Astromers: Nuclear Isomers in Astrophysics*

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Published 2020 December 17 © 2020. The American Astronomical Society. All rights reserved.
, , Citation G. Wendell Misch et al 2021 ApJS 252 2 DOI 10.3847/1538-4365/abc41d

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Abstract

We develop a method to compute thermally mediated transition rates between the ground state and long-lived isomers in nuclei. We also establish criteria delimiting a thermalization temperature above which a nucleus may be considered a single species and below which it must be treated as two separate species: a ground-state species and an astrophysical isomer ("astromer") species. Below the thermalization temperature, the destruction rates dominate the internal transition rates between the ground state and the isomer. If the destruction rates also differ greatly from one another, the nuclear levels fall out of or fail to reach thermal equilibrium. Without thermal equilibrium, there may not be a safe assumption about the distribution of occupation probability among the nuclear levels when computing nuclear reaction rates. In these conditions, the isomer has astrophysical consequences and should be treated as a separate astromer species which evolves separately from the ground state in a nucleosynthesis network. We apply our transition-rate methods and perform sensitivity studies on a few well-known astromers. We also study transitions in several other isomers of likely astrophysical interest.

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1. Introduction

Certain excited nuclear states may live much longer than the typical picosecond or femtosecond lifetimes of other states. The nuclear structure community uses an informal threshold of 1 ns to distinguish these: an excited state which lives for longer than a nanosecond is considered metastable and called a nuclear isomer. The term "isomer" in nuclear physics probably came from Frederick Soddy (Soddy 1917), who applied it to nuclei—in analogy with chemical isomers—to describe long-lived nuclear states; we take this term and modify it for those states that impact astrophysics. The discovery of nuclear isomerism is usually credited to the work of Otto Hahn in 1921 in an experiment with uranium (Hahn 1921). v. Weizsäcker (1936) pointed out that the combination of a large angular momentum change and low transition energy could lead to a long half-life for electromagnetic decay in nuclei. Bohr & Mottelson (1953) discussed specific isomeric transitions of the electric quadrupole type. Today, it is well known that various nuclear structure effects can lead to isomeric states, the best known being spin traps (the excited state has a large difference in spin from lower-lying states), K isomers (the orientation of spin relative to the axis of symmetry in a deformed nucleus is very different from lower-lying states), and shape isomers (the excited state is a very different shape from lower-lying states; Walker & Dracoulis 1999).

Astrophysical nucleosynthesis calculations rely on accurate nuclear reaction rate inputs. Indeed, even a single reaction rate can profoundly influence astrophysical evolution (see, e.g., Kirsebom et al. 2019). Researchers have therefore done a tremendous amount of work over the decades to compute the rates of nuclear weak interactions (Fuller et al. 1982; Oda et al. 1994; Langanke & Martínez-Pinedo 2001), neutron capture cross sections (Dillmann et al. 2010), and so on. Typically, one of two treatments is used to compute nucleosynthesis rates. Either only the ground-state rate is used, or the levels are considered to be in a thermal-equilibrium probability distribution. The presence of an isomeric state can diminish the accuracy of both approaches. When a nucleus is produced, it decays (usually by γ-ray emission) to a lower state. If it is caught in an isomer before it reaches the ground state, it will not necessarily undergo subsequent reactions at the ground-state rate. Isomers can also cause the probability distribution of nuclear energy levels to fail to reach thermal equilibrium. The destruction rates (e.g., β decay) of long-lived states (the ground state and isomers) of a single nuclear species can be vastly different from one another; the most famous example in astrophysics is 26Al, which has a ground-state β-decay half-life of 717 kyr, but an isomer with a β-decay half-life of 6.346 s. If the destruction rates are also fast relative to the transition rates between the long-lived states, a rapidly destroyed state will become depopulated relative to the thermal-equilibrium population because the population will tend to stay trapped in the other state. Although the existence of isomeric states in nuclei has been known for about a century, there remains much to learn about their influence on the creation of elements in astrophysical nucleosynthesis; they are expected to have a significant impact due to their unique decay properties (Aprahamian & Sun 2005).

Not all isomers have an impact on astrophysical nucleosynthesis. Most isomers transition to lower-energy states preferentially over destruction channels (e.g., the 103.00 keV isomer in 81Se, which transitions to ground 99.949% of the time; Baglin 2008), and sufficient connection to ground ensures destruction cannot cause deviation from thermal equilibrium. Furthermore, isomers that can have an effect will not make a difference in all environments; an isomer may prevent thermalization at low temperature, but in a hotter environment, thermally driven transitions through intermediate states can enable equilibration. There are also isomers that may be isolated from the ground state in the astrophysical site where they are produced, yet are not populated during the production of the nucleus (see, e.g., 182Hf in Section 3.5 and 113Cd in Section 3.6).

We thus see that some isomers can play an influential role in astrophysical nucleosynthesis, but most do not. This distinction defines astrophysical isomers, or "astromers": they are nuclear isomers that have influence as such in an astrophysical environment of interest.

Astromers by definition do not behave the same as their associated ground states. Consequently, it behooves nucleosynthesis networks to treat them as separate species that can be destroyed and created by transitions into and out of the ground state. In this work, we develop a framework to rigorously treat astromers and these thermally mediated transitions. We apply our methods to several nuclei of interest in a number of astrophysical sites, including analyses of the effects of uncertainty for three well-known isomers. We also provide data tables for use in nucleosynthesis networks.

We develop in Section 2 a highly precise means of calculating effective transition rates between long-lived nuclear states in hot environments. In Section 3, we apply our methods to several well-known and potential astromers, including 26Al, 34Cl, and 85Kr. We give some further observations and concluding thoughts in Section 4. Because astromer ↔ ground transitions are facilitated by intermediate states, it is helpful to trace which intermediate transitions contribute most to the effective transition rate so that we may efficiently assess the effects of uncertainty; the Appendix describes how we find the greatest contributors and makes important notes about symmetries and detailed balance.

2. Transition-rate Formalism

Consider a connected system in which every state is reachable from every other state via some set of transitions. We divide these states into two classes: endpoint states E, which in our application are the ground state and isomers in an atomic nucleus; and intermediate states I, which for us are nonisomeric excited states. This discussion specializes to the case of two endpoint states (a single isomer), but the arguments readily generalize. This section and Section Appendix ignore destruction of the states via β decay, etc. Destruction will be introduced later as simply another set of rates that do not impact internal transition rates.

We will keep this section general by using the labels A and B for endpoint states and i, j, etc. for intermediate states. For the sake of concreteness, take A to be the ground state and B to be an isomer of a nucleus. Figure 1 provides a schematic for thermally driven transitions from A to B via intermediate states i, j, and k. When a system transitions out of state s, it goes to state t with probability bst.

Figure 1.

Figure 1. Schematic of transitions from state A to state B when A and B have little or no direct coupling. If energy is increasing in the upward direction, then red arrows show up transitions and blue arrows show down transitions. The bst are the probabilities that when the system leaves s, it transitions directly to t. Because A cannot transition directly to B, transitions between the two require intermediate states.

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The transition probabilities bst are related to the transition rates λst by

Equation (1)

By inspection, ∑tbst = 1, ensuring that there are no sources or sinks in the system. We compute the λst using the spontaneous γ-decay rates ${\lambda }_{{hl}}^{s}$ from a higher state h to a lower state l. In this article, we follow the example of Ward & Fowler (1980) and Coc et al. (1999) and consider only the photon bath:

Equation (2)

Equation (3)

Equation (4)

These may be combined to obtain the useful relation

Equation (5)

The factor u is the Bose–Einstein distribution of a thermal photon bath and captures the fact that the bath stimulates transitions from h to l and induces transitions from l to h. As Ward & Fowler (1980) point out, there can be other thermal interactions which affect the λst;  Equations (2)–(4) can be extended to include other interactions if needed. These equations represent our only physical assumptions in this section and the Appendix.

With the individual transition probabilities, we are now prepared to compute the effective thermal transition rates between endpoint states.

2.1. Effective Transition Rate

We express the effective transition rate ΛAB from A to B as

Equation (6)

The rate λAB is for transitions directly from A to B; this quantity may be negligible, but in some cases it is not, so we include it. The sum is over intermediate states i, and PiB is the probability the system follows a chain of internal transitions from intermediate state i to the endpoint state B without passing through A. We require that the system not pass through A as that would be like starting over, amounting to a failed transition. In effect, Equation (6) sums the transition rate from A to each other state times that state's probability of going to B.

