arXiv subjects

Surjeet Singh

Publications and source records attributed to Surjeet Singh.

At least 19 recordsLinked to original sources

arXiv2026

Microscopic Origin of Random Singlet Behavior in B-site Disordered Spin-1/2 Perovskite BaCu_1/3Nb_2/3O_3 Revealed by EXAFS and Thermodynamics

We report a combined structural and thermodynamic study of the ABO$_3$-type disordered perovskite BaCu$_{1/3}$Nb$_{2/3}$O$_3$ (BCNO), whose B site is jointly occupied by Cu and Nb in the $1:2$ ratio. Using synchrotron powder x-ray diffraction (XRD) and x-ray absorption fine structure (XAFS) spectroscopy, we investigate the microscopic nature of Cu$^{2+}$/Nb$^{5+}$ disorder on the pseudo-cubic B-sublattice and its relation to the emergent random-singlet (RS) behavior evidenced at low temperatures. While XRD reveals no long-range Cu/Nb ordering and average site occupancy consistent with stoichiometry, XAFS reveals a peculiar local chemical order characterized by preferential heteroatomic Cu$:$Nb correlations. This local arrangement strongly suppresses direct Cu$:$Cu linkages, despite the Cu concentration being close to the percolation threshold of a cubic lattice. The resulting exchange network explains the absence of spin-glass freezing or long-range magnetic order in the presence of substantial antiferromagnetic interactions, as indicated by a Curie-Weiss temperature $Θ_{CW}\approx -50$ K. Instead, the magnetic susceptibility $χ(T)$ and specific heat $c_p(T)$ exhibit power-law behavior and characteristic single-parameter $T/H$ scaling over broad temperature and magnetic-field ranges, consistent with random-singlet phenomenology. Notably, at very low temperatures, the specific heat behavior transitions from $T^{1-γ}$ ($γ\approx 0.6$ from the $T/H$ scaling) in zero-field to a T-linear dependence under high field, indicating a crossover to a distinct low-energy regime whose microscopic origin remains to be established.

cond-mat.str-el↗

arXiv2026

Emergent Random Spin Singlets in Disordered Spin-1/2 perovskite BaCu$_{1/3}$Ta$_{2/3}$O$_3$

We investigate the disordered perovskite BaCu$_{1/3}$Ta$_{2/3}$O$_3$, where Cu (spin-1/2) and Ta randomly occupy a pseudo-cubic lattice. Synchrotron X-ray diffraction and X-ray absorption spectroscopy establish the local nature of the disorder, revealing the presence of structurally constrained magnetic exchange paths. No magnetic ordering or spin freezing is observed down to 0.1 K. The low-temperature magnetic and thermodynamic behavior is captured by a broad but non-singular distribution $P(J)$ of exchange couplings $J$. These results open the possibility of realizing a disordered quantum ground state where the exchange randomness is broad yet intrinsically bounded, departing from the conventional infinite-randomness fixed point driven random-singlet phase.

cond-mat.str-el↗

arXiv2025

Interplay of phonons, intertwined density waves, and induced spin density wave in trilayer nickelates Pr4-xLaxNi3O10

Lattice degrees of freedom (DoF) play a central role in correlated electron systems, strongly influencing the dynamics of the underlying charge carriers and spin excitations. In nickelates, understanding the role of lattice is essential to unravel the interplay between charge, orbital, and spin degree of freedom in giving rise to various emergent phenomena reported recently. Here, we investigate the phononic DoF in a series of trilayer nickelates, namely Pr4-xLaxNi3O10 (where x = 0, 0.4, 1, 2, 3.6, and 4) using temperature and polarization dependent Raman scattering measurements. Our in-depth analysis of the phonon evolution with temperature and doping, gives interesting insights into the behaviour of these materials. All these systems undergo a metal-to-metal transition (TMMT), characterized by the development of intertwined spin and charge density waves, with the spin density wave preceding the charge density wave. These transitions manifest as pronounced anomalies in phonon self-energy parameters i.e. peak frequency and linewidth in the vicinity of the metal-to-metal transition. Several phonon modes show dramatic change (nearly an order of magnitude for some modes) in their softening rates across the TMMT, highlighting the sensitivity of the lattice dynamics to spin and charge order. These findings emphasize the crucial role of lattice DoF in mediating correlated ground states in layered nickelates.

cond-mat.str-el↗

arXiv2025

A novel Gapless Quantum Spin Liquid in the S = 1 4d4-honeycomb material Cu$_3$LiRu$_2$O$_6$

