arXiv subjects

Andrew J. Millis

Publications and source records attributed to Andrew J. Millis.

At least 55 records · Page 3Linked to original sources

arXiv2024

Deep learning analysis of polaritonic waves images

Deep learning (DL) is an emerging analysis tool across sciences and engineering. Encouraged by the successes of DL in revealing quantitative trends in massive imaging data, we applied this approach to nano-scale deeply sub-diffractional images of propagating polaritonic waves in complex materials. We developed a practical protocol for the rapid regression of images that quantifies the wavelength and the quality factor of polaritonic waves utilizing the convolutional neural network (CNN). Using simulated near-field images as training data, the CNN can be made to simultaneously extract polaritonic characteristics and materials parameters in a timescale that is at least three orders of magnitude faster than common fitting/processing procedures. The CNN-based analysis was validated by examining the experimental near-field images of charge-transfer plasmon polaritons at Graphene/α-RuCl3 interfaces. Our work provides a general framework for extracting quantitative information from images generated with a variety of scanning probe methods.

cond-mat.mtrl-sci↗

arXiv2024

Uniaxial plasmon polaritons $\textit{via}$ charge transfer at the graphene/CrSBr interface

Graphene is a privileged 2D platform for hosting confined light-matter excitations known as surface plasmon-polaritons (SPPs), as it possesses low intrinsic losses with a high degree of optical confinement. However, the inherently isotropic optical properties of graphene limit its ability to guide and focus SPPs, making it less suitable than anisotropic elliptical and hyperbolic materials as a platform for polaritonic lensing and canalization. Here, we present the graphene/CrSBr heterostructure as an engineered 2D interface that hosts highly anisotropic SPP propagation over a wide range of frequencies in the mid-infrared and terahertz. Using a combination of scanning tunneling microscopy (STM), scattering-type scanning near-field optical microscopy (s-SNOM), and first-principles calculations, we demonstrate mutual doping in excess of 10$^{13}$ cm$^{-2}$ holes/electrons between the interfacial layers of graphene/CrSBr heterostructures. SPPs in graphene activated by charge transfer interact with charge-induced anisotropic intra- and interband transitions in the interfacial doped CrSBr, leading to preferential SPP propagation along the quasi-1D chains that compose each CrSBr layer. This multifaceted proximity effect both creates SPPs and endows them with anisotropic transport and propagation lengths that differ by an order-of-magnitude between the two in-plane crystallographic axes of CrSBr.

cond-mat.mes-hall↗

arXiv2024

Downfolding from Ab Initio to Interacting Model Hamiltonians: Comprehensive Analysis and Benchmarking of the DFT+cRPA Approach

Model Hamiltonians are regularly derived from first-principles data to describe correlated matter. However, the standard methods for this contain a number of largely unexplored approximations. For a strongly correlated impurity model system, here we carefully compare a standard downfolding technique with the best possible ground-truth estimates for charge-neutral excited state energies and wavefunctions using state-of-the-art first-principles many-body wave function approaches. To this end, we use the vanadocene molecule and analyze all downfolding aspects, including the Hamiltonian form, target basis, double counting correction, and Coulomb interaction screening models. We find that the choice of target-space basis functions emerges as a key factor for the quality of the downfolded results, while orbital-dependent double counting correction diminishes the quality. Background screening to the Coulomb interaction matrix elements primarily affects crystal-field excitations. Our benchmark uncovers the relative importance of each downfolding step and offers insights into the potential accuracy of minimal downfolded model Hamiltonians

cond-mat.str-el↗

arXiv2024

Keldysh field theory of dynamical exciton condensation transitions in nonequilibrium electron-hole bilayers

Recent experiments have realized steady-state electrical injection of interlayer excitons in electron-hole bilayers subject to a large bias voltage. In the ideal case in which interlayer tunneling is negligibly weak, the system is in quasi-equilibrium with a reduced effective band gap. Interlayer tunneling introduces a current and drives the system out of equilibrium. In this work we derive a nonequilibrium field theory description of interlayer excitons in biased electron-hole bilayers. In the large bias limit, we find that p-wave interlayer tunneling reduces the effective band gap and increases the effective temperature for intervalley excitons. We discuss possible experimental implications for InAs/GaSb quantum wells and transition metal dichalcogenide bilayers.