We now must find the PiB. These can be computed by considering the first step of all allowed routes from i to B. A step from i to state s occurs with probability bis. Now, PiB can be identified as the sum over the probabilities of the possible first steps from i folded with the probabilities PsB that the new state eventually reaches B. That is,

Equation (7)

The sum is over all states s. If s = A, the transition has failed, and if s = B, the transition is complete; therefore, PAB ≡ 0 and PBB ≡ 1. States do not transition to themselves, so bss ≡ 0 s. These features allow a slight rewrite:

Equation (8)

The summation in the second term is now only over intermediate states. From here, we may express the problem in matrix form,

Equation (9)

In this expression, the subscript I reminds us that the vector and matrix indices run over the intermediate states. So, ${\overrightarrow{P}}_{{IB}}$ is the vector with components PiB, ${\overrightarrow{b}}_{{IB}}$ is the vector with components biB, and bII is the matrix with elements bij; in each of these, i and j are intermediate states. Equations (7) and (9) represent a system of N linear equations in N variables, where N is the number of intermediate states included in the calculation. Thus, ${\overrightarrow{P}}_{{IB}}$ can be found with a linear equation solver, and inserting ${\overrightarrow{P}}_{{IB}}$ into Equation (6) yields the effective transition rate from A to B.

In the case of a system with more than two endpoint states, Equation (6) holds for all pairs of initial and final endpoint states. The method is straightforwardly extended by redefining PiE as the probability of eventually reaching endpoint state E from intermediate state i without passing through any other endpoints, and all of the same arguments apply.

2.2. Proof of Solvability

By the invertible matrix theorem, if 1 − bII is invertible, then a unique solution to Equation (9) exists:

Equation (10)

To show that that 1 − bII is invertible, we will use the logic of Gupta & Meyer (2001).

We note that the full transition matrix b with elements bst (which includes endpoint and intermediate states) is a stochastic matrix: its rows sum to unity. Obviously, b is nonnegative (all entries are real and positive or zero). Furthermore, because every state is reachable via some path from every other state, b is irreducible, meaning the rows and columns cannot be permuted to produce a block diagonal form. If it were reducible, there would be at least two sets of states that communicate only with members of their set, and the graph of the system would not be connected.

Stochastic matrices have an eigenvector with eigenvalue 1; to see this, observe that ${\boldsymbol{b}}\overrightarrow{1}=\overrightarrow{1}$, where $\overrightarrow{1}$ is the column vector with all entries equal to 1. From the Gershgorin circle theorem on upper bounds of spectral radii, the largest absolute value among eigenvalues (the spectral radius) of b is 1. Because b is nonnegative and irreducible, the Perron–Frobenius theorem guarantees that there is exactly one eigenvector corresponding to an eigenvalue equal to the spectral radius, i.e., 1.

We now rely on a corollary to the Perron–Frobenius theorem: any principal submatrix of an irreducible nonnegative matrix has a spectral radius that is strictly less than the full matrix. A principal submatrix is obtained by deleting rows and columns from a matrix, with the row and column indices being equal. The matrix bII is a principal submatrix of b obtained by deleting the rows containing transitions from endpoints and the columns containing transitions to endpoints. Therefore, it has a spectral radius less than 1, and all of its eigenvalues have absolute value (modulus) less than 1.

Finally, let M and N be square matrices with N = M + 1. For every eigenvalue Mλi of M, there will be an eigenvalue Nλi = Mλi + 1 of N. To see this, let $\overrightarrow{x}$ be an eigenvector of M with eigenvalue λ. We then have

Equation (11)

Taking M = − bII and remembering that all eigenvalues of bII have modulus less than 1, we deduce that all eigenvalues of 1 − bII have a positive real component and are therefore nonzero, and the matrix is invertible by the invertible matrix theorem.

3. Applications

We will now compute the isomer-to-ground and ground-to-isomer effective transition rates and β-decay rates in several nuclei; all calculations assume an electron density of ρYe = 105 g cm−3. We will use the prescription from Gupta & Meyer (2001) to compute effective decay rates for ensembles of states corresponding to the ground state and the isomer. For the reader's convenience, we outline the derivation and result here.

Unlike our derivations in Section 2, the Gupta & Meyer (2001) method assumes intermediate states instantaneously reach steady-state equilibrium with the endpoint states (under most circumstances, a reasonable assumption that is backed up by a detailed analysis in that work). They obtain the steady-state occupation fractions Y by noting that the ratio of the intermediate state i to the endpoint state E occupations is related to the ratio of the direct transition rates between them; they call this the "reverse ratio" REi:

Equation (12)

In principle, we would compute this ratio using Equation (5). It is undefined if the direct transition rates are zero, but because the ratio is independent of the size of the rates, it remains constant in the limit that the rates approach zero; we find that

Equation (13)

Finally, each intermediate state has the probability PiE to eventually transition to endpoint state E before going to some other endpoint. Gupta & Meyer (2001) interpret this as the fraction of intermediate state i that is associated with endpoint state E. This interpretation—along with the assumption of instantaneous equilibration of intermediate states—enables them to assign a weight wiE to each state and use those weights to construct an ensemble associated with each endpoint. In effect, every state is assigned a modified Boltzmann factor for each ensemble:

Equation (14)

The delta function applies to pairs of endpoint states and ensures that each endpoint contributes only to its own ensemble. With these weights, we may now compute the effective β-decay rate ΛEβ (or any other rate) for the ensemble associated with endpoint E,

Equation (15)

In this expression, λsβ is the individual β-decay rate of state s. We are now prepared to compute the transition rates and β-decay rates of nuclei with isomers.

3.1. 26Al

26Al is produced by massive stars in substantial quantities. Its ground-state β-decay lifetime of ∼1 million years means that it lives long enough to be observed after a massive star dies, but not so long as to become uncorrelated with where that star died. Because massive stars have short lifetimes, we infer that if one died recently in a location, that location is probably a region of active star formation. Hence, 26Al is an important tracer of star formation (Mahoney et al. 1982; Diehl et al. 1995), and we are interested in accurately computing its abundance in nucleosynthesis networks. 26Al production is sensitive not only to the rates in which it is directly involved, but also to many other reaction rates in nearby nuclei (Iliadis et al. 2011). However, its treatment is complicated by a long-lived isomer at 228.305 keV that can greatly impact 26Al destruction rates (Ward & Fowler 1980; Coc et al. 1999; Gupta & Meyer 2001; Runkle et al. 2001; Banerjee et al. 2018; Reifarth et al. 2018).

To compute 26Al transition and β-decay rates, we included 67 total states: the two endpoint states and 65 intermediate states. In this nucleus and all others in this section, we used available experimental data for the spontaneous transition and β-decay rates (Basunia & Hurst 2016). In 26Al, we supplemented the data with transition and β-decay strengths computed using the shell model codes NuShellX (Brown & Rae 2014) and OXBASH (Brown et al. 2004) along with the USDB interaction (Brown & Richter 2006). When a transition rate is unmeasured and a shell model calculation is impractical, we use the Weisskopf approximation (Weisskopf & Wigner 1930). For the β-decay rates, we used the measured ft values for ground-state and isomer β decays, and we computed matrix elements with the shell model for all other weak transitions.

Once we have the bst, obtained from Equations (1)–(5), we use Equation (9) to compute the PIE. Figure 2 shows PIE for the first three intermediate states as functions of temperature; in this figure and Figure 3, the index g indicates the ground state, and m is the isomer.

Figure 2.

Figure 2. The probabilities PiE that intermediate state i reaches endpoint state E before reaching the other endpoint state for the three lowest intermediate states in 26Al. Solid (dashed) lines marked with dots (x) show probabilities of reaching the isomer m (ground g). Most are insensitive functions of temperature, though P3m climbs suddenly at T ≈ 30 keV (see text).

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Figure 3.

Figure 3. Contributions to Λgm and Λmg in 26Al from individual first steps out of the ground g (solid with dots) and isomeric m (dashed with x) states. The contribution is the product of the rate to transition directly from the initial state to the intermediate state and the probability of going from the intermediate state to the destination endpoint state.

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While most of the PIE are nearly constant, the jump in P3m at around 30 keV portends a behavioral change in the nucleus at this temperature. Indeed, this manifests as an increase in the rate for the ground state to transition to state 3 and from there ultimately to the isomer. Figure 3 illustrates this jump; it shows rates for endpoint states to transition to specific intermediate states, and from there to eventually transition to the other endpoint state. That is, Figure 3 shows the terms in Equation (6). Whereas most intermediate states' contributions increase smoothly with temperature, the third state going from g to m (black solid) has a kink at ∼30 keV.

It is no mere coincidence that the kink occurs at the same temperature where λm3P3g (black dashed) crosses λm4P4g (red dashed). As the temperature rises, state 4 becomes more accessible from the isomer, driving the rise of λm4P4g. Once it dominates λm3P3g, the most probable isomer-to-ground transition pathways change.9 Figure 4 shows the three most probable paths from ground to the isomer at T = 25 keV and 35 keV; by symmetry (Section A.3), it also shows the isomer-to-ground paths.

