arXiv subjects

A. J. Millis

Publications and source records attributed to A. J. Millis.

At least 19 recordsLinked to original sources

arXiv2026

Finite-temperature Green's function cluster expansion from thermofield doubles: Breakdown of the polaron picture

We introduce a method, numerically exact in principle, for computing the momentum- and frequency-resolved single-particle Green's function of a polaron at finite temperature. The method, which we refer to as the finite-temperature Green's function cluster expansion, combines two ingredients: the generalized Green's function cluster expansion, a numerically exact extension of the momentum average family of methods that solves the polaron problem at zero temperature through a hierarchy of equations of motion for restricted phonon cloud configurations; and the thermofield double formalism, which maps the thermal trace onto a pure-state expectation value over a doubled Hilbert space. The resulting equations of motion have the same algebraic structure as those of the multi-boson zero-temperature theory, with the temperature entering through a Bogoliubov-type mixing angle that controls the coupling to a set of fictitious bath bosons. We implement the method in our open-source software package and benchmark it on the one-dimensional Holstein polaron, computing spectral functions, dispersions, lifetimes, and effective masses across coupling regimes and temperatures up to $T/Ω\sim 1$. Where finite-temperature density matrix renormalization group results are available, we find quantitative agreement at affordable computational cost. The method recovers momentum-resolved spectra directly in frequency space, with no time evolution or analytic continuation. We also discuss the practical costs of the approach. In particular, since the doubled phonon Hilbert space has a non-trivial configuration structure in which real and fictitious clouds compete, convergence in the corresponding cloud parameters requires care.

cond-mat.str-el↗

arXiv2026

Quantum Light Nano-Imaging

Entanglement and quantum correlations are central to the physics of quantum materials, yet they have remained notoriously difficult to access experimentally. Accessing these phenomena in solids requires quantum optical probes that operate at the native length and time scales of material excitations, below the diffraction limit of light. Developing the requisite tools has previously been infeasible due to the weak intensities of state-of-the-art quantum light sources and the inefficiency of light coupling in near-field light-matter interactions. In this work, we address these challenges and report the development of a quantum light scattering-type scanning near-field optical microscope (q-SNOM) that enables quantum-optical studies of solid-state systems with nanoscale spatial resolution. As a first demonstration, we visualize the self-interference of single hybrid light-matter polaritons in the prototypical van der Waals semiconductor MoS2. We also introduce a polaritonic time-of-flight metrology that exploits the temporal correlations among entangled photons to observe the quasiparticle propagation dynamics at femtosecond time scales. This work establishes a new experimental paradigm for exploring quantum effects in materials at the nanoscale.

cond-mat.mes-hall↗

arXiv2026

Dimensionality-Driven Electronic and Orbital Transitions Mediating Interfacial Magnetism in LaNiO3/CaMnO3 Observed In Situ

Emergent magnetic states at oxide interfaces arise from the interplay of charge transfer, orbital reconstruction, and dimensional confinement, offering a route to engineered correlated-electron behavior in nanoscale spintronic materials. Here, we combine in situ synthesis, polarization-dependent angle-resolved photoelectron spectroscopy, X-ray magnetic circular dichroism, and first-principles electronic-structure calculations to investigate LaNiO3/CaMnO3 superlattices. We show that reducing the LaNiO3 thickness drives a metal-insulator transition accompanied by loss of electronic coherence and an orbital-polarization crossover in the ultrathin limit. These changes weaken charge transfer across the interface and suppress the interfacial Mn magnetic moment in CaMnO3, revealing that the emergent ferromagnetic state is directly governed by electronic confinement in LaNiO3. The insulating state and orbital reconstruction are reproduced by density functional theory combined with dynamical mean-field theory. Together, these results establish a direct and tunable coupling among electronic, orbital, and magnetic degrees of freedom in oxide heterostructures.

cond-mat.str-el↗

arXiv2025

Light-induced Asymmetric Pseudogap below T$_\text{c}$ in cuprates

To this day, high-temperature cuprate superconductors remain an unparalleled platform for studying the competition and coexistence of emergent, static and dynamic, quantum phases of matter exhibiting high transition temperature non-s-wave superconductivity, non-Fermi liquid transport and a still enigmatic pseudogap regime. However, how superconductivity emerges alongside and competes with the pseudogap regime remains an open question. Here, we present a high-resolution, time- and angle-resolved photoemission study of the near-antinodal region of optimally-doped Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$. For a sufficiently high excitation fluence, we disrupt superconductivity and drive a transient change from a symmetric superconducting-like to an asymmetric pseudogap-like density of states, for electronic temperatures well below the equilibrium superconducting critical temperature. Conversely, when the superconductivity is fully restored, the pseudogap is suppressed, as signaled by a fully particle-hole symmetric density of states. A unique aspect of our experiments is that the pseudogap coexists with superconducting features at intermediate times or at intermediate fluence. Our findings challenge the paradigm that superconductivity emerges by establishing phase coherence in the pseudogap. Instead, our experimental results, supported by phenomenological theory, demonstrate that the two states compete, and that the low-temperature ground state of the cuprates originates from a competition between superconducting and pseudogap states.

cond-mat.supr-con↗

arXiv2023

Orbital polarization, charge transfer, and fluorescence in reduced valence nickelates

