Focus on Advanced Nanomaterials for Energy, Environmental Science and Optoelectronic Devices

Figure

Size, shape and coupling-strength dependent optoelectronic properties of nanomaterials

Guest Editors

Sheng Hsiung Chang, Chung Yuan Christian University, Taiwan
Wei-Ren Liu, Chung Yuan Christian University, Taiwan
Chi-Tsu Yuan, Chung Yuan Christian University, Taiwan
Chiashain Chuang, Chung Yuan Christian University, Taiwan

Scope

Nanomaterials provide huge surface area, tunable optoelectronic properties and quantum confinement effects and thereby playing important roles on the manipulations of light-mater interactions, catalyses, energy flows and light emissions. However, the unpredictable complexities on the mutual interactions between the surface and bulk properties of nanostructured materials, nanocomposite materials and quantum materials impedes the developments of energy conversions, environmental protection and lighting devices based applications. Fortunately, the structural, surface, optoelectronic and chemical characteristics of nanomaterials can be manipulated by using vacuum based and/or solution-processed techniques. Therefore, the focus collection will address the recent developments and breakthroughs in the fields of nanomaterials based devices, including light-emitting diodes, photo-detectors, lasers, solar cells, batteries, energy converters, sensors, memory devices and flexible devices.

Submission process and deadline for submission

Researchers are invited to contribute their original research articles to this collection. Please submit using our online submission form.

The deadline for submissions is 31 March 2021. Nanotechnology publishes focus collections incrementally. This means that articles submitted early will be published as soon as they are accepted and prepared for publication, without being delayed waiting for other papers in the collection. If you are not able to meet the deadline, please let us know.

Topical Reviews

Synthesis, characterization, and applications of gold nanoparticles in development of plasmonic optical fiber-based sensors

Anamika Kumari et al 2023 Nanotechnology 34 042001

Gold nanoparticles (Au-NPs) are readily used nanoparticles which finds applications in fields like biosensors, drug delivery, optical bioimaging and many state of art systems used for detection. In the recent years fiber optic sensors have seen utilization of Au-NPs along with other nanoparticles for implementation of sensors for sensing various biomolecules like cholesterol, glucose, and uric acid. The cancer cells, creatinine and bacteria can also be detected with the fiber optic sensors. Given the significance of Au-NPs in fiber optic sensors, the current work is a review of the synthesis, the common methods used for characterization, and the applications of Au-NPs. It is important to discuss and analyse the work reported in the literature to understand the trend and gaps in developing plasmonic optical fiber sensors.

Papers

Synergistic coupling of IrNi/Ni(OH)2 nanosheets with polypyrrole and iron oxyhydroxide layers for efficient electrochemical overall water splitting

Zhongyao Duan et al 2023 Nanotechnology 34 275401

The design of electrocatalysts with excellent activity and stability for overall water splitting is highly desirable, and remains a challenge. Constructing heterojunctions onto the same substrate is beneficial for the integration of a water-splitting reaction. Herein, self-supported IrNi/Ni(OH)2@PPy and IrNi/Ni(OH)2@FeOOH are fabricated by coupling polypyrrole (PPy) and iron oxyhydroxide (FeOOH) on IrNi/Ni(OH)2 nanosheets array, respectively. Benefiting from the nanosheet structure, composition, and heterogeneous interface, the as-constructed IrNi/Ni(OH)2@PPy and IrNi/Ni(OH)2@FeOOH catalysts can efficiently drive the hydrogen evolution reaction and oxygen evolution reaction, respectively. Moreover, the electrolyzer consisting of IrNi/Ni(OH)2@PPy and IrNi/Ni(OH)2@FeOOH for water splitting requires only a low cell voltage of 1.49 V to deliver 10 mA cm−2. This study provides a useful strategy for constructing efficient electrocatalysts by synergistic composition modulation and interface engineering.

