arXiv subjects

Amit Pawbake

Publications and source records attributed to Amit Pawbake.

14 recordsLinked to original sources

arXiv2026

Manipulation of localized excitons in CrPS$_4$ by temperature and magnetic field

Layered van der Waals magnetic semiconductors provide a versatile platform for exploring excitonic phenomena intertwined with spin and lattice degrees of freedom, enabling excitons to act as sensitive probes of magnetic order. CrPS$_4$ is a layered antiferromagnetic semiconductor that hosts rich excitonic features whose microscopic origin and connection to magnetic ordering remain incompletely understood. Here, we investigate the electronic and excitonic properties of bulk CrPS$_4$ using a combination of many-body perturbation theory, dynamical mean-field theory, and photoluminescence-based experiments. Our calculations establish CrPS$_4$ as a direct-gap semiconductor with a bandgap of 2.48~eV in the antiferromagnetic phase. Several sub-bandgap excitonic transitions are predicted by theory, comprising multiple spin-allowed excitons and an additional spin-flip excitation, predominantly localized on the Cr$^{3+}$ ions. Temperature- and magnetic-field-dependent optical measurements reveal thermally driven exciton redistribution among localized states and identify characteristic energy shifts that provide clear optical signatures of magnetic phase transitions in CrPS$_4$. These results provide new insights into the excitonic transitions of antiferromagnets and suggest potential routes for all-optical sensing and light-driven control of their magnetic order.

cond-mat.str-el↗

arXiv2026

Probing Dielectric Screening in van der Waals Heterostructures via Pressure-Tuned Exciton Rydberg Series

Excitons in two-dimensional semiconductors are directly exposed to the environment and are sensitive to the dielectric properties of their surrounding. Here, we show that the Rydberg series of excited states of excitons in a monolayer WSe$_2$ encapsulated in hexagonal boron nitride (hBN) can be used to probe the pressure-induced modifications of the surrounding dielectric properties. We propose a model based on the pressure induced evolution of the interlayer distances in this van der Waals heterostructure and on the bulk dielectric properties of hBN. This approach allows a direct measurement of the dielectric constant of pressurized hBN and establishes a new methodology for dielectric sensing.

cond-mat.mes-hall↗

arXiv2026

Room-temperature antiferromagnetic resonance in NaMnAs

We report on antiferromagnetic resonance experiments in bulk tetragonal NaMnAs -- a room-temperature antiferromagnetic semiconductor. Our results corroborate previous ab initio studies, which propose that NaMnAs is an easy-axis antiferromagnet with the N\'eel vector oriented along the tetragonal axis. At $ B = 0 $, we find a single antiferromagnetic resonance line at 7 meV and associate it with a doubly degenerate ($ k = 0 $) magnon mode. Its energy softens considerably with increasing $ T $, but remains clearly visible in the data up to room temperature. From the experimental data, we estimate the single-ion anisotropy of the Mn ions in NaMnAs in the range 0.1-0.2 meV, a value that is relatively large compared to other manganese-based antiferromagnets.

cond-mat.mtrl-sci↗

arXiv2026

Van der Waals CrSBr alloys with tunable magnetic and optical properties

Van der Waals magnets are attracting a lot of attention for their potential integration in spintronic and magnonic technologies. CrSBr is an A-type antiferromagnet that shows a coupling between its electronic band structure and magnetic properties. This property is appealing for applications and it also offers the possibility to investigate magnetic ground states and GHz magnons using visible optics techniques. Using Raman scattering and (magneto)-optical experiments, we describe the magnetic and optical properties of alloys of CrSBr$_{(1-x)}$Cl$_x$ with $x<0.46$. Similar to CrSBr, these alloys are direct band gap semiconductors with a coupling of their electronic and magnetic properties. Exciton energies evolve weakly with composition and we describe the large changes in the saturation magnetic fields and their implications on the magnetic properties. We show that both the interlayer magnetic exchange and electronic interactions are modified by the halogen mixing, offering the possibility to tune magnon energies with alloy composition.

