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Two-dimensional (2D) van der Waals (vdW) materials with lower symmetry (triclinic, monoclinic or orthorhombic) exhibit intrinsic anisotropic in-plane structure desirable for future optoelectronic surface operating devices. Herein, we report one such material, 2D $p$-type semiconductor germanium sulfide (GeS), a group IV monochalcogenide with puckered orthorhombic morphology, in which in-plane optical and transport properties can be correlated with its electronic structure. We systematically investigate the electronic band structure of the bulk GeS with micro-focused angle-resolved photoemission spectroscopy ($\mu$-ARPES) and correspond the charge transport properties using the field-effect transistor (FET) device architecture, and optical anisotropy $via$ angle-resolved polarization dependent Raman spectroscopy (ARPRS) on a micron-sized rectangle-shaped exfoliated bulk flake. The experimental valence band dispersion along the two high symmetry directions indicate highly anisotropic in-plane behavior of the charge carrier that agrees well with the density functional theory (DFT) calculations. In addition, we demonstrate the variation of the in-plane hole mobility (ratio $\sim$ 3.4) from the electrical conductivity with gate-sweep in a GeS-on-SiO$_2$ FET. Moreover, we use the angle-resolved fluctuation of the Raman intensity of the characteristic phonon modes to precisely determine the armchair and zigzag edges of the particular flake. The unique structural motif of GeS with correlated electronic and optical properties are of great interest both for the physical understanding of the all-optical switch and their applications in memory devices.

Structural phase transition can occur due to complex mechanisms other than simple dynamical instability, especially when the parent and daughter structure is of low dimension. This article reports such an inversion symmetry-breaking structural phase transition in a quasi-1D compound (TaSe$_4$)$_3$I at T$_S\sim$ 141~K studied by Raman spectroscopy. Our investigation of collective lattice dynamics reveals three additional Raman active modes in the low-temperature non-centrosymmetric structure. Two vibrational modes become Raman active due to the absence of an inversion center, while the third mode is a soft phonon mode resulting from the vibration of Ta atoms along the \{-Ta-Ta-\} chains. Furthermore, the most intense Raman mode display Fano-shaped asymmetry, inferred as the signature of strong electron-phonon coupling. The group theory and symmetry analysis of Raman spectra confirm the displacive-first-order nature of the structural transition. Therefore, our results establish (TaSe$_4)_3$I as a model system with broken inversion symmetry and strong electron-phonon coupling in the quasi-1D regime., Comment: Main text - 6 figures, 11 pages, supplementary - 10 figures, 13 pages

Manipulation of long-range order in two-dimensional (2D) van der Waals (vdW) magnetic materials (e.g., CrI$_3$, CrSiTe$_3$ etc.), exfoliated in few-atomic layer, can be achieved via application of electric field, mechanical-constraint, interface engineering, or even by chemical substitution/doping. Usually, active surface oxidation due to the exposure in the ambient condition and hydrolysis in the presence of water/moisture causes degradation in magnetic nanosheets which, in turn, affects the nanoelectronic/spintronic device performance. Counterintuitively, our current study reveals that exposure to the air at ambient atmosphere results in advent of a stable nonlayered secondary ferromagnetic phase in the form of Cr$_2$Te$_3$ (T$_{C2}$ ~ 160 K) in the parent vdW magnetic semiconductor Cr$_2$Ge$_2$Te$_6$ (T$_{C1}$ ~ 69 K). In addition, the magnetic anisotropy energy (MAE) enhances in the hybrid by an order from the weakly anisotropic pristine Cr$_2$Ge$_2$Te$_6$ crystal, increasing the stability of the FM ground state with time. Comparing with the freshly prepared Cr$_2$Ge$_2$Te$_6$, the coexistence of the two ferromagnetic phases in the time elapsed bulk crystal is confirmed through systematic investigation of crystal structure along with detailed dc/ac magnetic susceptibility, specific heat, and magnetotransport measurement. To capture the concurrence of the two ferromagnetic phases in a single material, Ginzburg-Landau theory with two independent order parameters (as magnetization) with a coupling term can be introduced. In contrast to rather common poor environmental stability of the vdW magnets, our results open possibilities of finding air-stable novel materials having multiple magnetic phases.

In two-dimensional (2D) van der Waals (vdW) layered materials the application of pressure often induces a giant lattice collapse, which can subsequently drive an associated Mott transition. Here, we investigate room-temperature layer-dependent insulator-metal transition (IMT) and probable spin-crossover (SCO) in vdW magnet, FePS$_3$, under high-pressure using micro-Raman scattering. Experimentally obtained spectra, in agreement with the computed Raman modes, indicate evidence of IMT of FePS$_3$ started with a thickness-dependent critical pressure ($P_c$) which reduces to 1.5 GPa in trilayer flakes compared to 10.8 GPa for the bulk counterpart. Using a phenomenological model, we argue that strong structural anisotropy in few-layer flakes enhances the in-plane strain under applied pressure and is, therefore, ultimately responsible for reducing the critical pressure for the IMT with decreasing layer numbers. Reduction of the critical pressure for phase transition in vdW magnets to 1-2 GPa marks the possibility of using intercalated few-layers in the field-effect transistor device architecture, and thereby, avoiding the conventional use of the diamond anvil cell (DAC)., Comment: Accepted in Physical Review B

