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Atindra Nath Pal

Publications and source records attributed to Atindra Nath Pal.

At least 19 recordsLinked to original sources

Magnetic anisotropy in the near-stoichiometric van der Waals ferromagnet Fe$_3$GeTe$_2$

Quasi-two-dimensional (2D) van der Waals (vdW) ferromagnets such as the series Fe$_{3-x}$GeTe$_2$, with a relatively high Curie temperature and robust metallicity, offer an ideal platform for investigating itinerant magnetism in reduced dimensions. Here, we present a comprehensive electron spin resonance (ESR) investigation of single-crystalline almost-stoichiometric Fe$_{3.03 \pm 0.03}$GeTe$_{2}$ across wide ranges of frequencies, temperatures, and magnetic fields to gain quantitative insights into its magnetic anisotropy and spin dynamics. Frequency-dependent ESR measurements establish Fe$_{3}$GeTe$_{2}$ as an easy-axis ferromagnet. Temperature-dependent high-field ESR reveals a large internal field that gradually decreases at higher temperatures. Remarkably, this internal field persists even above $T_\mathrm{C}$, evidencing short-range spin correlations in Fe$_{3}$GeTe$_{2}$. Analysis of spin-wave modes yields a strong uniaxial magnetocrystalline anisotropy $K_{\text{int}} \approx - 5 \times 10^6$ erg cm$^{-3}$ at 3 K and a large magnon gap $Δ(3 \mathrm{K})$ $\approx$ 87.8 $\pm$ 13.7 GHz ($\approx$ 0.363 $\pm$ 0.057 meV). Our study highlights that small variations in Fe content in Fe$_{3}$GeTe$_{2}$ lead to substantial changes in the magnon gap at low temperatures, indicating the extreme sensitivity of spin dynamics to the chemical composition. These results establish Fe$_{3}$GeTe$_{2}$ as a model vdW ferromagnet for exploring tunable anisotropies and magnon excitations in metallic 2D magnets.

cond-mat.str-el

Observation of correlation-driven topological transport and robust ferromagnetism in 2D CrS$_2$

The realization of correlated layered magnets hosting robust ferromagnetism with emergent topological transport remains a key challenge in quantum materials. Here we report the first catalyst-free chemical vapour deposition growth of layered 1T-CrS$_2$, establishing a highly stable vdWs ferromagnet with an out-of-plane easy-axis anisotropy and a Curie temperature above room temperature. Transport measurements reveal a semimetal--insulator crossover near 80 K and pronounced negative magnetoresistance up to 350 K. A topological Hall effect emerges below 30 K, a rare signature of correlated transport in layered transition-metal dichalcogenide ferromagnets. First-principles calculations show that spin--orbit coupling gaps Dirac-like crossings, while electronic correlations reconstruct the Fermi surface by suppressing electron pockets and reducing the carrier density, enhancing momentum-dependent out-of-plane spin polarization. Magnetic measurements, supported by Heisenberg exchange calculations, reveal strong nearest-neighbour ferromagnetic exchange that stabilizes long-range ferromagnetism. Our results establish 1T-CrS$_2$ as a rare correlated 3$d$ layered ferromagnet in which electronic correlations and spin--orbit coupling cooperatively drive emergent topological transport.

cond-mat.mtrl-sci

Spin-phonon interaction in a symmetry-enforced spin-polarized state

Symmetry-governed magnetic materials have emerged as a promising platform for spintronic functionalities without net magnetization or stray magnetic fields, motivating the exploration of how lattice dynamics couple to symmetry-derived spin-polarized electronic states. Understanding spin-phonon coupling in these systems is therefore essential for uncovering the microscopic origin of spin-lattice interactions and for enabling their control in quantum materials. However, this mechanism remains poorly understood because spin polarization originates from crystal symmetry rather than conventional magnetic order. Here, we address this issue in the g-type altermagnet CoNb4Se8 using temperature- and polarization-resolved Raman spectroscopy, complemented by measurements on a structurally analogous Co-deficient compound lacking well-defined long-range magnetic order. We observe pronounced symmetry-selective phonon renormalization across the magnetic transition in CoNb4Se8, while related phonon anomalies persist in the Co-deficient system, demonstrating that the lattice response cannot be explained solely by conventional exchange-striction associated with coherent magnetic ordering. First-principles calculations reveal that spin-orbit coupling establishes a symmetry-dependent interaction channel between lattice vibrations and symmetry-governed electronic states. Our results identify an alternative mechanism for spin-phonon coupling in symmetry-governed magnetic materials and demonstrate that phonons provide a sensitive probe of symmetry-driven spin polarization even without robust magnetic order. More broadly, this work provides a framework for understanding and engineering spin-lattice functionality in symmetry-driven quantum materials, offering design principles for coupling lattice dynamics to spin-polarized electronic states.