cond-mat.mtrl-sci↗

arXiv2025

Multilayer Crystal Field states from locally broken centrosymmetry

Local charge, spin, or orbital degrees of freedom with intersite interactions are oftentimes sufficient to construct most quantum orders. This is conventionally true for f-electron systems, where the extent of the f-electrons and their associated crystal-electric-field (CEF) states are strongly localized. Here, polarized Raman spectroscopy measurements of a locally non-centrosymmetric compound, CeCoSi, unveil more CEF excitations than expected in the local model. We interpret this as experimental evidence for the entanglement of CEF states between cerium layers. This composite sublattice, spin, and orbital degree of freedom provides an unconsidered means to form novel orders, not only in this system, but in any system exhibiting globally preserved yet locally broken centrosymmetry.

cond-mat.str-el↗

arXiv2025

Extremely high excitonic $g$-factors in 2D crystals by alloy-induced admixing of band states

Monolayers (MLs) of semiconducting transition metal dichalcogenides (\mbox{S-TMDs}) emit light very efficiently and display rich spin-valley physics, with gyromagnetic ($g$-) factors of about -4. Here, we investigate how these properties can be tailored by alloying. Magneto-optical spectroscopy is used to reveal the peculiar properties of excitonic complexes in Mo$_{x}$W$_{1-x}$Se$_2$ MLs with different Mo and W concentrations. We show that the alloys feature extremely high $g$-factors for neutral excitons, that change gradually with the composition up to reaching values of the order of -10 for $x \approx 0.2$. First-principles calculations corroborate the experimental findings and provide evidence that alloying in S-TMDs results in a non-trivial band structure engineering, being at the origin of the high $g$-factors. The theoretical framework also suggests a higher strain sensitivity of the alloys, making them promising candidates for tailor-made optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2025

Laser patterning of the room temperature van der Waals ferromagnet 1$T$-CrTe$_2$

Lamellar crystalline materials, whose layers are bond by van der Waals forces, can be stacked to form ultrathin artificial heterostructures, and in particular vertical magnetic junctions when some of the stacked materials are (ferro)magnetic. Here, using the room temperature van der Waals ferromagnet 1$T$-CrTe$_2$, we report a method for patterning lateral magnetic junctions. Exploiting the heat-induced phase transformation of the material into Cr$_x$Te$_y$ compounds ($x/y>1/2$), we use local laser heating to imprint patterns at the micron-scale. Optimizing laser heat dissipation, we further demonstrate the crucial role of the substrate to control the phase transformation. If plain, unstructured poorly heat-conducting substrates allow for direct writing of magnetic patterns, structured $h$-BN layers can serve as heat stencils to draw potentially thinner patterns. Besides, $h$-BN encapsulation turns out to be heat-protective (in addition from protecting against oxidation as it is generally used for), allowing the demonstration of room temperature ferromagnetism in $<$7~nm-thick 1$T$-CrTe$_2$.

cond-mat.mtrl-sci↗

arXiv2025

Resonant X-ray spectroscopies on Chromium $3\textit{d}$ orbitals in CrSBr

We investigate the Cr electronic structure and excitations in CrSBr, a layered magnetic semiconductor, using a combination of resonant x-ray spectroscopic techniques. X-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) spectra collected at the Cr $L_{2,3}$ edges reveal significant linear dichroism, which arises from the distorted octahedral environment surrounding the Cr$^{3+}$ ions. The origin of the bright excitons observed in this compound is examined through a comparison of the d-d excitations identified in the RIXS spectra, the x-ray excited optical luminescence (XEOL) spectra, and previously reported optical spectroscopic and theoretical studies. To further understand these phenomena, we develop a multiplet model based on a crystal electric field (CEF) approach that accounts for the local environment of Cr ions. This model successfully reproduces several experimental features, while also suggesting strong hybridization effects between Cr $3\textit{d}$ orbitals and ligands that are not fully captured by the present framework. These findings advance our understanding of the electronic structure and excitonic behavior in CrSBr and provide a foundation for future $\textit{in-situ}$ and $\textit{operando}$ studies of CrSBr-based devices for spintronic and optoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2024

