arXiv subjects

D. V. S. Muthu

Publications and source records attributed to D. V. S. Muthu.

At least 19 recordsLinked to original sources

arXiv2024

Ultrafast Dynamics of Coherent Phonon Modes in Excitonic Insulator Ta$_2$NiSe$_5$

The spontaneous condensation of excitons in the excitonic insulating phase has been reported in Ta$_2$NiSe$_5$ below 325 K. In this context, we present the temperature-dependent optical pump optical probe spectroscopy of Ta$_2$NiSe$_5$, with a focus on coherent phonon dynamics. In addition to the fast relaxation process involving excitonic recombination, we observe a systematic behavior for the slow relaxation process associated with the relaxation of hot phonons. The asymmetry parameter and cubic anharmonicity of the 3 THz mode demonstrate the structural transition across T$_C$=325 K, whereas the order parameter nature and asymmetry of 2 THz modes reveal its coupling with the excitonic phase of Ta$_2$NiSe$_5$. Coherent phonon modes display less anharmonicity compared to the corresponding Raman modes. Continuous Wavelet Transform (CWT) reveals that the peak time t$_{peak}$ of phonons is similar for all modes except the 3 THz mode. The temperature dependence of t$_{peak}$ for the M3 mode exhibits a possible role of excitonic condensate below T$_c$ in the formation of quasiparticle (phonon). CWT analysis supports the time-dependent asymmetry of the M3 mode caused by photoexcited carriers. This study illustrates the role of photoexcited carriers in depicting a structural transition and dressing of coherent phonons and, hence, demonstrating many-body effects.

cond-mat.mtrl-sci↗

arXiv2024

Ultrafast Spectroscopy of Dirac Semimetal Cd3As2 under Pressure

Topological properties of a three-dimensional Dirac semimetal Cd3As2, protected by crystal rotation and time-reversal symmetry, can be tuned with the application of pressure. Ultrafast spectroscopy is a unique tool to investigate the character and time evolution of electronic states, emphasizing the signatures of transition. We designed an experimental setup for in-situ pressure-dependent ultrafast optical pump optical probe spectroscopy of Cd3As2 using a symmetric diamond anvil cell. The fast relaxation processes show significant changes across pressure-induced phase transitions at PC1, approximately 3 GPa, and PC2, approximately 9 GPa. A new sub-picosecond time scale relaxation dynamics emerges beyond PC2. Theoretical calculations of differential reflectivity for both interband and intraband processes indicate that the negative (positive) differential reflectivity (Delta R/R) results from the interband (intraband) processes. The pressure-dependent behavior of relaxation dynamics amplitudes beyond PC1 emphasized the necessity of incorporating quadratic band opening in the calculations, explaining the transition of Cd3As2 from a Dirac semimetal to a semiconducting phase. The time evolution of differential reflectivity is calculated using the electronic temperature as a function of time, as provided by the two-temperature model, which fits the experimental data.

cond-mat.mtrl-sci↗

arXiv2024

Pressure-induced phase transition in pyrochlore iridates (Sm$_{1-x}$Bi$_x$)$_2$Ir$_2$O$_7$ ($x =$ 0, 0.02, and 0.10): Raman and X-ray diffraction studies

The pyrochlore iridates, A$_2$Ir$_2$O$_7$, show a wide variety of structural, electronic, and magnetic properties controlled by the interplay of different exchange interactions, which can be tuned by external pressure. In this work, we report pressure-induced phase transitions at ambient temperature using synchrotron-based X-ray diffraction (up to ~ 20 GPa) and Raman-scattering measurements (up to ~ 25 GPa) of the pyrochlore series (Sm$_{1-x}$Bi$_x$)$_2$Ir$_2$O$_7$ ($x =$ 0, 0.02, and 0.10). Our Raman and X-ray data suggest an iso-structural transition in Sm$_2$Ir$_2$O$_7$ at Pc ~ 11.2 GPa associated with the rearrangement of IrO6 octahedra in the pyrochlore lattice. The transition pressure decreases to ~ 10.2 and 9 GPa for $x =$ 0.02 and 0.10, respectively. For all the samples, the linewidth of three phonons associated with Ir-O-Ir (A1g and Eg) and Ir-O (T$_2$g$_4$) vibrations show anomalous decrease up to Pc, due to decrease in electron-phonon interaction.

