Emerging Leaders

First-principles calculations based on density-functional theory including anharmonicity within the variational stochastic self-consistent harmonic approximation are applied to understand how the quantum character of the proton affects the candidate metallic molecular Cmca  −  4 structure of hydrogen in the 400–450 GPa pressure range, where metallization of hydrogen is expected to occur. Anharmonic effects, which become crucial due to the zero-point motion, have a large impact on the hydrogen molecules by increasing the intramolecular distance by approximately a 6%. This induces two new electron pockets at the Fermi surface opening new scattering channels for the electron–phonon interaction. Consequently, the electron–phonon coupling constant and the superconducting critical temperature are approximately doubled by anharmonicity and Cmca  −  4 hydrogen becomes a superconductor above 200 K in all the studied pressure range. Contrary to many superconducting hydrides, where anharmoncity tends to lower the superconducting critical temperature, our results show that it can enhance superconductivity in molecular hydrogen.

The temperature and concentration dependent phase diagrams of zero-valent copper, cobalt, and iron intercalated bismuth selenide are investigated using in situ transmission electron microscopy. Polytypic phase transitions associated with superlattice formation along with order-disorder transitions of the guest intercalant are determined. Dual-element intercalants of CuCo, CuFe, and CoFe-Bi ₂Se ₃ are also investigated. Hexagonal and striped domain formation consistent with two-dimensional ordering of the intercalant and Pokrovksy–Talapov theory is identified as a function of concentration. These studies provide a complete picture of the structural behavior of zero-valent metal intercalated Bi ₂Se ₃.

Using combined low-temperature scanning tunneling microscopy and Kelvin probe force microscopy we studied the local electronic structure and work function change of the (0 0 0 1)-oriented epitaxial ZnO layers on a Ag(1 1 1) substrate. Scanning tunneling spectroscopy (STS) revealed that the conduction band minimum monotonically downshifts as the number of the ZnO layers increases up to 4 monolayers (ML). However, it was found by field emission resonance (FER) spectroscopy that the local work function of Ag(1 1 1) slightly decreases for 2 ML thick ZnO but it dramatically changes and drops by about 1.2 eV between 2 and 3 ML, suggesting a structural transformation of the ZnO layer. The spatial variation of the conduction band minimum and the local work function change were visualized at the nanometer scale by mapping the STS and FER intensities. Furthermore, we found that the ZnO layers contained line defects with a few tens of nm long, which can be removed by the injection of a tunneling electron into the conduction band.

Colloidal particles are considered ideal building blocks to produce materials with enhanced physical properties. The state-of-the-art techniques for synthesizing these particles provide control over shape, size, and directionality of the interactions. In spite of these advances, there is still a huge gap between the synthesis of individual components and the management of their spontaneous organization towards the desired structures. The main challenge is the control over the dynamics of self-organization. In their kinetic route towards thermodynamically stable structures, colloidal particles self-organize into intermediate (mesoscopic) structures that are much larger than the individual particles and become the relevant units for the dynamics. To follow the dynamics and identify kinetically trapped structures, one needs to develop new theoretical and numerical tools. Here we discuss the self-organization of functionalized colloids (also known as patchy colloids) on attractive substrates. We review our recent results on the adsorption and relaxation and explore the use of annealing cycles to overcome kinetic barriers and drive the relaxation towards the targeted structures.

Quantum mechanical simulation of realistic models of nanostructured systems, such as nanocrystals and crystalline interfaces, demands computational methods combining high-accuracy with low-order scaling with system size. Blöchl’s projector augmented wave (PAW) approach enables all-electron (AE) calculations with the efficiency and systematic accuracy of plane-wave pseudopotential calculations. Meanwhile, linear-scaling (LS) approaches to density functional theory (DFT) allow for simulation of thousands of atoms in feasible computational effort. This article describes an adaptation of PAW for use in the LS-DFT framework provided by the ONETEP LS-DFT package. ONETEP uses optimisation of the density matrix through in situ-optimised local orbitals rather than the direct calculation of eigenstates as in traditional PAW approaches. The method is shown to be comparably accurate to both PAW and AE approaches and to exhibit improved convergence properties compared to norm-conserving pseudopotential methods.

The self-consistent theory of localization is generalized to account for a weak quadratic nonlinear potential in the wave equation. For spreading wave packets, the theory predicts the destruction of Anderson localization by the nonlinearity and its replacement by algebraic subdiffusion, while classical diffusion remains unaffected. In 3D, this leads to the emergence of a subdiffusion-diffusion transition in place of the Anderson transition. The accuracy and the limitations of the theory are discussed.