NbSe$_{2}$'s charge density wave collapse in the (LaSe)$_{1.14}$(NbSe$_{2}$)$_{2}$ misfit layer compound

Misfit layer compounds, heterostructures composed by a regular alternating stacking of rocksalt monochalcogenides bilayers and few-layer transition metal dichalchogenides, are an emergent platform to investigate highly doped transition metal dichalcogenides. Among them, (LaSe)$_{1.14}$(NbSe$_2$)$_2$ displays Ising superconductivity, while the presence of a charge density wave (CDW) in the material is still under debate. Here, by using polarized Raman spectroscopy and first-principles calculations, we show that NbSe$_2$ undergoes a doping-driven collapse of the CDW ordering within the misfit, and no signature of the CDW is detected down to 8~K. We provide a complete experimental and theoretical description of the lattice dynamics of this misfit compound. We show that the vibrational properties are obtained from those of the two subunits, namely the LaSe unit and the NbSe$_2$ bilayer, in the presence of a suitable field-effect doping, and then highlight the 2D nature of the lattice dynamics of NbSe$_2$ within the (LaSe)$_{1.14}$(NbSe$_2$)$_2$ 3D structure.

cond-mat.mtrl-sci↗

arXiv2024

Pressure-induced optical anisotropy of HfS$_2$

The effect of pressure on Raman scattering (RS) in the bulk HfS$_2$ is investigated under hydrostatic and non-hydrostatic conditions. The RS lineshape does not change significantly in the hydrostatic regime, showing a systematic blueshift of the spectral features. In a non-hydrostatic environment, seven peaks emerge in the spectrum ($P$=7 GPa) dominating the lineshape up to $P$=10.5 GPa. The change in the RS lineshape manifests a pressure-induced phase transition in HfS$_2$. The simultaneous observation of both low-pressure (LP) and high-pressure (HP) related RS peaks suggests the corresponding coexistence of two different phases over a large pressure range. We found that the HP-related phase is metastable, persisting during the decompression cycle down to $P$=1.2 GPa with the LP-related features finally recovering at even lower pressures. The angle-resolved polarized RS (ARPRS) performed under $P$=7.4 GPa revealed a strong in-plane anisotropy of both the LP-related A$_{1g}$ mode and the HP peaks. The anisotropy is related to the possible distortion of the structure induced by the non-hydrostatic component of the pressure. We describe the obtained results by the influence of the non-hydrostatic pressure on the observed phase transition. We interpret our results in terms of a distorted $Pnma$ phase as a possible HP induced structure of HfS$_2$.

cond-mat.mtrl-sci↗

arXiv2023

In-plane magnetocrystalline anisotropy in the van der Waals antiferromagnet FePSe$_3$ probed by magneto-Raman scattering

Magnon gap excitations selectively coupled to phonon modes have been studied in FePSe$_3$ layered antiferromagnet with magneto-Raman scattering experiments performed at different temperatures. The bare magnon excitation in this material has been found to be split (by $\approx~1.2$ cm$^{-1}$) into two components each being selectively coupled to one of the two degenerated, nearby phonon modes. Lifting the degeneracy of the fundamental magnon mode points out toward the biaxial character of the FePS$_3$ antiferromagnet, with an additional in-plane anisotropy complementing much stronger, out-of-plane anisotropy. Moreover, the tunability, with temperature, of the phonon- versus the magnon-like character of the observed coupled modes has been demonstrated.

cond-mat.mtrl-sci↗

arXiv2022

Raman scattering signatures of the strong spin-phonon coupling in the bulk magnetic van der Waals material CrSBr