We report the discovery of a novel gapless quantum spin liquid in the S=1 honeycomb system Cu$_3$LiRu$_2$O$_6$ with Ru$^{4+}$ ($4d^4$) where moments remain dynamic down to 50 mK. Heat capacity measurements show no sign of magnetic ordering down to 60 mK in spite of a Curie-Weiss temperature = -222 K indicating a strong antiferromagnetic interaction. In zero field, magnetic heat capacity shows a linear T-dependence with Sommerfeld coefficient = 107 mJ/mol K$^2$ is much larger than that found in typical Fermi liquids. Our local probe $^7$Li nuclear magnetic resonance (NMR) measurements find a significant temperature-independent $^7$Li NMR shift (and hence a non-zero spin susceptibility) at low-T and a linear T-variation of the $^7$Li NMR spin-lattice relaxation rate 1/T$_1$ at low-T reminiscent of fermionic excitations. Muon spin relaxation measurements detect neither long-range ordering nor spin freezing down to 50 mK and the temperature variation of the muon depolarization rate shows a gradual increase with decreasing temperature and a leveling off below about 1 K evincing a persistent spin dynamics common to several spin liquid candidates. Our results provide strong signatures of a quantum spin liquid in the titled honeycomb material.

cond-mat.str-el↗

arXiv2024

Dynamics of electron-electron correlated to electron-phonon coupled phase progression in trilayer nickelate La4Ni3O10

Trilayer nickelates are a rich class of materials exhibiting diverse correlated phenomena, including superconductivity, density wave transitions, non-Fermi liquid behavior along with an unusual metal-to-metal transition around T* ~ 150 K. Understanding the electronic correlations, lattice and charge dynamics are crucial to unreveal the origin of superconductivity and other instabilities in nickelates. Our in-depth Raman measurements shows that trilayer nickelate, La4Ni3O10, shows transition from electron-phonon coupled phase to the electron-electron correlated one below charge density wave transition around T* with an estimated energy gap of ~ 18-20 meV. The transition around T* is also accompanied by the emergence of zone folded phonon modes reflecting the transition into the charge density wave phase. Phonon modes self-energy parameters show anomalous changes around T* attributed to the electron-electron correlations, and renormalization rate of the phonon modes is much slower in the charge-ordered phase compared to the phase above T*. The transition around T* are marked by the suppression of electron-phonon coupling parameter by ~ 70 %, a change of the quasiparticle dynamics from non-Fermi liquid to the Landau-Fermi liquid type behaviour estimated using the low frequency Raman response.

cond-mat.str-el↗

arXiv2024

Crystal growth, magnetic, and magnetocaloric properties of J_eff = 1/2 quantum antiferromagnet CeCl_3

We report growth of high-quality single crystals of CeCl3 using a modified Bridgman Stockbarger method in an infrared image furnace. The grown crystals are characterized using single-crystal/powder X-ray diffraction, Laue X-ray diffraction, Raman spectroscopy, magnetization, and heat capacity probes. CeCl3 crystallizes in a hexagonal structure with a weak trigonal distortion. The Raman spectrum at 300 K showcases five, clearly resolvable, phonon modes at 106.8, 181.2, 189, 213, and 219.7 wavenumbers. The magnetic susceptibility show a large anisotropy with a broad peak in the perpendicular orientation, which is explained using the crystal field theory. The crystal field in CeCl3 splits the J = 5/2 manifold of Ce3+ into three Kramers doublets, resulting in a well-isolated ground state. In the specific heat, no magnetic ordering is detected above 2 K. However, in non-zero fields the low-temperature specific heat changes dramatically, showcasing a peak at 2.5 K under a moderate field of 30 kOe. The weak Ce-Ce exchange, large Ce moment in the crystal field ground state, and significant anisotropy are ingredients for realizing a high magnetocaloric effect. A maximum entropy change of 23 J/Kg/K is observed near 2.5 K in fields ranging from 50 kOe to 60 kOe. These values are comparable to some of the best Gd-based magnetocaloric materials, signifying the potential of CeCl3 as a magnetic coolant.

cond-mat.str-el↗

arXiv2024

Atypical antiferromagnetic ordering in single crystalline quasi-2D honeycomb magnet YbI$_3$