cond-mat.mes-hall↗

arXiv2024

Electrical Transport in the Hatsugai-Kohmoto Model

We show that in models with the Hatsugai-Kohmoto type of interaction that is local in momentum space thus infinite-range in real space, Kubo formulas neither reproduce the correct thermodynamic susceptibilities, nor yield sensible transport coefficients. Using Kohn's trick to differentiate between metals and insulators by threading a flux in a torus geometry, we uncover the striking property that Hatsugai-Kohmoto models with an interaction-induced gap in the spectrum sustain a current that grows as the linear size at any non-zero flux and which can be either diamagnetic or paramagnetic.

cond-mat.str-el↗

arXiv2024

Correlation Functions From Tensor Network Influence Functionals: The Case of the Spin-Boson Model

We investigate the application of matrix product state (MPS) representations of the influence functionals (IF) for the calculation of real-time equilibrium correlation functions in open quantum systems. Focusing specifically on the unbiased spin-boson model, we explore the use of IF-MPSs for complex time propagation, as well as IF-MPSs for constructing correlation functions in the steady state. We examine three different IF approaches: one based on the Kadanoff-Baym contour targeting correlation functions at all times, one based on a complex contour targeting the correlation function at a single time, and a steady state formulation which avoids imaginary or complex times, while providing access to correlation functions at all times. We show that within the IF language, the steady state formulation provides a powerful approach to evaluate equilibrium correlation functions.

physics.chem-ph↗

arXiv2024

Good plasmons in a bad metal

Correlated materials may exhibit unusually high resistivity increasing linearly in temperature, breaking through the Mott-Ioffe-Regel bound, above which coherent quasiparticles are destroyed. The fate of collective charge excitations, or plasmons, in these systems is a subject of debate. Several studies suggest plasmons are overdamped while others detect unrenormalized plasmons. Here, we present direct optical images of low-loss hyperbolic plasmon polaritons (HPPs) in the correlated van der Waals metal MoOCl2. HPPs are plasmon-photon modes that waveguide through extremely anisotropic media and are remarkably long-lived in MoOCl2. Many-body theory supported by photoemission results reveals that MoOCl2 is in an orbital-selective and highly incoherent Peierls phase. Different orbitals acquire markedly different bonding-antibonding character, producing a highly-anisotropic, isolated Fermi surface. The Fermi surface is further reconstructed and made partly incoherent by electronic interactions, renormalizing the plasma frequency. HPPs remain long-lived in spite of this, allowing us to uncover previously unseen imprints of electronic correlations on plasmonic collective modes.

cond-mat.str-el↗

arXiv2024

Superconductivity in twisted bilayer WSe$_2$

The discovery of superconductivity in twisted bilayer and twisted trilayer graphene has generated tremendous interest. The key feature of these systems is an interplay between interlayer coupling and a moiré superlattice that gives rise to low-energy flat bands with strong correlations. Flat bands can also be induced by moiré patterns in lattice-mismatched and or twisted heterostructures of other two-dimensional materials such as transition metal dichalcogenides (TMDs). Although a wide range of correlated phenomenon have indeed been observed in the moiré TMDs, robust demonstration of superconductivity has remained absent. Here we report superconductivity in 5 degree twisted bilayer WSe$_2$ (tWSe$_2$) with a maximum critical temperature of 426 mK. The superconducting state appears in a limited region of displacement field and density that is adjacent to a metallic state with Fermi surface reconstruction believed to arise from antiferromagnetic order. A sharp boundary is observed between the superconducting and magnetic phases at low temperature, reminiscent of spin-fluctuation mediated superconductivity. Our results establish that moiré flat-band superconductivity extends beyond graphene structures. Material properties that are absent in graphene but intrinsic among the TMDs such as a native band gap, large spin-orbit coupling, spin-valley locking, and magnetism offer the possibility to access a broader superconducting parameter space than graphene-only structures.

cond-mat.mes-hall↗

arXiv2024

Stoner instabilities and Ising excitonic states in twisted transition metal dichalcogenides

Moiré transition metal dichalcogenide (TMD) systems provide a tunable platform for studying electron-correlation driven quantum phases. Such phases have so far been found at rational fillings of the moiré superlattice, and it is believed that lattice commensurability plays a key role in their stability. In this work, we show via magnetotransport measurements on twisted WSe2 that new correlated electronic phases can exist away from commensurability. The first phase is an antiferromagnetic metal that is driven by proximity to the van Hove singularity. The second is a re-entrant magnetic field-driven insulator. This insulator is formed from a small and equal density of electrons and holes with opposite spin projections - an Ising excitonic insulator.

cond-mat.str-el↗

arXiv2024

On the Adequacy of the Dynamical Mean Field Theory for Low Density and Dirac Materials

