SearcharxivSearch

arXiv subjects

Anushree Roy

Publications and source records attributed to Anushree Roy.

At least 19 recordsLinked to original sources

Phonon anomalies and critical scaling in the spin-$1/2$ trimer chain Na$_2$Cu$_3$Ge$_4$O$_{12}$

Low-dimensional quantum magnets provide an ideal platform to explore spin-lattice coupling-mediated quantum correlations, which give rise to emergent quasiparticle excitations. The antiferromagnetically coupled spin-1/2 trimer chain of copper ions in Na$_2$Cu$_3$Ge$_4$O$_{12}$ (NCGO) hosts high-energy spin excitations of different species, whose energy scales overlap with those of lattice vibrations. Here, we report a comprehensive temperature-dependent Raman spectroscopic study performed between 80 and 400 K. The dynamic spin susceptibility, as obtained from the analysis of the broad spectral background, reveals the emergence of quasiparticle excitations below 170 K. We further identify an unusual crossover of phonon dynamics when the material transits from a normal paramagnetic state to a correlated quantum magnetic state. A power law dependence of the integrated Raman susceptibility of the phonon modes, $I_{\chi^{\prime\prime}}^{i}\sim|T-T_{c}|^\beta$, is observed with the critical temperature $T_c$=167$\pm$1 K, and critical exponent $\beta = 0.24\pm 0.02$. The combined results obtained from the broad spectral background and sharp phonon peaks further indicate that the phonon renormalization observed across the crossover is driven by dynamic spin states. Additionally, statistical correlations among phonon energy eigenvalues, quantified through matrix-norm and power-test analyses of 200 spectra recorded at 80 K, reveal an unexpected linear correlation among phonon modes, also indicating that the collective lattice response is governed by spin correlations. These findings establish NCGO as a model system for investigating cooperative spin-lattice coupling and critical scaling behavior of phonon dynamics in low-dimensional magnetic materials.

cond-mat.str-el

Contrasting anisotropic electron-phonon-spin coupling in Fe$_{3}$GeTe$_{2}$ and Fe$_{5}$GeTe$_{2}$: A helicity-resolved Raman study

Two-dimensional van der Waals ferromagnets Fe$_3$GeTe$ _2$ (F3GT) and Fe$_5$GeTe$_2$ (F5GT) exhibit pronounced magneto-optical responses, which open promising platforms for investigating the interplay among lattice, electronic, and magnetic degrees of freedom. Here, we present a comparative study of optical resonance-induced anisotropic electron-phonon coupling and its association with magnetic ordering in these systems using wavelength- and temperature-dependent helicity-resolved Raman spectroscopy. By resolving the doubly degenerate E modes under left- and right-circularly polarized excitations, we demonstrate that the temperature evolution of the chiral mode splitting ($\Delta f$) does not track the magnetization behavior, indicating that the helicity-dependent Raman response arises not solely from time-reversal symmetry breaking due to magnetic order, but also from spin-orbit-coupled electronic interactions. Notably, in F3GT, the out-of-plane magnetization indirectly governs the in-plane anisotropic electron-phonon coupling under optical resonance, whereas F5GT exhibits static anisotropic interactions. The Fano asymmetry parameter $1/q$ reveals mode- and temperature-dependent coupling strengths between phonons and the electronic continuum, with pronounced angular anisotropy in F3GT but isotropic behavior in F5GT--- a consequence of its multiple Fe sites and enhanced interlayer hybridization in the latter. Our results demonstrate the role of crystal structure and magnetic anisotropy in shaping the anisotropically coupled electron-phonon-spin dynamics in these layered metallic ferromagnets, and highlight Fe$_x$GeTe$_2$ as a versatile platform for microscopic insight into chiral light-matter interactions in layered metallic ferromagnets.

cond-mat.str-el

Anisotropic electron-phonon coupling and chiral phonons in van der Waals room temperature ferromagnet Fe$_{5}$GeTe$_{2}$