Here, we study YbI$_3$, a quasi-2D layered material with Yb atoms arranged on an ideal honeycomb network of edge-sharing YbI$_6$ octahedra, analogous to the low-temperature phase of $α-$RuCl$_3$. High quality single crystals of YbI$_3$ are grown from Yb and I as starting precursors, using the vapor transport technique. The grown crystals are characterized by single crystal x-ray diffraction, Raman spectroscopy, magnetization, and heat capacity probes. The crystal-field split ground state of Yb$^{3+}$ in \Yb~ is a well-isolated Kramers doublet with an effective moment $\rm J_{eff} = 1/2$. Upon cooling, the low-temperature heat capacity of \Yb~ reveals a broad peak at $\rm T_1 = 0.95$~K due to short-range ordering of the Yb moments, followed by a sharp peak at $\rm T_2 = T_N = 0.6$~K due to long-range ordering. The magnetic behavior is found to be weakly anisotropic with $χ^\parallel > χ^\perp$, where $χ^\parallel$ and $χ^\perp$ refers to the in-plane ($H \parallel ab$) and out-of-plane ($H \perp ab$) susceptibilities. The 2~K isothermal magnetization saturates at $\rm \approx~1.5~μ_B/Yb^{3+}$ (in-plane) and $\rm \approx~1~μ_B/Yb^{3+}$ (out-of-plane), suggesting the anisotropy to be easy-plane type. Low-temperature heat capacity, well below T$_N$, is found to vary as T$^α$ with $α~\approx~2.5$, indicating a possible unconventional magnetic ground state for YbI$_3$.

cond-mat.str-el↗

arXiv2024

Spatial-temporal analysis of neural desynchronization in sleep-like states reveals critical dynamics

Sleep is characterized by non-rapid eye movement (nREM) sleep, originating from widespread neuronal synchrony, and REM sleep, with neuronal desynchronization akin to waking behavior. While these were thought to be global brain states, recent research suggests otherwise. Using time-frequency analysis of mesoscopic voltage-sensitive dye recordings of mice in a urethane-anesthetized model of sleep, we find transient neural desynchronization occurring heterogeneously across the cortex within a background of synchronized neural activity, in a manner reminiscent of a critical spreading process and indicative of an "edge-of-synchronization phase" transition.

q-bio.NC↗

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

Upconversion of terahertz phonons in spin-ladder compounds via nonlinear coupling

We demonstrate dynamic control of the lattice by THz light by exploiting the coupling of phonon modes. The low-energy sliding phonon modes in the spin-ladder system, Sr$_{14}$Cu$_{24}$O$_{41}$, are excited using THz radiation with high electric fields. Due to the nonlinearities induced by the THz electric fields, the low-energy phonon mode couples to the higher energy, silent optical phonon modes at $\approx$ 1.17 THz. This indirect excitation of the silent phonon mode is reflected as an enhancement of the THz transmission near 1.17 THz. Our results demonstrate that it is possible to indirectly control inaccessible phonon modes with THz frequency electromagnetic radiation, which provides opportunities to alter such material systems' electronic and magnetic properties dynamically using THz radiation.

cond-mat.str-el↗

arXiv2023

Investigating the cause of crossover from charge/spin stripe insulator to correlated metallic phase in layered T' nickelates -- R$_4$Ni$_3$O$_8$

The $T^{\prime}$ infinite layered nickelates have recently garnered significant attention owing to the discovery of superconductivity in hole-doped RNiO$_2$ (R $=$ La, Pr, or Nd), which is the $n = \infty$ member of the series R$_{n+1}$Ni$_n$O$_{2n+2}$. Here, we investigate the $n = 3$ member, namely R$_4$Ni$_3$O$_8$ (R $=$ La, Pr, or Nd) of this family. The compound La$_4$Ni$_3$O$_8$ exhibits simultaneous charge/spin-stripe ordering at T$_N^\ast$ $=$ 105 K, which is also concomitant with the onset of metal-to-insulator (MIT) transition upon lowering the temperature below T$_N^\ast$. We investigate the conspicuous absence of this transition in the Pr and Nd analogues of La$_4$Ni$_3$O$_8$. To achieve this purpose, we synthesized solid-solutions of the form (La, Pr)$_4$Ni$_3$O$_8$ and (La, Nd)$_4$Ni$_3$O$_8$ and examined the behavior of T$_N^\ast$ as a function of the average R-site ionic radius ($r_{\overline{R}}$). We show that after an initial quasilinear decrease with decreasing $r_{\overline{R}}$, T$_N^\ast$ suddenly vanishes in the narrow range 1.134 $Å$ $\leq$ $r_{\overline{R}}$ $\leq$ 1.143 $Å$. In the same range, we observed the emergence of a new transition below T$^\ast$, whose onset temperature increases as $r_{\overline{R}}$ further decreases. We, therefore, argue that the sudden vanishing of charge/spin-stripe/MIT ordering upon decreasing $r_{\overline{R}}$ is due to the appearance of a new competing phase. The point $r_{\overline{R}}$ $\approx$ $r_c$, where T$_N^\ast$ vanishes and T$^\ast$ appears -- a quantum critical point -- should be investigated further. In this regard, Pr$_4$Ni$_3$O$_8$ and Pr-rich samples should be useful due to the weak magnetization response associated with the Pr-sublattice, as shown here.

