arXiv subjects

Satyendra Nath Gupta

Publications and source records attributed to Satyendra Nath Gupta.

12 recordsLinked to original sources

arXiv2025

New plasmon-like mode in PdTe$_{2}$: Raman scattering and memory function study

PdTe$_2$ is a type II Dirac semimetal that has garnered significant attention due to its intriguing electronic and topological properties. Here, we report temperature dependent Raman scattering study of PdTe$_2$ in the temperature range from 10 K to 300 K. Our study reveals emergence of a new unreported peak below 100 K, centered around 250 cm$^{-1}$. We argue that the new mode is not a phonon mode because the Raman spectra calculated using Density Functional Theory shows only two intense peaks at 85 $ cm^{-1}$ and 128 $cm^{-1}$. To ascertain the origin of this new peak, we constructed a microscopic model of electrons coupling to a single plasmon mode at 250 $cm^{-1}$ and using the memory function formalism, we obtained that the Raman relaxation rate is linear in frequency. We also performed phenomenological analysis of the Raman response from the experimental data and computed frequency dependent Raman relaxation rate, which is also found to exhibit a linear dependence on frequency. With the congruence of our theoretical and phenomenological results we could ascertain that the new mode observed at low temperatures is indeed a plasmon-like mode. Further, phonon frequencies and line widths of the two phonon modes exhibit anomalous behavior above 100 K.

cond-mat.str-el↗

arXiv2022

Higher-Order Photon Statistics as a New Tool to Reveal Hidden Excited States in a Plasmonic Cavity

Among the best known quantities obtainable from photon correlation measurements are the $g^{(m)}$~correlation functions. Here, we introduce a new procedure to evaluate these correlation functions based on higher-order factorial cumulants $C_{\text{F},m}$ which integrate over the time dependence of the correlation functions, i.e., summarize the available information at different time spans. In a systematic manner, the information content of higher-order correlation functions as well as the distribution of photon waiting times is taken into account. Our procedure greatly enhances the sensitivity for probing correlations and, moreover, is robust against a limited counting efficiency and time resolution in experiment. It can be applied even in case $g^{(m)}$ is not accessible at short time spans. We use the new evaluation scheme to analyze the photon emission of a plasmonic cavity coupled to a single quantum dot. We derive criteria which must hold if the system can be described by a generic Jaynes-Cummings model. A violation of the criteria can be explained by the presence of an additional excited quantum dot state.

cond-mat.mes-hall↗

arXiv2021

Pressure-induced 1T to 3R structural phase transition in metallic VSe2: X-ray diffraction and first-principles theory

We study pressure-induced structural evolution of vanadium diselenide (VSe2), a 1T polymorphic member of the transition metal di-chalcogenide (TMD) family using synchrotron-based powder X-ray diffraction (PXRD) and first-principles density functional theory (DFT). Our XRD results reveal anomalies at P ~4 GPa in c/a ratio, V-Se bond length and Se-V-Se bond angle signalling an isostructural transition. This is followed by a first order structural transition from 1T (space group P-3m1) phase to a 3R (space group R-3m) phase at P ~11 GPa due to sliding of adjacent Se-V-Se layers. We present various scenarios to understand the experimental results within DFT and find that the 1T to 3R transition can be captured only after inclusion of enthalpic correction associated with errors in cell volume with underestimated transition pressure. The abrupt increase in the Debye-Waller factors of Se atoms by a factor of ~4 and hence the anharmonic effects across the structural transition pressure are hitherto not reported so far and hint a possible way to understand the mismatch between the experimental and theoretical transition pressure values.

cond-mat.mtrl-sci↗

arXiv2021

Complex plasmon-exciton dynamics revealed through quantum dot light emission in a nanocavity

Plasmonic cavities can confine electromagnetic radiation to deep sub-wavelength regimes. This facilitates strong coupling phenomena to be observed at the limit of individual quantum emitters. Here we report an extensive set of measurements of plasmonic cavities hosting one to a few semiconductor quantum dots. Scattering spectra show Rabi splitting, demonstrating that these devices are close to the strong coupling regime. Using Hanbury Brown and Twiss interferometry, we observe non-classical emission, allowing us to directly determine the number of emitters in each device. Surprising features in photoluminescence spectra point to the contribution of multiple excited states. Using model simulations based on an extended Jaynes Cummings Hamiltonian, we find that the involvement of a dark state of the quantum dots explains the experimental findings. The coupling of quantum emitters to plasmonic cavities thus exposes complex relaxation pathways and emerges as an unconventional means to control dynamics of quantum states.