Magnetic excitations in layered magnetic materials that can be thinned down the two-dimensional (2D) monolayer limit are of high interest from a fundamental point of view and for applications perspectives. Raman scattering has played a crucial role in exploring the properties of magnetic layered materials and, even-though it is essentially a probe of lattice vibrations, it can reflect magnetic ordering in solids through the spin-phonon interaction or through the observation of magnon excitations. In bulk CrSBr, a layered A type antiferromagnet (AF), we show that the magnetic ordering can be directly observed in the temperature dependence of the Raman scattering response i) through the variations of the scattered intensities, ii) through the activation of new phonon lines reflecting the change of symmetry with the appearance of the additional magnetic periodicity, and iii) through the observation, below the Neel temperature (TN) of second order Raman scattering processes. We additionally show that the three different magnetic phases encountered in CrSBr, including the recently identified low temperature phase, have a particular Raman scattering signature. This work demonstrates that magnetic ordering can be observed directly in the Raman scattering response of bulk CrSBr with in-plane magnetization, and that it can provide a unique insight into the magnetic phases encountered in magnetic layered materials.

cond-mat.mes-hall↗

arXiv2022

High pressure tuning of magnon-polarons in the layered antiferromagnet FePS$_3$

Magnetic layered materials have emerged recently as promising systems to introduce magnetism in structures based on two-dimensional (2D) materials and to investigate exotic magnetic ground states in the 2D limit. In this work, we apply high hydrostatic pressures up to P = 8.7 GPa to the bulk layered antiferromagnet FePS$_3$ to tune the collective lattice excitations (phonons) in resonance with magnetic excitations (magnons). Close to P = 4 GPa, the magnon-phonon resonance is achieved and the strong coupling between these collective modes leads to the formation of new quasi-particles, the magnon-polarons, evidenced in our low temperature Raman scattering experiments by a particular avoided crossing behavior between the phonon and the doubly degenerate antiferromagnetic magnon. At the pressure-induced magnon-phonon resonance, three distinct coupled modes emerge. As it is mainly defined by intralayer properties, we show that the energy of the magnon is nearly pressure independent. We additionally apply high magnetic fields up to B = 30 T to fully identify and characterize the magnon excitations, and to explore the different magnon-polaron regimes for which the phonon has an energy lower-, equal to-, or higher- than the magnon energy. The description of our experimental data requires introducing a phonon-phonon coupling not taken into account in actual calculations.

cond-mat.mes-hall↗

arXiv2020

Raman Fingerprint of Pressure-Induced Phase Transitions in TiS3 Nanoribbons: Implications for Thermal Measurements under Extreme Stress Conditions

Two-dimensional layered trichalcogenide materials have recently attracted the attention of the scientific community because of its robust mechanical, thermal properties and applications in opto and nanoelectronics devices. We report the pressure dependence of out-of plane Ag Raman modes in high quality few-layers titanium trisulfide (TiS3) nanoribbons grown using a direct solid-gas reaction method and infer their cross-plane thermal expansion coefficient.Both mechanical stability and thermal properties of the TiS3 nanoribbons are elucidated using phonon-spectrum analyses. Raman spectroscopic studies at high pressure (up to 34 GPa) using a diamond anvil cell identify four prominent Ag Raman bands; a band at 557 cm-1 softens under compression, and others at 175, 300, and 370 cm-1 show normal hardening. Anomalies in phonon mode frequencies and excessive broadening in line-width of the soft phonon about ~ 13 GPa are attributed to the possible onset of a reversible structural transition. A complete structural phase transition at 43 GPa is inferred from Ag soft mode frequency (557 cm-1) versus pressure extrapolation curve, consistent with recent reported theoretical predictions. Using the experimental mode Grüneisen parameters i of Raman modes, the cross-plane thermal expansion coefficient Cv of the TiS3 nanoribbons at ambient phase is estimated to be1.32110-6K-1. The observed results are expected to be useful in calibration and performance of next generation nano-electronics and optical devices under extreme stress conditions.

cond-mat.mtrl-sci↗