The qualitative reliability of the dynamical mean field theory (DMFT) is investigated for systems in which either the actual carrier density or the effective carrier density is low, by comparing the exact perturbative and dynamical mean field expressions of electron scattering rates and optical conductivities. We study two interacting systems: tight binding models in which the chemical potential is near a band edge and Dirac systems in which the chemical potential is near the Dirac point. In both systems it is found that DMFT underestimates the low frequency, near-Fermi surface single particle scattering rate by a factor proportional to the particle density. The quasiparticle effective mass is qualitatively incorrect for the low density tight binding model but not necessarily for Dirac systems. The dissipative part of the optical conductivity is more subtle: in the exact calculation vertex corrections, typically neglected in DMFT calculations, suppress the low frequency optical absorption, compensating for some of the DMFT underestimate of the scattering rate. The role of vertex corrections in calculating the conductivity for Dirac systems is clarified and a systematic discussion is given of the approach to the Galilean/Lorentz invariant low density limit. Relevance to recent calculations related to Weyl metals is discussed.

cond-mat.str-el↗

arXiv2024

Machine learning-based compression of quantum many body physics: PCA and autoencoder representation of the vertex function

Characterizing complex many-body phases of matter has been a central question in quantum physics for decades. Numerical methods built around approximations of the renormalization group (RG) flow equations have offered reliable and systematically improvable answers to the initial question -- what simple physics drives quantum order and disorder? The flow equations are a very high dimensional set of coupled nonlinear equations whose solution is the two particle vertex function, a function of three continuous momenta that describes particle-particle scattering and encodes much of the low energy physics including whether the system exhibits various forms of long ranged order. In this work, we take a simple and interpretable data-driven approach to the open question of compressing the two-particle vertex. We use PCA and an autoencoder neural network to derive compact, low-dimensional representations of underlying physics for the case of interacting fermions on a lattice. We quantify errors in the representations by multiple metrics and show that a simple linear PCA offers more physical insight and better out-of-distribution (zero-shot) generalization than the nominally more expressive nonlinear models. Even with a modest number of principal components (10 - 20), we find excellent reconstruction of vertex functions across the phase diagram. This result suggests that many other many-body functions may be similarly compressible, potentially allowing for efficient computation of observables. Finally, we identify principal component subspaces that are shared between known phases, offering new physical insight.

cond-mat.str-el↗

arXiv2024

Sublattice structure and topology in spontaneously crystallized electronic states

The prediction and realization of the quantum anomalous Hall effect are often intimately connected to honeycomb lattices in which the sublattice degree of freedom plays a central role in the nontrivial topology. Two-dimensional Wigner crystals, on the other hand, form triangular lattices without sublattice degrees of freedom, resulting in a topologically trivial state. In this Letter, we discuss the possibility of spontaneously formed honeycomb-lattice crystals that exhibit the quantum anomalous Hall effect. Starting from a single-band system with nontrivial quantum geometry, we derive the mean-field energy functional of a class of crystal states and express it as a model of sublattice pseudospins in momentum space. We find that nontrivial quantum geometry leads to extra terms in the pseudospin model that break an effective `time-reversal symmetry' and favor a topologically nontrivial pseudospin texture. When the effects of these extra terms dominate over the ferromagnetic exchange coupling between pseudospins, the anomalous Hall crystal state becomes energetically favorable over the trivial Wigner crystal state.

cond-mat.str-el↗

arXiv2023

Observation of an electronic microemulsion phase emerging from a quantum crystal-to-liquid transition

Strongly interacting electronic systems possess rich phase diagrams resulting from the competition between different quantum ground states. A general mechanism that relieves this frustration is the emergence of microemulsion phases, where regions of different phase self-organize across multiple length scales. The experimental characterization of these phases often poses significant challenges, as the long-range Coulomb interaction microscopically mingles the competing states. Here, we use cryogenic reflectance and magneto-optical spectroscopy to observe the signatures of the mixed state between an electronic Wigner crystal and an electron liquid in a MoSe2 monolayer. We find that the transit into this 'microemulsion' state is marked by anomalies in exciton reflectance, spin susceptibility, and Umklapp scattering, establishing it as a distinct phase of electronic matter. Our study of the two-dimensional electronic microemulsion phase elucidates the physics of novel correlated electron states with strong Coulomb interactions.

cond-mat.str-el↗

arXiv2023

Edge zeros and boundary spinons in topological Mott insulators

We introduce a real-space slave rotor theory of the physics of topological Mott insulators, using the Kane-Mele-Hubbard model as an example, and use it to show that a topological gap in the Green function zeros corresponds to a gap in the bulk spinon spectrum and that a zero edge mode corresponds to a spinon edge mode. We then consider an interface between a topological Mott insulator and a conventional topological insulator showing how the spinon edge mode of the topological Mott insulator combines with the spin part of the conventional electron topological edge state leaving a non-Fermi liquid edge mode described by a gapless propagating holon and gapped spinon state. Our work demonstrates the physical meaning of Green function zeros and shows that interfaces between conventional and Mott topological insulators are a rich source of new physics.