Figure 4.

Figure 4. The three paths giving the greatest contribution to the transition rate between the ground state and isomer in 26Al at temperatures T = 25 keV (top) and T = 35 keV (bottom). Although only transitions from 1 to 2 are shown, path reversal symmetry guarantees that the routes from 2 to 1 are the same.

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At T = 25 keV, the dominant pathway between 1 (ground) and 2 (isomer) is simply through state 3. But at T = 35 keV, state 4 is thermally accessible from 2, and because it is much more strongly coupled to the isomer than is state 3 (P4m ≫ P3m in Figure 2),10 2 preferentially transitions to 4. State 4 is only weakly coupled to ground (P4g in Figure 2), and the preferred route from 4 to 1 is via 3. Therefore, when the isomer preferentially transitions to state 4 (above T = 30 keV), the most probable isomer-to-ground path is 2 → 4 → 3 → 1. This "opens up" the 1 → 3 → 4 → 2 path and creates the kinks. Figure 5 further illustrates this point by showing the probabilities for state 3 to go directly to the isomer (b3m), to go to 4, and then eventually to the isomer (b34P4m, and to go to 5 and then eventually to the isomer (b35P5m).

Figure 5.

Figure 5. Probabilities of following routes from the third state to the isomer m in 26Al. Once the nucleus is in the third state, b3m is the probability that it transitions directly to the isomer, while ${b}_{3i}{P}_{{im}}$ is the probability of going to state i and from there via some path that leads to m without going through ground.

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Finally, we use Equation (6) to compute the effective transition rates Λ12 and Λ21, shown in Figure 6. From here on, 1 should be understood as the ensemble corresponding to the ground state, and 2 is the ensemble corresponding to the isomer; the ensembles are constructed as described at the beginning of this section in Equations (12)–(15). The figure also shows various β-decay rates: the ensemble decay rates Λ1β and Λ2β;  the thermal decay rate Λβ therm, computed using a thermal distribution of level occupations; the steady-state decay rate Λβ SS;  the steady-state decay rates ${{\rm{\Lambda }}}_{\beta \,{SS}}^{P1}$ and ${{\rm{\Lambda }}}_{\beta \,{SS}}^{P2}$ when the nucleus is produced exclusively in either the ground state (P1) or isomer (P2) ensemble; and—for comparison—the effective decay rate found by Coc et al. (1999). We computed the steady-state rates with the formalism of Misch et al. (2018) assuming a two-level system comprised of 1 and 2. At low temperatures, we compute a slightly higher β-decay rate than Coc et al. (1999); this is because they used laboratory rates, whereas our electron capture rates are enhanced by the dense environment. We are otherwise in good agreement.

Figure 6.

Figure 6. 26Al transition rates and β-decay rates. Solid lines with no markers show the effective ground ↔ isomer transition rates, and other lines show β-decay rates. Red: ground-state ensemble transition and β-decay rates; down triangles show the steady-state decay rate when only the ground state is produced. Green: isomer ensemble transition and β-decay rates; up triangles show the steady-state decay rate when only the isomer is produced. Black (crosses): steady-state β-decay rate in the absence of production. Blue (X): thermal-equilibrium β-decay rate. Gray (circles): effective decay rate from Coc et al. (1999).

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Let us first understand Λ12, Λ21, Λ1β, and Λ2β. Below T ≈ 7 keV, excited states are inaccessible. The isomer transitions directly to ground at a slow trickle, the ground state cannot reach the isomer, and each β decays at its laboratory rate. Above T ≈ 7 keV, state 3 becomes accessible, the path 1 ↔ 3 ↔ 2 opens up, and the transition rates begin to rise. At T ≈ 13 keV, Λ12 surpasses Λ1β, and the dominant "destruction" channel for ensemble 1 is transitions to ensemble 2. At T ≈ 17 keV, the weight w31 of state 3 in ensemble 1 grows great enough that it contributes significantly to the ensemble β-decay rate. State 3 has allowed decays to 26Mg, and Λ1β rises accordingly. At T ≈ 30 keV, the path 1 ↔ 3 ↔ 4 ↔ 2 opens up, and the transition rates rise faster. At T ≈ 35 keV, Λ21 surpasses Λβ2, and the dominant destruction channel for ensemble 2 is transitions to ensemble 1.

Now let us examine Λβ therm and Λβ SS, which are the thermal-equilibrium β-decay rate and the steady-state (without any 26Al production) β-decay rate, respectively. The thermal decay rate is straightforward to understand. If 26Al had no isomer, the nuclear level occupation probabilities would simply follow a Boltzmann distribution. At T ≈ 8 keV, the first excited state would be sufficiently populated to contribute to Λβ therm, and the decay rate would rise concomitantly. However, 26Al does have an isomer that suppresses thermally driven transitions up from ground. Because there is no thermally accessible path to populate the isomer, it decays away rapidly, is not replenished, and has a less-than-thermal population in steady state; this suppresses Λβ SS. Once Λ12 exceeds Λ1β at T ≈ 13 keV, the ground state begins to appreciably feed the isomer. But up until T ≈ 35 keV, the isomer essentially always β decays. Furthermore, Λ2β ≫ Λ1β, so 26Al decays as fast as the isomer is fed, and the steady-state β-decay rate is approximately equal to Λ12. At T ≈ 35 keV, when Λ21 exceeds Λ2β, transitions between the ensembles dominate the ensemble decay rates, and the system at last reaches the thermal equilibrium found by other authors (Coc et al. 1999; Iliadis et al. 2011; Banerjee et al. 2018). This defines the thermalization temperature below which the 26Al isomer is an astromer.

This leaves us to understand ${{\rm{\Lambda }}}_{\beta \,{SS}}^{P1}$ and ${{\rm{\Lambda }}}_{\beta \,{SS}}^{P2}$, which are the steady-state decay rates when 26Al is produced solely in the ground-state or isomer ensembles, respectively. Observe that ${{\rm{\Lambda }}}_{\beta \,{SS}}^{P1}$ tracks Λβ SS at all temperatures. This is because in steady state without production, essentially all of the population is in the ground state anyway, so it makes no difference if 26Al is produced in the ground-state ensemble.

In contrast, when 26Al is produced in the isomer ensemble at low temperature, the ground state is fed exceedingly slowly. Gradually, a small equilibrium amount of material will build up in the ground state that brings down the total decay rate, though this may take many years (see Misch et al. 2018; Figure 5), and it will never be enough to bring the decay rate to near the ground-state rate. At T ≈ 7 keV, Λ21 increases dramatically, so the ground state is more rapidly fed. The increased feeding yields a larger quantity of ground-state material, and the steady-state decay rate consequently falls. Once Λ12 overtakes Λ1β at T ≈ 13 keV, the steady-state decay rate goes to the thermal-equilibrium rate. This follows from Equation (18) in Misch et al. (2018) using our two-ensemble system. That equation is expressed in matrix notation, but we may analyze one of the embedded scalar equations by selecting a single vector component. Taking the first element of the vectors, we have

Equation (16)

Here, n1 and n2 are the occupation fractions of the two ensembles, and p1 is the fraction of 26Al production that goes into the ground-state ensemble. By assumption, p1 = 0, and we are considering a regime where Λ12 dominates Λ1β;  the latter point implies that Λ12n1 + Λ1βn1 ≈ Λ12n1. Using these facts along with Equation (A13), we find

Equation (17)

which is precisely a thermal distribution between the ground state and isomer. We conclude that the nuclear levels are thermally distributed when Λ12 ≫Λ1β, leading to the observed agreement between ${{\rm{\Lambda }}}_{\beta \,{SS}}^{P2}$ and Λβ therm. Note that this is not necessarily an excuse to just use the thermal decay rate, because it may take many thousands of years to reach steady state.

Up to now, we have used exact values for the λst. However, uncertainties in the individual rates lead to uncertainty in the effective transition rates. We therefore performed a sensitivity study by varying the λst. Figure 7 shows the results of adjusting measured rates all up or all down by one or two standard deviations and shell model rates all up or all down by a factor of 3 or 30. Shell model rates using the USDB Hamiltonian tend to be good to within a factor of a couple with occasional large errors relative to experiment of one to two orders of magnitude (see Banerjee et al. 2018), so this choice of variations should reasonably probe the range of the ΛAB. Dark bands show the smaller variations, and light bands show the larger. Because the λst were adjusted up and down together, the bands represent reasonable bounds on the effective rates. Furthermore, our analysis finds that the thermalization temperature of 26Al is uncertain within the range between 30 and 40 keV; this is at odds with Coc et al. (1999), who concluded that the thermalization temperature is insensitive to remaining nuclear uncertainties.

Figure 7.