cond-mat.mtrl-sci↗

arXiv2023

Strong coupling of lattice and orbital excitations in quantum magnet Ca$_{10}$Cr$_7$O$_{28}$: Anomalous temperature dependence of Raman phonons

We report low-temperature Raman signatures of the Heisenberg quantum magnet Ca$_{10}$Cr$_7$O$_{28}$, showing clear anomalies in phonon mode frequencies and linewidths below $\sim$100 K. This crossover temperature lies in between the Jahn-Teller (JT) temperature scale ($>$ room temperature) and the temperature scale associated with the spin exchange interactions ($<$ 12 K). Our experimental observation is well captured by a novel secondary JT transition associated with a cooperative reorientation of the orbitals giving rise to anomalies in the temperature dependence of Raman frequencies and linewidths. Such orbital reorganisation, in turn, affects the spin-spin exchange interactions that decide the fate of the magnet at lower temperatures and hence provide important clues to understand the energetics of the possible lower temperature quantum paramagnetic phase.

cond-mat.str-el↗

arXiv2022

Pressure tuning of structure, magnetic frustration and carrier conduction in Kitaev spin liquid candidate Cu$_2$IrO$_3$: X-ray, Raman, magnetic susceptibility, resistivity and first-principles analysis

The layered honeycomb lattice iridate Cu$_2$IrO$_3$ is the closest realization of the Kitaev quantum spin liquid, primarily due to the enhanced interlayer separation and nearly ideal honeycomb lattice. We report pressure-induced structural evolution of Cu$_2$IrO$_3$ by powder x-ray diffraction (PXRD) up to $\sim$17 GPa and Raman scattering measurements up to $\sim$25 GPa. A structural phase transition (monoclinic $C2/c \: \rightarrow$ triclinic $P\bar{1}$) is observed with a broad mixed phase pressure range ($\sim$4 to 15 GPa). The triclinic phase consists of heavily distorted honeycomb lattice with Ir-Ir dimer formation and a collapsed interlayer separation. In the stability range of the low-pressure monoclinic phase, structural evolution maintains the Kitaev configuration up to 4 GPa. This is supported by the observed enhanced magnetic frustration in dc susceptibility without emergence of any magnetic ordering and an enhanced dynamic Raman susceptibility. High-pressure resistance measurements up to 25 GPa in the temperature range 1.4--300 K show resilient non-metallic $R$($T$) behaviour with significantly reduced resistivity in the high-pressure phase. The Mott 3D variable-range-hopping conduction with much reduced characteristic energy scale $T_0$ suggests that the high-pressure phase is at the boundary of localized-itinerant crossover. Using first-principles density functional theoretical (DFT) calculations, we find that at ambient pressure $\rm Cu_2IrO_3$ exists in monoclinic $P2_1/c$ phase which is energetically lower than $C2/c$ phase (both the structures are consistent with experimental XRD pattern). DFT reveals structural transition from $P2_1/c$ to $P\bar{1}$ structure at 7 GPa (involving dimerization of Ir-Ir bonds) in agreement with experimentally observed transition pressure.

cond-mat.str-el↗

arXiv2022

Raman fingerprints of fractionalized Majorana excitations in honeycomb iridate Ag$_3$LiIr$_2$O$_6$

We report low-temperature (down to $\sim$5 K) Raman signatures of the recently discovered intercalated honeycomb magnet Ag$_3$LiIr$_2$O$_6$, a putative Kitaev quantum spin liquid (QSL) candidate. The Kitaev QSL is predicted to host Majorana fermions as its emergent elementary excitations through a thermal fractionalization of entangled spins $S = 1/2$. We observe evidence of this fractionalization in the low-energy magnetic continuum whose temperature evolution harbours signatures of the predicted Fermi statistics obeyed by the itinerant Majorana quasiparticles. The magnetic Raman susceptibility evinces a crossover from the conventional to a Kitaev paramagnetic state below the temperature of $\sim$80 K. Additionally, the development of the Fano asymmetry in the low frequency phonon mode and the enhancement of integrated Raman susceptibilities below the crossover temperature signifies prominent coupling between the vibrational and Majorana fermionic excitations.

cond-mat.str-el↗

arXiv2021

Raman and first-principles study of the pressure induced Mott-insulator to metal transition in bulk FePS$_3$

