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Dipanjan Chaudhuri

Publications and source records attributed to Dipanjan Chaudhuri.

At least 19 recordsLinked to original sources

Momentum-resolved EELS study of collective charge excitations in 1$T$-TaS$_2$

We use momentum-resolved electron energy-loss spectroscopy (M-EELS) to study the low-energy charge excitations of 1$T$-TaS$_2$ across the nearly commensurate-to-commensurate charge-density-wave (CDW) transition. Single-crystal x-ray diffraction and elastic M-EELS measurements confirm the expected rotation of the CDW wave vector upon entering the commensurate phase. In the nearly commensurate phase, the low-energy M-EELS spectra reveal an acoustic phonon branch and two optical phonon features whose energies and dispersions are broadly consistent with previous calculations and inelastic x-ray measurements. Across the transition, the optical phonon energies remain nearly unchanged, while their spectral intensity develops a pronounced temperature dependence near the CDW ordering wave vector. At higher energies, the finite-momentum charge response undergoes a substantial redistribution of spectral weight below the transition, consistent with the opening of an energy gap. These results demonstrate that M-EELS provides simultaneous access to lattice dynamics and finite-momentum valence band charge excitations in 1$T$-TaS$_2$, revealing their evolution across the commensurate CDW transition.

cond-mat.str-el

Decoupling momentum and energy relaxation rates in cuprate strange metals via giant THz nonlinearities

Understanding the $T$-linear normal-state resistivity of cuprates remains a central physics challenge. The associated momentum relaxation rate, $Γ_M$, saturates near the conjectured ``Planckian" bound $Γ_M\sim kT/\hbar$, but the mechanism underlying the anomalous scattering remains unresolved. Here we employ nonlinear terahertz spectroscopy to systematically study La$_{2-x}$Sr$_x$CuO$_4$ across a broad temperature and doping range. We measure the normal-state third-order susceptibility, $|χ^{(3)}|\approx 6\times10^{-9}$ m$^2$/V$^2$, among the largest in the THz regime, enabling direct access to the rarely measured electronic energy relaxation rate, $Γ_E$. Strikingly, $Γ_E$ is 10-40 times smaller than $Γ_M$, revealing that the scatterings responsible for momentum loss and $T$-linear resistivity do not remove appreciable energy from the electrons. While $Γ_M (T)$ is consistent with quasi-elastic scattering from bosonic modes above their characteristic energy scale, this is incompatible with the increasing temperature dependence of $Γ_E(T)$. Our results exclude phonons as the source of $T$-linear resistivity and impose strong constraints on possible mechanisms.

cond-mat.supr-con

Kondo driven suppression of charge density wave in Van der Waals material UTe$_3$

Competing electronic instabilities lie at the heart of emergent phenomena in quantum materials. In low-dimensional metals, Fermi-surface nesting can drive charge density wave (CDW) formation through a Peierls-like mechanism, while in strongly correlated systems, Kondo hybridization reconstructs the electronic structure by entangling localized moments with itinerant electrons. How these two fundamentally different instabilities interact$-$whether they coexist, compete, or mutually exclude each other$-$remains an open question. Here, we present suppression of charge density wave via the Kondo interaction in van der Waals material UTe$_3$. The angle-resolved photoemission spectroscopy (ARPES) data reveals Fermi surface nesting under similar conditions as seen in RETe$_3$ compounds. Despite that, no CDW is found in UTe$_3$ after an extensive search. We demonstrate that strong hybridization between U 5$f$ electrons and Te $p$ states reconstructs the low-energy electronic structure, removes the instability, and preempts CDW formation. Our results reveal a rare example where Kondo hybridization preempts density wave formation, offering a new route to controlling ordering phenomena in correlated 2D materials.

cond-mat.str-el

Reexamining the strange metal charge response with transmission inelastic electron scattering