cond-mat.mtrl-sci

Impact of Disorder Dynamics and Multi-Domain Kinetics on the Sliding Ferroelectricity of CVD-Grown 3R-WSe2 Bilayers

Sliding ferroelectricity in van der Waals (vdW) layered systems has emerged as a promising route toward non-volatile nanoscale devices, where interlayer displacement in non-centrosymmetric bilayers generates an out-of-plane polarization. In particular, 3R-stacked bilayer transition metal dichalcogenides (TMDs) grown via chemical vapor deposition (CVD) have been shown to host such polarization due to broken inversion symmetry. However, a detailed investigation of the 2D ferroelectric (FE) properties of CVD-grown 2D films, particularly the role of intrinsic disorder, such as structural defects and domain structure, remains poorly understood. Here, we investigate the FE switching characteristics of CVD-grown 3R-stacked WSe2 using a graphene-based ferroelectric field-effect transistor (graphene-FE-FET) architecture, where graphene serves as a highly sensitive probe of induced charge modulation due to polarization switching of FEs. We show that the growth-induced structural disorder significantly impacts polarization switching, while multi-domain kinetics governs the evolution of the FE response. These findings provide important insights into the design and optimization of FE devices based on vdW materials.

cond-mat.mtrl-sci

Intrinsic Electric Field Driven High Sensitive Photodetection in Alloy TMDC MoSSe

Alloying offers an effective way to improve the functionality of transition metal dichalcogenides (TMDCs) in both fundamental research and optoelectronic applications, as it allows for engineering their electronic and optical properties. This study investigates the optoelectronic properties of CVD-synthesized alloy MoSSe, which exhibits an inherent out-of-plane dipole moment, arising from asymmetry in S and Se atoms on either side of the Mo layer, as confirmed by piezoelectric force microscopy, polarization-resolved second harmonic generation studies and theoretical first-principles calculations. Time-resolved photoluminescence measurements reveal an extended exciton radiative recombination lifetime in MoSSe, attributed to electron-hole wavefunction separation by the dipole moment, which improves photodetection by facilitating enhanced electron-hole separation before recombination. The device demonstrates significant responsivity over broad spectral range. By employing the photogating effect, the device response can be switched from slow to fast modes. These findings are further supported by illumination intensity-dependent photoluminescence and Raman measurements, underscoring the potential of polar TMDCs in future optoelectronic devices.

cond-mat.mtrl-sci

Spin Reorientation Driven Renormalization of Spin-Phonon Coupling in Fe$_4$GeTe$_2$

Quasi-2D van der Waals ferromagnet Fe$_4$GeTe$_2$, featuring the simultaneous presence of high Curie temperature ($T_\mathrm{C}$ $\sim 270$ K) and a spin-reorientation transition at $T_\mathrm{SR}$ $\sim 110$ K, is a rare system where strong interplay of spin dynamics, lattice vibrations, and electronic structure leads to a wide range of interesting phenomena. Here, we investigate the lattice response of exfoliated Fe$_4$GeTe$_2$ nanoflakes using temperature-dependent Raman spectroscopy. Polarization-resolved measurements reveal that, while one Raman mode exhibits a purely out-of-plane character, the rest display mixed symmetry, reflecting interlayer vibrational nonuniformity and symmetry-driven mode degeneracies. Below $T_\mathrm{C}$, phonons harden, and the linewidth narrows, consistent with reduced anharmonicity, while across the spin reorientation transition at $T_\mathrm{SR}$ they display anomalous softening, linewidth broadening, and a peak in lifetime, which are signatures of strengthened spin-phonon coupling. Complementary DFT+DMFT calculations and atomistic spin dynamical simulations reveal temperature-dependent spin excitations whose energies overlap with the Raman-active phonons, providing a natural route for the observed magnon-phonon interaction. Together, these insights establish Fe$_4$GeTe$_2$ as a versatile platform for exploring intertwined spin, lattice, and electronic degrees of freedom, with relevance for dynamic spintronic and magneto-optic functionalities near technologically meaningful temperatures.