Recently discovered class of 2D materials based on transition metal phosphorous trichalcogenides exhibit antiferromagnetic ground state, with potential applications in spintronics. Amongst them, FePS$ _{3} $ is a Mott insulator with a band gap of $\sim$ 1.5 eV. This study using Raman spectroscopy along with first-principles density functional theoretical analysis examines the stability of its structure and electronic properties under pressure. Raman spectroscopy reveals two phase transitions at 4.6 GPa and 12 GPa marked by the changes in pressure coefficients of the mode frequencies and the number of symmetry allowed modes. FePS$_3$ transforms from the ambient monoclinic C2/m phase with a band gap of 1.54 eV to another monoclinic C2/m (band gap of 0.1 eV) phase at 4.6 GPa, followed by another transition at 12 GPa to the metallic trigonal P-31m phase. Our work complements recently reported high pressure X-ray diffraction studies.

cond-mat.mtrl-sci↗

arXiv2021

Thickness dependent transition from the 1T$^\prime$ to Weyl semimetal phase in ultrathin MoTe$ _{2} $: Electrical transport, Noise and Raman studies

Bulk 1T$^\prime$-MoTe$_2$ shows a structural phase transition from 1T$^\prime$ to Weyl semimetallic (WSM) $ T_{d} $ phase at $\sim$ 240 K. This phase transition and transport properties in the two phases have not been investigated on ultra-thin crystals. Here we report electrical transport, $1/f$ noise and Raman studies in ultra-thin 1T$^\prime$-MoTe$_2$ ($\sim$ 5 to 16 nm thick) field-effect transistors (FETs) devices as a function of temperature. The electrical resistivities for thickness 16 nm and 11 nm show maxima at temperatures 208 K and 178 K, respectively, making a transition from semiconducting to semi-metallic phase, hitherto not observed in bulk samples. Raman frequencies and linewidths for 11nm thick crystal show change around 178 K, attributed to additional contribution to the phonon self-energy due to enhanced electron-phonon interaction in the WSM phase. Further, the resistivity at low-temperature shows an upturn below 20 K along with the maximum in the power spectral density of the low frequency $1/f$ noise. The latter rules out the metal-insulator transition (MIT) being responsible for the upturn of resistivity below 20 K. The low temperature resistivity follows $ρ\propto 1/T$, changing to $ρ\propto T$ with increasing temperature supports electron-electron interaction physics at electron-hole symmetric Weyl nodes below 20 K. These observations will pave the way to unravel the properties of WSM state in layered ultra-thin van der Waals materials.

cond-mat.mes-hall↗

arXiv2021

Symmetry induced phonon renormalization in few layers of 2H-MoTe$_2$ transistors: Raman and first-principles studies

Understanding of electron-phonon coupling (EPC) in two dimensional (2D) materials manifesting as phonon renormalization is essential to their possible applications in nanoelectronics. Here we report in-situ Raman measurements of electrochemically top-gated 2, 3 and 7 layered 2H-MoTe$ _{2} $ channel based field-effect transistors (FETs). While the E$ ^{1}_{2g} $ and B$ _{2g} $ phonon modes exhibit frequency softening and linewidth broadening with hole doping concentration (\textit{p}) up to $\sim$ 2.3 $\times$10$ ^{13} $/cm$ ^{2} $, A$ _{1g}$ shows relatively small frequency hardening and linewidth sharpening. The dependence of frequency renormalization of the E$ ^{1}_{2g} $ mode on the number of layers in these 2D crystals confirms that hole doping occurs primarily in the top two layers, in agreement with recent predictions. We present first-principles density functional theory (DFT) analysis of bilayer MoTe$ _{2} $ that qualitatively captures our observations, and explain that a relatively stronger coupling of holes with E$ ^{1}_{2g} $ or B$ _{2g} $ modes as compared with the A$ _{1g} $ mode originates from the in-plane orbital character and symmetry of the states at valence band maximum (VBM). The contrast between the manifestation of EPC in monolayer MoS$ _{2} $ and those observed here in a few-layered MoTe$ _{2} $ demonstrates the role of the symmetry of phonons and electronic states in determining the EPC in these isostructural systems.

cond-mat.mes-hall↗

arXiv2021

Doping controlled Fano resonance in bilayer 1T$ ^{\prime} $-ReS$ _{2} $: Raman experiments and first-principles theoretical analysis

