| 1. |
- Chareev, Dmitriy A., et al.
(author)
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Growth of Transition-Metal Dichalcogenides by Solvent Evaporation Technique
- 2020
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In: Crystal Growth & Design. - : American Chemical Society (ACS). - 1528-7483 .- 1528-7505. ; 20:10, s. 6930-6938
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Journal article (peer-reviewed)abstract
- Due to their physical properties and potential applications in energy conversion and storage, transition-metal dichalcogenides (TMDs) have garnered substantial interest in recent years. Among this class of materials, TMDs based on molybdenum, tungsten, sulfur, and selenium are particularly attractive due to their semiconducting properties and the availability of bottom-up synthesis techniques. Here we report a method which yields high-quality crystals of transition-metal diselenide and ditelluride compounds (PtTe2, PdTe2, NiTe2, TaTe2, TiTe2, RuTe2, PtSe2, PdSe2, NbSe2, TiSe2, VSe2, ReSe2) from their solid solutions, via vapor deposition from a metal-saturated chalcogen melt. Additionally, we show the synthesis of rare-earth-metal polychalcogenides and NbS2 crystals using the aforementioned process. Most of the crystals obtained have a layered CdI2 structure. We have investigated the physical properties of selected crystals and compared them to state of the art findings reported in the literature. Remarkably, the charge density wave transition in 1T-TiSe2 and 2H-NbSe2 crystals is well-defined at TCDW ≈ 200 and 33 K, respectively. Angle-resolved photoelectron spectroscopy and electron diffraction are used to directly access the electronic and crystal structures of PtTe2 single crystals and yield state of the art measurements.
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| 2. |
- Danilovich, I. L., et al.
(author)
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Co(NO3)(2) as an inverted umbrella-type chiral noncoplanar ferrimagnet
- 2020
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In: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 102:9
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Journal article (peer-reviewed)abstract
- The low-dimensional magnetic systems tend to reveal exotic spin-liquid ground states or form peculiar types of long-range order. Among systems of vivid interest are those characterized by the triangular motif in two dimensions. The realization of either ordered or disordered ground state in triangular, honeycomb, or kagome lattices is dictated by the competition of exchange interactions, also being sensitive to anisotropy and the spin value of magnetic ions. While the low-spin Heisenberg systems may arrive to a spin-liquid long-range entangled quantum state with emergent gauge structures, the high-spin Ising systems may establish the rigid noncollinear structures. Here, we present the case of chiral noncoplanar inverted umbrella-type ferrimagnet formed in cobalt nitrate Co(NO3)(2) below T-C = 3 K with the comparable spin and orbital contributions to the total magnetic moment.
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| 3. |
- Gao, Jiajia, et al.
(author)
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Electrochemical impedance and X-ray absorption spectroscopy analyses of degradation in dye-sensitized solar cells containing cobalt tris(bipyridine) redox shuttles
- 2022
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In: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 24:31, s. 18888-18895
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Journal article (peer-reviewed)abstract
- Electrochemical impedance spectroscopy (EIS) is a commonly used steady-state technique to examine the internal resistance of electron-transfer processes in solar cell devices, and the results are directly related to the photovoltaic performance. In this study, EIS was performed to study the effects of accelerated ageing, aiming for insights into the degradation mechanisms of dye-sensitized solar cells (DSSCs) containing cobalt tris(bipyridine) complexes as redox mediators. Control experiments based on aged electrolytes differing in concentrations of the redox couple components and cation co-additives were conducted to reveal the correlation of the cell degradation with external and internal properties. The failure modes of the cells emerged as changes in the kinetics of charge- and ion-transfer processes. An insufficient concentration of the redox complexes, in particular Co(iii), was found to be the main reason for the inferior performance after ageing. The related characterization of electrolytes aged outside the solar cell devices confirms the loss of active Co(iii) complexes in the device electrolytes. A new EIS feature at low frequencies emerged during ageing and was analysed. The new EIS feature demonstrates the presence of an unexpected rate-limiting, charge-transfer process in aged devices, which can be attributed to the TiO2/electrolyte interface. High-resolution fluorescence detected X-ray absorption spectroscopy (HERFD-XAS) was performed to identify the reduction of a part of Co(iii) to Co(II) after ageing, by investigating the Co K absorption edge. The HERFD-XAS data suggested a partial reduction of Co(iii) to Co(ii), accompanied by a difference in symmetry of the reduced species.