Strain-induced ultrahigh power conversion efficiency in BP-MoSe2 vdW heterostructure

Jiarui Tu et al 2023 Nanotechnology 34 085403

Photocatalytic water splitting is a promising method for hydrogen production, and the search for efficient photocatalysts has received extensive attention. Two-dimensional van der Waals (vdW) heterostructures have recently been considered excellent candidates for photocatalytic water splitting. In this work, a BP-MoSe2 vdW heterostructure composed of a blue phosphorus (BP) and MoSe2 monolayer was studied as a potential photocatalyst for water splitting using first-principles calculations. The results show that the heterostructure has a type-II band structure, and the band edges straddle water redox potentials under biaxial strains from −3% to 2%, satisfying the requirements for photocatalytic water splitting. In addition, the heterostructure has excellent power conversion efficiency (PCE) and strong optical absorption in both visible light and near-ultraviolet region, indicating that it is a very promising candidate for photocatalytic water splitting. Specifically, the PCE was enhanced to ∼20.2% under a tensile strain of 2%. The Gibbs free energy profiles indicate that BP-MoSe2 vdW heterostructure exhibits good catalytic performance in hydrogen and oxygen evolution reactions. In particular, high carrier mobility implies that the transfer of carriers to reactive sites is easy, and the recombination probability of photogenerated electron–hole pairs is reduced.

Rh metallene with functionalized polypyrrole surface for hydrogen evolution over a wide pH range

Wenxin Wang et al 2023 Nanotechnology 34 045402

Interface engineering of two-dimensional (2D) materials by conductive polymer modification is one of the valid methods to promote hydrogen evolution reaction (HER) performance. Herein, we report a simple and universal strategy for the synthesis of polypyrrole (PPy) modified Rh metallene (Rh@PPy metallene) towards an efficient pH-universal HER. Due to the unique ultrathin 2D metallene structure and the optimized electronic structure between the metallene-PPy surfaces, the as-prepared Rh@PPy metallene not only exhibits excellent HER activity with low overpotentials of 16, 39 and 42 mV in 0.5 M H2SO4, 1 M KOH, and 1 M phosphate buffer solution at current density of 10 mA cm−2, but also displays outstanding stability and durability. This work provides a well-founded pathway to constructe metallene-organic interfaces for various electrocatalytic applications.

Fabrication of novel BiVO4/Bi2O3 heterostructure with superior visible light induced photocatalytic properties

Maira Liaqat et al 2023 Nanotechnology 34 015711

Heterostructure BiVO4/Bi2O3 nanocomposites with enhanced visible light activity are effectively synthesized through an easiest and single step hydrothermal route, using bismuth subnitrate and ammonium meta-vanadate as main raw materials in existence of citric acid. The phase and surface structure, topography and optical properties of synthesized composites are characterized by XRD, SEM, EDX, FTIR, UV–Visible and PL spectroscopy. It was found that 5%BiVO4/Bi2O3 (BOBV-5) nanocomposite exhibit excellent photocatalytic performance for rhodamine B dye degradation and tetracyclic under irradiation of visible light as compared to single component i.e. BiVO4. The increased photocatalytic activity should be ascribed for making p–n heterojunction among p-type Bi2O3 and n-type BiVO4. This p–n heterojunction successfully reduce the recombination of photogenerated charge carriers. Furthermore, the BOBV-5 novel photocatalyst shows good stability in constructive five cycles and photocatalytic activity is best for conquering photo corrosion of a photocatalysts. To explain charge migration route, whole photocatalytic mechanism was described in terms of energy band structures. Furthermore, the present work is helpful effort for design of new visible light photocatalytic materials with heterojunction structures.

Fe2O3 nanoparticles anchored on thermally oxidized MWCNTs as anode material for lithium-ion battery

Xiaoru Meng et al 2023 Nanotechnology 34 015602

Thermally oxidized MWCNTs (OMWCNTs) are fabricated by a thermal treatment of MWCNTs at 500 °C for 3 h in an oxygen-containing atmosphere. The oxygen content of OMWCNTs increases from 1.9 wt% for MWCNTs to 8.3 wt%. And the BET specific surface area of OMWCNTs enhances from 254.2 m2 g−1 for MWCNTs to 496.1 m2 g−1. The Fe2O3/OMWCNTs nanocomposite is prepared by a hydrothermal method. Electrochemical measurements show that Fe2O3/OMWCNTs still keeps a highly reversible specific capacity of 653.6 mA h g−1 after 200 cycles at 0.5 A g−1, which shows an obviously higher capacity than the sum of that of single Fe2O3 and OMWCNTs. The OMWCNTs not only buffer the volume changes of Fe2O3 nanoparticles but also provide high-speed electronic transmission channels in the charge–discharge process. The thermal oxidation method of OMWCNTs avoids using strong corrosive acids such as nitric acid and sulfuric acid, which has the advantages of safety, environmental protection, macroscopic preparation, etc.

