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A. K. Sood

Publications and source records attributed to A. K. Sood.

At least 19 recordsLinked to original sources

Anomalies in G and 2D Raman Modes of Twisted Bilayer Graphene Near the Magic Angle

The role of twist angle ($θ_t$) in tailoring the physical properties of heterostructures is emerging as a new paradigm in two-dimensional materials. The influence of flat electronic bands near the magic angle ($\sim$1.1$^{\circ}$) on the phononic properties of twisted bilayer graphene (t-BLG) is not well understood. In this work, we systematically investigate the G and 2D Raman modes of t-BLG samples with twist angles ranging from $\sim$0.3$^{\circ}$ to $\sim$3$^{\circ}$ using micro-Raman spectroscopy. A key finding of our work is the splitting of the G mode near the magic angle due to moiré potential induced phonon hybridization. The linewidth of the low-frequency component of the G mode (G$^-$), as well as the main component of the 2D mode, exhibits enhanced broadening near the magic angle due to increased electron-phonon coupling, driven by the emergence of flat electronic bands. Additionally, temperature-dependent Raman measurements (6-300 K) of magic-angle twisted bilayer graphene sample ($θ_t \sim$ 1$^{\circ}$) reveal an almost tenfold increase in phonon anharmonicity-induced temperature variation in both components of the split G mode, as compared to Bernal-stacked bilayer graphene sample, further emphasizing the role of phonon hybridization in this system. These studies could be important for understanding the thermal properties of the twisted bilayer graphene systems.

cond-mat.mes-hall

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

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

Intermediate-range order governs dynamics in dense colloidal liquids

The conventional wisdom is that liquids are completely disordered and lack non-trivial structure beyond nearest-neighbor distances. Recent observations have upended this view and demonstrated that the microstructure in liquids is surprisingly rich and plays a critical role in numerous physical, biological, and industrial processes. However, approaches to uncover this structure are either system-specific or yield results that are not physically intuitive. Here, through single-particle resolved three-dimensional confocal microscope imaging and the use of a recently introduced four-point correlation function, we show that bidisperse colloidal liquids have a highly non-trivial structure comprising alternating layers with icosahedral and dodecahedral order, which extends well-beyond nearest-neighbor distances and grows with supercooling. By quantifying the dynamics of the system on the particle level, we establish that it is this intermediate-range order, and not the short-range order, which has a one-to-one correlation with dynamical heterogeneities, a property directly related to the relaxation dynamics of glassy liquids. Our experimental findings provide a direct and much sought-after link between the structure and dynamics of liquids and pave the way for probing the consequences of this intermediate-range order in other liquid state processes.

cond-mat.soft

Shear jamming and fragility in fractal suspensions under confinement

Under applied stress, the viscosity of many dense particulate suspensions increases drastically, a response known as discontinuous shear-thickening (DST). In some cases, the applied stress can even transform the suspension into a solid-like shear jammed state. Although shear jamming (SJ) has been probed for dense suspensions with particles having well-defined shapes, such a phenomenon for fractal objects has not been explored. Here, using rheology and in situ optical imaging, we study the flow behaviour of ultra-dilute fractal suspensions of multi-walled carbon nanotubes (MWCNT) under confinement. We show a direct transition from flowing to SJ state without a precursory DST in fractal suspensions at an onset volume fraction, $ϕ\sim$ 0.5\%, significantly lower than that of conventional dense suspensions ($ϕ\sim$ 55\%). The ultra-low concentration enables us to demonstrate the fragility and associated contact dynamics of the SJ state, which remain experimentally unexplored in suspensions. Furthermore, using a generalized Wyart-Cates model, we propose a generic phase diagram for fractal suspensions that captures the possibility of SJ without prior DST over a wide range of shear stress and volume fractions.

cond-mat.soft

Pressure-induced superconductivity in weak topological insulator BiSe

Quasi-two-dimensional layered BiSe, a natural super-lattice with Bi2Se3-Bi2-Bi2Se3 units, has recently been predicted to be a dual topological insulator, simultaneously weak topological insulator as well as topological crystalline insulator. Here using structural, transport, spectroscopic measurements and density functional theory calculations, we show that BiSe exhibits rich phase diagram with the emergence of superconductivity with Tc ~8K under pressure. Sequential structural transitions into SnSe-type energetically tangled orthorhombic and CsCl-type cubic structures having distinct superconducting properties are identified at 8 GPa and 13 GPa respectively. Our observation of weak-antilocalization in magneto-conductivity suggests that spin-orbit coupling (SOC) plays a significant role in retaining non-trivial band topology in the trigonal phase with possible realization of 2D topological superconductivity. Theoretical analysis reveals that SOC significantly enhances superconducting Tc of the high-pressure cubic phase through an increase in electron-phonon coupling strength. Simultaneous emergence of Dirac-like surface states suggests cubic BiSe as a suitable candidate for the 3D-topological superconductor.

cond-mat.supr-con

Active nonreciprocal attraction between motile particles in an elastic medium

We show from experiments and simulations on vibration-activated granular matter that self-propelled polar rods in an elastic medium on a substrate turn and move towards each other. We account for this effective attraction through a coarse-grained theory of a motile particle as a moving point-force density that creates elastic strains in the medium that reorient other particles. Our measurements confirm qualitatively the predicted features of the distortions created by the rods, including the $|x|^{-1/2}$ tail of the trailing displacement field and non-reciprocal sensing and pursuit. A discrepancy between the magnitudes of displacements along and transverse to the direction of motion remains. Our theory should be of relevance to the interaction of motile cells in the extracellular matrix or in a supported layer of gel or tissue.

