arXiv subjects

Fahad Mahmood

Publications and source records attributed to Fahad Mahmood.

At least 19 recordsLinked to original sources

arXiv2026

Revealing the origin of ionic conduction in silver-iodide-doped silver phosphate glass

Fast ionic transport is a defining feature of many solid electrolytes, yet its microscopic origin is not fully understood. In the absence of microscopic insights, the development of next-generation solid-state batteries remains largely empirical. Most existing measurements access either the low-frequency transport response or the high-frequency bound polarization, yet the intermediate mesoscopic frequency regime is where ionic transport emerges. By varying the $\mathrm{AgI}$ concentration ($x$) and performing time-domain terahertz spectroscopy (TDTS) in a prototypical glassy electrolyte $\left(\mathrm{AgI}\right)_{x}\left(\mathrm{AgPO_3}\right)_{(1-x)}$, we reveal this intermediate frequency regime and identify a crossover from bound-current-dominated conduction to conductivity arising from short-range dispersive ionic transport. We find that bound polarization associated with the bond-bending motion of the $\mathrm{P{-}O^- -Ag^+}$ motif is present across compositions but is insufficient to produce ionic transport on its own. Transport emerges only when this polarization is embedded in a sufficiently soft $\mathrm{AgPO_3}$ glassy matrix and accompanied by a high carrier density. These ingredients together take the system from a vibrationally bound response to short-range dispersive motion.

cond-mat.mtrl-sci↗

arXiv2026

Plasmon-driven exciton formation in a non-equilibrium Fermi liquid

Collective modes in Fermi liquids are usually regarded as dissipation channels that relax electronic excitations through Landau damping. Whether such modes can instead mediate the formation of correlated electronic states under non-equilibrium conditions remains an open question. Here we show that, under optical photo-doping, a bulk plasmon can drive correlated inter-band transfer within a transient electronic continuum. Using time- and angle-resolved photoemission spectroscopy (Tr-ARPES) on EuCd$_2$As$_2$ supported by electronic structure calculations, we observe that at high excitation density, plasmons transfer energy from a weakly dispersing bulk band into unoccupied surface states. This bulk-to-surface redistribution stabilizes a long-lived, energy-localized spectral feature consistent with a Mahan exciton. Our results uncover a non-equilibrium regime of Fermi-liquid physics in which collective modes do not merely dissipate energy, but also stabilize correlated bound states.

cond-mat.mes-hall↗

arXiv2026

Manipulation of ferromagnetism with a light-driven nonlinear Edelstein-Zeeman field

Optical control of magnetization is often symmetry-forbidden because electric fields and magnetization transform differently under inversion and time-reversal. However, through even-order nonlinear response, optical excitation can generate a nonequilibrium magnetic density (the nonlinear Edelstein effect) that acts as an internal Edelstein-Zeeman field coupling to slower magnetic degrees of freedom. Here we demonstrate non-thermal, ultrafast optical control of ferromagnetism in the centrosymmetric van der Waals semiconductor Cr$_2$Ge$_2$Te$_6$ via a resonant nonlinear Edelstein effect. Using time-domain THz emission spectroscopy under near-infrared excitation, we directly observe magnetic dipole radiation arising from optically driven magnetization dynamics. The polarization, fluence, and temperature dependences of the THz emission are quantitatively captured by a mean-field description of a weakly anisotropic Heisenberg ferromagnet subject to an Edelstein-Zeeman field. Our results establish a general nonequilibrium route to optical control of magnetism in centrosymmetric materials.

cond-mat.mes-hall↗

arXiv2025

Dynamic competition between phason and amplitudon observed by ultrafast multimodal scanning tunneling microscopy

The intertwining between two ordered states that arise from the same interactions is reflected in the dynamics of their coupled collective excitations. While the equilibrium phase diagram resulting from such intertwined orders has been extensively studied, the dynamic competition between non-equilibrium modes is a largely unexplored territory. Here, we introduce a multimodal STM-based pump-probe technique, that combines ultrafast tunneling microscopy (USTM), ultrafast point-contact spectroscopy (UPC), and optical pump-probe reflectance (OPPR) on femtosecond timescale, all within a single instrument. Using this platform, we investigate the collective excitations of the unconventional charge density wave insulator (TaSe4)2I. Our UPC measurements reveal charge oscillations at 0.22 THz, with a temperature dependence that matches the theoretically predicted behavior of the long-sought massive phason gaining mass through the Anderson-Higgs mechanism. Unexpectedly, the data also reveals a second mode at 0.11 THz exhibiting similar temperature and polarization dependence with comparable mode intensity. These features, along with the robust 1/2 frequency ratio locking suggest that the 0.11 THz phason is a 'daughter mode' that arises from the splitting of the 0.22 THz massive phason into two massless phasons via parametric amplification, analogous to the decay of a neutral pion into two photons. Strikingly, comparison with OPPR data reveals that the daughter phason competes with and suppresses the amplitudon at proximate frequency. Our studies reveal an unexplored mechanism for the generation and extinction of collective excitations in quantum materials and pave the way for a microscopic understanding of ultrafast phenomena.