cond-mat.str-el↗

arXiv2023

Evidence of Charge-Phonon coupling in Van der Waals materials Ni1-xZnxPS3

NiPS3 is a Van der Waals antiferromagnet that has been found to display spin-charge and spin-phonon coupling in its antiferromagnetically ordered state below TN = 155 K. Here, we study high-quality crystals of site-diluted Ni1-xZnxPS3 (0 < x < 0.2) using temperature-dependent specific heat and Raman spectroscopy probes. The site dilution suppresses the antiferromagnetic ordering in accordance with the mean-field prediction. In NiPS3, we show that the phonon mode P2 (176 cm-1) associated with Ni vibrations show a distinct asymmetry due to the Fano resonance, which persists only in the paramagnetic phase, disappearing below T_N = 155 K. This was further supported by temperature-dependent Raman data on an 8% Zn-doped crystal (T_N = 135 K) where Fano resonance similarly van in the magnetically ordered phase. This is contrary to the behaviour of the Raman mode P9 (570 cm-1), which shows a Fano resonance at low temperatures below T_N due to its coupling with the two-magnon continuum. We show that the Fano resonance of P2 arises from its coupling with an electronic continuum that weakens considerably upon cooling to low temperatures. In the doped crystals, the Fano coupling is found to enhance with Zn-doping. These observations suggest the presence of strong electron-phonon coupling in the paramagnetic phase of NiPS3 due to charge density fluctuations associated with the negative charge transfer state of Ni.

cond-mat.str-el↗

arXiv2023

Optimization for truss design using Bayesian optimization

In this work, geometry optimization of mechanical truss using computer-aided finite element analysis is presented. The shape of the truss is a dominant factor in determining the capacity of load it can bear. At a given parameter space, our goal is to find the parameters of a hull that maximize the load-bearing capacity and also don't yield to the induced stress. We rely on finite element analysis, which is a computationally costly design analysis tool for design evaluation. For such expensive to-evaluate functions, we chose Bayesian optimization as our optimization framework which has empirically proven sample efficient than other simulation-based optimization methods. By utilizing Bayesian optimization algorithms, the truss design involves iteratively evaluating a set of candidate truss designs and updating a probabilistic model of the design space based on the results. The model is used to predict the performance of each candidate design, and the next candidate design is selected based on the prediction and an acquisition function that balances exploration and exploitation of the design space. Our result can be used as a baseline for future study on AI-based optimization in expensive engineering domains especially in finite element Analysis.

stat.AP↗

arXiv2023

Systematic design space exploration by learning the explored space using Machine Learning

Current practice in parameter space exploration in euclidean space is dominated by randomized sampling or design of experiment methods. The biggest issue with these methods is not keeping track of what part of parameter space has been explored and what has not. In this context, we utilize the geometric learning of explored data space using modern machine learning methods to keep track of already explored regions and samples from the regions that are unexplored. For this purpose, we use a modified version of a robust random-cut forest along with other heuristic-based approaches. We demonstrate our method and its progression in two-dimensional Euclidean space but it can be extended to any dimension since the underlying method is generic.

cs.LG↗

arXiv2022

Synergistic approach towards reproducible high zT in superionic thermoelectric Ag2Te

Recently, the superionic thermoelectrics, which typify the novel `phonon-liquid electron-crystal' concept, have attracted enormous attention due to their ultralow thermal conductivity and high figure-of-merit (zT). However, their high zT is generally obtained deep inside the superionic phase, e.g., near 1000~K in the Cu$_2$X (X: chalcogen atom) family where the superionic transition is close to 400~K. At such high temperatures, the liquid-like flow of the metal ions under an electric field or a temperature gradient, both of which are integral to the working of a thermoelectric device, results in device degradation. To harness the full potential of the superionic thermoelectrics, it is, therefore, necessary to reach high zT at low temperatures where the metal-ion diffusion is not an issue. Here, we present a novel all-room-temperature route to fabricate 100\% dense, nanostructured Ag$_2$Te with highly reproducible thermoelectric properties and a high zT of 1.2 at 570~K, i.e., merely 150~K above its superionic transition. The samples show a broad particle-size distribution ranging from a few nm to a few $μ$m. This hierarchical nanostructuring is shown to suppress the thermal conductivity of Ag$_2$Te beyond the phonon-liquid electron-crystal limit to ultralow values, leading to a remarkable enhancement of 87\% in the zT over that of the ingot sample. These values supersede the zT of any Ag$_2$Te previously reported. Our results are supported by first-principles density functional theory calculations of the electronic and thermal properties.