As the complexity of strongly correlated systems and high temperature superconductors increases, so does also the essential complexity of defects found in these materials and the complexity of the supercurrent pathways. It can be therefore convenient to realize a solid-state system with regular supercurrent pathways and without the disguising effects of disorder in order to capture the essential characteristics of a collective dynamics. Using a square array of superconducting islands placed on a normal metal, we observe a state in which magnetic field-induced vortices are frozen in the dimples of the egg crate potential by their strong repulsion interaction. In this system a dynamic vortex Mott insulator transition has been previously observed. In this work, we will show the symmetric dynamic behaviour with respect to field reversal and we will compare it with the asymmetric behaviour observed at the dynamic vortex Mott transition.

Magnetic susceptibility, electrical resistivity, and heat capacity results are reported for the chemical substitution series URu ₂Si _{2− x} P _x for . This study expands in detail on work recently reported in Gallagher et al (2016 Nat. Commun. 10712), which focused on the small x region of this substitution series. Measurements presented here reveal persistent hybridization between the f- and conduction electrons and strong variation of the low temperature behavior with increasing x. Hidden order and superconductivity are rapidly destroyed for and are replaced for by a region with Kondo coherence but no ordered state. Antiferromagnetism abruptly appears for . This phase diagram differs significantly from those produced by most other tuning strategies in URu ₂Si ₂, including applied pressure, high magnetic fields, and isoelectronic chemical substitution (i.e. Ru  →  Fe and Os), where hidden order and magnetism share a common phase boundary. Besides revealing an intriguing evolution of the low temperature states, this series provides a setting in which to investigate the influence of electronic tuning, where probes that are sensitive to the Fermi surface and the symmetry of the ordered states will be useful to unravel the anomalous behavior of URu ₂Si ₂.

Quantitative tracking of features from video images is a basic technique employed in many areas of science. Here, we present a method for the tracking of features that partially overlap, in order to be able to track so-called colloidal molecules. Our approach implements two improvements into existing particle tracking algorithms. Firstly, we use the history of previously identified feature locations to successfully find their positions in consecutive frames. Secondly, we present a framework for non-linear least-squares fitting to summed radial model functions and analyze the accuracy (bias) and precision (random error) of the method on artificial data. We find that our tracking algorithm correctly identifies overlapping features with an accuracy below 0.2% of the feature radius and a precision of 0.1 to 0.01 pixels for a typical image of a colloidal cluster. Finally, we use our method to extract the three-dimensional diffusion tensor from the Brownian motion of colloidal dimers.

Three-dimensional (3D) Dirac semimetals are featured by 3D linear energy-momentum dispersion relation, which have been proposed to be a desirable system to study Dirac fermions in 3D space and Weyl fermions in solid-state materials. Significantly, to reveal exotic transport properties of Dirac semimetals, the Fermi level should be close to the Dirac point, around which the linear dispersion is retained. Here we report the magnetotransport properties near the Dirac point in Cd ₃As ₂ nanowires, manifesting the evolution of band structure under magnetic field. Ambipolar field effect is observed with the Dirac point at V _g  =  3.9 V. Under high magnetic field, there is a resistivity dip in transfer curve at the Dirac point, which is caused by the Zeeman splitting enhanced density of state around the Dirac point. Furthermore, the low carrier density in the nanowires makes it feasible to enter into the quantum limit regime, resulting in the quantum linear magnetoresistance being observed even at room temperature. Besides, the dramatic reduction of bulk conductivity due to the low carrier density, together with a large surface to volume ratio of the nanowire, collectively help to reveal the Shubnikov–de Haas oscillations from the surface states. Our studies on transport properties around the Dirac point therefore provide deep insights into the emerging exotic physics of Dirac and Weyl fermions.

We present a numerical study on the thermal activated avalanche dynamics in granular materials composed of ferromagnetic clusters embedded in a non-magnetic matrix. A microscopic dynamical simulation based on the reaction-diffusion process is developed to model the magnetization process of such systems. The large-scale simulations presented here explicitly demonstrate inter-granular collective behavior induced by thermal activation of spin tunneling. In particular, we observe an intriguing criticality controlled by the rate of energy dissipation. We show that thermal activated avalanches can be understood in the framework of continuum percolation and the emergent dissipation induced criticality is in the universality class of 3D percolation transition. Implications of these results to the phase-separated states of colossal magnetoresistance materials and other artificial granular magnetic systems are also discussed.