cond-mat.mes-hall

Disentangling the unusual magnetic anisotropy of the near-room-temperature ferromagnet Fe$_{4}$GeTe$_{2}$

In the quest for two-dimensional conducting materials with high ferromagnetic ordering temperature the new family of the layered Fe$_{n}$GeTe$_{2}$ compounds, especially the near-room-temperature ferromagnet Fe$_{4}$GeTe$_{2}$, receives a significant attention. Fe$_{4}$GeTe$_{2}$ features a peculiar spin reorientation transition at $T_\mathrm{SR} \sim 110$ K suggesting a non-trivial temperature evolution of the magnetic anisotropy (MA) - one of the main contributors to the stabilization of the magnetic order in the low-D systems. An electron spin resonance (ESR) spectroscopic study reported here provides quantitative insights into the unusual magnetic anisotropy of Fe$_{4}$GeTe$_{2}$. At high temperatures the total MA is mostly given by the demagnetization effect with a small contribution of the counteracting intrinsic magnetic anisotropy of an easy-axis type, whose growth below a characteristic temperature $T_{\rm shape} \sim 150$ K renders the sample seemingly isotropic at $T_\mathrm{SR}$. Below one further temperature $T_{\rm d} \sim 50$ K the intrinsic MA becomes even more complex. Importantly, all the characteristic temperatures found in the ESR experiment match those observed in transport measurements, suggesting an inherent coupling between magnetic and electronic degrees of freedom in Fe$_{4}$GeTe$_{2}$. This finding together with the observed signatures of the intrinsic two-dimensionality should facilitate optimization routes for the use of Fe$_{4}$GeTe$_{2}$ in the magneto-electronic devices, potentially even in the monolayer limit.

cond-mat.str-el

Single-Defect Spectroscopy via Random Telegraph Noise in Graphene-Contacted ReS$_2$-hBN Heterostructures

Defect spectroscopy in two-dimensional (2D) field-effect transistors (FETs) requires device architectures that suppress contact and disorder artifacts while preserving intrinsic carrier dynamics. Here, we demonstrate ReS$_2$-hBN FETs with few-layer graphene (FLG) van der Waals contacts that form nearly barrier-free interfaces, enabling intrinsic transport in ReS$_2$, an anisotropic, low-symmetry TMDC rarely exhibiting disorder-free behavior. The clean ReS$_2$-FLG platform allows direct observation of random telegraph noise (RTN) even in micron-scale channels, manifested as discrete two-level current fluctuations between 90-150 K arising from stochastic trapping at localized hBN defect sites. With increasing temperature, the RTN evolves into a 1/f spectrum as multiple traps activate. Statistical analysis of RTN amplitudes and capture-emission kinetics identifies substitutional carbon-related centers in hBN as dominant defects. These findings establish a generalizable approach for probing dielectric-origin defect dynamics in intrinsically conducting, low-symmetry 2D semiconductors.

cond-mat.mes-hall

Skyrmionic Transport and First Order Phase Transitions in Twisted Bilayer Graphene Quantum Hall Ferromagnet

Large-angle twisted bilayer graphene (TBLG) realizes a multicomponent quantum Hall (QH) platform of spin, valley and layer pseudospins with strong Coulomb interaction-driven symmetry broken phases. Here, we investigate the low energy Landau-level spectrum of layer-decoupled TBLG and identify skyrmion-textured charged excitations and a field-induced insulating transition to an intervalley coherent state at zero-filling factor. Symmetric potential difference perpendicular to TBLG demonstrated layer coherent population of ground states with uniform energy barriers, while the charge imbalance in the layers at finite displacement field led to multidomain nucleation and a pronounced hysteresis in the exchange-dominated transport regime suggesting first order phase transitions between different QH ferromagnetic ground states.