Figure 7. Range of 26Al effective transition rates. Dark bands: measured rates increased/decreased by one standard deviation, shell model rates multiplied/divided by a factor of 3. Light bands: measured rates increased/decreased by two standard deviations, shell model rates multiplied/divided by a factor of 30.

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A more detailed picture emerges when the λst are varied separately. We identified which individual rates to change by examining the dominant transition paths; if a transition existed in paths carrying a total of at least 1% of the effective rate and that transition's uncertainty was at least 10%, we varied it. We adjusted measured rates up and down by one standard deviation and shell model rates up and down by a factor of 3. Table 1 shows the sensitivity of the effective transition rate to variations in the individual rates.

Table 1.  Most-uncertain Individual Transitions in the Dominant Pathways through 26Al

T Trans Type Fraction Variation Impact
10 3 → 2 SM 0.9999  × 3 0.3334–2.9997
15 3 → 2 SM 1.0000  × 3 0.3333–3.0000
20 3 → 2 SM 1.0000  × 3 0.3334–2.9998
25 3 → 2 SM 0.9800  × 3 0.3466–2.9602
  4 → 2 Exp 0.0199 20% 1.0
  4 → 3 SM 0.0199  × 3 0.9867–1.0399
30 3 → 2 SM 0.4070  × 3 0.7287–1.8139
  4 → 2 Exp 0.5930 20% 1.0
  4 → 3 SM 0.5930  × 3 0.6046–2.1860
35 3 → 2 SM 0.0315  × 3 0.9790–1.0630
  4 → 2 Exp 0.9685 20% 1.0
  4 → 3 SM 0.9685  × 3 0.3543–2.9369
40 3 → 2 SM 0.0033  × 3 0.9978–1.0066
  4 → 2 Exp 0.9967 20% 1.0
  4 → 3 SM 0.9967  × 3 0.3355–2.9933

Note. The Type column indicates whether this spontaneous transition rate comes from shell model calculations (SM) or from experiment (Exp). The column labeled Fraction shows what fraction of the effective transitions flow through paths containing the individual transition (or its reverse). Variation is an estimate of the uncertainty; we use the published uncertainty for experimental rates and a factor of 3 for SM rates. The last column shows the fractional change in effective transition rates when the individual rate is adjusted up and down by one "unit" of uncertainty.

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Our results generally agree quite well with Gupta & Meyer (2001). The greatest uncertainty in the effective transition rates arise from λ32 at lower temperatures and λ43 at higher temperatures.

3.2. 34Cl

34Cl may be observable immediately after a nova (Coc et al. 1999), which means that accurately computing its abundance could be interesting. However, it has a long-lived isomer at 146.36 keV, bringing with it the familiar difficulty. But unlike 26Al and the other nuclei in this paper, the 34Cl isomer is more β-stable than the ground state; the ground-state β-decay half-life is 1.5266 s, while the isomer's total half-life is 31.99 minutes (Nica & Singh 2012).

We computed the 34Cl rates using 30 states. As with 26Al, we supplemented unmeasured transition rates and β-decay ft values with calculations from NuShellX, OXBASH, and the USDB interaction. Experimental data for the key 3 → 2 transition consist only of an upper bound, so we used our shell model result. Our computed effective transition rates and β-decay rates are shown in Figure 8 along with the rates computed by Coc et al. (1999). As with 26Al, we are in good agreement with the earlier work.

Figure 8.

Figure 8. 34Cl transition and β-decay rates. The lines are as in Figure 6.

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Below T ≈ 10 keV, no paths apart from the direct transition contribute meaningfully to the transition rate, but above this temperature, the path 2 ↔ 3 ↔ 1 opens up and Λ21 begins to rise. Because 2 is the more β-stable state, ${{\rm{\Lambda }}}_{\beta \,{SS}}^{P2}$ mostly tracks Λβ SS. Once Λ21 dominates Λ2β, Λβ SS follows until it joins Λβ therm, while ${{\rm{\Lambda }}}_{\beta \,{SS}}^{P1}$ is delayed slightly; 34Cl thermalizes at T ≈ 20 keV. Below this temperature, the isomer is an astromer. With ground being the less stable state, Λβ therm and ${{\rm{\Lambda }}}_{\beta \,{SS}}^{P1}$ both track Λ1β until T ≈ 30 keV, at which point the isomer ensemble is thermally populated at a sufficient level to pull the thermal and steady-state rates down a bit.

Figure 9 shows the uncertainty bands in the 34Cl ΛAB. The uncertainty is driven almost entirely by the 3 → 2 transition. Even up to T = 50 keV, all dominant paths travel through states no higher than state 4, and apart from λ32, the λst are measured with small experimental uncertainties. Our dark uncertainty bands (smaller variations) agree well with the findings of Coc et al. (1999). The light bands (larger variations) exhibit some asymmetry: the lower bands are narrower than the upper bands at higher temperatures. As λ32 is increased, the nucleus flows more freely through the 1 → 3 → 2 path, and 3 → 2 is the bottleneck. But when λ32 is sufficiently decreased, the 1 → 4 → 2 path dominates at higher temperatures, and the effective transition rate becomes insensitive to further decrease in λ32.

Figure 9.

Figure 9. Range of 34Cl effective transition rates. Dark bands: measured rates increased/decreased by one standard deviation, shell model rates multiplied/divided by a factor of 3. Light bands: measured rates increased/decreased by two standard deviations, shell model rates multiplied/divided by a factor of 30. The uncertainties are dominated by the 3 → 2 transition.

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3.3. 85Kr

In slow neutron capture (s-process) nucleosynthesis, neutron captures are generally slow relative to β decays, so few nuclei are produced, which are more than one or two steps from stability. In most cases, this makes it easy to trace out the s-process path in the chart of nuclides. Starting with a seed nucleus, add neutrons until you make a β-unstable nucleus. Allow that unstable nucleus to β decay until it is stable. Resume adding neutrons and repeat until you have lead, bismuth, or no more neutron source.

85Kr lies along the s-process nucleosynthesis path, but the simple procedure above is derailed by the ground state's long, but not too long, β-decay half-life of 10.739 yr. This creates competition between β decay and neutron capture, which influences the production of nearby nuclei (Abia et al. 2001). Because the s-process path can go in two different directions at 85Kr, it is known as a branch-point nucleus and serves as an interesting diagnostic of the s-process environment. However, its current usefulness as such is greatly diminished by two complications: an uncertain neutron capture cross section (Dillmann et al. 2010) and an isomer at 304.871 keV with a total half-life of 4.480 hours (Singh & Chen 2014).

We will not address the neutron capture cross section, but we did apply our method to study the isomer's effect on β decay. We used experimental data on the lowest 30 levels of 85Kr. We supplemented unmeasured transition rates with the Weisskopf approximation; 85Kr (N = 49) is near a closed neutron shell (N = 50)—which diminishes the effectiveness of shell model calculations—so we made no further data supplements. Figure 10 shows our results.

Figure 10.

Figure 10. 85Kr transition and β-decay rates. The lines are as in Figure 6.

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For the most part, 85Kr does not behave in any remarkable way; the thermal and steady-state decay rates track each other, including when 85Kr is produced in the ground state, so the isomer is not an astromer. This is because in contrast with 26Al, Λ21 exceeds Λ2β (the green lines cross) at a lower temperature than Λ12 exceeds Λ1β (the red lines cross). Therefore, by the time the ground-state ensemble can appreciably feed it, the isomer ensemble preferentially transitions back to ground rather than β decays, and the thermal β-decay rate is appropriate for all situations except when 85Kr is produced in the isomer ensemble.

The latter case, however, can give rise to interesting behavior. Below T ≈ 21 keV, material produced in the isomer ensemble has an  ∼ 80% chance to β decay rather than transition to ground; this drives up the decay rate of the species and favors β decay over neutron capture, rendering the 85Kr isomer an astromer. Above T ≈ 25 keV, the nuclear levels thermalize, and the thermal β-decay rate is always correct. The weak component of the s-process occurs in massive stars with temperatures between 30 and 90 keV, well above the 85Kr thermalization temperature. But interestingly, the main s-process occurs in pulsing asymptotic giant branch (AGB) stars of mass 1 − 3 M;  short pulses reach temperature T ∼ 30 keV, while longer interpulse periods have a temperature of T ∼ 8 keV. The entire cycle has a period of ∼50,000 yr (Busso et al. 1999). This means that the 85Kr isomer alternates being an astromer in the main s-process.

The uncertainties in the 85Kr effective transition rates are somewhat different from the 26Al and 34Cl cases in two ways. First, the experimental uncertainties are asymmetric (see table 2). Second, the unmeasured rates are estimated with the Weisskopf approximation rather than the shell model; the Weisskopf approximation tends to only be precise to one or two orders of magnitude.

