Strain-shear coupling in bilayer MoS2

Layered materials such as graphite and transition metal dichalcogenides have extremely anisotropic mechanical properties owing to orders of magnitude difference between in-plane and out-of-plane interatomic interaction strengths. Although effects of mechanical perturbations on either intra- or inter-layer interactions have been extensively investigated, mutual correlations between them have rarely been addressed. Here we show that layered materials have an inevitable coupling between in-plane uniaxial strain and interlayer shear. Because of this, the uniaxial in-plane strain induces an anomalous splitting of the degenerate interlayer shear phonon modes such that the split shear mode along the tensile strain is not softened but hardened contrary to the case of intralayer phonon modes. We confirm the effect by measuring Raman shifts of shear modes of bilayer MoS2 under strain. Moreover, by analyzing the splitting, we obtain an unexplored off-diagonal elastic constant, demonstrating that Raman spectroscopy can determine almost all mechanical constants of layered materials.Comment: 36 pages, 10 figure

Rapid suppression of quantum many-body magnetic exciton in doped van der Waals antiferromagnet (Ni,Cd)PS3

The unique discovery of magnetic exciton in van der Waals antiferromagnet NiPS3 arises between two quantum many-body states of a Zhang-Rice singlet excited state and a Zhang-Rice triplet ground state. Simultaneously, the spectral width of photoluminescence originating from this exciton is exceedingly narrow as 0.4 meV. These extraordinary properties, including the extreme coherence of the magnetic exciton in NiPS3, beg many questions. We studied doping effects using Ni1-xCdxPS3 using two experimental techniques and theoretical studies. Our experimental results show that the magnetic exciton is drastically suppressed upon a few % Cd doping. All these happen while the width of the exciton only gradually increases, and the antiferromagnetic ground state is robust. These results highlight the lattice uniformity's hidden importance as a prerequisite for coherent magnetic exciton. Finally, an exciting scenario emerges: the broken charge transfer forbids the otherwise uniform formation of the coherent magnetic exciton in (Ni,Cd)PS3.Comment: 40 pages, 4 main figures, 13 supporting figures, accepted by Nano Letter

Negative Thermal Expansion Coefficient of Graphene Measured by Raman Spectroscopy

The thermal expansion coefficient (TEC) of single-layer graphene is estimated with temperature-dependent Raman spectroscopy in the temperature range between 200 and 400 K. It is found to be strongly dependent on temperature but remains negative in the whole temperature range, with a room temperature value of -8.0x10^{-6} K^{-1}. The strain caused by the TEC mismatch between graphene and the substrate plays a crucial role in determining the physical properties of graphene, and hence its effect must be accounted for in the interpretation of experimental data taken at cryogenic or elevated temperatures.Comment: 17 pagese, 3 figures, and supporting information (4 pages, 3 figures); Nano Letters, 201

Optical Detection of SnSe2 Formation on CZTSSe Thin-Film Solar Cells

Cu2ZnSn(S1-xSex)4 (CZTSSe) is a promising candidate for the absorber layer of low-cost thin-film solar cells, thanks to the advantage of using earth-abundant, non-toxic elements. However, since the stable phase region of CZTSSe is very narrow, secondary phases are easily formed during the thinfilm deposition or the post-deposition treatments, and some of the secondary phases are detrimental to the solar conversion efficiency. In this work, we investigated the influence of the SnSe2 secondary phase to the performance of a solar cell using laser-beam-induced current (LBIC) measurements and resonance Raman spectroscopy. We found that the SnSe2 secondary phase has a critical impact on the characteristics of the solar cell even if the amount of the secondary phase is so little that it can be detected only with a resonant excitation source. We established that the points with the SnSe2 secondary phase Raman signal had a lower photocurrent. From macro-scale resonance Raman measurements, we show that the existence of the SnSe2 secondary phase directly correlated with the lower efficiency of a cell. Therefore, we conclude that controlling the formation of the SnSe2 secondary phase is a crucial factor to obtain CZTSSe solar cells with high efficiencies. © 2022 American Chemical Society.FALS

Solution-processed Cu2ZnSnS4 absorbers prepared by appropriate inclusion and removal of thiourea for thin film solar cells

We studied how to effectively add/remove organic chemicals to/from CZTS precursor thin films to prepare uniform CZTS thin films that show optimal properties. We used multi-functional thiourea, as both a stabiliser and a source of sulphur, to prepare the precursor solutions. This is because it forms complexes with metal chlorides, which stabilise the CZTS precursor solutions and enable CZTS thin films to be spin-coated onto substrates thereby enabling fabrication of CZTS absorbers. However, the excess thiourea, required to stabilise the CZTS precursor solutions, induced the formation of a ZnS secondary phase in the CZTS thin films, which deteriorated the photovoltaic properties of the CZTS solar cells. We therefore pre-annealed the thin films to inhibit ZnS formation. We used the thiourea-stabilized CZTS precursor solutions and simple solution processing techniques to prepare CZTS precursor thin films, and optimized the pre-annealing temperature to fabricate CZTS solar cells that showed 5.29% efficiency. © 2014 The Royal Society of Chemistry.FALS

Effects of S and Se contents on the physical and photovoltaic properties of Cu2ZnSn(S-X, Se1-X)(4) thin films: achieving a PCE of 9.47%

CZTSSe absorbers are synthesized by a one-step annealing process from Cu, SnS and ZnS stacks prepared by sputtering deposition. CZTSSe thin films are fabricated by a selenization process using an optimized precursor stack structure. The selenization temperature has a strong influence on the phase and reactions of the elements in the films. CZTSSe formation is initially triggered by the interaction of Cu with Sn(S, Se) to form CuSn(S, Se) compounds, which then react with ZnS. CZTSSe films obtained at 590 °C exhibit a kesterite structure. Sulfo-selenization is performed using an optimized selenization process. Based on the mass ratio of the chalcogen sources, selenium disulfide and selenium, the effect of the S/(S + Se) compositional ratio on the structural and morphological properties of the as-grown films and the optoelectronic parameters of solar cells fabricated using these absorber films are studied. Using this single-step sulfo-selenization method, CZTSSe devices with conversion efficiencies up to 9.47% are obtained. This journal is © The Royal Society of Chemistry.1

Large scale production of highly conductive reduced graphene oxide sheets by a solvent-free low temperature reduction

A novel one-pot process that can produce freestanding reduced graphene oxide (RGO) sheets in large scale through a mechanochemical method is presented, which is based on a 1:1 adduct of hydrazine and carbon dioxide (H_3N^+NHCO_2^−, solid hydrazine). We were able to synthesize RGO sheets by grinding solid hydrazine with graphene oxide (GO), followed by storing the mixed powder at 50 °C for 10 min. No solvents, nor large vessels, nor post-annealing at high temperatures are required. The resulting RGO sample was characterized by elemental analysis, X-ray diffraction, X-ray photoelectron spectroscopy, Raman spectroscopy, Brunauer–Emmett–Teller measurement, thermo gravimetric analysis, Fourier transform infrared spectroscopy, solid state nuclear magnetic resonance spectroscopy, and conductivity measurement. It exhibits excellent conductivity and possesses a high specific surface area. This reduction method was successfully applied for the fabrication of inkjet-printed RGO devices on a flexible substrate