Self-powered ultraviolet/visible photodetector based on graphene-oxide via triboelectric nanogenerators performing by finger tapping

Faezeh Ejehi et al 2022 Nanotechnology 33 475205

Self-sufficient power sources provide a promising application of abundant electronic devices utilized in detection of ambient properties. Recently, triboelectric nanogenerators (TENGs) have been widely investigated to broaden the self-powered systems by converting the ambient mechanical agitations into electrical voltage and current. Graphene oxide (GO), not only for sensing applications but also as a brilliant energy-related nanomaterial, provides a wide range of controllable bandgap energies, as well as facile synthesis route. In this study, GO-based self-powered photodetectors have been fabricated by conflating the photosensitivity and triboelectric characteristics of freestanding GO paper. In this regard, photodetection via TENGs has been investigated in two forms of active and passive circuits for ultraviolet (UV) and visible illumination. The photodetector responsivity upon UV enhanced from 0.011 mA W−1 for conventional GO-photoresistors up to 13.41 mA W−1 by active photodetection setup. Moreover, applying the active-TENG improved the efficiency from 0.25% (in passive TENG) to 4.21%. Our findings demonstrate that active TENGs might enable materials with insignificant optical response to represent considerably higher light-sensitivity by means of synergizing the effect of TENG output changes with opto-electronical properties of desired layers.

Interfacial engineering of 1D/2D heterostructured photoanode for efficient photoelectrochemical water splitting

Ziyu Wang et al 2022 Nanotechnology 33 495402

Solar-driven photoelectrochemical (PEC) water splitting for hydrogen generation is regarded as a sustainable strategy to relieve fossil resource issue. However, its PEC conversion efficiency still suffers from the low light absorption and high electron–hole recombination. Herein, we report 1D/2D hierarchical heterostructured photoelectrode constructed by ordered ZnO nanorod array and intimately attached ultra-thin Hematene (thickness of monolayer: 1–2 nm) for effective PEC water oxidation with visible light irradiation. The onset potential of Hematene/ZnO NRs photoanode (0.28 V versus RHE) for PEC water oxidation has an obvious negative shift compared with that of ZnO NRs (0.32 V versus RHE) indicating the enhanced PEC kinetics. Furthermore, reduced charge transport resistance (18.82 KΩ cm−2), a high carrier density of 9.03 × 1018 cm−3 and the resulting significantly enhanced incident photon-to-current efficiency enhancement compared with ZnO NRs photoanode were obtained for Hematene/ZnO NRs photoanode. All these were ascribed to the formation of large built-in electric field which was arising from the charge redistribution at the ZnO and Hematene interface, and the band alignment engineering between the components. In summary, such interfacial engineering may inspire the future development of 1D/2D hierarchical heterostructured photoanodes in the field of PEC water splitting.

Construction of a photo-controlled fluorescent switching with diarylethene modified carbon dots

Shiqi Liuye et al 2022 Nanotechnology 33 405705

Photo-controlled fluorescent switching is of great utility in fluorescence sensors, reversible data storage, and logic circuit, based on their modifiable emission intensity and spectra. In this work, a novel photo-controlled reversible fluorescent switching system was constructed based on photochromic diarylethene (DT) molecular modified fluorescent carbon dots (CDs). The fluorescent CDs acted as fluorescent donors and the photochromic diarylethene molecular functioned as acceptors in this fluorescent switching system. The fluorescence modulation efficiency of the fluorescent switching was determined to be 97.1%. The result was attributable to Förster resonance energy transfer between the CDs and the diarylethene molecular. The fluorescent switching could undergo 20 cycles without significant decay.

Doping Mn2+ in hybrid Ruddlesden–Popper phase of layered double perovskite (BA)4AgBiBr8

Priyesh Yadav et al 2022 Nanotechnology 33 415706

The layered hybrid double perovskites emerged as excellent semiconductor materials owing to their environment compatibility and stability. However, these materials are weakly luminescent, and their photoluminescence (PL) properties can be modulated via doping. While Mn2+ doping in perovskites is well known, but to the best of our knowledge the doping of Mn2+ in layered double perovskites (LDPs) is yet to be explored. Herein, for the first time, we demonstrate the doping of Mn2+ in hybrid inorganic-organic two-dimensional (2D) LDPs, (BA)4AgBiBr8 (BA = n-butyl amine) via a simple solid-state mechanochemical route. The powder x-ray diffraction pattern, and electron paramagnetic resonance analysis confirm the successful incorporation of Mn2+ ions inside (BA)4AgBiBr8 lattice. The Mn2+ doped 2D LDP shows energy transfer from host excitons to d-electrons of Mn2+ ions, which results in red-shifted broad Mn2+ emission band centered at 625 nm, attributed to the spin-forbidden4T1 to 6A1 internal transition. This work opens up new possibilities to dope metal ions in 2D LDPs to tune the optical as well as magnetic properties.