The layered van der Waals Fe$_5$GeTe$_2$ (F5GT) compound exhibits room-temperature ferromagnetism, making it a promising candidate for technological applications. In our study, combined temperature, wavelength, and polarization-dependent Raman measurements, along with {\it ab initio} calculations reveal important aspects of lattice dynamics and electron-phonon interactions. The angle-resolved Raman intensity under linear polarization configurations exhibits a strong tilt in the laboratory coordinate system, indicating the existence of anisotropic electron-phonon coupling. The temperature evolution of this anisotropy is discussed by extracting the phase factor of the Raman tensor elements from the angle-resolved intensity measured at different temperatures, also uncovering a spin-orbit coupling-mediated electron-phonon response in F5GT. The thermal evolution of electron-phonon coupling is also examined by measuring the temperature dependence of the Fano parameter of the asymmetric peak in the Raman spectra, while wavelength-dependent measurements establish the role of optical resonance in enhancing the anisotropic interaction. Finally, the threefold rotational symmetry guarantees the existence of chiral phonons. We present direct spectroscopic evidence for these chiral vibrational modes through cross-circularly polarized Raman measurements, complemented by theoretical calculations of phonon circular polarization. Together, these results identify F5GT as an ideal platform for investigating emergent couplings among lattice, electronic, and magnetic degrees of freedom and for advancing the understanding of chiral phonons in magnetic van der Waals materials.

cond-mat.mtrl-sci

Fermionic Band Dispersions and an Evidence of Cooperon Excitations in a Spin-$1/2$ Trimer Chain

We obtain the solution of the Hamiltonian of an antiferromagnetically coupled spin-$1/2$ trimer chain in terms of three bands that host three different species of fermions. While the lowest two bands correspond to spin-$1/2$ fermions, the fermions in the highest band are of spin-$3/2$. Because the bands are for different species of fermions, the particle-hole excitation channel across the bands is closed. However, fractionalized excitations as spin-$1/2$ and spin-$3/2$ fermions in pairs open a cooperon channel of excitations in Raman scattering. The background spectral intensity profile obtained by Raman scattering measurements in Na$_2$Cu$_3$Ge$_4$O$_{12}$ having a trimer chain consisting of spin-$1/2$ Cu ions, has comprehensively been shown to be consistent with these excitations.

cond-mat.str-el

Non-trivial phonon dynamics and significant electron-phonon coupling of the high frequency modes in a Dirac semimetal

Using finite temperature Raman spectroscopy, we investigate the electron-phonon interactions (EPI) and phonon-phonon scattering dynamics in the Dirac semimetal Cd3As2 in different fre quency regimes. Strong softening of the Raman shifts below 200 K is observed for almost all the phonon modes with a marked deviation from the standard anharmonic behavior. The experimen tally observed Raman linewidth seems to be captured well by a combination of EPI, relevant at low temperature (LT) and phonon-phonon scattering, which is predominant at high temperatures (HT), leading to an observable minima in the thermal evolution of the linewidth. While this fea ture is most prominently observed in the highest-frequency Raman mode (196 cm-1), its intensity gradually diminishes as the Raman frequency decreases. Computation of the electronic contribution to the phonon linewidth, for both the high and low frequency modes, from the phonon self-energy shows that it qualitatively mimics the experimental observations. It is found that phonon-induced interband scattering results in the presence of a maxima in phonon linewidth that crucially depends on the finiteness of the chemical potential.

cond-mat.str-el

Evidences for local non-centrosymmetricity and strong phonon anomaly in EuCu2As2: A Raman spectroscopy and lattice dynamics study