cond-mat.mes-hall↗

arXiv2020

Vacuum Rabi splitting of a dark plasmonic cavity mode revealed by fast electrons

Recent years have seen a growing interest in strong coupling between plasmons and excitons, as a way to generate new quantum optical testbeds and influence chemical dynamics and reactivity. Strong coupling to bright plasmonic modes has been achieved even with single quantum emitters. Dark plasmonic modes fare better in some applications due to longer lifetimes, but are difficult to probe as they are subradiant. Here, we apply electron energy loss (EEL) spectroscopy to demonstrate that a dark mode of an individual plasmonic bowtie can interact with a small number of quantum emitters, as evidenced by Rabi-split spectra. Coupling strengths of up to 85 meV place the bowtie-emitter devices at the onset of the strong coupling regime. Remarkably, the coupling occurs at the bowtie gap periphery, even while the electron beam probes their center. Our findings pave the way for using EEL spectroscopy to study exciton-plasmon interactions involving non-emissive photonic modes.

cond-mat.mes-hall↗

arXiv2019

Plasmon-induced efficient hot carrier generation in graphene on gold ultrathin film with periodic array of holes: Ultrafast pump-probe spectroscopy

Using ultrafast pump-probe reflectivity with 3.1 eV pump and coherent white light probe (1.1 to 2.6 eV), we show that graphene on gold nanostructures exhibits a strong coupling to the plasmonic resonances of the ordered lattice hole array, thus injecting a high density of hot carriers in graphene through plasmons. The system being studied is single-layer graphene on ultrathin film of gold with periodic arrangements of holes showing anomalous transmission. A comparison is made with gold film with and without hole array. By selectively probing transient carrier dynamics in the spectral regions corresponding to plasmonic resonances, we show efficient plasmon-induced hot carrier generation in graphene. We also show that due to high electromagnetic field intensities at the edge of the sub-micron holes, fast decay time (10-100 fs) and short decay length (1 nm) of plasmons, a highly confined density of hot carriers (very close to edge of the holes) is generated by Landau damping of plasmons within the holey gold film. A contribution to transient decay dynamics due to diffusion of initial non-uniform distribution of hot carriers away from the hole edges is observed. Our results are important for future applications of novel hot carrier device concepts where hot carriers with tunable energy can be generated in different graphene regions connected seamlessly.

cond-mat.mes-hall↗

arXiv2017

Pressure-induced Lifshitz transition in NbP: Raman, x-ray diffraction, electrical transport and density functional theory

We report high pressure Raman, synchrotron x-ray diffraction and electrical transport studies on Weyl semimetals NbP and TaP along with first-principles density functional theoretical (DFT) analysis. The frequencies of first-order Raman modes of NbP harden with increasing pressure and exhibit a slope change at P$_c$ $\sim$ 9 GPa, and its resistivity exhibits a minimum at P$_c$. The pressure-dependent volume of NbP exhibits a change in its bulk modulus from 207 GPa to 243 GPa at P$_c$. Using DFT calculations, we show that these anomalies are associated with pressure induced Lifshitz transition which involves appearance of electron and hole pockets in its electronic structure. In contrast, results of Raman and synchrotron x-ray diffraction experiments on TaP and DFT calculations show that TaP is quite robust under pressure and does not undergo any phase transition.

cond-mat.mtrl-sci↗

arXiv2017

Raman anomalies as signatures of pressure induced electronic topological and structural transitions in black phosphorus: Experiments and Theory

We report high pressure Raman experiments of Black phosphorus up to 24 GPa. The line widths of first order Raman modes A$^1_g$, B$_{2g}$ and A$^2_g$ of the orthorhombic phase show a minimum at 1.1 GPa. Our first-principles density functional analysis reveals that this is associated with the anomalies in electron-phonon coupling at the semiconductor to topological insulator transition through inversion of valence and conduction bands marking a change from trivial to nontrivial electronic topology. The frequencies of B$_{2g}$ and A$^2_g$ modes become anomalous in the rhombohedral phase at 7.4 GPa, and new modes appearing in the rhombohedral phase show anomalous softening with pressure. This is shown to originate from unusual structural evolution of black phosphorous with pressure, based on first-principles theoretical analysis.