When the motion of a probe strongly disturbs the thermal equilibrium of the solvent or bath, the nonlinear response of the latter must enter the probe’s effective evolution equation. We derive that induced stochastic dynamics using second order response around the bath thermal equilibrium. We discuss the nature of the new term in the evolution equation which is no longer purely dissipative, and the appearance of a novel time-scale for the probe related to changes in the dynamical activity of the bath. A major application for the obtained nonlinear generalized Langevin equation is in the study of colloid motion in a visco-elastic medium.

Bulk phase separation is responsible for the occurrence of stacks of different layers in sedimentation of colloidal mixtures. A recently proposed theory (de las Heras and Schmidt 2013 Soft Matter 9 8636) establishes a unique connection between the bulk phase behaviour and sedimentation-diffusion-equilibrium. The theory constructs a stacking diagram of all possible sequences of stacks under gravity in the limit of very high (infinite) sample heights. Here, we study the stacking diagrams of colloidal mixtures at finite sample height, h. We demonstrate that h plays a vital role in sedimentation-diffusion-equilibrium of colloidal mixtures. The region of the stacking diagram occupied by a given sequence of stacks depends on h. Hence, two samples with different heights but identical colloidal concentrations can develop different stacking sequences. In addition, the stacking diagrams for different heights can be qualitatively different since some stacking sequences occur only in a given interval of sample heights. We use the theory to investigate the stacking diagrams of both model bulk systems and mixtures of patchy particles that differ either by the number or by the types of patches.

The drying of a drop containing particles often results in the accumulation of the particles at the contact line. In this work, we investigate the drying of an aqueous colloidal drop surrounded by a hydrogel that is also evaporating. We combine theoretical and experimental studies to understand how the surrounding vapor concentration affects the particle deposit during the constant radius evaporation mode. In addition to the common case of evaporation on an otherwise dry surface, we show that in a configuration where liquid is evaporating from a flat surface around the drop, the singularity of the evaporative flux at the contact line is suppressed and the drop evaporation is homogeneous. For both conditions, we derive the velocity field and we establish the temporal evolution of the number of particles accumulated at the contact line. We predict the growth dynamics of the stain and the drying timescales. Thus, dry and wet conditions are compared with experimental results and we highlight that only the dynamics is modified by the evaporation conditions, not the final accumulation at the contact line.

We investigate the atomic structure of Sn dimer chains grown on the Si(1 0 0) surface using non-contact atomic force microscopy (NC-AFM) at cryogenic temperatures. We find that similar to the native Si(1 0 0) dimer structure, the ground state of the Sn dimer structure is buckled at low temperature. At 5 K we show that the buckling state of the Sn dimers may be controllably, and reversibly, manipulated with atomic precision by close approach of the tip, without modification of the underlying substrate buckling structure. At intermediate cryogenic temperatures we observe changes in the configuration of the dimer chains in the region where the tip-sample interaction is very weak, suggesting that the energy barrier to transit between configurations is sufficiently small to be surmounted at 78 K.

Electrostatic interactions between DNA molecules have been extensively studied experimentally and theoretically, but several aspects (e.g. its role in determining the pitch of the cholesteric DNA phase) still remain unclear. Here, we performed large-scale all-atom molecular dynamics simulations in explicit water and 150 mM sodium chloride, to reconstruct the potential of mean force (PMF) of two DNA oligomers 24 base pairs long as a function of their interaxial angle and intermolecular distance. We find that the potential of mean force is dominated by total DNA charge, and not by the helical geometry of its charged groups. The theory of homogeneously charged cylinders fits well all our simulation data, and the fit yields the optimal value of the total compensated charge on DNA to  ≈65% of its total fixed charge (arising from the phosphorous atoms), close to the value expected from Manning’s theory of ion condensation. The PMF calculated from our simulations does not show a significant dependence on the handedness of the angle between the two DNA molecules, or its size is on the order of . Thermal noise for molecules of the studied length seems to mask the effect of detailed helical charge patterns of DNA. The fact that in monovalent salt the effective interaction between two DNA molecules is independent on the handedness of the tilt may suggest that alternative mechanisms are required to understand the cholesteric phase of DNA.