cond-mat.mes-hall

Unconventional Electromechanical Response in Ferrocene Assisted Gold Atomic Chain

Atomically thin metallic chains serve as pivotal systems for studying quantum transport, with their conductance strongly linked to the orbital picture. Here, we report a non-monotonic electro-mechanical response in a gold-ferrocene junction, characterized by an unexpected conductance increase over a factor of ten upon stretching. This response is detected in the formation of ferrocene-assisted atomic gold chain in a mechanically controllable break junction at a cryogenic temperature. DFT based calculations show that tilting of molecules inside the chain modifies the orbital overlap and the transmission spectra, leading to such non-monotonic conductance evolution with stretching. This behavior, unlike typical flat conductance plateaus observed in metal atomic chains, pinpoints the unique role of conformational rearrangements during chain elongation. Our findings provide a deeper understanding of the role of orbital hybridization in transport properties and offer new opportunities for designing nanoscale devices with tailored electro-mechanical characteristics.

cond-mat.mes-hall

Alloying as a new route to generating interlayer excitons

Heterobilayers formed by stacking two-dimensional atomic crystals are particularly promising for low-dimensional semiconductor optics, as they host interlayer excitons, bound states of electrons and holes residing in different layers. They inherit the valley-contrasting physics of the individual monolayers, leading to a range of unique properties that distinguish them from other solid-state nanostructures. Here, we propose a novel route for the generation of interlayer excitons based on the synthesis of a transition metal dichalcogenide bilayer alloy material, WS$_{2x}$Se$_{2(1-x)}$. Using piezoelectric force microscopy, we demonstrate the existence of an internal electric field oriented in the out-of-plane direction. Interlayer excitons have so far been mostly observed in heterostructures with a type-II band alignment. In the presence of an internal electric field, a similar alignment occurs in the alloy bilayer resulting in an efficient generation of interlayer excitons. Photoluminescence spectroscopy measurements involving circularly polarised light come up with key observations like a negative degree of circular polarization of the interlayer excitons which increases as a function of temperature. A simple theoretical model provides a physical understanding of the major experimentally observed features. With experimentally fitted parameter values, the dominant contribution to the degree of circular polarization is shown to arise from spin polarization and not from valley polarization, a consequence of the spin-valley-layer coupling characteristic of a TMDC bilayer. The room-temperature interlayer excitonic transition in bilayer TMDCs has key implications for fundamental physics, including Bose-Einstein condensation and high-temperature superfluidity, while enabling advanced valleytronic and quantum information functionalities.

cond-mat.mes-hall

Valley polarization and photocurrent generation in transition metal dichalcogenide alloy MoS$_{2x}$Se$_{2(1-x)}$

Monolayer transition metal dichalcogenides (TMDCs) constitute the core group of materials in the emerging semiconductor technology of valleytronics. While the coupled spin-valley physics of pristine TMDC materials and their heterstructures has been extensively investigated, less attention was given to TMDC alloys, which could be useful in optoelectronic applications due to the tunability of their band gaps. We report here our experimental investigations of the spin-valley physics of the monolayer and bilayer TMDC alloy, MoS$_{2x}$Se$_{2(1-x)}$, in terms of valley polarization and the generation as well as electrical control of a photocurrent utilising the circular photogalvanic effect. Piezoelectric force microscopy provides evidence for an internal electric field perpendicular to the alloy layer, thus breaking the out-of-plane mirror symmetry. The experimental observation is supported by first principles calculations based on the density functional theory. A comparison of the photocurrent device, based on the alloy material, is made with similar devices involving other TMDC materials.

cond-mat.mes-hall

Detection of nontrivial topology driven by charge density wave in a semi-Dirac metal