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| 4. |
- Ghosh, Anirudha, et al.
(author)
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Magnetic circular dichroism in the dd excitation in the van der Waals magnet CrI3 probed by resonant inelastic x-ray scattering
- 2023
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In: Physical Review B. - : American Physical Society (APS). - 2469-9950 .- 2469-9969. ; 107:11
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Journal article (peer-reviewed)abstract
- We report on a combined experimental and theoretical study on CrI3 single crystals by employing the polarization dependence of resonant inelastic x-ray scattering (RIXS). Our investigations reveal multiple Cr 3d orbital splitting (dd excitations) as well as magnetic dichroism (MD) in the RIXS spectra. The dd excitation energies are similar on the two sides of the ferromagnetic transition temperature, T-C similar to 61 K, although MD in RIXS is predominant at 0.4 T magnetic field below TC. This demonstrates that the ferromagnetic superexchange interaction that is responsible for the interatomic exchange field is vanishingly small compared with the local exchange field that comes from exchange and correlation interaction among the interacting Cr 3d orbitals. The recorded RIXS spectra reported here reveal clearly resolved Cr 3d intraorbital dd excitations that represent transitions between electronic levels that are heavily influenced by dynamic correlations and multiconfiguration effects. Our calculations taking into account the Cr 3d hybridization with the ligand valence states and the full multiplet structure due to intra-atomic and crystal field interactions in Oh and D3d symmetry clearly reproduced the dichroic trend in experimental RIXS spectra.
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| 5. |
- Grubisic-Cabo, Antonija, et al.
(author)
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In Situ Exfoliation Method of Large-Area 2D Materials
- 2023
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In: Advanced Science. - : Wiley. - 2198-3844. ; 10:22
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Journal article (peer-reviewed)abstract
- 2D materials provide a rich platform to study novel physical phenomena arising from quantum confinement of charge carriers. Many of these phenomena are discovered by surface sensitive techniques, such as photoemission spectroscopy, that work in ultra-high vacuum (UHV). Success in experimental studies of 2D materials, however, inherently relies on producing adsorbate-free, large-area, high-quality samples. The method that yields 2D materials of highest quality is mechanical exfoliation from bulk-grown samples. However, as this technique is traditionally performed in a dedicated environment, the transfer of samples into vacuum requires surface cleaning that might diminish the quality of the samples. In this article, a simple method for in situ exfoliation directly in UHV is reported, which yields large-area, single-layered films. Multiple metallic and semiconducting transition metal dichalcogenides are exfoliated in situ onto Au, Ag, and Ge. The exfoliated flakes are found to be of sub-millimeter size with excellent crystallinity and purity, as supported by angle-resolved photoemission spectroscopy, atomic force microscopy, and low-energy electron diffraction. The approach is well-suited for air-sensitive 2D materials, enabling the study of a new suite of electronic properties. In addition, the exfoliation of surface alloys and the possibility of controlling the substrate-2D material twist angle is demonstrated.
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| 6. |
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| 7. |
- Jain, Sagar M., et al.