We introduce a generalization of the adiabatic frequency conversion method for an efficient conversion of ultrashort pulses in the full nonlinear regime. Our analysis takes into account dispersion as well as two-photon processes and Kerr effect, allowing complete analysis of any three waves with arbitrary phase mismatched design and any nonlinear optical process. We use this analysis to design an efficient and robust second harmonic generation, the most widely used nonlinear process for both fundamental and applied research. We experimentally show that such design not only allows for very efficient conversion of various of ultrashort pulses, but is also very robust to variations in the parameters of both the nonlinear crystal and the incoming light. These include variation of more than 100 °C in the crystal temperature, a wide bandwidth of up to 75 nm and a chirp variation of 300 fs to 3.5 ps of the incoming pulse. Also, we show the dependency of the adiabatic second harmonic generation design on the pump intensity and the crystal length. Our study shows that two photon absorption plays a critical role in such high influence nonlinear dynamics, and that it must be considered in order to achieve agreement with experimental results.

The dissolution of sodium chloride (NaCl) in water is a frequently encountered process in our daily lives. While the NaCl dissolution process in liquid water has been extensively studied, whether and how the dissolution occurs below the freezing point is still not clear. Using a low-temperature scanning tunneling microscope (STM), here we were able to directly visualize the dissolution of Au-supported NaCl (0 0 1) bilayer islands by water at atomic level. We found that the single water molecule on the STM tip can assist the extraction of single Na ⁺ from the NaCl surface even at 5 K, while leaving the Cl ⁻ intact. When covered with a full water monolayer, the NaCl islands started to dissolve from the step edges and also showed evidence of dissolution inside the terraces as the temperature was raised up to 145 K. At 155 K, the water molecules completely desorbed from the surface, which was accompanied with the decomposition and restructuring of the bilayer NaCl islands. Those results suggest that the dissolution of NaCl may occur well below the freezing point at the ice/NaCl interfaces and is mainly driven by the interaction between the water molecules and the Na ⁺, which is in clear contrast with the NaCl dissolution in liquid water.

We have developed a drift-diffusion equation of spin transport in collinear bipartite metallic antiferromagnets. Starting from a model tight-binding Hamiltonian, we obtain the quantum kinetic equation within Keldysh formalism and expand it to the lowest order in spatial gradient using Wigner expansion method. In the diffusive limit, these equations track the spatio-temporal evolution of the spin accumulations and spin currents on each sublattice of the antiferromagnet. We use these equations to address the nature of the spin transfer torque in (i) a spin-valve composed of a ferromagnet and an antiferromagnet, (ii) a metallic bilayer consisting of an antiferromagnet adjacent to a heavy metal possessing spin Hall effect, and in (iii) a single antiferromagnet possessing spin Hall effect. We show that the latter can experience a self-torque thanks to the non-vanishing spin Hall effect in the antiferromagnet.

We simulate electron transport through graphene nanoribbons of realistic size containing a p–n junction patterned by electrostatic gates. For a sharp p–n interface, Klein tunneling leads to refocusing of a divergent beam forming a Veselago lens. Wider transition regions allow only electrons with near-perpendicular incidence to pass the junction, forming a Klein collimator. Using a third nearest neighbor tight binding description we explore the influence of interface roughness and bulk disorder on guiding properties. We provide bounds on disorder amplitudes and p–n junction properties to be satisfied in order to experimentally observe the focusing effect and compare our predictions to very recent realizations.

Propulsion at low Reynolds numbers is often studied by defining artificial microswimmers which exhibit a particular stroke. The disadvantage of such an approach is that the stroke does not adjust to the environment, in particular the fluid flow, which can diminish the effect of hydrodynamic interactions. To overcome this limitation, we simulate a microswimmer consisting of three beads connected by springs and dampers, using the self-developed waLB erla and framework based on the lattice Boltzmann method and the discrete element method. In our approach, the swimming stroke of a swimmer emerges as a balance of the drag, the driving and the elastic internal forces. We validate the simulations by comparing the obtained swimming velocity to the velocity found analytically using a perturbative method where the bead oscillations are taken to be small. Including higher-order terms in the hydrodynamic interactions between the beads improves the agreement to the simulations in parts of the parameter space. Encouraged by the agreement between the theory and the simulations and aided by the massively parallel capabilities of the waLB erla- framework, we simulate more than ten thousand such swimmers together, thus presenting the first fully resolved simulations of large swarms with active responsive components.