The strange metal remains one of the great unsolved problems for 21st century science. Since the early development of the marginal Fermi liquid phenomenology, it has been clear that progress requires detailed knowledge of the momentum- and frequency-dependent charge susceptibility, $χ(\mathbf{q},ω)$, particularly at large momenta. Electron energy-loss spectroscopy (EELS), performed in either reflection or transmission geometry, provides the most direct probe of $χ(\mathbf{q},ω)$. However, measurements over the past four decades have yielded conflicting results, with some studies reporting a dispersing RPA-like plasmon and others observing a strongly overdamped, incoherent response. Here we report a transmission EELS study of Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$ (Bi-2212) that simultaneously achieves high energy resolution ($ΔE \approx 30$ meV) and high momentum resolution ($Δq \approx 0.01$ Å$^{-1}$). To address issues of reproducibility, measurements were repeated ten times on five different Bi-2212 flakes, benchmarked against aluminum, a well-characterized Fermi liquid, and quantitatively compared with prior studies spanning four decades. At momenta $q < 0.15$ Å$^{-1}$, we observe a highly damped plasmon whose linewidth is comparable to its energy. At larger momenta, $q > 0.15$ Å$^{-1}$, this excitation does not disperse but instead evolves into an incoherent continuum, with no evidence for the RPA-like dispersion reported in some earlier works. Comparison with recent RIXS measurements on Bi-based cuprates supports the view that Bi-2212 is an incoherent metal with strongly damped charge excitations.

cond-mat.str-el

Topology-Driven Vibrations in a Chiral Polar Vortex Lattice

The ordering of magnetic or electric dipoles leading to real-space topological structures is at the forefront of materials research as their quantum mechanical nature often lends itself to emergent properties. Atomic lattice vibrations (phonons) are often a key contributor to the formation of long-range dipole textures based on ferroelectrics and impact the properties of the emergent phases. Here, using monochromated, momentum-resolved electron energy-loss spectroscopy (qEELS) with nanometer spatial resolution and meV-spectral-precision, we demonstrate that polar vortex lattices in PbTiO$_3$ spatially modulate the material's vibrational spectrum in patterns that directly reflect the overlying symmetry of the topological patterns. Moreover, by combining experiments with molecular dynamics simulations using machine learned potentials we reveal how these structures modify phonon modes across the vibrational spectrum. Beyond simple intensity modulation, we find that the chirality of the vortex topology imparts its unique symmetry onto phonons, producing a distinctive asymmetrical spectral shift across the vortex unit cell. Finally, the high spatial resolution of the technique enables topological defects to be probed directly, demonstrating a return to trivial PbTiO$_3$ modes at vortex dislocation cores. These findings establish a fundamental relationship between ferroelectric-ordering-induced topologies and phonon behavior, opening new avenues for engineering thermal transport, electron-phonon coupling, and other phonon-mediated properties in next-generation nanoscale devices.

cond-mat.mtrl-sci

Comparative analysis of plasmon modes in layered Lindhard metals and strange metals

The enigmatic strange metal remains one of the central unsolved problems of 21st century science. Understanding this phase of matter requires knowledge of the momentum- and energy-resolved dynamic charge susceptibility, $χ(q,ω)$, especially at finite momentum. Inelastic electron scattering (EELS), performed in either transmission (T-EELS) or reflection (R-EELS) geometries, is a powerful probe of $χ(q,ω)$. For the prototypical strange metal Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$, T-EELS, R-EELS, and infrared (IR) spectroscopy agree at $q \sim 0$, all revealing a highly damped plasmon near 1 eV. At larger $q$, however, EELS results show unresolved discrepancies. Since IR data are highly reproducible, it is advantageous to use IR data to calculate what the expected EELS response should be at modest $q$. Building on prior R-EELS work [J. Chen \textit{et al.}, Phys. Rev. B. \textbf{109}, 045108 (2024)], we extend this approach to T-EELS for finite stacks of metallic layers, comparing a "textbook" Lindhard metal to a strange metal. In the Lindhard case, the low-$q$ response is dominated by long-lived, standing wave plasmon modes arising from interlayer Coulomb coupling, with in-plane dispersions that resemble the well-known Fetter modes of layered metals. This behavior depends only on the geometry and the long-ranged nature of the Coulomb interaction, and is largely insensitive to layer details. At larger $q$, the response reflects the microscopic properties of individual layers. For the strange metal, calculations based on IR data predict a highly damped plasmon with weak dispersion and no distinct surface mode. While our results match IR and R-EELS at low $q$, they do not reproduce any published EELS spectra at large $q$, highlighting unresolved discrepancies that demand further experimental investigation.