Table 2.  Most-uncertain Individual Transitions in the Dominant Pathways through 85Kr

T Trans Type Fraction Variation Impact
21 3 → 2 W 0.0605  ×10 0.9995–1.0001
  4 → 1 Exp 0.0698 −40, +80% 0.9901–1.0085
  4 → 3 W 0.0605  ×10 0.9492–1.1517
  5 → 2 W 0.0047  ×10 1.0
  5 → 4 W 0.0047  ×10 0.9965–1.0301
  6 → 2 Exp 0.0047 −17, +25% 0.9995–1.0007
  6 → 4 W 0.0084  ×10 0.9962–1.0015
23 3 → 2 W 0.5725  ×10 0.9941–1.0006
  4 → 1 Exp 0.6797 −40, +80% 0.8964–1.0907
  4 → 3 W 0.5725  ×10 0.5248–2.3960
  5 → 2 W 0.0487  ×10 1.0
  5 → 4 W 0.0487  ×10 0.9633–1.3098
  6 → 2 Exp 0.0585 −17, +25% 0.9938–1.0087
  6 → 4 W 0.1051  ×10 0.9506–1.0200
25 3 → 2 W 0.7312  ×10 0.9914–1.0009
  4 → 1 Exp 0.9219 −40, +80% 0.8526–1.1312
  4 → 3 W 0.7312  ×10 0.4008–2.7348
  5 → 2 W 0.0971  ×10 1.0
  5 → 4 W 0.0671  ×10 0.9490–1.4223
  6 → 2 Exp 0.0936 −17, +25% 0.9900–1.0139
  6 → 4 W 0.1979  ×10 0.9174–1.0335
  6 → 5 W 0.0300  ×10 0.9822–1.1087

Note. The Type column indicates whether this spontaneous transition rate comes from experiment (Exp) or the Weisskopf approximation (W). The column labeled Fraction shows what fraction of the effective transitions flow through paths containing the individual transition (or its reverse). Variation is an estimate of the uncertainty; we use the published uncertainty for experimental rates and a factor of 10 for Weisskopf rates. The last column shows the fractional change in effective transition rates when the individual rate is adjusted up and down by one "unit" of uncertainty.

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Figure 11 shows the uncertainties in the 85Kr ΛAB. The upper light band is much narrower than the lower light band due to a bottlenecking effect similar to 34Cl. As the λst are turned up together, the experimental λ41 becomes a bottleneck; because its uncertainty is much less than the Weisskopf rates, it is turned up less than the Weisskopf rates and eventually controls the ΛAB. However, as the rates are turned down, the opposite happens: λ41 is reduced much more slowly, the Weisskopf rates become the bottleneck, and the lower band is wider than the upper band. If we decrease the Weisskopf rates much more, then as with 34Cl, the 1 → 2 direct transition will be favored up to higher temperatures, and the ΛAB will be insensitive to further decreases.

Figure 11.

Figure 11. Range of 85Kr effective transition rates. Dark bands: measured rates increased/decreased by one standard deviation, Weisskopf rates multiplied/divided by a factor of 10. Light bands: measured rates increased/decreased by two standard deviations, Weisskopf rates multiplied/divided by a factor of 100.

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We show the sensitivity of the ΛAB to selected λst in Table 2; we used the same selection criteria as with 26Al. Similarly, we only vary by one "unit" of uncertainty, which will avoid the bottleneck effect. We examine the fairly narrow range of temperatures from 21–25 keV because that is the range of thermalization temperatures found from Figure 11. At all temperatures, the unmeasured λ43 is the largest contributor to the effective transition-rate uncertainty. At T = 23 keV, the unmeasured λ54 plays a significant role, and at T = 25 keV, the unmeasured λ65 and the measured (but uncertain) λ41 are also important sources of uncertainty in the ΛAB.

3.4. Other s-process Astromers

To reiterate from Section 3.3, the main s-process occurs in thermally pulsing AGB stars. The total pulsation period is ∼50 thousand years, with a pulse temperature of T ∼ 30 keV and an interpulse temperature of T ∼ 8 keV (Busso et al. 1999).

All rates in this section were computed using all measured levels in each nucleus (up to 30 levels) with unmeasured γ-decay rates computed from the Weisskopf approximation. We do not provide sensitivity studies for these nuclei because nearly all of the intermediate-level lifetimes (and hence γ rates) along dominant transition paths are unknown, and the uncertainties in the ΛAB are driven by the Weisskopf approximation.

The 6.31 keV isomer of 121Sn (T1/2 = 43.9 y) is more stable than the ground state (T1/2 = 27.03 h). Unlike other isomers considered in this work, this one decays primarily to the ground state (77.6%) rather than β decay, so Λ21 always exceeds Λ2β. However, Figure 12 shows that Λ12 does not catch up to Λ1β until temperature T ∼ 20 keV, making this an astromer in the interpulse periods of the main s-process. Moreover, the long half-life of the astromer provides ample time for it to capture a neutron rather than deexcite or β decay. This would reduce the s-process production of 121Sb, 122Te, and 123Te.

Figure 12.

Figure 12. 121Sn transition and β-decay rates. The lines are as in Figure 6.

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Takahashi & Yokoi (1987) took advantage of the 122.845 keV isomer to compute a thermal β-decay rate for 176Lu. We also computed the transition and β-decay rates in this isotope; the results are in Figure 13. Takahashi & Yokoi (1987) performed a very careful calculation, but two of their temperature points (0.05 and 0.1 GK) fall in the range where the two states should be treated as separate species. Furthermore, 176Lu is made in the main s-process, and the ∼10 keV thermalization temperature implies its isomer could be an astromer during the main s-process interpulse periods.

Figure 13.

Figure 13. 176Lu transition and β-decay rates. The lines are as in Figure 6.

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3.5. r-process Astromers

All rates in this section were computed using all measured levels in each nucleus (up to 30 levels) with unmeasured γ-decay rates computed from the Weisskopf approximation. We do not provide sensitivity studies for these nuclei because nearly all of the intermediate-level lifetimes (and hence γ rates) are unknown, and the uncertainties in the ΛAB are driven entirely by the Weisskopf approximation.

Isomers may play an important role in the rapid neutron capture process (r-process). Fujimoto & Hashimoto (2020) identified nine nuclei with isomers that could affect the light curve of a post-neutron-star-merger kilonova, four of which were particularly impactful: 123,125,127Sn with isomers at 24.6, 27.50, and 5.07 keV respectively, and 128Sb with an isomer of unknown energy. Figures 14, 15, and 16 show the transition and β-decay rates for the Sn isotopes. Indeed, each of these thermalizes at T ≈ 25 keV, well above the expected ambient temperature when the isotopes are populated in such environments. The disparity between the ground-state and isomer β-decay rates could have a marked impact on the radioactive heating as nuclei decay back to stability, so further investigation is in order.

Figure 14.

Figure 14. 123Sn transition and β-decay rates. The lines are as in Figure 6.

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Figure 15.

Figure 15. 125Sn transition and β-decay rates. The lines are as in Figure 6.

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Figure 16.

Figure 16. 127Sn transition and β-decay rates. The lines are as in Figure 6.

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The fourth isotope identified by Fujimoto & Hashimoto (2020), 128Sb, suffers from incomplete data. The rates are shown in Figure 17, but it does not thermalize within the computed temperature range. This is almost certainly due to missing data in the excited states. The ground state has spin and parity Jπ = 8, the isomer has Jπ = 5+, and all other measured states have J ≤ 4. Furthermore, the isomer has unknown energy (we take the likely upper bound of 20 keV), and all other excited states have energies measured with respect to that unknown energy (Elekes & Timar 2015). Because this is such a potentially important nucleus, closer investigation is warranted. If the isomer is indeed influential, this would motivate experiments to measure the excited-state properties.

Figure 17.

Figure 17. 128Sb transition and β-decay rates. The lines are as in Figure 6.

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182Hf is a cosmochronometer that may be produced in the s-process (Lugaro et al. 2014) or the r-process (Wu et al. 2019). It has an isomer at 1172.87 keV; Figure 18 shows the rates for this isotope. Although 182Hf thermalizes at a fairly low T ≈ 6 keV and is therefore not an s-process astromer, this is nevertheless higher than the expected temperature at which it would be produced in some r-process events; the two-minute β-decay half-life of 182Lu likely implies that a rapid neutron capture event would have adequate time to cool. However, the 182Lu β decay exclusively feeds the 182Hf ground-state ensemble (Kirchner et al. 1982). With this information, we conclude that the 182Hf isomer does not affect the γ-ray signal predicted by Wu et al. (2019).

Figure 18.

Figure 18. 182Hf transition and β-decay rates. The lines are as in Figure 6.