cond-mat.str-el↗

arXiv2023

Dynamical exciton condensates in biased electron-hole bilayers

Bilayer materials may support interlayer excitons comprised of electrons in one layer and holes in the other. In experiments, a non-zero exciton density is typically sustained by a bias chemical potential, implemented either by optical pumping or by electrical contacts connected to the two layers. We show that if charge can tunnel between the layers, the chemical potential bias means that an exciton condensate is in the dynamical regime of ac Josephson effect. It has physical consequences such as tunneling currents and the ability to tune a condensate from bright (emitting coherent photons) to dark by experimental controlling knobs. If the system is placed in an optical cavity, coupling with cavity photons favors different dynamical states depending on the bias, realizing superradiant phases.

cond-mat.mes-hall↗

arXiv2023

Exciton-spin interactions in antiferromagnetic charge-transfer insulators

We derive exciton-spin interactions from a microscopic correlated model that captures important aspects of the physics of charge-transfer (CT) insulators to address magnetism associated with exciton creation. We present a minimal model consisting of coupled clusters of transition metal d and ligand p orbitals that captures the essential features of the local atomic and electronic structure. First, we identify the lowest-energy state and optically allowed excited states within a cluster by applying the molecular orbital picture to the ligand p orbitals. Then, we derive the effective interactions between two clusters mediated by intercluster hoppings, which include exciton-spin couplings. The interplay of the correlations and the spatial structure of the CT exciton leads to strong magnetic exchange couplings with spatial anisotropy. Finally, we calculate an optical excitation spectrum in our effective model to obtain insights into magnetic sidebands optically observed in magnetic materials. We demonstrate that the spin-flip excitation due to the strongly enhanced local spin interactions around the exciton gives rise to the magnetic sidebands.

cond-mat.str-el↗

arXiv2023

Magnetism and Metallicity in Moiré Transition Metal Dichalcogenides

The ability to control the properties of twisted bilayer transition metal dichalcogenides in situ makes them an ideal platform for investigating the interplay of strong correlations and geometric frustration. Of particular interest are the low energy scales, which make it possible to experimentally access both temperature and magnetic fields that are of the order of the bandwidth or the correlation scale. In this manuscript we analyze the moiré Hubbard model, believed to describe the low energy physics of an important subclass of the twisted bilayer compounds. We establish its magnetic and the metal-insulator phase diagram for the full range of magnetic fields up to the fully spin polarized state. We find a rich phase diagram including fully and partially polarized insulating and metallic phases of which we determine the interplay of magnetic order, Zeeman-field, and metallicity, and make connection to recent experiments.

cond-mat.str-el↗

arXiv2023

Picosecond volume expansion drives a later-time insulator-metal transition in a nano-textured Mott Insulator

Technology moves towards ever faster switching between different electronic and magnetic states of matter. Manipulating properties at terahertz rates requires accessing the intrinsic timescales of electrons (femtoseconds) and associated phonons (10s of femtoseconds to few picoseconds), which is possible with short-pulse photoexcitation. Yet, in many Mott insulators, the electronic transition is accompanied by the nucleation and growth of percolating domains of the changed lattice structure, leading to empirical time scales dominated by slow coarsening dynamics. Here, we use time-resolved X-ray diffraction and reflectivity measurements to investigate the photoinduced insulator-to-metal transition in an epitaxially strained thin film Mott insulator Ca2RuO4. The dynamical transition occurs without observable domain formation and coarsening effects, allowing the study of the intrinsic electronic and lattice dynamics. Above a fluence threshold, the initial electronic excitation drives a fast lattice rearrangement, followed by a slower electronic evolution into a metastable non-equilibrium state. Microscopic calculations based on time-dependent dynamical mean-field theory and semiclassical lattice dynamics within a recently published equilibrium energy landscape picture explain the threshold-behavior and elucidate the delayed onset of the electronic phase transition in terms of kinematic constraints on recombination. Analysis of satellite scattering peaks indicates the persistence of a strain-induced nano-texture in the photoexcited film. This work highlights the importance of combined electronic and structural studies to unravel the physics of dynamic transitions and elucidates the role of strain in tuning the timescales of photoinduced processes.

cond-mat.str-el↗