cond-mat.str-el↗

arXiv2025

The Future of the Correlated Electron Problem

A central problem in modern condensed matter physics is the understanding of materials with strong electron correlations. Despite extensive work, the essential physics of many of these systems is not understood and there is very little ability to make predictions in this class of materials. In this manuscript we share our personal views on the major open problems in the field of correlated electron systems. We discuss some possible routes to make progress in this rich and fascinating field. This manuscript is the result of the vigorous discussions and deliberations that took place at Johns Hopkins University during a three-day workshop January 27, 28, and 29, 2020 that brought together six senior scientists and 46 more junior scientists. Our hope, is that the topics we have presented will provide inspiration for others working in this field and motivation for the idea that significant progress can be made on very hard problems if we focus our collective energies.

cond-mat.str-el↗

arXiv2025

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, $\Gamma_M$, saturates near the conjectured ``Planckian" bound $\Gamma_M\sim kT/\hbar$, 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, $|\chi^{(3)}|\approx 6\times10^{-9}$ m$^2$/V$^2$, among the largest in the THz regime, enabling direct access to the rarely measured electronic energy relaxation rate, $\Gamma_E$. Strikingly, $\Gamma_E$ is 10-40 times smaller than $\Gamma_M$, revealing that the scatterings responsible for momentum loss and $T$-linear resistivity do not remove appreciable energy from the electrons. While $\Gamma_M (T)$ is consistent with quasi-elastic scattering from bosonic modes above their characteristic energy scale, this is incompatible with the increasing temperature dependence of $\Gamma_E(T)$. Our results exclude phonons as the source of $T$-linear resistivity and impose strong constraints on possible mechanisms.

cond-mat.supr-con↗

arXiv2025

Observation of a dynamic magneto-chiral instability in photoexcited tellurium

In a system of charged chiral fermions driven out of equilibrium, an electric current parallel to the magnetic field can generate a dynamic instability by which electromagnetic waves become amplified. Whether a similar instability can occur in chiral solid-state systems remains an open question. Using time-domain terahertz (THz) emission spectroscopy, we detect signatures of what we dub a ``dynamic magneto-chiral instability" in elemental tellurium, a structurally chiral crystal. Upon transient photoexcitation in a moderate external magnetic field, tellurium emits THz radiation consisting of coherent modes that amplify over time. An explanation for this amplification is proposed using a theoretical model based on a dynamic instability of electromagnetic waves interacting with infrared-active oscillators of impurity acceptor states in tellurium to form an amplifying polariton. Our work not only uncovers the presence of a magneto-chiral instability but also highlights its promise for THz-wave amplification in chiral materials.

cond-mat.mes-hall↗

arXiv2024

Revealing the hidden Dirac gap in a topological antiferromagnet using Floquet-Bloch manipulation

Manipulating solids using the time-periodic drive of a laser pulse is a promising route to generate new phases of matter. Whether such `Floquet-Bloch' manipulation can be achieved in topological magnetic systems with disorder has so far been unclear. In this work, we realize Floquet-Bloch manipulation of the Dirac surface-state mass of the topological antiferromagnet (AFM) MnBi$_2$Te$_4$. Using time- and angle-resolved photoemission spectroscopy (tr-ARPES), we show that opposite helicities of mid-infrared circularly polarized light result in substantially different Dirac mass gaps in the AFM phase, despite the equilibrium Dirac cone being massless. We explain our findings in terms of a Dirac fermion with a random mass. Our results underscore Floquet-Bloch manipulation as a powerful tool for controlling topology even in the presence of disorder, and for uncovering properties of materials that may elude conventional probes.

cond-mat.mes-hall↗

arXiv2024

Measuring the Debye Energy in Superconductors via two Electron Photoemission Spectroscopy