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Finally, we raise the interesting case of 170Ho. This nuclide has only two measured levels: the ground state with Jπ = 6+ and a β-decay half-life of 2.76 minutes, and a 120 keV isomer with Jπ = 1+ and a β-decay half-life of 43 s. We anticipate that this difference in decay rates could affect energy generation in an r-process event with observable effects in the light curve of a kilonova. 170Ho is produced by β decay of 170Dy, but the parent β-decay intensities are unmeasured. However, the parent ground state has Jπ = 0+, so it likely decays predominantly to the 170Ho isomer. This fact—coupled with the lack of data on 170Ho excited states (which greatly hinders estimating the ΛAB), the computed abundance of A = 170 nuclei (Sprouse et al. 2020; Vassh et al. 2020), and the potential kilonova implications—motivates experimental examination of this pair of nuclei.

3.6. Other Cases

We show here two examples of isomers that look promising as astromers but for which we are unaware of any environments where they may behave as such. We computed unmeasured γ-decay rates using the Weisskopf approximation.

58Mn is an important antineutrino source in presupernova stellar cores (Patton et al. 2017), and it has an isomer at 71.77 keV. We computed effective transition and β-decay rates using the lowest 30 measured levels. As shown in Figure 19, 58Mn thermalizes at T < 5 keV, far below the presupernova core temperatures of 300−900 keV, so it is not an astromer in this environment. Nevertheless, there is a point to be made about this isomer. Because 58Mn is such a prodigious antineutrino source (with consequences for presupernova detection), we naturally desire precise weak-interaction rates. In most cases, we must rely entirely on theory for the weak-interaction strengths of excited states, but the existence of a low-lying isomer gives precise experimental data that reduces uncertainties in the high-temperature weak-interaction rates of 58Mn.

Figure 19.

Figure 19. 58Mn transition and β-decay rates. The lines are as in Figure 6.

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113Cd has a 14.1 yr isomer at 263.54 keV that nearly always β decays (Blachot 2010). Because it lies on the s-process path and the isomer β-decay rate could make it a branch point, it is worth taking a closer look at. We computed effective transition rates and β-decay rates in 113Cd using the 30 lowest measured energy levels; our results are shown in Figure 20.

Figure 20.

Figure 20. 113Cd transition and β-decay rates. The lines are as in Figure 6.

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The 113Cd rates are qualitatively similar to 85Kr in that Λ21 overtakes Λ2β at a lower temperature than Λ12 exceeds Λ1β, with similar consequences for the β-decay rates. The major difference is that the thermalization temperature for 113Cd is only ∼5 keV. This is below any s-process temperatures, so this isomer is likely never an s-process astromer.

Of course, as with 58Mn, the existence of the isomer means that we have a precise measurement of the β-decay rate for the first excited state in this nucleus, providing a more precise value of the thermal β-decay rate for this species. Also, if there exists an environment where the isomer is produced at a cooler temperature, 113Cd that is produced in the ground state will remain nearly stable, but that produced in the isomer will decay to 113In. However, we are unaware of any specific astrophysical environments where this would play a role, as 113Ag—the 113Cd β decay parent produced in the r-process—essentially always decays to the ground-state ensemble.

4. Discussion and Conclusions

We have developed an effective means of computing thermally driven transition rates between the ground state and long-lived isomers in atomic nuclei. We focus on the case of a single isomer, but generalization to multiple isomers is straightforward by simply including more endpoint states that obey all of our well-defined rules. Our technique does not rely on any physical assumptions apart from the assumption of a thermal photon bath, and, as discussed below, even this can be relaxed. While the technique itself is uncomplicated, we have extensively and rigorously proved its validity, including developing a detailed means of analyzing which transitions are important at a given temperature.

Although we developed our method independently from Gupta & Meyer (2001), our computed rates will be numerically similar to calculations using the technique of that work because we ultimately arrive at similar conclusions. Nevertheless, ours has some advantages. First, whereas Gupta & Meyer (2001) assume that intermediate states equilibrate essentially instantaneously, we do not rely on physical assumptions. Second, we do not use a Taylor expansion to solve Equation (9); a solution always exists, and a linear equation solver will quickly find it. This eliminates any concern about including enough terms of the expansion for any nucleus at any temperature.

We do, however, owe a great debt to Gupta & Meyer (2001) for our calculations of ensemble β-decay rates. While these rely on the assumption of fast equilibration of intermediate states, it is in general a very good assumption, and their method of assigning ensemble weights to the intermediate states is a powerful way to accurately break the nucleus into two species for nucleosynthesis network calculations.

We have applied our methods to several interesting nuclei, and we used the formulation of Gupta & Meyer (2001) and Misch et al. (2018) to compute β-decay rates for these nuclei, treating the ground state and isomers as separate species. For most of our case studies, we find that for a given set of destruction rates (in this case, β decay, though it applies to all destruction channels), there is a clear "thermalization temperature." Above this temperature, the nuclear levels may be assumed to be in thermal equilibrium, and below it, the isotope should be treated as two independent species: the ground state and an astromer. We summarize in Table 3 the astrophysically relevant nuclear isomers studied in this work.

Table 3.  Summary of Data for Nuclei in This Paper

Isotope Em ${J}_{g}^{\pi }$ ${J}_{m}^{\pi }$ T1/2, g T1/2, m Bmβ # States Ttherm Sitea Notes
  (keV)     (s) (s) (%)   (keV)    
26Al 228.31 5+ 0+ 2.26 × 1013 6.35 × 100 100 67 35 p λ32, λ43 unmeasured
34Cl 146.36 0+ 3+ 1.53 × 100 1.92 × 103 55 30 20 Sne λ32 poorly constrained
58Mn 71.77 1+ 4+ 3.00 × 100 6.54 × 101 90 30 5 PSne λij unmeasured for 3-7
85Kr 304.87 9/2+ 1/2 3.39 × 108 1.61 × 104 78.8 30 25 s λij poorly measured for 3-7
113Cd 263.54 1/2+ 11/2 2.54 × 1023 4.45 × 108 99.86 30 5 r λ42 unmeasured
121Sn 6.31 3/2+ 11/2 9.73 × 104 1.39 × 109 22.4 30 20 s, r λij unmeasured for 3-6
123Sn 24.6 11/2 3/2+ 1.12 × 107 2.4 × 103 100 30 30 r λij unmeasured for 3-7
125Sn 27.50 11/2 3/2+ 8.33 × 105 5.71 × 102 100 30 30 r λij unmeasured for 3-8
127Sn 5.07 11/2 3/2+ 7.56 × 103 2.48 × 102 100 30 30 r λij unmeasured for 3-8
128Sb 0.0 + X 8 5+ 3.26 × 104 6.25 × 102 96.4 9 unknown r Em unknown; Note 2 below
170Ho 120 (6) (1+) 1.66 × 102 4.3 × 101 100 2 unknown r Note c below
176Lu 122.845 7 1 1.19 × 1018 1.32 × 104 100 30 10 s λij unmeasured for 5-13, 16, 17
182Hf 1172.87 0+ (8) 2.81 × 1014 3.69 × 103 54 30 10 s, r λij unmeasured for 2-9, 11, 12

Notes. The column headers use g and m as shorthand for the ground state and isomer, respectively. The state number (starting with ground ng = 1) of the isomer is nm = 2 for all nuclei except 182Hf, which has nm = 10. The isomer energy is Em, and the Jπ are the spin and parity of the respective levels (parentheses denote uncertain Jπ). The half-lives (T1/2) and β-decay branching for the isomer (Bmβ) are as measured in the laboratory; Bmβ is the percent of isomer decays which are β decays rather than internal transitions to another nuclear state. The column # States tells how many measured levels we included in our calculations, and our computed approximate thermalization temperature is indicated by Ttherm. The Site column indicates the astrophysical site of interest. Notes highlights important points about available data; specific states or ranges of states are deemed relevant from our pathfinding in that nucleus. All experimental data is taken from the ENSDF database at http://www.nndc.bnl.gov/ensarchivals/.

aAstrophysical site key: p: p-process. r: r-process. s: s-process. Sne: supernovae. PSne: presupernovae. bIntermediate states unmeasured. cEm uncertain; intermediate states of 170Ho unmeasured and 170Dy β intensities unmeasured.

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We have shown that the isomers in 121,123,125,127Sn, 128Sb, and 176Lu have high thermalization temperatures relative to the environments where they are created. Our results reinforce the claim by Fujimoto & Hashimoto (2020) that some of these isomers play important roles in the r-process and show that there may be impact from astromers on the s-process. We have also identified 170Ho as another potentially impactful r-process astromer. These findings motivate more detailed study of astromers in nucleosynthesis.

We find that there is currently insufficient data on the excited states of 128Sb and 170Ho to compute transition rates and thermalization temperatures. This lack of data and their probable importance in the r-process highlight a need for experimental inquiry into their excited-state properties. Additionally, we have shown that uncertainties in individual intermediate-state transitions can dramatically influence the effective transition rates and thermalization temperatures. The success of precise measurements of 34Cl transitions in producing precise effective transition rates demonstrates the value of measuring the unknown transitions in nuclei with isomers.