Phonon modes and their association with the electronic states have been investigated for the metallic EuCu$_{2}$As$_{2}$ system. In this work, we present the Raman spectra of this pnictide system which clearly shows the presence of seven well defined peaks above $100$~cm$^{-1}$ that is consistent with the locally non-centrosymmetric {\it P4/nmm} crystal structure, contrary to that what is expected from the accepted symmorphic {\it I4/mmm} structure. Lattice dynamics calculations using the {\it P4/nmm} symmetry attest that there is a commendable agreement between the calculated phonon spectra at the $\Gamma$ point and the observed Raman mode frequencies, with the most intense peak at $\sim 232$~cm$^{-1}$ being ascribed to the A$_{1g}$ mode. Temperature dependent Raman measurements show that there is a significant deviation from the expected anharmonic behaviour around $165$~K for the A$_{1g}$ mode, with anomalies being observed for several other modes as well, although to a lesser extent. Attempts are made to rationalize the observed anomalous behavior related to the hardening of the phonon modes, with parallels being drawn from metal dichalcogenide and allied systems. Similarities in the evolution of the Raman peak frequencies with temperature seem to suggest a strong signature of a subtle electronic density wave instability below $165$~K in this compound.

cond-mat.str-el

Decoupling the Roles of Defects/Impurities and Wrinkles in Thermal Conductivity of Wafer-scale hBN Films

We demonstrate a non-monotonic evolution of thermal conductivity of large-area hexagonal boron nitride films with thickness. Wrinkles and defects/impurities are present in these films. Raman spectroscopy, an optothermal non-contact technique, is employed to probe the temperature and laser power dependence property of the Raman active E2ghigh phonon mode, which in turn is used to estimate the rise in the temperature of the films under different laser powers. As the conventional Fourier law of heat diffusion cannot be directly employed analytically to evaluate the thermal conductivity of these films with defects and wrinkles, finite element modeling is used instead. In the model, average heat resistance is used to incorporate an overall defect structure, and Voronoi cells with contact resistance at the cell boundaries are constructed to mimic the wrinkled domains. The effective thermal conductivity is estimated to be 87, 55, and 117 W/m.K for the 2, 10, and 30 nm-thick films, respectively. We also present a quantitative estimation of the thermal resistance by defects and wrinkles individually to the heat flow. Our study reveals that the defects/impurities render a much higher resistance to heat transfer in the films than wrinkles.

cond-mat.mtrl-sci

Possible signature of broken symmetry state near the quantum critical point in P doped BaFe$_2$As$_2$: A Raman spectroscopy study

We study the iron-pnictide compound BaFe$_2$(As$_{1-x}$P$_x$)$_2$ for x $\sim$0.23, with a doping concentration near quantum criticality and enhanced nematic fluctuating state in the doping-temperature phase diagram. Transport measurements confirm the presence of a magneto-structural transition at 60K from the tetragonal to the orthorhombic phase, followed by a superconducting transition below 16K. The temperature and polarisation dependent Raman spectra reveal that there is a phonon mode at 211 cm$^{-1}$, followed by two broad modes (BM) between 400 and 700 cm$^{-1}$, having an energy difference of 15 meV, in the temperature range between 300K and 80K. In the non-superconducting state, the phonon mode exhibits expected polarization dependence as well as temperature evolution due to anharmonicity, strong anisotropic and thermally inert behaviour are observed for the BM. Electronic structure calculations for doped and undoped BaFe$_2$As$_2$ show that while Fe $d_{xz}$ and $d_{yz}$ orbitals do not split in the tetragonal phase, the splitting energy is 13.5 meV in the orthorhombic phase of the doped system, which is reasonably close to the experimentally observed value of the energy separation of the BM. We believe that reported BM possibly are the signature of electronic Raman scattering involving the crystal field levels of $d$-orbitals of Fe$^{2+}$ due to local breaking of the C$_4$ symmetry of the parent compound in the doped system.

cond-mat.str-el

Analog Raychaudhuri equation in mechanics

Usually, in mechanics, we obtain the trajectory of a particle in a given force field by solving Newton's second law with chosen initial conditions. In contrast, through our work here, we first demonstrate how one may analyse the behaviour of a suitably defined family of trajectories of a given mechanical system. Such an approach leads us to develop a mechanics analog following the well-known Raychaudhuri equation largely studied in Riemannian geometry and general relativity. The idea of geodesic focusing, which is more familiar to a relativist, appears to be analogous to the meeting of trajectories of a mechanical system within a finite time. Applying our general results to the case of simple pendula, we obtain relevant quantitative consequences. Thereafter, we set up and perform a straightforward experiment based on a system with two pendula. The experimental results on this system are found to tally well with our proposed theoretical model. In summary, the simple theory, as well as the related experiment, provides us with a way to understand the essence of a fairly involved concept in advanced physics from an elementary standpoint.