cond-mat.str-el

Tuning Incommensurate Charge Order in Ba$_{1-x}$Sr$_x$Al$_4$ and Ba$_{1-y}$Eu$_y$Al$_4$

The BaAl$_4$-type structure family is home to a vast landscape of interesting and exotic properties, with descendant crystal structures hosting a variety of electronic ground states including magnetic, superconducting and strongly correlated electron phenomena. BaAl$_4$ itself hosts a non-trivial topological band structure, but is otherwise a paramagnetic metal. However, the other members of the $A$Al$_4$ family ($A$= alkali earth), including SrAl$_4$ and EuAl$_4$, exhibit symmetry-breaking ground states including charge density wave (CDW) and magnetic orders. Here we investigate the properties of the solid solution series Ba$_{1-x}$Sr$_x$Al$_4$ and Ba$_{1-y}$Eu$_y$Al$_4$ using transport, thermodynamic and scattering experiments to study the evolution of the charge-ordered state as it is suppressed with Ba substitution to zero near 50% substitution in both systems. Neutron and x-ray diffraction measurements reveal an incommensurate CDW state in SrAl$_4$ with $c$-axis-oriented ordering vector (0, 0, 0.097) that evolves with Ba substitution toward a shorter wavelength. A similar progression is observed in the Ba$_{1-y}$Eu$_y$Al$_4$ series that also scales with the ordering temperature, revealing a universal correlation between charge-order transition temperature and ordering vector that points to a critical wavevector that stabilizes CDW order in both systems. We study the evolution of the phonon band structure in the Ba$_{1-x}$Sr$_x$Al$_4$ system, revealing the suppression of the CDW phase matches the suppression of a phonon instability at precisely the same momentum as observed in experiments, confirming the electron-phonon origin of charge order in this system.

cond-mat.str-el

Does rainfall create buoyant forcing at the ocean surface?

Rain affects the buoyancy of the upper ocean in two ways: The freshwater flux in rain makes the water fresher and lighter, stabilizing the ocean (a negative buoyancy flux). The convective systems that produce rain are often accompanied by cold, dry air, often called 'cold pools', and reduced short-wave radiation, which makes the water colder and heavier, destabilizing the ocean (a positive buoyancy flux). We estimate net buoyancy fluxes using in situ measurements from twenty-two moored buoys in the equatorial oceans under different rainfall categories. We find that buoyancy fluxes tend to destabilize the ocean during light rain (0.2-4 mm/hr) and stabilize the ocean during heavy rain (>4 mm/hr). Furthermore, buoyancy fluxes during rain tend to be more positive at night than during the day, with nighttime rain twice as likely to cause instability compared to daytime rain, even at the same rainfall intensity. Average buoyancy fluxes across the tropics during rain can have either sign. These findings challenge the common assumption that rainfall makes the ocean surface lighter and provide a starting point for focusing on the overall effect of precipitation on the ocean.