Our calculations have focused on β decay, but the ensemble destruction rates can be just as readily computed for any other destruction channel. We must simply recognize that a fast destruction rate will tend to raise the thermalization temperature. For example, an isomer that decays solely via internal transition to the ground state will thermalize under most conditions. But if the isomer has a very different neutron capture cross section from the ground state, it may fall out of equilibrium in the r-process, ultimately affecting nuclear flow.

Another concern is the "feeding factors" of the ground state and isomer during production—that is, for a given production channel and environment, what fraction of the material goes to which ensemble. For example, consider the 26Al rates shown in Figure 6. Assume for the sake of argument that we produce this nucleus at T = 10 keV with a 50/50 split of ground state and isomer. Before an appreciable population of the species has had a chance to build up, we would measure an instantaneous effective β-decay rate for the species that is the average of the ground-state and isomer decay rates. However, as time goes on, a population of the ground state will build up while the isomer decays away. When we again measure the instantaneous effective β-decay rate, it will be skewed toward the ground-state rate because the ground state will have a greater population. We therefore see that the species effective β-decay rate can be time dependent irrespective of production mechanism.

Of course, the PiE for the states where the isotope is produced are the feeding factors into the ground and isomeric ensembles. Consider 26Al produced by 25Mg(p,γ). In this reaction, the initial states of 26Al are a small handful of resonant levels above the proton separation energy of 6306.31 keV. If we can reliably calculate the PiE for these states, we will know how much material lands in each of the isomer and ground state. The same is true for the daughter levels in 84Kr(n,γ)85Kr, 170Dy(β)170Ho, and so on.

It is also important to note that while many of the finer details (path reversibility, etc.) rely on a thermal bath, the general method of computing effective isomer ↔ ground-state transitions does not. As long as λst and λts are measured or calculable for every relevant pair of states s and t, we may use Equation (9) to compute the effective transition rates. This may have applications when nuclei with isomers are exposed to nonthermal sources of radiation. In this vein, our method applies to random walks through any general weighted network of connected nodes where you wish to get from node A to node B without going through node C (or D, E, etc.) Here, the nodes are nuclear levels and the connections are internal nuclear transitions.

A nuclear isomer has astrophysical consequences and is hence an "astromer" below the thermalization temperature. This temperature is sensitive to the various destruction rates that the nuclear species faces, with rapid rates increasing the temperature, thereby widening the range of conditions for which a metastable state is an astromer. At sufficiently high temperatures, the transition rates dominate the destruction rates, the astromer property fades, and the isotope may be considered a single species.

5. Supporting Data

We provide ASCII-formatted data files in a tar.gz package containing the effective transition and weak-interaction rates for the isotopes presented in this paper. The rates are compiled into two data files for each isotope (one for the ground state and one for the isomer) along with relevant metadata, including publication data, the nuclear level energy, the assumed density of the environment, and descriptions of the columns. We always take ρYe = 105 g cm−3, which should be adequate for most environments where electrons are not degenerate and electron capture is not the dominant weak interaction. We also provide the rates from our sensitivity studies of 26Al and 85Kr. These data are intended for unlimited release under Los Alamos report LA-UR-20-26010.

We thank Frank Timmes, Aaron Couture, Brad Meyer, Alex Heger, and George Fuller for helpful astrophysics discussions. Calvin Johnson deserves credit for the term "astromer." Timothy Elling, Jonah Miller, Peter Polko, Joseph Schaeffer, and Marc Verriere provided insights on pathfinding. Alice Shih helped create Figure 1. G.W.M. would like to acknowledge Presh Talwalkar and his YouTube channel Mind Your Decisions for inspiring Equations (7) and (9). G.W.M and M.R.M. were supported by the US Department of Energy through the Los Alamos National Laboratory. The Los Alamos National Laboratory is operated by Triad National Security, LLC, for the National Nuclear Security Administration of the US Department of Energy (Contract No. 89233218CNA000001). G.W.M and M.R.M. were also supported by the Laboratory Directed Research and Development program of Los Alamos National Laboratory under project number 20190021DR. This research was partially supported by the National Natural Science Foundation of China (No. U1932206) and the National Key Program for S&T Research and Development (No. 2016YFA0400501).

Software: WebPlotDigitizer (v4.3; https://automeris.io/WebPlotDigitizer), MatPlotLib (v3.3.1; Hunter 2007), NumPy (v1.19.0; van der Walt et al. 2011), SciPy (v1.5.2; Virtanen et al. 2020).

Appendix: Transition Pathways

In determining the effect of unmeasured individual transition rates on total effective transition rates, it is helpful to identify those paths through intermediate states which a nucleus is most likely to follow. We describe here the probabilities of following specific paths, the algorithm we employed to identify the dominant paths, and comment on the symmetry of reverse paths.

A.1. Path Probabilities

The probability of following a path is the product of the weights bij for each step in the path. We will show here precisely what that means. A probability quantifies how frequently an outcome will occur from a set of possibilities, and the probabilities must sum to unity. In discussing path probabilities, we must define the possibilities under consideration.

The first set of possibilities we discuss is not directly applicable to calculations of effective transition rates, but rather is useful in interpreting the PiE. Consider the set of all paths of length N which begin at state i and end anywhere. Naturally, the probabilities of following these paths must sum to unity because the system must end up somewhere. For paths of length 1, we can easily see that the probability of following each path to each final state f is bif. Those are the individual transition probabilities, and we know that they sum over f to unity. Now consider paths of length 2: i → j → f. We know the probabilities of the individual transitions, so we may simply multiply them then sum the products over all values of j and f to get a normalization factor K for the total probability:

Equation (A1)

The inner sum is unity, which implies that the total sum is unity, and the normalization factor is simply 1. Considering paths of greater length simply extends the number of sums, and we see that paths of length N form a well-defined set of possibilities with probabilities computed from direct multiplication of the individual transition probabilities.

Our graph represents an irreducible Markov chain (every state is reachable from every other state by at least one path), so all states are members of a single communicating class (Gagniuc 2017). Consequently, each intermediate state can reach A via at least one path with a finite number of steps N and that path has a positive probability with respect to other paths of length N. This implies that with repeated transitions, the probability of not having followed a path that reaches A will decay toward zero. Thus, A is recurrent, meaning the system will eventually reach A with unit probability. Recurrence is a class property (all members of a communicating class are either recurrent or not recurrent), so a system will eventually reach A with probability 1 and it will eventually reach every other endpoint state with probability 1.

The PiE from Section 2 quantify the probability of starting from intermediate state i and reaching endpoint E before reaching any other endpoint. The system definitely reaches every endpoint eventually, and it must reach one of them first; the probabilities PiE therefore sum to 1:

Equation (A2)

Now we describe a more directly applicable set of possibilities. We are interested in starting at A, leaving to some state s (which in principle could be B), and finding the subsequent probability of successfully transitioning to endpoint state B. Again, for every state s, the sum over t of bst is unity, which combines with Equation (A2) to give a set of possibilities whose probabilities sum to unity:

Equation (A3)

In words, the set of possibilities for which we compute probabilities is paths that begin at A, terminate at an endpoint state, and do not have any endpoint states in between. When the system leaves A, it must eventually reach an endpoint state (Equation (A2)), so the probabilities of all possibilities sum to 1 (Equation (A3)). The possibilities are also mutually exclusive (no two paths are alike), giving a well-defined set of possibilities and associated probabilities.

Iterated expansion of the PjB in Equation (8) reveals that PiB is the sum over all paths of any length from i to B of the compounded individual transition probabilities:

Equation (A4)

Note that this includes short paths that might not have a j or k. Multiplying Equation (8) by bAi gives an unnormalized probability that when the system leaves A, it goes to i, and from there via some path that eventually leads to B, with the contribution of each path to that probability explicitly computable. Likewise, we may compute the unnormalized probabilities of paths that begin at A and go to any endpoint E (including returning to A) by using the PiE. But comparison with Equation (A3) shows that the sum of the compounded individual transition probabilities for all paths that start at A and end at any endpoint is unity. In other words, the compounded individual transition probabilities for these paths directly answer the question "when the system leaves A, what is its probability of following a particular path to a particular endpoint state given that the path terminates at an endpoint state?" Naturally, we may replace A with any endpoint state.

The total effective transition rate ΛAB is ultimately the product of the rate λA at which systems leave A and the sum of the probabilities of paths from A to B (see Equation (6) in the context of the arguments in this section). Each path A → ... → B contributes to the total effective transition rate in proportion to its probability, and we may now ask which paths contribute the most to transition rates.