(author)
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An effective approach of vapour assisted morphological tailoring for reducing metal defect sites in lead-free, (CH3NH3)(3)Bi2I9 bismuth-based perovskite solar cells for improved performance and long-term stability
- 2018
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In: Nano Energy. - : ELSEVIER SCIENCE BV. - 2211-2855 .- 2211-3282. ; 49, s. 614-624
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Journal article (peer-reviewed)abstract
- We present a controlled, stepwise formation of methylammonium bismuth iodide (CH3NH3)(3)Bi2I9 perovskite films prepared via the vapour assisted solution process (VASP) by exposing BiI3 films to CH3NH3I (MAI) vapours for different reaction times, (CH3NH3)(3)Bi2I9 semiconductor films with tunable optoelectronic properties are obtained. Solar cells prepared on mesoporous TiO2 substrates yielded hysteresis-free efficiencies upto 3.17% with good reproducibility. The good performance is attributed mainly to the homogeneous surface coverage, improved stoichiometry, reduced metallic content in the bulk, and desired optoelectronic properties of the absorbing material. In addition, solar cells prepared using pure BiI3 films without MAI exposure achieved a power conversion efficiency of 0.34%. The non-encapsulated (CH3NH3)(3)Bi2I9 devices were found to be stable for as long as 60 days with only 0.1% drop in efficiency. This controlled formation of (CH3NH3)(3)Bi2I9 perovskite films highlights the benefit of the VASP technique to optimize material stoichiometry, morphology, solar cell performance, and long-term durability.
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| 8. |
- Jana, Somnath, et al.
(author)
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Atom-specific magnon driven ultrafast spin dynamics in Fe1-xNix alloys
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Other publication (other academic/artistic)abstract
- By employing element specific ultrafast spectroscopy in Fe1-xNix alloys alloys, we find a composition dependent effect in the demagnetization that we relate to changes in electron-magnon scattering. In all six measured alloys of different composition, the demagnetization of Ni compared to Fe exhibits a delay, an effect which we find is inherent in alloys but not in elemental Fe and Ni. Using a model based on electron-magnon scattering, we extract a spin-wave stiffness from all alloys that show excellent agreement with values obtained from other techniques. The result establishes the atom-specific sd-exchange induced magnon generation as an underlying mechanism during ultrafast demagnetization in Fe1-xNix alloys
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| 9. |
- Jana, Somnath, et al.
(author)
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Atom-specific magnon-driven ultrafast spin dynamics in Fe1-xNix alloys
- 2023
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In: Physical Review B. - : American Physical Society (APS). - 2469-9950 .- 2469-9969. ; 107:18
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Journal article (peer-reviewed)abstract
- By employing element-specific spectroscopy in the ultrafast time scale in Fe1-xNix alloys, we find a composition-dependent effect in the demagnetization that we relate to electron-magnon scattering and changes in the spin-wave stiffness. In all six measured alloys of different composition, the demagnetization of Ni compared to Fe exhibits a delay, an effect which we find is inherent in alloys but not in elemental Fe and Ni. Using a model based on electron-magnon scattering, we extract a spin-wave stiffness from all alloys that show excellent agreement with values obtained from other techniques.
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| 10. |
- Jana, Somnath, et al.
(author)
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Charge disproportionate antiferromagnetism at the verge of the insulator-metal transition in doped LaFeO3
- 2019
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In: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 99:7
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Journal article (peer-reviewed)abstract
- We explore the effects of electron doping in lanthanum ferrite, LaFeO3 by doping Mo at the Fe sites. Based on magnetic, transport, scanning tunneling spectroscopy, and x-ray photoelectron spectroscopy measurements, we find that the large gap, charge-transfer, antiferromagnetic (AFM) insulator LaFeO3 becomes a small gap AFM band insulator at low Mo doping. With increasing doping concentration, Mo states, which appear around the Fermi level, is broadened and become gapless at a critical doping of 20%. Using a combination of calculations based on density functional theory plus Hubbard U (DFT+U) and x-ray absorption spectroscopy measurements, we find that the system shows charge disproportionation (CD) in Fe ions at 25% Mo doping, where two distinct Fe sites, having Fe2+ and Fe3+ nominal charge states appear. A local breathing-type lattice distortion induces the charge disproportionation at the Fe site without destroying the antiferromagnetic order. Our combined experimental and theoretical investigations establish that the Fe states form a CD antiferromagnet at 25% Mo doping, which remains insulating, while the appearance of Mo states around the Fermi level is showing an indication towards the insulator-metal transition.
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