cond-mat.mtrl-sci↗

arXiv2022

High pressure structural and magneto-transport studies on type-II Dirac semimetal candidate Ir2In8S: Emergence of superconductivity upon decompression

The structural and magneto-transport properties of type-II Dirac semimetal candidate Ir2In8S have been investigated under high pressure. The ambient tetragonal structure (P4_2/mnm) is found to be stable up to 7 GPa, above which the system takes an orthorhombic Pnnm structure, possibly destroying the Dirac cones due to the loss of the four-fold screw symmetry. In the tetragonal structure, a gradual suppression of the transverse magneto-resistance and a rapid change in the magnetic field dependence above 50K suggest possible T-dependent Fermi surface modification. In the high pressure phase, the metallic character increases marginally (as evident from the increased RRR value) accompanied with suppressed magneto-resistance, without emergence of superconductivity up to 20 GPa and down to 1.4K. Most surprisingly, upon release of pressure to 0.2 GPa, a sharp resistance drop below 4K is observed, field varying measurements confirm this as the onset of superconductivity. The observed changes of the carrier density and mobility in the pressure-released tetragonal phase indicate electronic structural modification resulting from the irreversible polyhedral distortion. A simultaneous increase in the residual resistivity and carrier density upon decompression indicates that an enhanced impurity scattering play a key role in the emergence of superconductivity in the tetragonal Ir2In8S, making it an ideal platform to study topological superconductivity.

cond-mat.supr-con↗

arXiv2021

Protracting the Weyl phase by a giant negative lattice expansion in Bi doped Sm$_2$Ir$_2$O$_7$

We show that the Weyl phase in $\rm Sm_2Ir_2O_7$ is protracted up to at least 2~\% alloying with Bi by an anomalous negative lattice expansion with $\rm Δa \sim- 0.01$Å. With further doping, the magnetic ordering disappears and electrical resistivity decreases by orders of magnitude; the resistivity upturn remains but with $\rm 1/T$ dependence of Weyl phase changed to $\rm -lnT$ dependence characteristic of the Quadratic Band Touching (QBT). At the Weyl-QBT phase boundary, a new phase is evidenced whose resistivity scales as $\rm -T^{1/4}$ possibly due to proximity to a quantum critical point proposed several years ago [Phys. Rev. X 4, 041027 (2014)], but whose experimental evidence has remained elusive thus far.

cond-mat.str-el↗

arXiv2021

Role of spin-phonon and electron-phonon interactions in phonon renormalization of (Eu$_{1-x}$Bi$_x$)$_2$Ir$_2$O$_7$ across the metal-insulator phase transition: Temperature-dependent Raman and X-ray studies

We report temperature-dependent Raman scattering and X-ray diffraction studies of pyrochlore iridates, (Eu$_{1-x}$Bi$_x$)$_2$Ir$_2$O$_7$, for x=0, 0.02, 0.035, 0.05 and 0.1. The temperature variation in Raman experiments spans from 4 K to 300 K, covering the metal-insulator phase transition accompanied by paramagnetic to all-in/all-out (AIAO) spin ordering (T$_N$). These systems also show a Weyl semi-metal (WSM) phase at low temperatures (below ~50 K). We show that the Ir-O-Ir bond bending mode, A$_{1g}$ (510 cm$^{-1}$), shows anomalous softening in the magnetically ordered AIAO state, arising primarily from the spin-phonon interaction due to the phonon-modulation of the Dzyaloshinskii-Moriya (DM) spin-exchange interaction. The two stretching modes, T$_{2g}^1$ (307 cm$^{-1}$) and T$_{2g}^2$ (382 cm$^{-1}$) harden significantly in the magnetic insulating phase. The T$_{2g}$ phonons also show anomalous temperature dependence of their mode frequencies, hitherto unreported, due to strong electron-phonon coupling. The signatures of the WSM state are observed in phonon renormalization below 50 K due to strong electron-phonon interaction. Our experimental results establish strong magneto-elastic coupling below T$_N$ and significant electron-phonon interactions in the metallic phase above T$_N$ as well as in the low-temperature WSM state.

cond-mat.str-el↗