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1. Cascade synthesis and optoelectronic applications of intermediate bandgap Cu3VSe4 nanosheets

   https://doi.org/10.1038/s41598-020-78649-9  

   Liu, Mimi ; Lai, Cheng-Yu ; Zhang, Meng ; Radu, Daniela R. ( December 2020 , Scientific Reports)

   Two-dimensional (2D) ternary materials recently generated interest in optoelectronics and energy-related applications, alongside their binary counterparts. To date, only a few naturally occurring layered 2D ternary materials have been explored. The plethora of benefits owed to reduced dimensionality prompted exploration of expanding non-layered ternary chalcogenides into the 2D realm. This work presents a templating method that uses 2D transition metal dichalcogenides as initiators to be converted into the corresponding ternary chalcogenide upon addition of copper, via a solution-phase synthesis, conducted in high boiling point solvents. The process starts with preparation of VSe₂nanosheets, which are next converted into Cu₃VSe₄sulvanite nanosheets (NSs) which retain the 2D geometry while presenting an X-ray diffraction pattern identical with the one for the bulk Cu₃VSe₄. Both the scanning electron microscopy and transmission microscopy electron microscopy show the presence of quasi-2D morphology. Recent studies of the sulfur-containing sulvanite Cu₃VS₄highlight the presence of an intermediate bandgap, associated with enhanced photovoltaic (PV) performance. The Cu₃VSe₄nanosheets reported herein exhibit multiple UV–Vis absorption peaks, related to the intermediate bandgaps similar to Cu₃VS₄and Cu₃VSe₄nanocrystals. To test the potential of Cu₃VSe₄NSs as an absorber for solar photovoltaic devices, Cu₃VSe₄NSs thin-films deposited on FTO were subjected to photoelectrochemical testing, showing p-type behavior and stable photocurrents of up to ~ 0.036 mA/cm². The photocurrent shows a ninefold increase in comparison to reported performance of Cu₃VSe₄nanocrystals. This proves that quasi-2D sulvanite nanosheets are amenable to thin-film deposition and could show superior PV performance in comparison to nanocrystal thin-films. The obtained electrical impedance spectroscopy signal of the Cu₃VSe₄ NSs-FTO based electrochemical cell fits an equivalent circuit with the circuit elements of solution resistance (R_s), charge-transfer resistance (R_ct), double-layer capacitance (C_dl), and Warburg impedance (W). The estimated charge transfer resistance value of 300 Ω cm²obtained from the Nyquist plot provides an insight into the rate of charge transfer on the electrode/electrolyte interface.

    

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2. Oxygen‐Induced Structural Disruption for Improved Li + Transport and Electrochemical Stability of Li 3 PS 4

   https://doi.org/10.1002/aenm.202302785  

   Deck, Michael J. ; Chien, Po‐Hsiu ; Poudel, Tej P. ; Jin, Yongkang ; Liu, Haoyu ; Hu, Yan‐Yan ( December 2023 , Advanced Energy Materials)

   The performance of all‐solid‐state batteries (ASSBs) relies on the Li⁺transport and stability characteristics of solid electrolytes (SEs). Li₃PS₄is notable for its stability against lithium metal, yet its ionic conductivity remains a limiting factor. This study leverages local structural disorder via O substitution to achieve an ionic conductivity of 1.38 mS cm⁻¹with an activation energy of 0.34 eV for Li₃PS_4−xO_x(x = 0.31). Optimal O substitution transforms Li⁺transport from 2D to 3D pathways with increased ion mobility. Li₃PS_3.69O_0.31exhibits improvements in the critical current density and stability against Li metal and retains its electrochemical stability window compared with Li₃PS₄. The practical implementation of Li₃PS_3.69O_0.31in ASSBs half‐cells, particularly when coupled with TiS₂as the cathode active material, demonstrates substantially enhanced capacity and rate performance. This work elucidates the utility of introducing local structural disorder to ameliorate SE properties and highlights the benefits of strategically combining the inherent strengths of sulfides and oxides via creating oxysulfide SEs.

    

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3. Monolayer Superconductivity and Tunable Topological Electronic Structure at the Fe(Te,Se)/Bi 2 Te 3 Interface

   https://doi.org/10.1002/adma.202210940  

   Moore, Robert G. ; Lu, Qiangsheng ; Jeon, Hoyeon ; Yao, Xiong ; Smith, Tyler ; Pai, Yun‐Yi ; Chilcote, Michael ; Miao, Hu ; Okamoto, Satoshi ; Li, An‐Ping ; et al ( April 2023 , Advanced Materials)