physics.ao-ph

Quantum Fisher Information Reveals UV-IR Mixing in the Strange Metal

The density-density response in optimally doped Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$ has recently been shown to exhibit conformal symmetry. Using, the experimentally inferred conformal dynamic susceptibility, we compute the resultant quantum Fisher information (QFI), a witness to multi-partite entanglement. For a Fermi liquid, we find that the QFI grows quadratically as the temperature increases, consistent then with the phase space available for scattering in the standard theory of metals. By contrast, the QFI in a strange metal increases as a power law at as the temperature decreases, but ultimately extrapolates to a constant at $T=0$. The constant is of the form, $ω_g^{2Δ}$, where $Δ$ is the conformal dimension and $ω_g$ is the UV cutoff which is on the order of the pseudogap. As this constant {depends on both UV and IR properties}, it illustrates that multipartite entanglement in a strange metal exhibits UV-IR mixing, a benchmark feature of doped Mott insulators as exemplified by dynamical spectral weight transfer. We conclude with a discussion of the implication of our results for low-energy reductions of the Hubbard model.

cond-mat.str-el

Measurement of the dynamic charge susceptibility near the charge density wave transition in ErTe$_3$

A charge density wave (CDW) is a phase of matter characterized by a periodic modulation of the valence electron density accompanied by a distortion of the lattice structure. The microscopic details of CDW formation are closely tied to the dynamic charge susceptibility, $χ(q,ω)$, which describes the behavior of electronic collective modes. Despite decades of extensive study, the behavior of $χ(q,ω)$ in the vicinity of a CDW transition has never been measured with high energy resolution ($\sim$meV). Here, we investigate the canonical CDW transition in ErTe$_3$ using momentum-resolved electron energy loss spectroscopy (M-EELS), a technique uniquely sensitive to valence band charge excitations. Unlike phonons in these materials, which undergo conventional softening due to the Kohn anomaly at the CDW wavevector, the electronic excitations display purely relaxational dynamics that are well described by a diffusive model. The diffusivity peaks around 250 K, just below the critical temperature. Additionally, we report, for the first time, a divergence in the real part of $χ(q,ω)$ in the static limit ($ω\rightarrow 0$), a phenomenon predicted to characterize CDWs since the 1970s. These results highlight the importance of energy- and momentum-resolved measurements of electronic susceptibility and demonstrate the power of M-EELS as a versatile probe of charge dynamics in materials.

cond-mat.str-el

Conformally invariant charge fluctuations in a strange metal

The strange metal is a peculiar phase of matter in which the electron scattering rate, $τ^{-1} \sim k_B T/\hbar$, which determines the electrical resistance, is universal across a wide family of materials and determined only by fundamental constants. In 1989, theorists hypothesized that this universality would manifest as scale-invariant behavior in the dynamic charge susceptibility, $χ''(q,ω)$. Here, we present momentum-resolved inelastic electron scattering measurements of the strange metal Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$ showing that the susceptibility has the scale-invariant form $χ''(q,ω) = T^{-ν} f(ω/T)$, with exponent $ν= 0.93$. We find the response is consistent with conformal invariance, meaning the dynamics may be thought of as occurring on a circle of radius $1/T$ in imaginary time, characterized by conformal dimension $Δ= 0.05$. Our study indicates that the strange metal is a universal phenomenon whose properties are not determined by microscopic properties of a particular material.

cond-mat.str-el

Absence of a bulk charge density wave signature in x-ray measurements of UTe$_2$

The long-sought pair density wave (PDW) is an exotic phase of matter in which charge density wave (CDW) order is intertwined with the amplitude or phase of coexisting, superconducting order \cite{Berg2009,Berg2009b}. Originally predicted to exist in copper-oxides, circumstantial evidence for PDW order now exists in a variety of materials. Recently, scanning tunneling microscopy (STM) studies have reported evidence for a three-component charge density wave (CDW) at the surface of the heavy-fermion superconductor, UTe$_2$, persisting below its superconducting transition temperature. Here, we use hard x-ray diffraction measurements on crystals of UTe$_2$ at $T = 1.9$ K and $12$ K to search for a bulk signature of this CDW. Using STM measurements as a constraint, we calculate the expected locations of CDW superlattice peaks, and sweep a large volume of reciprocal space in search of a signature. We failed to find any evidence for a CDW near any of the expected superlattice positions in many Brillouin zones. We estimate an upper bound on the CDW lattice distortion of $u_{max} \lesssim 4 \times 10^{-3} \mathrmÅ$. Our results suggest that the CDW observed in STM is either purely electronic, somehow lacking a signature in the structural lattice, or is restricted to the material surface.