Open access
Phosphine free synthesis of copper telluride nanocrystals in 1D and 2D shapes using Dipehylditelluride (DPDTe) as an air-stable source

Mohini Mishra et al 2022 Nanotechnology 33 305602

In this paper, we have developed a ‘phosphine-free’ method for synthesising copper telluride nanocrystals using diphenyl ditelluride as an air-stable tellurium source. The diphenyl ditelluride is shown to have optimal reactivity for the colloidal synthesis of Cu2Te, allowing optimal control over the phase and morphology. Using this unexplored Te precursor for copper telluride synthesis, 1D nanorods of hexagonal phase (Cu2Te) were synthesised at a moderate temperature of 180 °C. The precise control over key parameters for this system results in Cu2−xTe nanocrystals forming with varied shapes (1D nanorods and 2D nanoplates), sizes, and crystal phases (hexagonal Cu2Te and orthorhombic Cu1.43Te).

V2O5/NaV6O15 nanocomposites synthesized by molten salt method as a high-performances cathode material for aqueous zinc-ion batteries

Yan Ran et al 2022 Nanotechnology 33 115402

Aqueous zinc-ion batteries (ZIBs) is a potential energy storage system due to its advantages of low cost, good safety, and high theoretical capacity (820 mAh g−1). However, the lack of cathode materials with long cycle stability severely restricts the development of ZIBs. In this paper, V2O5/ NaV6O15 nanocomposites are synthesized by molten salt method in one step and used as cathode material for ZIBs, which have good electrochemical performances. The specific capacity of the materials remain 160 mAh g−1 when the current density is 0.5 A g−1 after 1000 cycles, and the capacity retention rate is 102.03% when the current density is 5 A g−1 for 1000 cycles. This is mainly due to the large number of active sites generated by crystal defects and the synergistic interaction between the dual-phase materials, which reduces the stress of ions inserted/extracted during the Zn2+ storage process and improves the electrochemical performance.

High-pressure vapor-solid transformation of 2D template to derive 2D Co–N–C electrocatalysts for oxygen reduction reaction

Li Lin et al 2022 Nanotechnology 33 105601

Two-dimensional (2D) cobalt zeolitic imidazolate frameworks (ZIF-67) have attracted significant research interests to synthesize cobalt and nitrogen co-doped carbon-based (Co–N–C) catalyst for oxygen reduction reaction (ORR). However, most of the current synthetic approaches of 2D ZIF-67 are energy-intensive, environmentally hazardous and low-yield. Herein, a feasible and efficient ‘morphology-retaining method via a high-pressure vapor-solid reaction’ are reported to synthesize 2D ZIF-67 nanosheets by using 2D cobalt carbonate hydroxide template. In the strategy, the high-pressure vapor caused by sublimation of 2-Melm and the pores formed from effusion of CO2 during transformation ensure the complete transformation from 2D template to 2D ZIF-67. The corresponding 2D Co–N–C catalyst exhibits comparable ORR electrocatalytic activity and better stability than Pt/C in alkaline media. The present method is expected to offer a feasible and universal way to efficiently synthesize 2D M–N–C catalysts.

Flexible synthesis of high-performance electrode materials of N-doped carbon coating MnO nanowires for supercapacitors

Ting Zhou et al 2022 Nanotechnology 33 085602

The MnO/C composites were obtained by co-precipitation method, which used Mn3O4 nanomaterials as precursors and dopamine solution after ultrasonic mixing and calcination under N2 atmosphere at different temperatures. By studying the difference of MnO/C nanomaterials formed at different temperatures, it was found that with the increase of calcination temperature, the materials appear obvious agglomeration. The optimal calcination temperature is 400 °C, and the resulting MnO/C is a uniformly dispersed slender nanowire structure. The specific capacitance of MnO/C nanowires can reach 356 F g−1 at 1 A g−1. In the meantime, the initial capacitance of MnO/C nanowires remains 106% after 5000 cycles. Moreover, the asymmetric supercapacitor was installed, which displays a tremendous energy density of 30.944 Wh kg−1 along with a high power density of 10 kW kg−1. The composite material reveals a promising prospect in the application of supercapacitors.