gr-qc

Analysing the anisotropy in morphological evolution and readjustment effects in cluster-cluster aggregation of AuNPs using Shannon entropy

We have used information theory analogue of entropy, Shannon entropy, for estimating the variations during the isotropic and anisotropic AuNP fractal growth process. We have firstly applied the Shannon entropy on the simulated fractal aggregates obtained from DLA model with noise reduction scheme. In conventional noise reduction scheme used in past, the growth process of identical particles was performed and no effect of the evolving cluster on the incoming particle was considered, hence the noise is reduced in discrete amount and do not account for the noise fluctuations present during the morphological evolution of the fractals. The Shannon entropy is shown to capture the emergence of the anisotropic morphological evolution. The imaging tool was further found to be promising for capturing the readjustment effects during cluster-cluster aggregation.

physics.atm-clus

Electronic band structure engineering in InAs/InSbAs and InSb/InSbAs superlattice heterostructures

We report a detailed ab initio study of two superlattice heterostructures, one component of which is a unit cell of CuPt ordered InSb_(0.5)As_(0.5). This alloy part of the heterostructures is a topological semimetal. The other component of each system is a semiconductor, zincblende-InSb, and wurtzite-InAs. Both heterostructures are semiconductors. Our theoretical analysis predicts that the variation in the thickness of the InSb layer in InSb/InSb_(0.5)As_(0.5) heterostructure renders altered band gaps with different characteristics (i.e. direct or indirect). The study holds promise for fabricating heterostructures, in which the modulation of the thickness of the layers changes the number of carrier pockets in these systems.

cond-mat.mtrl-sci

Geometrically frustrated GdInO$_3$: An exotic system to study negative thermal expansion and spin-lattice coupling

In this article, we report negative thermal expansion and spin frustration in hexagonal GdInO$_{3}$. Rietveld refinement of the XRD patterns reveal that the negative thermal expansion in the temperature range of 50-100K stems from the triangular lattice of Gd$^{3+}$ ions. At low temperature, the downward deviation of the inverse susceptibility ($χ^{-1}$) vs. $T$ plot from the Curie-Weiss law indicates spin frustration which inhibits long-range magnetic ordering down to 2K. Magnetostriction measurements clearly demonstrate a strong spin-lattice coupling. Low temperature anomalous phonon softening, as obtained from temperature dependent Raman measurements, also reveals the same. Our experimental observations are supported by first principles density functional theory calculations of the electronic and phonon dispersion of GdInO$_3$. The calculations suggest that the GdInO$_3$ lattice is highly frustrated at low temperature. Further, the calculated normal mode frequencies of the Gd related $Γ$ point phonons are found to depend on the magnetic structure of the lattice, suggesting significant magneto-elastic coupling.

cond-mat.mtrl-sci

Mapping of Electronic Band Gap along the Axis of Single InAs/InSbxAs1-x Heterostructured Nanowire

We report the graded electronic band gap along the axis of individual heterostructured WZ-ZB InAs/InSb0.12As0.88 nanowires. Resonance Raman imaging has been exploited to map the axial variation in the second excitation gap energy (E1) at the high symmetry point (L point) of the Brillouin zone. We relate the origin of the observed evolution of the gap energy to the fine tuning of the alloy composition from the tip towards the interface of the nanowire. The electronic band structures of InAs, InSb and InSbxAs1-x alloy systems at x=0.125, 0.25, 0.50, 0.75 and 0.875, using all electron density functional theory code Wien2k, are reported. The measured band gap along the axis of the InAs/InSb0.12As0.88 nanowire is correlated with the calculated gap energy at the A point and the L point of the Brillouin zone for InAs and InSb0.125As0.875, respectively. We draw a one-to-one correspondence between the variation of the E1 gap and the fundamental E0 gap in the calculated electronic band structure and propose the graded fundamental gap energy across the axis of the nanowire.