We demonstrate theoretically that double angle resolved photoemission spectroscopy (2eARPES) can directly probe the existence of Cooper pairs away from the Fermi surface, and can thus provide insight into the characteristic energy scale around the Fermi surface, the Debye energy, in which electrons are bound into Cooper pairs. To this end, we compute the photoelectron counting rate $P^{(2)}$ in two different types of unconventional superconductors, a $d_{x^2-y^2}$-wave superconductor, and a topological superconductor with a broken time-reversal symmetry. We show that $P^{(2)}$ provides insight into the relative strength of intra- and inter-band pairing in multi-band systems, as well as into the spin polarization of the bands.

cond-mat.supr-con↗

arXiv2024

Charge Conservation Beyond Uniformity: Spatially Inhomogeneous Electromagnetic Response in Periodic Solids

Nonlinear electromagnetic response functions have reemerged as a crucial tool for studying quantum materials. Most attention has been paid to responses to spatially uniform electric fields, relevant to optical experiments in conventional materials. However, magnetic and magnetoelectric phenomena are naturally connected by responses to spatially varying electric fields due to Maxwell's equations. Furthermore, in moiré materials, characteristic lattice scales are much longer, allowing spatial variation of optical electric fields to potentially have a measurable effect in experiments. To address these issues, we develop a formalism for computing linear and nonlinear responses to spatially inhomogeneous electromagnetic fields. Starting with the continuity equation, we derive an expression for the current operator that is manifestly conserved and model independent. Crucially, our formalism makes no assumptions on the form of the microscopic Hamiltonian and so is applicable to model Hamiltonians derived from tight-binding or ab initio calculations. We then develop a diagrammatic Kubo formalism for computing the wavevector dependence of linear and nonlinear conductivities, using Ward identities to fix the value of the diamagnetic current order-by-order in the vector potential. We apply our formula to compute the magnitude of the Kerr effect at oblique incidence for a model of a moiré Chern insulator and demonstrate the experimental relevance of spatially inhomogeneous fields in these systems. We further show how our formalism allows us to compute the magnetic multipole moments and magnetic susceptibility in insulators. We next use our formalism to compute the second-order transverse response to spatially varying transverse electric fields in our moiré Chern insulator model, with an eye towards the next generation of experiments in these systems.

cond-mat.mes-hall↗

arXiv2024

Disorder and diffuse scattering in single-chirality (TaSe$_4$)$_2$I crystals

The quasi-one-dimensional chiral compound (TaSe$_4$)$_2$I has been extensively studied as a prime example of a topological Weyl semimetal. Upon crossing its phase transition temperature $T_\textrm{CDW}$ $\approx$ 263 K, (TaSe$_4$)$_2$I exhibits incommensurate charge density wave (CDW) modulations described by the well-defined propagation vector $\sim$(0.05, 0.05, 0.11), oblique to the TaSe$_4$ chains. Although optical and transport properties greatly depend on chirality, there is no systematic report about chiral domain size for (TaSe$_4$)$_2$I. In this study, our single-crystal scattering refinements reveal a bulk iodine deficiency, and Flack parameter measurements on multiple crystals demonstrate that separate (TaSe$_4$)$_2$I crystals have uniform handedness, supported by direct imaging and helicity dependent THz emission spectroscopy. Our single-crystal X-ray scattering and calculated diffraction patterns identify multiple diffuse features and create a real-space picture of the temperature-dependent (TaSe$_4$)$_2$I crystal structure. The short-range diffuse features are present at room temperature and decrease in intensity as the CDW modulation develops. These transverse displacements, along with electron pinning from the iodine deficiency, help explain why (TaSe$_4$)$_2$I behaves as an electronic semiconductor at temperatures above and below $T_\textrm{CDW}$, despite a metallic band structure calculated from density functional theory of the ideal structure.

cond-mat.str-el↗

arXiv2024

Spin-Resolved Topology and Partial Axion Angles in Three-Dimensional Insulators

Symmetry-protected topological crystalline insulators (TCIs) have primarily been characterized by their gapless boundary states. However, in time-reversal- ($\mathcal{T}$-) invariant (helical) 3D TCI$\unicode{x2014}$termed higher-order TCIs (HOTIs)$\unicode{x2014}$the boundary signatures can manifest as a sample-dependent network of 1D hinge states. We here introduce nested spin-resolved Wilson loops and layer constructions as tools to characterize the intrinsic bulk topological properties of spinful 3D insulators. We discover that helical HOTIs realize one of three spin-resolved phases with distinct responses that are quantitatively robust to large deformations of the bulk spin-orbital texture: 3D quantum spin Hall insulators (QSHIs), "spin-Weyl" semimetals, and $\mathcal{T}$-doubled axion insulator (T-DAXI) states with nontrivial partial axion angles indicative of a 3D spin-magnetoelectric bulk response and half-quantized 2D TI surface states originating from a partial parity anomaly. Using ab-initio calculations, we demonstrate that $β$-MoTe$_2$ realizes a spin-Weyl state and that $α$-BiBr hosts both 3D QSHI and T-DAXI regimes.