In-situ sputtered 2D-MoS2 nanoworms reinforced with molybdenum nitride towards enhanced Na-ion based supercapacitive electrodes

Bhanu Ranjan et al 2021 Nanotechnology 32 455402

We report the fabrication of binder-free, low-cost and efficient hybrid supercapacitive electrode based on the hexagonal phase of two-dimensional MoS2 nanoworms reinforced with molybdenum nitride nanoflakes deposited on stainless steel (SS) substrate using reactive magnetron sputtering technique. The hybrid nanostructured MoS2–Mo2N/SS thin film working electrode delivers a high gravimetric capacitance (351.62 F g−1 at 0.25 mA cm−2) investigated in 1 M Na2SO4 aqueous solution. The physisorption/intercalation of sodium (Na+) ions in electroactive sites of MoS2–Mo2N composite ensures remarkable electrochemical performance. The deposited porous nanostructure with good electrical conductivity and better adhesion with the current collector demonstrates a high-energy density of 82.53 Wh kg−1 in addition to a high-power density of 24.98 kW kg−1. Further, excellent capacitance retention of 93.62% after 4000 galvanostatic charge–discharge cycles elucidated it as a promising candidate for realizing high-performance supercapacitor applications.

Efficiency improvement of P3CT-Na based MAPbI3 solar cells with a simple wetting process

Said Kassou et al 2021 Nanotechnology 32 345402

The averaged power conversion efficiency of polyelectrolytes (P3CT-Na) based MAPbI3 solar cells can be increased from 14.94% to 17.46% with a wetting method before the spin-coating process of MAPbI3 precursor solutions. The effects of the wetting process on the surface, structural, optical and excitonic properties of MAPbI3 thin films are investigated by using the atomic-force microscopic images, x-ray diffraction patterns, transmittance spectra, photoluminescence spectra and Raman scattering spectra. The experimental results show that the wetting process of MAPbI3 precursor solution on top of the P3CT-Na/ITO/glass substrate can be used to manipulate the molecular packing structure of the P3CT-Na thin film, which determines the formation of MAPbI3 thin films.

Suppressing ion migration of CsPbBrxI3-x nanocrystals by Nickel doping and the application in high-efficiency WLEDs

Supeng Yang et al 2021 Nanotechnology 32 335601

All inorganic perovskite nanocrystals CsPbX3(X = Cl, Br, I) are the great potential candidates for the application of high-performance light emitting diodes (LED) due to their high Photoluminescence Quantum Yield (PLQY), high defect tolerance, narrow full-width half-maximum and tunable wavelength of 410–700 nm. However, the application of red-emitting (630–650 nm) CsPbBrxI3-x nanocrystals are perplexed by phase segregation due to the composition of mixed halides and the difference in halide ion mobility. Herein, we provide an effective strategy to suppressing the migration of Br/I ions through Ni2+ doping via a facile Hot-Injection method and the PLQY was improved as well. DFT calculations show that the introduction of Ni2+ causes a slight contraction of the host crystal structure, which improves the bond energy between Pb and halides and reduces the level of surface defects. Therefore, the phase stability is improved by Ni2+ doping because the phase segregation caused by ion migration in the mixed phase is effectively inhibited. Meanwhile, the non-radiative recombination in the exciton transition process is reduced and the PLQY is improved. What’s more, benefiting from the suppressed ion migration and enhanced PLQY, we combine the Ni2+-doped CsPbBrxI3-x nanocrystals with different Br/I ratios and YAG: Ce3+ phosphors as color conversion layers to fabricate high efficiency WLED. When the ratio of Br/I is 9:11, WLED has a color coordinate of (0.3621, 0.3458), the color temperature of 4336 K and presents a high luminous efficiency of 113.20 lm W−1, color rendering index of 94.9 under the driving current of 20 mA and exhibits excellent stability, which shows great potential in the application of LED.