A.2. Pathfinding Algorithm

To find the most probable paths through intermediate states, we use a version of the A* pathfinding algorithm (Hart et al. 1968). In its original form, A* finds the single path of least cost between two vertices that does not revisit intermediate vertices on a weighted graph. The edge costs are also typically nonnegative and additive. For our purposes, each of the emphasized points requires generalizing.

The first generalization is well known: finding the k shortest paths, rather than the single shortest (Eppstein 1998). Although k is the standard symbol for finding multiple shortest paths, we will for the remainder of this section use N to avoid confusion with a state labeled k.

The second generalization requires a notion of "legality." Consider a graph that represents a geographic map, and we are looking for routes from A to B. We would not be interested in paths that revisit vertices as it would effectively be backtracking. We would therefore declare any paths that include revisiting to be illegal and not consider such paths as candidates. In general, at each iteration of the algorithm described below, we would determine whether each next increment in the path is legal according to our specific needs, then as appropriate either add it to or exclude it from the list of candidate paths.

In the class of cases under consideration here, a physical system may meander between intermediate states—even tracing loops in the graph—before reaching B. If we exclude paths that revisit intermediate states, we will miss the contribution of these meanderings to the total effective transition rate. Indeed, some paths with loops may contribute more than some direct paths. This leads to our statement of path legality: we allow any path that starts at A, ends at B, and does not have A or B as intermediates.

The final generalization addresses how we compute cost. In the graphs considered here, the edge weights are multiplicative probabilities. These may be converted to nonnegative additive weights by taking the negative logarithm:

Equation (A5)

But this is an unnecessary step if we change the optimization criterion from "least cost" to "highest probability." We may just as easily compute the cumulative effect of each incremental addition to a path; we simply multiply instead of add, and we prefer paths with higher cost (probability) instead of lower.

A* requires a heuristic function h(v) that estimates the cost from each vertex v to the goal (here, the goal is B). Candidate paths are then selected according to the criterion of optimizing the computed actual cost to get to the current vertex combined with the estimated cost to get the rest of the way to the goal. This heuristic must be "admissible," meaning it never overestimates the actual cost. With our multiplicative weights, our choice of heuristic must therefore never underestimate the probability. For simplicity, we take h(v) = 1v. In principle, we could achieve better performance with a more intelligent choice of h(v), but we will not worry about that here.

Finally, we describe our algorithm in detail. To find the N most probable paths from A to B, follow these steps.

  • 1.  
    Start an empty list of candidate paths.
  • 2.  
    Add to this list all possible paths of length 1 (one increment) that start at A. Using the graph in Figure 1 as an example, the list will now consist of the paths A → i, A → j, and A → k.
  • 3.  
    Select the highest probability path from the candidate list and delete it from the list.
  • 4.  
    If the selected path does not end at B, add to the candidate list all legal paths that are one increment farther along and return to step 3. If, for example, the most probable candidate path is A → i, delete it from the list and append to the list the candidates A → i → B, A → i → j, and A → i → k.
  • 5.  
    If the selected path ends at B, record it as the nth most probable path, where n is the number of most probable paths found so far. If N most probable paths have been found, you are done. Otherwise, return to step 3.

It is worth mentioning that it is in principle possible to get caught in a loop of transitions where probability decays slowly with each iteration, and a path may traverse this loop many times before it fails to be selected in step 3. This can be avoided if in step 4 we augment the legality condition to say that a path may not include more than N − 1 total loops. Because every path increment at best does not increase a path's probability, we may be assured that a path P that visits a state n times will be at least as probable as an otherwise identical path that includes a loop to visit the state n + 1 times. Therefore, there will be at least n − 1 paths at least as probable as P, and we may safely reject all paths with more than N − 1 loops.

A.3. Path Symmetry

In a general weighted digraph, the optimal path from A to B is not necessarily the optimal path from B to A. But when transitions are mediated by a thermal bath, the most probable path between two states—and hence the greatest contributor to the transition rate—is the same in both directions. In fact, all paths maintain their relative probability when traversed in either direction. For example, the second most probable path from A to B is also the second most probable path from B to A, and so on. Figure 21 illustrates this for the five most probable paths through 26Al at temperature T = 500 keV. This is an unrealistically high temperature for 26Al production, but it nicely illustrates the symmetry. The states are labeled in increasing order of energy starting with ground = 1 and isomer = 2. In the figure, the most probable path (rank = 1) from ground to the isomer is 1 → 36 → 47 → 21 → 8 → 4 → 2, while from the isomer to ground it is 2 → 4 → 8 → 21 → 47 → 36 → 1. All other ranks exhibit the same symmetry. We detail the inputs to our calculations in Section 3.1.

Figure 21.

Figure 21. The five most probable paths from the ground state to the isomer (top) and from the isomer to ground (bottom) in 26Al at a temperature T = 500 keV. The paths in one direction are the reverse of the paths in the other direction.

Standard image High-resolution image

A stochastic process for which all paths obey the symmetry described above is known as a reversible Markov chain (RMC), and there are at least three ways to show that nuclear energy levels with thermally mediated transitions comprise such.

First, and most simply, a system that meets the detailed balance condition is an RMC. The detailed balance condition is that there exists a configuration of occupation probabilities for which the transition rates between every pair of states is the same forward and backward. That is, if we denote the occupation probability of state i as ni, there must be some set of occupations such that niλij = njλji for all i and j (Durrett 1999). The thermal-equilibrium distribution ${n}_{i}\propto (2{J}_{i}+1){e}^{-{E}_{i}/T}$ satisfies this equation (see Equation (5)), guaranteeing reversibility. Importantly, the system need not be in this configuration; the configuration must only exist.

Second, the specific symmetry here is directly provable, which we will do presently. Third, by a trivial extension of the direct proof, we can show that thermally mediated transitions satisfy Kolmogorov's criterion, which states that a Markov chain is reversible if for every closed loop, the probability of following the loop is the same in both directions (Kelly 2011).

To directly prove path reversal symmetry, we begin with the probability pAi...jB that a transition out of state A follows the path A → i → ... → j → B:

Equation (A6)

Rewrite the b's terms of the λ's:

Equation (A7)

We use Equation (5) to reverse the indices of the numerators, using gs ≡ 2Js + 1 for brevity:

Equation (A8)

The exponents contain a collapsing sum, and the gsA,B all cancel, yielding

Equation (A9)

We now multiply by ${\lambda }_{B}/{\lambda }_{B}$ and shift all of the numerators to the right:

Equation (A10)

Rewrite the λ's in terms of the b's:

Equation (A11)

Finally, we recognize that this product of b's is the reverse path probability:

Equation (A12)

The factor relating the forward and reverse path probabilities is path independent, and depends only on temperature and the properties of the endpoint states. Therefore, the fractional contribution of each path to transition rates from endpoint to endpoint is the same forward and backward; if a path contributes 10% of the rate from ground to isomer, then it contributes 10% of the rate from isomer to ground. Reversal factors that are not equal to unity imply that one endpoint state or the other is more likely to fail to transition, returning to its starting point.

To demonstrate satisfaction of Kolmogorov's criterion, we need only set A = B in the direct proof. Because the proof does not rely on any special properties of A and B (e.g., longevity), A and B may be taken to be arbitrary and equal. Then, per Equation (A12), the reverse probability is identical to the forward probability for all closed loops.

As a final point, the rate to follow a particular path starting at endpoint E is the product of the rate to leave E and the probability of following that path. That is, λpath = λE ppath. Note from Equation (A12) that the rates to follow each path in the forward and reverse directions obey the same relationship as the direct transition rates in Equation (5). Summing over all paths from A to B leads us to conclude that effective transition rates between endpoint states exhibit the thermal relationship

Equation (A13)

This result is not surprising given an intuition of detailed balance, but it is nevertheless useful to have it made explicit and to observe that it does not require the nuclear levels to be in a thermal-equilibrium distribution. Indeed, relying on methods that do not include path reversal symmetry can lead to erroneous results. Reifarth et al. (2018) made the seemingly reasonable assumption that all dominant paths consist of one up transition from a long-lived state followed by a cascade of down transitions through intermediate states; this is justified by the fact that down transitions are much faster than up transitions and therefore dominate the deexcitation of intermediate states. However, from the present analysis and Figure 4, we see that at temperature T = 35 keV, this misses the single greatest contributing path (1 → 3 → 4 → 2) from the ground state to the isomer in 26Al; the consequence is a drastic underestimate of the effective transition rate in an important temperature range.

Footnotes

  • This article is intended for unlimited release under LA-UR-20-22828.

  • Transition paths, the algorithm we use to find them, and an important symmetry are detailed in the Appendix.

  • 10 

    To be precise, we should use b3m, b4m, etc. rather than P. Nevertheless, P is adequate for the present qualitative analysis.

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10.3847/1538-4365/abc41d