Tuning the ambipolar behavior in charge carrier transport via defect-engineering is crucial for achieving high mobility transistors for nonlinear logic circuits. Here, we present the electric-field tunable electron and hole transport in a microchannel device consisting of highly air-stable van der Waals (vdW) noble metal dichalcogenide (NMDC), PdSe$_\mathrm{2}$, as an active layer. Pristine bulk PdSe$_\mathrm{2}$ constitutes Se surface vacancy defects created during the growth or exfoliation process and offers an ambipolar transfer characteristics with a slight electron dominance recorded in field-effect transistor (FET) characteristics showing an ON/OFF ratio < 10 and electron mobility ~ 21 cm$^2$/V.s. However, transfer characteristics of PdSe$_\mathrm{2}$ can be tuned to a hole-dominated transport while using hydrochloric acid (HCl) as a $p$-type dopant. On the other hand, the chelating agent EDTA, being a strong electron donor, enhances the electron-dominance in PdSe$_\mathrm{2}$ channel. In addition, $p$-type behavior with a 100 times higher ON/OFF ratio is obtained while cooling the sample down to 10 K. Low-temperature angle-resolved photoemission spectroscopy resembles the $p$-type band structure of PdSe$_\mathrm{2}$ single crystal. Also, first principle density functional theory calculations justify the tunability observed in PdSe$_\mathrm{2}$ as a result of defect-engineering. Such a defect-sensitive ambipolar vdW architecture may open up new possibilities towards future CMOS (Complementary Metal-Oxide-Semiconductor) device fabrications and high performance integrated circuits.

Induced magnetic order in a topological insulator (TI) can be realized either by depositing magnetic adatoms on the surface of a TI or engineering the interface with epitaxial thin film or stacked assembly of two-dimensional (2D) van der Waals (vdW) materials. Herein, we report the observation of spin-phonon coupling in the otherwise non-magnetic TI Bi$_\mathrm{2}$Te$_\mathrm{3}$, due to the proximity of FePS$_\mathrm{3}$ (an antiferromagnet (AFM), $T_\mathrm{N}$ $\sim$ 120 K), in a vdW heterostructure framework. Temperature-dependent Raman spectroscopic studies reveal deviation from the usual phonon anharmonicity originated from spin-lattice coupling at the Bi$_{2}$Te$_{3}$/FePS$_{3}$ interface at/below 60 K in the peak position (self-energy) and linewidth (lifetime) of the characteristic phonon modes of Bi$_{2}$Te$_{3}$ (106 cm$^{-1}$ and 138 cm$^{-1}$) in the stacked heterostructure. The Ginzburg-Landau (GL) formalism, where the respective phonon frequencies of Bi$_{2}$Te$_{3}$ couple to phonons of similar frequencies of FePS$_{3}$ in the AFM phase, has been adopted to understand the origin of the hybrid magneto-elastic modes. At the same time, the reduction of characteristic $T_\mathrm{N}$ of FePS$_3$ from 120 K in isolated flakes to 65 K in the heterostructure, possibly due to the interfacial strain, which leads to smaller Fe-S-Fe bond angles as corroborated by computational studies using density functional theory (DFT). Besides, inserting hexagonal boron nitride within Bi$_{2}$Te$_{3}$/FePS$_{3}$ stacking regains the anharmonicity in Bi$_{2}$Te$_{3}$. Controlling interfacial spin-phonon coupling in stacked heterostructure can have potential application in surface code spin logic devices., Comment: Accepted in Advanced Functional Materials

One-dimensional (1D) van der Waals (vdW) materials offer nearly defect-free strands as channel material in the field-effect transistor (FET) devices and probably, a better interconnect than conventional copper with higher current density and resistance to electro-migration with sustainable down-scaling. We report a new halide based "truly" 1D few-chain atomic thread, PdBr$_2$, isolable from its bulk which crystallizes in a monoclinic space group C2/c. Liquid phase exfoliated nanowires with mean length (20$\pm$1)$\mu$m transferred onto SiO$_2$/Si wafer with a maximum aspect ratio of 5000 confirms the lower cleavage energy perpendicular to chain direction. Moreover, an isolated nanowire can also sustain current density of 200 MA/cm$^\mathrm{2}$ which is atleast one-order higher than typical copper interconnects. However, local transport measurement via conducting atomic force microscopy (CAFM) tip along the cross direction of the single chain records a much lower current density due to the anisotropic electronic band structure. While 1D nature of the nanoobject can be linked with non-trivial collective quantum behavior, vdW nature could be beneficial for the new pathways in interconnect fabrication strategy with better control of placement in an integrated circuit (IC).