Improved lithium-ion battery performance by introducing oxygen-containing functional groups by plasma treatment

Xudong Zhang et al 2021 Nanotechnology 32 275401

Metal sulfides are often used as cathode materials for lithium-ion batteries (LIBs) owing to their high theoretical specific capacity; however, excessively fast capacity decay during charging/discharging and rapid shedding during cycling limits their practical application in batteries. In this study, we proposed a strategy using plasma treatment combined with the solvothermal method to prepare cobalt sulfide (Co1−xS)-carbon nanofibers (CNFs) composite. The plasma treatment could introduce oxygen-containing polar groups and defects, which could improve the hydrophilicity of the CNFs for the growth of the Co1−xS, thereby increasing the specific capacity of the composite electrode. The results show that the composite electrode present a high discharge specific capacity (839 mAh g−1 at a current density of 100 mA g−1) and good cycle stability (the capacity retention rate almost 100% at 2000 mA g−1 after 500 cycles), attributing to the high conductivity of the CNFs. This study proves the application of plasma treatment and simple vulcanization method in high-performance LIBs.

Investigation of plant leaf-derived graphene quantum dot clusters via magnetic force microscopy

Chiashain Chuang et al 2021 Nanotechnology 32 245704

Magnetic force microscopy (MFM) is utilized to characterize the magnetic moment in nanostructured plant leaf-derived graphene quantum dot clusters (GQDCs). The MFM signal reveals that the magnetic response of the GQDCs depends on the height and width of the GQDCs. However, individual GQDs, and smaller clusters with widths of less than 20 nm, have not shown any observable magnetic signal. Importantly, experimental analyses suggest that the magnetic signal of GQDCs distributed in a plane can be effectively detected at room temperature. These results could pave the way for future graphene-based magnetic storage media and spin manipulation quantum devices.

Photocatalytic activity and photoelectrochemical properties of Ag/ZnO core/shell nanorods under low-intensity white light irradiation

M J Kadhim et al 2021 Nanotechnology 32 195706

Zinc oxide (ZnO) nanorod thin films were prepared by CBD onto glass and FTO/glass substrates. Silver (Ag) nanoparticles were synthesized on the surface of the prepared ZnO nanorod thin films using electrochemical methods. The scanning electron microscopy images of the Ag/ZnO/glass core/shell nanostructure confirmed that the average particles size is 20 nm while it was 41 nm for Ag NPs that synthesized onto ZnO/FTO NRs. The photocatalytic activity of the prepared Ag/ZnO core/shell nanostructure was studied by analyzing the degradation of methylene blue (MB) dye under visible light. Various pH values (6 and 10) and exposure time (30–240) min were controlled to investigate the photocatalytic activity of as-prepared Ag/ZnO core/shell nanostructure and that annealed at 200 °C and 300 °C for 1 h. It was observed that when the pH was 6, the degradation rate increased with the annealing temperature and irradiation time reaching 51% at the annealing temperature of 300 °C and exposure time of 240 min. In other hands, when the pH was 10, and the sample was annealed at 200 °C, it showed a good degradation rate of 100% at the irradiation time of 90 min. By contrast, the sample annealed at 300 °C required 180 min to degrade the MB dye completely. The photoelectrochemical cell measurement based on photocurrent density revealed a slight response to light. Cycle voltammetry (CV) measurement was conducted, and the CV curves of the Ag/ZnO core/shell electrodes indicated nonfaradaic and pseudocapacitance behavior. The electrodes showed nearly rectangular CV curves, which indicated the dominance of the nonfaradaic capacitance behavior. The specific capacitance of the electrodes remained at approximately 99%. Mott–Schottky analysis revealed that the semiconductor was an n-type with dependence on flat band potential VFB deviation in the negative direction.

Deposition amount effects on the microstructure of ion-beam-sputtering grown Mn0.03Ge0.97 quantum dots for spintronic applications

Yahui Li et al 2021 Nanotechnology 32 140001

Here, a relative simpler and lower cost method, ion beam sputtering deposition was applied to fabricate diluted magnetic MnxGe1−x quantum dots (QDs). The effects of Ge–Mn co-deposition amount on the morphology and crystallization of Mn0.03Ge0.97 QDs were investigated systematically by employing the atomic force microscopy and Raman spectroscopy techniques. It can be seen that the morphology, density, and crystallinity of Mn0.03Ge0.97 QDs exhibit unique evolution processes with the increase of Ge–Mn co-sputtering amount. The optimal deposition amount for realizing well size-uniform, large-aspect-ratio, and high-density QDs is also determined. The unique evolution route of diluted magnetic semiconductor QDs and the amount of co-sputtering are also discussed sufficiently.