We explore an alternate way of looking at the rheological response of a yield stress fluid: using discrete geometry to probe the heterogeneous distribution of stress in soap froth. We present quasi-static, uniaxial, isochoric compression and extension of three-dimensional random monodisperse soap froth in periodic boundary conditions and examine the stress and geometry that result. The stress and shape anisotropy of individual cells is quantified by Q, a scalar measure derived from the interface tensor that gauges each cell’s contribution to the global stress. Cumulatively, the spatial distribution of highly deformed cells allows us to examine how stress is internally distributed. The topology of highly deformed cells, how they arrange relative to one another in space, gives insight into the heterogeneous distribution of stress.

In this work, a model for the interaction force between a small bubble and a wall or another bubble is presented. The formulation is especially designed for Lagrangian calculations of bubble or soft sphere trajectories, with or without resolution of the continuous fluid. The force only relies on position and velocity of the bubble. The model does not include any empirical parameter that would have to be calibrated. Therefore, this force model is easy to implement. The formulation of the force is explicit, which means low computational effort. The collision of a small bubble with an inclined top wall is investigated numerically and experimentally. The computational results achieved with the new collision model show good agreement with the experiment.

We investigate spin correlations in the dipolar Heisenberg antiferromagnet Gd ₂Sn ₂O ₇ using polarised neutron-scattering measurements in the correlated paramagnetic regime. Using Monte Carlo methods, we show that our data are sensitive to weak further-neighbour exchange interactions of magnitude  ∼0.5% of the nearest-neighbour interaction, and are compatible with either antiferromagnetic next-nearest-neighbour interactions, or ferromagnetic third-neighbour interactions that connect spins across hexagonal loops. Calculations of the magnetic scattering intensity reveal rods of diffuse scattering along [1 1 1] reciprocal-space directions, which we explain in terms of strong antiferromagnetic correlations parallel to the set of directions that connect a given spin with its nearest neighbours. Finally, we demonstrate that the spin correlations in Gd ₂Sn ₂O ₇ are highly anisotropic, and correlations parallel to third-neighbour separations are particularly sensitive to critical fluctuations associated with incipient long-range order.

We have carried out the growth of h-RFeO ₃ (0 0 1) (R  =  Lu, Yb) thin films on Fe ₃O ₄ (1 1 1)/Al ₂O ₃ (0 0 1) substrates, and studied the effect of the h-RFeO ₃ (0 0 1)/Fe ₃O ₄ (1 1 1) interfaces on the epitaxy and magnetism. The observed epitaxial relations between h-RFeO ₃ and Fe ₃O ₄ indicate an unusual matching of Fe sub-lattices rather than a matching of O sub-lattices. The out-of-plane direction was found to be the easy magnetic axis for h-YbFeO ₃ (0 0 1) but the hard axis for Fe ₃O ₄ (1 1 1) in the h-YbFeO ₃ (0 0 1)/Fe ₃O ₄ (1 1 1)/Al ₂O ₃ (0 0 1) films, suggesting a perpendicular magnetic alignment at the h-YbFeO ₃ (0 0 1)/Fe ₃O ₄ (1 1 1) interface. These results indicate that Fe ₃O ₄ (1 1 1)/Al ₂O ₃ (0 0 1) could be a promising substrate for epitaxial growth of h-RFeO ₃ films of well-defined interface and for exploiting their spintronic properties.

We present a methodology to predict magnetic systems using ab initio methods. By employing crystal structure method and spin-polarized calculations, we explore the relation between crystalline structures and their magnetic properties. In this work, testbed cases of transition metal alloys (FeCr, FeMn, FeCo and FeNi) are study in the ferromagnetic case. We find soft-magnetic properties for FeCr, FeMn while for FeCo and FeNi hard-magnetic are predicted. In particular, for the family of FeNi, a candidate structure with energy lower than the tetrataenite was found. The structure has a saturation magnetization ( M _s) of 1.2 MA m ⁻¹, magnetic anisotropy energy (MAE) above 1200 kJ m ⁻³ and hardness value close to 1. Theoretically, this system made of abundant elements could be the right candidate for permanent magnet applications. Comparing with the state-of-the-art (Nd ₂Fe ₁₄B) hard-magnet, ( M _s of 1.28 MA m ⁻¹ and MAE of 4900 kJ m ⁻³) is appealing to explore this low energy polymorph of FeNi further. Considering the relatively limited number of magnets, predicting a new system may open routes for free rare-earth magnets. Furthermore, the use of the computational algorithm as the one presented in this work, hold promises in this field for which in near future improvements will allow to study numerous complex systems, larger simulations cells and tackled long-range antiferromagnetic cases.