The presence of electron correlations in a system with topological order can lead to exotic ground states. Considering single crystals of LaAgSb2 which has a square net crystal structure, one finds multiple charge density wave transitions (CDW) as the temperature is lowered. We find large planar Hall (PHE) signals in the CDW phase, which are still finite in the high temperature phase though they change sign. Optimising the structure within first-principles calculations, one finds an unusual chiral metallic phase. This is because as the temperature is lowered, the electrons on the Ag atoms get more localized, leading to stronger repulsions between electrons associated with atoms on different layers. This leads to successive layers sliding with respect to each other, thereby stabilising a chiral structure in which inversion symmetry is also broken. The large Berry curvature associated with the low temperature structure explains the low temperature PHE. At high temperature the PHE arises from the changes induced in the tilted Dirac cone in a magnetic field. Our work represents a route towards detecting and understanding the mechanism in a correlation driven topological transition through electron transport measurements, complemented by ab-initio electronic structure calculations.

cond-mat.mtrl-sci

Resonant transport in a highly conducting single molecular junction via metal-metal covalent bond

Achieving highly transmitting molecular junctions through resonant transport at low bias is key to the next-generation low-power molecular devices. Although, resonant transport in molecular junctions was observed by connecting a molecule between the metal electrodes via chemical anchors by applying a high source-drain bias (> 1V), the conductance was limited to < 0.1 G$_0$, G$_0$ being the quantum of conductance. Here, we report electronic transport measurements by directly connecting a Ferrocene molecule between Au electrodes at the ambient condition in a mechanically controllable break junction setup (MCBJ), revealing a conductance peak at ~ 0.2 G$_0$ in the conductance histogram. A similar experiment was repeated for Ferrocene terminated with amine (-NH2) and cyano (-CN) anchors, where conductance histograms exhibit an extended low conductance feature including the sharp high conductance peak, similar to pristine ferrocene. Statistical analysis of the data along with density functional theory-based transport calculation suggests the possible molecular conformation with a strong hybridization between the Au electrodes and Fe atom of Ferrocene molecule is responsible for a near-perfect transmission in the vicinity of the Fermi energy, leading to the resonant transport at a small applied bias (< 0.5V). Moreover, calculations including Van der Waals/dispersion corrections reveal a covalent like organometallic bonding between Au and the central Fe atom of Ferrocene, having bond energies of ~ 660 meV. Overall, our study not only demonstrates the realization of an air-stable highly transmitting molecular junction, but also provides an important insight about the nature of chemical bonding at the metal/organo-metallic interface.

cond-mat.mes-hall

Establishing Magnetic Coupling in Spin-crossover-2D Hybrid Nanostructures via Interfacial Charge-transfer Interaction

Despite a clear demonstration of bistability in spin-crossover (SCO) materials, the absence of long-range magnetic order and poor electrical conductivity limit their prospect in spintronic and nanoelectronic applications. Intending to create hybrid devices made of spin-crossover (SCO)-2D architecture, here, we report an easily processable Fe-based SCO nanostructures grown on 2D reduced graphene oxide (rGO). The heterostructure shows enhanced cooperativity due to formation of interfacial charge transfer induced inter-molecular interaction. The spin transition temperature is controlled by tuning the coverage area of SCO nanostructured networks over the 2D surfaces, thus manipulating hysteresis (aka memory) of the heterostructure. The enhanced magnetic coupling of the heterostructure leads to the spontaneous magnetization states with a large coercive field of $\sim$ 3000 Oe. Additionally, the low conductivity of the pristine SCO nanostructures is addressed by encapsulating them on suitable 2D rGO template, enabling detection of magnetic bistable spin states during high-spin/low-spin conductance change. This adds spin functionality in conductance switching for realizing hybrid 2D spintronic devices. Ab-inito calculations, on the experimentally proposed nanostructures, corroborate the enhanced magnetic interaction in the proposed architecture facilitated by interfacial charge transfer and provide insights on the microscopic mechanism.

cond-mat.mtrl-sci

Structural regulation of mechanical gating in molecular junctions

In contrast to silicon-based transistors, single molecule junctions can be gated by simple mechanical means. Specifically, charge can be transferred between the junction's electrodes and its molecular bridge when the interelectrode distance is modified, leading to variations in the electronic transport properties of the junction. While this effect has been studied extensively, the influence of the molecule orientation on mechanical gating has not been addressed, despite its potential influence on the gating effectiveness. Here, we show that the same molecular junction can experience either clear mechanical gating or none, depending on the molecule orientation in the junctions. The effect is found in silver-ferrocene-silver break junctions, and analyzed in view of ab-initio and transport calculations, where the influence of molecular orbitals geometry on charge transfer to or from the molecule is revealed. The molecule orientation is thus a new degree of freedom that can be used to optimize mechanically-gated molecular junctions.

