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Magnetodielectric (MD) materials are important for their ability to spin-charge conversion, magnetic field control of electric polarization and vice versa. Among these, two-dimensional (2D) van der Waals (vdW) magnetic materials are of particular interest due to the presence of magnetic anisotropy (MA) originating from the interaction between the magnetic moments and the crystal field. Also, these materials indicate a high degree of stability in the long-range spin order and may be described using suitable spin Hamiltonians of the Heisenberg, XY, or Ising type. Recent reports have suggested effective interactions between magnetization and electric polarization in 2D magnets. However, MD coupling studies on layered magnetic materials are still few. This review covers the fundamentals of magnetodielectric coupling by explaining related key terms. It includes the necessary conditions for having this coupling and sheds light on the possible physical mechanisms behind this coupling starting from phenomenological descriptions. Apart from that, this review classifies 2D magnetic materials into several categories for reaching out each and every class of materials. Additionally, this review summarizes recent advancements of some pioneer 2D magnetodielectric materials. Last but not the least, the current review provides possible research directions for enhancing magnetodielectric coupling in those and mentions the possibilities for future developments., Comment: 19 pages, 8 figures

We investigate the pressure-driven structural and electronic evolution of PdSe\(_2\) using powder X-ray diffraction, Raman spectroscopy, and first-principles calculations. Beyond 2.3 GPa, suppression of the Jahn-Teller distortion induces in-plane lattice expansion and metallization. Around 4.8 GPa, the interlayer \(d_{z^2}-\pi^*\) orbital hybridization drives the dimensional crossover, facilitating the transformation from the 2D distorted to a 3D undistorted pyrite phase. Above 9 GPa, a novel phase emerges, characterized by octahedral distortions in the $d$ orbitals of Pd. Structural analysis suggests the presence of marcasite (\(Pnnm\)) or arsenopyrite (\(P2_1/c\)) phase with orthorhombic and monoclinic configurations, respectively. Furthermore, the observed phonon anomaly and electronic structure modifications, including the emergence of flat bands in the high-pressure phases, elucidate the fundamental mechanisms underlying the previously reported exotic superconductivity with an enhanced critical temperature. These results highlight the pivotal role of dimensional crossover and structural transitions in tuning the electronic properties of puckered materials, providing pathways for novel functionalities.

We present a fully analytical model of hybridization between magnon, and phonons observed experimentally in magneto-Raman scattering in van der Waals (vdW) antiferromagnets (AFM). Here, the representative material, FePS3, has been shown to be a quasi-two-dimensional-Ising antiferromagnet, with additional features of spin-phonon coupling in the Raman spectra emerging below the N\'eel temperature (TN) of approximately 120 K. Using magneto-Raman spectroscopy as an optical probe of magnetic structure, we show that one of these Raman-active modes in the magnetically ordered state is a magnon with a frequency of 3.7 THz (~ 122 cm-1). In addition, one magnon band and three phonon bands are coupled via the magneto-elastic coupling evidenced by anti-crossing in the complete spectra. We consider a simple model involving only in-plane nearest neighbor exchange couplings (designed to give rise to a similar magnetic structure) and perpendicular anisotropy in presence of an out-of-plane magnetic field. Exact diagonalization of the Hamiltonian leads to energy bands which show that the interaction term gives rise to avoided crossings between the hybridized magnon and phonon branches. Realizing magnon-phonon coupling in two-dimensional (2D) AFMs is important for the verification of the theoretical predictions on exotic quantum transport phenomena like spin-caloritronics, topological magnonics, etc., Comment: 5 pages, 2 figures

We report a sequential two-step vapor deposition process for growing mixed-dimensional van der Waals (vdW) materials, specifically Te nanowires (1D) and MoS$_2$ (2D), on a single SiO$_2$ wafer. Our growth technique offers a unique potential pathway to create large scale, high-quality, defect-free interfaces. The assembly of samples serves a twofold application: first, the as-prepared heterostructures (Te NW/MoS$_2$) provide insights into the atomically thin depletion region of a 1D/2D vdW diode, as revealed by electrical transport measurements and density functional theory-based quantum transport calculations. The charge transfer at the heterointerface is confirmed using Raman spectroscopy and Kelvin probe force microscopy (KPFM). We also observe modulation of the rectification ratio with varying applied gate voltage. Second, the non-hybrid regions on the substrate, consisting of the as-grown individual Te nanowires and MoS$_2$ microstructures, are utilized to fabricate separate p- and n-FETs, respectively. Furthermore, the ionic liquid gating helps to realize low-power CMOS inverter and all basic logic gate operations using a pair of n- and p- field-effect transistors (FETs) on Si/SiO$_2$ platform. This approach also demonstrates the potential for unifying diode and CMOS circuits on a single platform, opening opportunities for integrated analog and digital electronics.