   The interface between 2D topological Dirac states and ans‐wave superconductor is expected to support Majorana‐bound states (MBS) that can be used for quantum computing applications. Realizing these novel states of matter and their applications requires control over superconductivity and spin‐orbit coupling to achieve spin‐momentum‐locked topological interface states (TIS) which are simultaneously superconducting. While signatures of MBS have been observed in the magnetic vortex cores of bulk FeTe_0.55Se_0.45, inhomogeneity and disorder from doping make these signatures unclear and inconsistent between vortices. Here superconductivity is reported in monolayer (ML) FeTe_1–ySe_y(Fe(Te,Se)) grown on Bi₂Te₃by molecular beam epitaxy (MBE). Spin and angle‐resolved photoemission spectroscopy (SARPES) directly resolve the interfacial spin and electronic structure of Fe(Te,Se)/Bi₂Te₃heterostructures. Fory = 0.25, the Fe(Te,Se) electronic structure is found to overlap with the Bi₂Te₃TIS and the desired spin‐momentum locking is not observed. In contrast, fory = 0.1, reduced inhomogeneity measured by scanning tunneling microscopy (STM) and a smaller Fe(Te,Se) Fermi surface with clear spin‐momentum locking in the topological states are found. Hence, it is demonstrated that the Fe(Te,Se)/Bi₂Te₃system is a highly tunable platform for realizing MBS where reduced doping can improve characteristics important for Majorana interrogation and potential applications.

    

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4. Mid‐ to Far‐Infrared Anisotropic Dielectric Function of HfS 2 and HfSe 2

   https://doi.org/10.1002/adom.202200933  

   Kowalski, Ryan A. ; Nolen, Joshua Ryan ; Varnavides, Georgios ; Silva, Sebastian Mika ; Allen, Jack E. ; Ciccarino, Christopher J. ; Juraschek, Dominik M. ; Law, Stephanie ; Narang, Prineha ; Caldwell, Joshua D. ( September 2022 , Advanced Optical Materials)

   The far‐infrared (far‐IR) remains a relatively underexplored region of the electromagnetic spectrum extending roughly from 20 to 100 µm in free‐space wavelength. Research within this range has been restricted due to a lack of optical materials that can be optimized to reduce losses and increase sensitivity, as well as by the long free‐space wavelengths associated with this spectral region. Here the exceptionally broad Reststrahlen bands of two Hf‐based transition metal dichalcogenides (TMDs) that can support surface phonon polaritons (SPhPs) within the mid‐infrared (mid‐IR) into the terahertz (THz) are reported. In this vein, the IR transmission and reflectance spectra of hafnium disulfide (HfS₂) and hafnium diselenide (HfSe₂) flakes are measured and their corresponding dielectric functions are extracted. These exceptionally broad Reststrahlen bands (HfS₂: 165 cm⁻¹; HfSe₂: 95 cm⁻¹) dramatically exceed that of the more commonly explored molybdenum‐ (Mo) and tungsten‐ (W) based TMDs (≈5–10 cm⁻¹), which results from the over sevenfold increase in the Born effective charge of the Hf‐containing compounds. This work therefore identifies a class of materials for nanophotonic and sensing applications in the mid‐ to far‐IR, such as deeply sub‐diffractional hyperbolic and polaritonic optical antennas, as is predicted via electromagnetic simulations using the extracted dielectric function.

    

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5. Anisotropic Properties of Quasi‐1D In 4 Se 3 : Mechanical Exfoliation, Electronic Transport, and Polarization‐Dependent Photoresponse

   https://doi.org/10.1002/adfm.202106459  

   Vorobeva, Nataliia S. ; Lipatov, Alexey ; Torres, Angel ; Dai, Jun ; Abourahma, Jehad ; Le, Duy ; Dhingra, Archit ; Gilbert, Simeon J. ; Galiy, Pavlo V. ; Nenchuk, Taras M. ; et al ( September 2021 , Advanced Functional Materials)

   Theoretical and experimental investigations of various exfoliated samples taken from layered In₄Se₃crystals are performed. In spite of the ionic character of interlayer interactions in In₄Se₃and hence much higher calculated cleavage energies compared to graphite, it is possible to produce few‐nanometer‐thick flakes of In₄Se₃by mechanical exfoliation of its bulk crystals. The In₄Se₃flakes exfoliated on Si/SiO₂have anisotropic electronic properties and exhibit field‐effect electron mobilities of about 50 cm² V⁻¹ s⁻¹at room temperature, which are comparable with other popular transition metal chalcogenide (TMC) electronic materials, such as MoS₂and TiS₃. In₄Se₃devices exhibit a visible range photoresponse on a timescale of less than 30 ms. The photoresponse depends on the polarization of the excitation light consistent with symmetry‐dependent band structure calculations for the most expectedaccleavage plane. These results demonstrate that mechanical exfoliation of layered ionic In₄Se₃crystals is possible, while the fast anisotropic photoresponse makes In₄Se₃a competitive electronic material, in the TMC family, for emerging optoelectronic device applications.

    

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