cond-mat.str-el↗

arXiv2016

Spin liquid like Raman signatures in hyperkagome iridate Na$_4$Ir$_3$O$_8$

Combining Raman scattering measurements with mean field calculations of the Raman response we show that Kitaev-like magnetic exchange is dominant in the hyperkagome iridate Na$_4$Ir$_3$O$_8$. In the measurements we observe a broad Raman band at $\sim$~3500 cm$^{-1}$ with a band-width $\sim 1700$~cm$^{-1}$. Calculations of the Raman response of the Kitaev-Heisenberg model on the hyperkagome lattice shows that the experimental observations are consistent with calculated Raman response where Kitaev exchange interaction ($J_K$) is much larger than the Heisenberg term J$_1$ ($J_1/J_K \sim 0.1$). A comparison with the theoretical model gives an estimate of the Kitaev exchange interaction parameter.

cond-mat.str-el↗

arXiv2016

Metallic monoclinic phase in VO$_2$ induced by electrochemical gating: in-situ Raman study

We report in-situ Raman scattering studies of electrochemically top gated VO$_2$ thin film to address metal-insulator transition (MIT) under gating. The room temperature monoclinic insulating phase goes to metallic state at a gate voltage of 2.6 V. However, the number of Raman modes do not change with electrolyte gating showing that the metallic phase is still monoclinic. The high frequency Raman mode A$_g$(7) near 616 cm$^{-1}$ ascribed to V-O vibration of bond length 2.06 Å~ in VO$_6$ octahedra hardens with increasing gate voltage and the B$_g$(3) mode near 654 cm$^{-1}$ softens. This shows that the distortion of the VO$_6$ octahedra in the monoclinic phase decreases with gating. The time dependent Raman data at fixed gate voltages of 1 V (for 50 minute, showing enhancement of conductivity by a factor of 50) and 2 V (for 130 minute, showing further increase in conductivity by a factor of 5) show similar changes in high frequency Raman modes A$_g$(7) and B$_g$(3) as observed in gating. This slow change in conductance together with Raman frequency changes show that the governing mechanism for metalization is more likely to the diffusion controlled oxygen vacancy formation due to the applied electric field.

cond-mat.str-el↗

arXiv2016

Raman Signatures of Strong Kitaev Exchange Correlations in (Na$_{1-x}$Li$_x$)$_2$IrO$_3$ : Experiments and Theory

Inelastic light scattering studies on single crystals of (Na$_{1-x}$Li$_x$)$_2$IrO$_3$ ($x = 0, 0.05$ and $0.15$) show a polarization independent broad band at $\sim $~2750 cm$^{-1}$ with a large band-width $\sim 1800$~cm$^{-1}$. For Na$_2$IrO$_3$ the broad band is seen for temperatures $ \leq 200$~K and persists inside the magnetically ordered state. For Li doped samples, the intensity of this mode increases, shifts to lower wave-numbers and persists to higher temperatures. Such a mode has recently been predicted (Knolle et.al.) as a signature of the Kitaev spin liquid. We assign the observation of the broad band to be a signature of strong Kitaev-exchange correlations. The fact that the broad band persists even inside the magnetically ordered state suggests that dynamically fluctuating moments survive even below $T_{N}$. This is further supported by our mean field calculations. The Raman response calculated in mean field theory shows that the broad band predicted for the spin liquid state survives in the magnetically ordered state near the zigzag-spin liquid phase boundary. A comparison with the theoretical model gives an estimate of the Kitaev exchange interaction parameter to be $J_K\approx 57$~meV.

cond-mat.str-el↗

arXiv2016

Electron-Hole Asymmetry in the Electron-phonon Coupling in Top-gated Phosphorene Transistor

Using in-situ Raman scattering from phosphorene channel in an electrochemically top-gated field effect transistor, we show that its phonons with A$_g$ symmetry depend much more strongly on concentration of electrons than that of holes, while the phonons with B$_g$ symmetry are insensitive to doping. With first-principles theoretical analysis, we show that the observed electon-hole asymmetry arises from the radically different constitution of its conduction and valence bands involving $π$ and $σ$ bonding states respectively, whose symmetry permits coupling with only the phonons that preserve the lattice symmetry. Thus, Raman spectroscopy is a non-invasive tool for measuring electron concentration in phosphorene-based nanoelectronic devices.

cond-mat.mes-hall↗