cond-mat.soft

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

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

Negative differential resistance state in the free-flux-flow regime of driven vortices in a single crystal of 2H-NbS$_2$

Time series measurements in 2H-NbS$_2$ crystal had unravelled a drive induced transition wherein the critical current (Ic) changes from a low to a high Ic jammed vortex state, via a negative differential resistance (NDR) transition. Here, using multiple current (I) - voltage (V) measurement cycles, we explore the statistical nature of observing the NDR transition in the free-flux-flow (FF) regime in a single crystal of 2H-NbS$_2$. The probability of observing the NDR transition always remains finite for a vortex state created with either fast or slow rate of magnetic field. The probability of observing the NDR transition in the FF regime is found to systematically increase with magnetic field (B) in weak collective pinning regime. In the strong pinning regime, the said probability becomes B-independent. We show that the higher Ic state is unique and cannot be accessed via any conventional route. While the I-V curves do not distinguish between zero field cooled (ZFC) and field cooled (FC) modes of preparing the vortex state, the probability for observing an NDR transition has different B-dependences for the vortex matter prepared in the ZFC and FC modes. We find that the NDR occurs in a high dissipation regime, where the flow resistivity is well above the theoretical value expected in the FF regime. We understand our results on the basis of a rapid drop in vortex viscosity at high drives in 2H-NbS$_2$, which triggers a rapid increase in the vortex velocity and reorganization in the moving vortex matter leading to a dynamical unstable vortex flow. This dynamical instability leads to the NDR transition into a high entropy vortex state with high Ic.

cond-mat.supr-con

Dipole alignment of water molecules flowing through a carbon nanotube

The fast flow rate of water through nanochannels has promising applications in desalination, energy conversion, and nanomedicine. We have used molecular dynamics simulations to show that the water molecules passing through a wide single-walled carbon nanotube (CNT) cavity get aligned by flow to have a net dipole moment along the flow direction. With increasing flow velocity, the net dipole moment first increases and eventually saturates to a constant value. This behavior is similar to the Langevin theory of paraelectricity with the flow velocity acting as an effective aligning field. We show conclusively that the microscopic origin of this behavior is the preferential entry of water molecules with their dipole vectors pointing inward along the CNT axis.

cond-mat.soft

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

Synergistic action in colloidal heat engines coupled by non-conservative flows

Collective operation of multiple engines to achieve a common objective is a vital step in the design of complex machines. Recent studies have reduced the length scales of engine design to micro and nanometers. While strategies to build complex machines from these remain to be devised, even the basic design principles remain obscure. Here, we construct and analyze the simplest collection of two engines from a pair of colloidal microspheres in optical traps at close separation. We demonstrate that at such proximity, non-conservative scattering forces that were hitherto neglected, affect the particle motion and hydrodynamics arising from dissipating these results in violating zeroth law of thermodynamics. Leveraging this in a manner analogous to microswimmers and active Brownian particles, we show that a collection of two interacting engines outperform those that are well separated. While these results explore the simplest case of two engines, the underlying concepts could aid in designing larger collections akin to biological systems.

cond-mat.soft

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

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

Imaging the coherent propagation of collective modes in the excitonic insulator candidate Ta$_2$NiSe$_5$ at room temperature

Excitonic insulators host a condensate of electron-hole pairs at equilibrium, giving rise to collective many-body effects. Although several materials have emerged as excitonic insulator candidates, evidence of long-range coherence is lacking and the origin of the ordered phase in these systems remains controversial. Here, using ultrafast pump-probe microscopy, we investigate the possible excitonic insulator Ta$_2$NiSe$_5$. Below 328 K, we observe the anomalous micrometer-scale propagation of coherent modes at velocities of the order of $\sim10^5$ m/s, which we attribute to the hybridization between phonon modes and the phase mode of the condensate. We develop a theoretical framework to support this explanation and propose that electronic interactions provide a significant contribution to the ordered phase in Ta$_2$NiSe$_5$. These results allow us to understand how the condensate's collective modes transport energy and interact with other degrees of freedom. Our study provides a unique paradigm for the investigation and manipulation of these properties in strongly correlated materials.

cond-mat.str-el

Shear-induced ordering of nano-pores and instabilities in concentrated surfactant mesh phases

Mixed surfactant systems with strongly bound counterions show many interesting phases such as the random mesh phase consisting of a disordered array of defects (water-filled nano-pores in the bilayers). The present study addresses the non-equilibrium phase transition of the random mesh phase under shear to an ordered mesh phase with a high degree of coherence between nano-pores in three-dimension. In-situ small-angle synchrotron X-ray study under different shear stress conditions shows sharp Bragg peaks in the X-ray diffraction, successfully indexed to the rhombohedral lattice with R$\bar{3}$m space group symmetry. The ordered mesh phase shows isomorphic twinning and buckling at higher shear stress. Our experimental studies bring out rich non-equilibrium phase transitions in concentrated cationic surfactant systems with strongly bound counterions hitherto not well-explored and provide motivation for a quantitative understanding.

cond-mat.soft

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