cond-mat.mes-hall

New perspectives on the fluorite-pyrochlore phase transition in La2Zr2O7 and the importance of local oxygen-related disordered states

The fluorite to pyrochlore phase transition in La2Zr2O7 has been studied in the literature for decades in the context of thermal barrier coatings and reinforcement materials. However, the nature of the phase transition in this system is still not well understood. In this article we have investigated the phase transition in La2Zr2O7, calcined at different temperatures, using powder x-ray diffraction and Raman measurements. Rietveld analyses of the x-ray data suggest a fluorite to pyrochlore phase transition in the system occurring between 1000-1450oC. Nonetheless, Raman spectra, recorded with different excitation wavelengths (λ_ex) reveal that the dynamics of phase transition is different in the near-surface region and in the bulk inside. While the near-surface region carried the signatures of a pure pyrochlore phase, the temperature dependent Raman measurements with λ_ex=785 nm suggest that locally formed oxygen related disordered states are present in the bulk of the system.

cond-mat.mtrl-sci

Mapping of Axial Strain in InAs/InSb Heterostructured Nanowires

The article presents a mapping of the residual strain along the axis of InAs/InSb heterostructured nanowires. Using confocal Raman measurements, we observe a gradual shift in the TO phonon mode along the axis of these nanowires. We attribute the observed TO phonon shift to a residual strain arising from the InAs/InSb lattice mismatch. We find that the strain is maximum at the interface and then monotonically relaxes towards the tip of the nanowires. We also analyze the crystal structure of the InSb segment through selected area electron diffraction measurements and electron diffraction tomography on individual nanowires.

cond-mat.mtrl-sci

Strain induced band alignment in wurtzite-zincblende InAs heterostructured nanowires

We study band alignment in wurtzite-zincblende polytype InAs heterostructured nanowires using temperature dependent resonance Raman measurements. Nanowires having two different wurtzite fractions are investigated. Using visible excitation wavelengths in resonance Raman measurements, we probe the electronic band alignment of these semiconductor nanowires near a high symmetry point of the Brillouin zone (E$_{1}$ gap). The strain in the crystal structure, as revealed from the shift of the phonon mode, explains the observed band alignment at the wurtzite-zincblende interface. Our experimental results are further supported by electronic structure calculations for such periodic heterostructured interface.

cond-mat.mtrl-sci

Electronic Band Structure of Wurtzite GaP Nanowires via Resonance Raman Spectroscopy

Raman measurements are performed on defect-free wurzite GaP nanowires. Resonance Raman measurements are carried out over the excitation energy range between 2.19 and 2.71 eV. Resonances at 2.38 eV and 2.67 eV of the E1(LO) mode and at 2.67 eV of the A1(LO) are observed. The presence of these intensity resonances clearly demonstrates the existence of energy states with Gamma_9hh and Gamma_7V (Gamma_7C) symmetries of the valence (conduction) band and allows to measure WZ phase GaP band energies at the Gamma point. In addition, we have investigated temperature dependent resonant Raman measurements, which allowed us to extrapolate the zero temperature values of Gamma point energies, along with the crystal field and spin-orbit splitting energies. Above results provide a feedback for refining available theoretical calculations to derive the correct wurtzite III-V semiconductor band structure.

cond-mat.mes-hall

Internal field induced enhancement and effect of resonance in Raman scattering of InAs nanowires

An internal field induced resonant intensity enhancement of Raman scattering of phonon excitations in InAs nanowires is reported. The experimental observation is in good agreement with the simulated results for the scattering of light under varying incident wavelengths, originating from the enhanced internal electric field in an infinite dielectric cylinder. Our analysis demonstrates the combined effect of the first higher lying direct band gap energy (E1) and the refractive index of the InAs nanowires in the internal field induced resonant Raman scattering. Furthermore, the difference in the relative contribution of electro-optic effect and deformation potential in Raman scattering of nanowires and bulk InAs over a range of excitation energies is discussed by comparing the intensity ratio of their LO and TO phonon modes.

cond-mat.mes-hall