cond-mat.str-el

Energy Relaxation and dynamics in the correlated metal Sr$_2$RuO$_4$ via THz two-dimensional coherent spectroscopy

Separating out the contributions of different scattering channels in strongly interacting metals is crucial in identifying the mechanisms that govern their properties. While momentum or current relaxation rates can be readily probed via \textit{dc} resistivity or optical/THz spectroscopy, distinguishing different kinds of inelastic scattering can be more challenging. Using nonlinear THz 2D coherent spectroscopy, we measure the rates of energy relaxation after THz excitation in the strongly interacting Fermi liquid, Sr$_2$RuO$_4$. Energy relaxation is a bound on the total scattering and specifically a measure of contributions to the electron self-energy that arise from {\it inelastic} coupling to a bath. We observe two distinct energy relaxation channels: a fast process that we interpret as energy loss to the phonon system and a much slower relaxation that we interpret as arising from a non-equilibrium phonon effects and subsequent heat loss through diffusion. Interestingly, even the faster energy relaxation rate is at least an order of magnitude slower than the overall momentum relaxation rate, consistent with strong electron interactions and the dominance of energy-conserving umklapp or interband electron-electron scattering in momentum relaxation. The slowest energy relaxation rate decays on a sub-GHz scale, consistent with the relaxation dynamics of non-equilibrium phonons. Our observations reveal the versatility of nonlinear THz spectroscopy to measure the energy relaxation dynamics in correlated metals. Our work also highlights the need for improved theoretical understanding of such processes in interacting metals.

cond-mat.str-el

Consistency between reflection M-EELS and optical spectroscopy measurements of the long-wavelength density response of Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$

The density fluctuation spectrum captures many fundamental properties of strange metals. Using momentum-resolved electron energy-loss spectroscopy (M-EELS), we recently showed that the density response of the strange metal Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$ (Bi-2212) at large momentum, $q$, exhibits a constant-in-frequency continuum [Mitrano, PNAS $\textbf{115}$, 5392 (2018); Husain, PRX $\textbf{9}$, 041062 (2019)] reminiscent of the marginal Fermi liquid (MFL) hypothesis of the late 1980s [Varma, PRL $\textbf{63}$, 1996 (1989)]. However, reconciling this observation with infrared (IR) optics experiments, which show a well-defined plasmon excitation at $q \sim 0$, has been challenging. Here we report M-EELS measurements of Bi-2212 using 4$\times$ improved momentum resolution, allowing us to reach the optical limit. For momenta $q<0.04$ r.l.u., the M-EELS data show a plasmon feature that is quantitatively consistent with IR optics. For $q>0.04$ r.l.u., the spectra become incoherent with an MFL-like, constant-in-frequency form. We speculate that, at finite frequency, $ω$, and nonzero $q$, some attribute of this Planckian metal randomizes the probe electron, causing it to lose information about its own momentum.

cond-mat.str-el

Anomalous high-temperature THz nonlinearity in superconductors near the metal-insulator transition

The interplay of strong disorder and superconductivity is a topic of long-term interest in condensed matter physics. Here we explore the nonlinear THz response of superconducting NbN films close to the 3D metal-insulator transition. For the least disordered samples, the magnitude of the nonlinear $χ^{(3)}$ response follows the temperature dependence of the superfluid density as expected. In contrast, for high disorder samples near the metal-insulator transition the $χ^{(3)}$ nonlinearity persists to temperatures as high as even 4 times the $T_c$ of the cleanest sample. We discuss the possible origins of this remarkably large nonlinearity, including the possibility that it arises in an enhancement of the temperature scales of superconductivity close to localization. Our work highlights the importance of finite frequency nonlinear THz experiments in detecting superconducting correlations even into regions where long-range ordered superconductivity does not persist.