Electron-magnon coupling reveals key insights into the interfacial properties between non-magnetic metals and magnetic insulators, influencing charge transport and spin dynamics. Here, we present temperature-dependent Raman spectroscopy and magneto-transport measurements of few-layer graphene (FLG)/antiferromagnetic FePS\(_3\) heterostructures. The magnon mode in FePS\(_3\) softens below 40 K, and effective magnon stiffness decreases with cooling. Magnetotransport measurements show that FLG exhibits negative magnetoresistance (MR) in the heterostructure at low fields (\(\pm 0.2 \, \text{T}\)), persisting up to 100 K; beyond this, MR transitions to positive. Notably, as layer thickness decreases, the coupling strength at the interface reduces, leading to a suppression of negative MR. Additionally, magnetodielectric measurements in the FLG/FePS\(_3\)/FLG heterostructure show an upturn at temperatures significantly below ($T_\text{N}$), suggesting a role for the magnon mode in capacitance, as indicated by hybridization between magnon and phonon bands in pristine FePS\(_3\) \textit{via} magnetoelastic coupling.

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.

The study investigates the influence of negative capacitance on the transfer characteristics of vdW FETs on the heterophase of CIPS ferroelectric. Notably, a less pronounced NC resulting from the spatial distribution of the ferroelectric and paraelectric phases plays crucial role in stabilizing of n-channel-conductance. This results into the emergence of a non-volatile logic state, between the two binary states of TFETs. Concerned study proposed NC-TFETs based on ferroionic crystals as promising devices for generating a stable logic state below Vth., Comment: 21 pages, 4 figures

We investigate thickness-dependent transformation from a paramagnetic to ferromagnetic phase in Cr$_{2}$Ge$_{2}$Te$_{6}$ (CGT) in bulk and few-layer flake forms. 2D Ising-like critical transition in bulk CGT occurs at $T_{c}$ = 67 K with out-of-plane magnetic anisotropy. Few-layer CGT on hBN/SiO$_{2}$/Si substrate displays the same $T_{c}$ but also exhibits a new critical transition at $T^{\prime}_c$ = 14.2 K. Here, critical scaling analysis reveals the critical exponents differ significantly from those in bulk and do not align with the known universality classes. Our Density Functional Theory (DFT) and classical calculations indicate competition between magnetocrystalline and dipolar anisotropy emerges with reduced dimensions. The observed behavior is due to minor structural distortions in low dimensional CGT, which modify the balance between spin-orbit coupling, exchange interactions and dipolar anisotropy. This triggers a critical crossover at $T^{\prime}_c$. Our study shows the emergence of a complex interplay of short- and long-range interactions below $T^{\prime}_c$ as CGT approaches the 2D limit., Comment: Paper to appear in Physical Review B (in press, 2024)

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).

We report anisotropic magnetodielectric (MD) coupling in layered van der Waals (vdW) antiferromagnetic (AFM) FePS$_3$ (N\'eel temperature $T_{\mathrm{N}}$ $\sim$ 120K) with perpendicular anisotropy. Above $T_N$, while dielectric response function along \textit{c}-axis shows frequency dependent relaxations, in-plane data is frequency independent and reveals a deviation from phonon-anharmonicity in the ordered state, thereby implying a connection to spin-phonon coupling known to be indicative of onset of magnetic ordering. At low temperature (below 40 K), atypical anomaly in the dielectric constant is corroborated with temperature dependent DC and AC susceptibility. The magnetodielectric response across this anomaly differs significantly for both, in-plane and out-of-plane cases. We have explained this in terms of preferential orientation of magnetic AFM-z alignment, implied by the in-plane structural anisotropy as confirmed by \textit{ab-initio} calculations. Controlling relative strength of magnetodielectric coupling with magnetic anisotropy opens up a strategy for tracking subtle modifications of structure, such as in-plane anisotropy, with potential application to spintronic technologies., Comment: Accepted in PRB as Letter

We apply periodic control to realize a quantum thermal transistor, which we term as the Floquet Quantum thermal Transistor. Periodic modulation allows us to control the heat flows and achieve large amplification factors even for fixed bath temperatures. Importantly, this transistor effect persists in the cut-off region, where traditional quantum thermal transistors operating in absence of periodic modulation, fail to act as viable heat modulation devices., Comment: 16 pages, 12 figures