In the bilayer ReS$ _{2} $ channel of a field-effect transistor (FET), we demonstrate using Raman spectroscopy that electron doping (n) results in softening of frequency and broadening of linewidth of the in-plane vibrational modes, leaving out-of-plane vibrational modes unaffected. Largest change is observed for the in-plane Raman mode at $\sim$ 151 cm$^{-1} $, which also shows doping induced Fano resonance with the Fano parameter 1/q = -0.17 at doping concentration of $\sim 3.7\times10^{13}$ cm$^{-2} $. A quantitative understanding of our results is provided by first-principles density functional theory (DFT), showing that the electron-phonon coupling (EPC) of in-plane modes is stronger than that of out-of-plane modes, and its variation with doping is independent of the layer stacking. The origin of large EPC is traced to 1T to 1T$ ^{\prime} $ structural phase transition of ReS$ _{2} $ involving in-plane displacement of atoms whose instability is driven by the nested Fermi surface of the 1T structure. Results are also compared with the isostructural trilayer ReSe$ _{2} $.

cond-mat.mes-hall↗

arXiv2021

Probing signatures of fractionalization in candidate quantum spin liquid Cu2IrO3 via anomalous Raman scattering

Long-range entanglement in quantum spin liquids (QSLs) lead to novel low energy excitations with fractionalised quantum numbers and (in 2D) statistics. Experimental detection and manipulation of these excitations present a challenge particularly in view of diverse candidate magnets. A promising probe of fractionalisation is their coupling to phonons. Here we present Raman scattering results for the S = 1/2 honeycomb iridate Cu2IrO3, a candidate Kitaev QSL with fractionalised Majorana fermions and Ising flux excitations. We observe anomalous low temperature frequency shift and linewidth broadening of the Raman intensities in addition to a broad magnetic continuum both of which, we derive, are naturally attributed to the phonon decaying into itinerant Majoranas. The dynamic Raman susceptibility marks a crossover from the QSL to a thermal paramagnet at ~120 K. The phonon anomalies below this temperature demonstrate a strong phonon-Majorana coupling. These results provide for evidence of spin fractionalisation in Cu2IrO3.

cond-mat.str-el↗

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

Magnetic and electronic ordering phenomena in the [Ru$_2$O$_6$] honeycomb lattice compound AgRuO$_3$

The silver ruthenium oxide AgRuO$_3$ consists of honeycomb [Ru$_2^{5+}$O$_6^{2-}$] layers, and can be considered an analogue of SrRu$_2$O$_6$ with a different intercalation stage. We present measurements of magnetic susceptibility and specific heat on AgRuO$_3$ single crystals which reveal a sharp antiferromagnetic transition at 342(3)K. The electrical transport in single crystals of AgRuO$_3$ is determined by a combination of activated conduction over an intrinsic semiconducting gap of $\approx$ 100 meV and carriers trapped and thermally released from defects. From powder neutron diffraction data a Néel-type antiferromagnetic structure with the Ru moments along the $c$ axis is derived. Raman and muon spin rotation spectroscopy measurements on AgRuO$_3$ powder samples indicate a further weak phase transition or a crossover in the temperature range 125-200 K. The transition does not show up in magnetic susceptibility and its origin is argued to be related to defects but cannot be fully clarified. The experimental findings are complemented by DFT-based electronic structure calculations. It is found that the magnetism in AgRuO$_3$ is similar to that of SrRu$_2$O$_6$, however with stronger intralayer and weaker interlayer magnetic exchange interactions.

cond-mat.str-el↗

arXiv2020

Tuning the structure of Skyrmion lattice system Cu2OSeO3 under pressure

The insulating ferrimagnet Cu2OSeO3 shows a rich variety of phases such as skyrmion lattice and helical magnetism controlled by interplay of different exchange interactions which can be tuned by external pressure. In this work we have investigated pressure-induced phase transitions at room temperature using synchrotron based x- ray diffraction and Raman scattering measurements. With first-principles theoretical analysis, we show that spin-spin exchange couplings in the ambient cubic phase are affected notably by hydrostatic pressure. The ambient cubic phase transforms to a monoclinic phase above 7 GPa and then to the triclinic phase above 11 GPa. Emergence of new phonon modes in the Raman spectra confirms these structural phase transitions. Notably, upon decompression, the crystal undergoes transition to a new monoclinic structure. Atomic coordinates have been refined in the low pressure cubic phase to capture the Cu-tetrahedra evolution responsible for the earlier reported magnetic behavior under pressure. Our experiments will motivate further studies of its emergent magnetic behavior under pressure.

cond-mat.mtrl-sci↗

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↗