cond-mat.supr-con

An optical investigation of the heavy fermion normal state in superconducting UTe$_2$

The recently discovered superconductor, UTe$_2$, has attracted immense scientific interest due to the experimental observations that suggest odd-parity superconductivity. It is believed that the material becomes a heavy-fermion metal at low temperatures although details of the normal state are unclear. Using Fourier transform infrared spectroscopy (FTIR), the normal state electronic structure of UTe$_2$ was investigated at zero applied magnetic field. Combining the measured reflectivity with the dc resistivity, the complex optical conductivity was obtained over a large frequency range. The frequency dependence of the real part of the optical conductivity exhibits a MIR peak around 4000 cm$^{-1}$ and a narrow Drude peak that develops below 40 K. A combination of density functional and dynamic mean field theory (DFT + DMFT) gives spectra in close correspondence to the experiment. Via this comparison we attribute the prominent MIR peak to inter-band transitions involving a narrow U 5$f$ feature that develops near the Fermi level. In this regard, our data gives spectroscopic evidence for the existence of a low energy Kondo resonance at temperatures just above the onset of superconductivity and implicates heavy electrons in the formation of the superconducting state. We find that the coherent Kondo resonance is primarily associated with a collapse of scattering and less with a transfer of spectral weight.

cond-mat.supr-con

Ambipolar magneto-optical response of ultra-low carrier density topological insulators

We have investigated the THz range magneto-optical response of ultralow carrier density films of Sb$_2$Te$_3$ using time-domain THz polarimetry. Undoped Sb$_2$Te$_3$ has a chemical potential that lies inside the bulk valence band. Thus its topological response is masked by bulk carriers. However, with appropriate buffer layer engineering and chemical doping, Sb$_2$Te$_3$ thin films can be grown with extremely low electron or hole densities. The ultralow carrier density samples show unusual optical properties and quantized response in the presence of magnetic fields. Consistent with the expectations for Dirac fermions, a quantized Hall response is seen even in samples where the zero field conductivity falls below detectable levels. The discontinuity in the Faraday angle with small changes in the filling fraction across zero is manifestation of the parity anomaly in 2D Dirac systems with broken time reversal symmetry.

cond-mat.mes-hall

Observation of a marginal Fermi glass using THz 2D coherent spectroscopy

A longstanding open problem in condensed matter physics is whether or not a strongly disordered interacting insulator can be mapped to a system of effectively non-interacting localized excitations. We investigate this issue on the insulating side of the 3D metal-insulator transition (MIT) in phosphorus doped silicon using the new technique of terahertz two dimensional coherent spectroscopy. Despite the intrinsically disordered nature of these materials, we observe coherent excitations and strong photon echoes that provide us with a powerful method for the study of their decay processes. We extract the first measurements of energy relaxation ($T_1$) and decoherence ($T_2$) times close to the MIT in this classic system. We observe that (i) both relaxation rates are linear in excitation frequency with a slope close to unity, (ii) the energy relaxation timescale $T_1$ counterintuitively increases with increasing temperature and (iii) the coherence relaxation timescale $T_2$ has little temperature dependence between 5 K and 25 K, but counterintuitively increases as the material is doped towards the MIT. We argue that these features imply that (a) the system behaves as a well isolated electronic system on the timescales of interest, and (b) relaxation is controlled by electron-electron interactions. We discuss the potential relaxation channels that may explain the behavior. Our observations constitute a qualitatively new phenomenology, driven by the interplay of strong disorder and strong electron-electron interactions, which we dub the marginal Fermi glass.

cond-mat.str-el