cond-mat.mes-hall↗

arXiv2023

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↗

arXiv2023

Angle-Resolved Pair Photoemission Theory for Correlated Electrons

In this paper we consider the possibility and conditions for pair photoemission whereby two incident photons emit pairs of electrons from a candidate material as a novel method to measure and visualize electronic correlations. As opposed to double photoemission - where a single photon precipitates the ejection of a pair electrons via a subsequent electron energy loss scattering process - we show that pair photoemission need not be limited to interference between initial photoelectrons and valence electrons, and moreover, can occur without the energy penalty of two work functions. This enables detection of pairs of electrons at high energy resolution that may be correlated in the same quantum many-body states.

cond-mat.str-el↗

arXiv2022

Ultrafast x-ray scattering reveals composite amplitude collective mode in the Weyl charge density wave material (TaSe$_4$)$_2$I

We report ultrafast x-ray scattering experiments of the quasi-1D charge density wave (CDW) material (TaSe$_4$)$_2$I following photoexcitation with femtosecond infrared laser pulses. From the time-dependent diffraction signal at the CDW sidebands we identify an amplitude mode derived primarily from the transverse acoustic component of the CDW static distortion. The dynamics of this acoustic amplitude mode are described well by a model of a displacive excitation, which we interpret as mediated through a coupling to the optical phonon component associated with the tetramerization of the Ta chains.

cond-mat.mtrl-sci↗

arXiv2022

Anharmonic multiphonon origin of the valence plasmon in SrTi1-xNbxO3

Doped SrTi1-xNbxO3 exhibits superconductivity and a mid-infrared optical response reminiscent of copper-oxide superconductors. Strangely, its plasma frequency, omega_p, increases by a factor of ~3 when cooling from 300 K to 20 K, without any accepted explanation. Here, we present momentum-resolved electron energy loss spectroscopy (M-EELS) measurements of SrTi1-xNbxO3 at nonzero momentum, q. We find that the infrared feature previously identified as a plasmon is present at large q in insulating SrTiO3, where it exhibits the same temperature dependence and may be identified as an anharmonic, multiphonon background. Doping with Nb increases its peak energy and total spectral weight, drawing this background to lower q where it becomes visible in IR optics experiments. We conclude that the "plasmon" in doped SrTi1-xNbxO3 is not a free-carrier mode, but a composite excitation that inherits its unusual properties from the lattice anharmonicity of the insulator.

cond-mat.str-el↗

arXiv2022

Observation of the massive Lee-Fukuyama phason in a charge density wave insulator

The lowest-lying fundamental excitation of an incommensurate charge density wave (CDW) material is widely believed to be a massless phason -- a collective modulation of the phase of the CDW order parameter. However, as first pointed out by Lee and Fukuyama, long-range Coulomb interactions should push the phason energy up to the plasma energy of the CDW condensate, resulting in a massive phason and a fully gapped spectrum. Whether such behavior occurs in a CDW system has been unresolved for more than four decades. Using time-domain THz emission spectroscopy, we investigate this issue in the material (TaSe$_4$)$_2$I, a classical example of a quasi-one-dimensional CDW insulator. Upon transient photoexcitation at low temperatures, we find the material strikingly emits coherent, narrow-band THz radiation. The frequency, polarization and temperature-dependence of the emitted radiation imply the existence of a phason that acquires mass by coupling to long-range Coulomb interaction. Our observations constitute the first direct evidence of the massive "Lee-Fukuyama" phason and highlight the potential applicability of fundamental collective modes of correlated materials as compact and robust sources of THz radiation.

cond-mat.str-el↗

arXiv2022

Two-electron photoemission spectroscopy in Topological Superconductors

We demonstrate that the photo-electron counting rate, $P^{(2)}$, measured in two electron coincidence spectroscopy (2$e$-ARPES) experiments, provides unprecedented insight into the nature of topological superconductivity. In particular, we show that the spin dependence of $P^{(2)}$ allows one to detect superconducting spin-triplet correlations that are induced in a topological superconductor even in the absence of an associated triplet superconducting order parameter. This ability to detect spin-triplet correlations allows one to distinguish between two recently proposed scenarios for the microscopic origin of topological superconductivity in FeSe$_{0.45}$Te$_{0.55}$. Finally, we show that $P^{(2)}$ exhibits a characteristic intensity maximum that can be employed to detect topological phase transitions.

cond-mat.supr-con↗