cond-mat.mes-hall

Unusual magnetotransport and anomalous Hall effect in quasi-two-dimensional van der Waals ferromagnet Fe$_4$GeTe$_2$

Fe$_4$GeTe$_2$, an itinerant vdW ferromagnet (FM) having Curie temperature (T$_C$) close to room temperature ($\sim 270$ K), exhibits another transition (T$_{SR}$ $\sim$ 120 K) where the easy axis of magnetization changes from in-plane to the out-of-plane direction in addition to T$_C$. Here, we have studied the magnetotransport in a multilayer Hall bar device fabricated on 300 nm Si/SiO$_2$ substrate. Interestingly, the zero field resistivity shows a negligible change in resistivity near T$_C$ unlike the typical metallic FM, whereas, it exhibits a dramatic fall below T$_{SR}$. Also, the resistivity shows a weak anomaly at T $ \sim $ 38 K (T$_Q$), below which the resistivity shows a quadratic temperature dependence according to the Fermi liquid behavior. Temperature-dependent Hall data exhibits important consequences. The ordinary Hall coefficient changes sign near T$_{SR}$ indicating the change in majority carriers. In a similar manner, the magnetoresistance (MR) data shows significantly large negative MR near T$_{SR}$ and becomes positive below T$_Q$. The observations of anomaly in the resistivity, sign-change of the ordinary Hall coefficient and maximum negative MR near T$_{SR}$, together suggest a possible Fermi surface reconstruction associated with the spin reorientation transition. Furthermore, analysis of the Hall data reveals a significant anomalous Hall conductivity (AHC) from $\sim 123 Ω^{-1}$ cm$^{-1}$ (at T $\approx$ 5 K) to the maximum value of $\sim 366 Ω^{-1}$ cm$^{-1}$ near T$_{SR}$. While the low-temperature part may originate due to the intrinsic KL mechanism, our analysis indicates that the temperature-dependent AHC is primarily appearing due to the side-jump mechanism as a result of the spin-flip electron-magnon scattering. Our study demonstrates an interplay between magnetism and band topology and its consequence on electron transport in Fe$_4$GeTe$_2$.

cond-mat.mes-hall

Exciton-Plasmon Coupling Mediated Superior Photoresponse in 2D Hybrid Phototransistors

The possibility of creating heterostructure of two-dimensional (2D) materials has emerged as a viable route towards realizing novel optoelectronic devices. However, the low light absorption due to their small absorption cross section, limits their realistic application. While light-matter interaction mediated by strong exciton-plasmon coupling has been demonstrated to improve absorbance and spontaneous emission in a coupled TMDC and metallic nanostructures, the fabrication of tunable broadband phototransistor with high quantum yield is still a challenging task. By synthesizing Ag nanoparticles (Ag NPs) capped with a thin layer of polyvinylpyrrolidone (PVP) through chemical route, we report a lithography-free fabrication of a large area broadband superior gate-tunable hybrid phototransistor based on monolayer graphene decorated by WS$_2$-Ag NPs in a three-terminal device configuration. The fabricated device exhibits extremely high photoresponsivity (up to $3.2\times 10^4$ A/W) which is more than 5 times higher than the bare graphene/WS$_2$ hybrid device, along with a low noise equivalent power (NEP) (~10$^{-13}$ W/Hz$^{0.5}$, considering 1/f noise) and high specific detectivity ~1010 Jones in the wide (325-730 nm) wavelength region. The additional PVP capping of Ag NPs helps to suppress the direct charge and heat transfer and most importantly, increases the device stability by preventing the degradation of WS$_2$-Ag hybrid system. The enhanced optical properties of the hybrid device are explained via dipole mediated strong exciton-plasmon coupling, corroborated by COMSOL Multiphysics simulation. Our work demonstrates a strategy towards obtaining an environment-friendly, scalable, high-performance broadband phototransistor by tuning the exciton-plasmon coupling for new generation opto-electronic devices.

cond-mat.mes-hall