This paper presents a simple formalism for calculating X-ray absorption (XAS) and resonant inelastic x-ray scattering (RIXS) that has as input orbital-resolved density of states from a single-particle or many-body \textit{ab initio} calculation and is designed to capture itinerant-like features. We use this formalism to calculate both the XAS and RIXS with input from DFT and DFT+DMFT for the recently studied reduced valence nickelates $R_4$Ni$_3$O$_8$ and $R$NiO$_2$ ($R$ a rare earth), and these results are then contrasted with those for the cuprate CaCuO$_2$ and the unreduced nickelate $R_4$Ni$_3$O$_{10}$. In contrast to the unreduced $R_4$Ni$_3$O$_{10}$, the reduced valence nickelates as well as the cuprate show strong orbital polarization due to the dominance of $x^2-y^2$ orbitals for the unoccupied $3d$ states. We also reproduce two key aspects of a recent RIXS experiment for $R_4$Ni$_3$O$_8$: (i) a charge transfer feature between $3d$ and oxygen $2p$ states whose energy we find to decrease as one goes from $R$NiO$_2$ to $R_4$Ni$_3$O$_8$ to the cuprate, and (ii) an energy-dependent polarization reversal of the fluorescence line that arises from hybridization of the unoccupied $z^2$ states with $R$ 5d states. We end with some implications of our results for the nature of the $3d$ electrons in reduced valence nickelates.

cond-mat.str-el↗

arXiv2023

Bipolaronic high-temperature superconductivity

Electron-lattice interactions play a prominent role in quantum materials, making a deeper understanding of direct routes to phonon-mediated high-transition-temperature ($T_{\mathrm{c}}$) superconductivity desirable. However, it has been known for decades that weak electron-phonon coupling gives rise to low values of $T_{\mathrm{c}}$, while strong electron-phonon coupling leads to lattice instability or formation of bipolarons, generally assumed to be detrimental to superconductivity. Thus, the route to high-$T_{\mathrm{c}}$ materials from phonon-mediated mechanisms has heretofore appeared to be limited to raising the phonon frequency as in the hydrogen sulfides. Here we present a simple model for phonon-mediated high-$T_{\mathrm{c}}$ superconductivity based on superfluidity of light bipolarons. In contrast to the widely studied Holstein model where lattice distortions modulate the electron's potential energy, we investigate the situation where lattice distortions modulate the electron hopping. This physics gives rise to small-size, yet light bipolarons, which we study using an exact sign-problem-free quantum Monte Carlo approach, demonstrating a new route to phonon-mediated high-$T_\mathrm{c}$ superconductivity. We find that $T_\mathrm{c}$ in our model generically and significantly exceeds typical upper bounds based on Migdal-Eliashberg theory or superfluidity of Holstein bipolarons. The key ingredient in this bipolaronic mechanism that gives rise to high $T_\mathrm{c}$ is the combination of light mass and small size of bipolarons. Our work establishes principles towards the design of high-$T_{\mathrm{c}}$ superconductors via functional material engineering.

cond-mat.supr-con↗

arXiv2022

Bipolaronic superconductivity out of a Coulomb gas

Employing unbiased sign-problem-free quantum Monte Carlo, we investigate the effects of long-range Coulomb forces on BEC of bipolarons using a model of bond phonon-modulated electron hopping. In absence of long-range repulsion, this model was recently shown to give rise to small-size, light-mass bipolarons that undergo a superfluid transition at high values of the critical transition temperature $T_\mathrm{c}$. We find that $T_\mathrm{c}$ in our model even with the long-range Coulomb repulsion remains much larger than that of Holstein bipolarons, and can be on the order of or greater than the typical upper bounds on phonon-mediated $T_\mathrm{c}$ based on the Migdal-Eliashberg and McMillan approximations. Our work points to a physically simple mechanism for superconductivity in the low-density regime that may be relevant to current experiments on dilute superconductors.

cond-mat.supr-con↗

arXiv2022

Coupling of Magnetic Phases at Nickelate Interfaces

In this work we present a model system built out of artificially layered materials, allowing us to understand the interrelation of magnetic phases with that of the metallic-insulating phase at long length-scales, and enabling new strategies for the design and control of materials in devices. The artificial model system consists of superlattices made of SmNiO$_3$ and NdNiO$_3$ layers -- two members of the fascinating rare earth nickelate family, having different metal-to-insulator and magnetic transition temperatures. By combining two complementary techniques -- resonant elastic x-ray scattering and muon spin relaxation -- we show how the magnetic order evolves, in this complex multicomponent system, as a function of temperature and superlattice periodicity. We demonstrate that the length scale of the coupling between the antiferromagnetic and paramagnetic phases is longer than that of the electronic metal-insulator phase transition -- despite being subsidiary to it. This can be explained via a Landau theory -- where the bulk magnetic energy plus a gradient cost between magnetic and non magnetic phases are considered. These results provide a clear understanding of the coupling of magnetic transitions in systems sharing identical order parameters.

cond-mat.str-el↗

arXiv2022

Infrared Plasmons Propagate through a Hyperbolic Nodal Metal

Metals are canonical plasmonic media at infrared and optical wavelengths, allowing one to guide and manipulate light at the nano-scale. A special form of optical waveguiding is afforded by highly anisotropic crystals revealing the opposite signs of the dielectric functions along orthogonal directions. These media are classified as hyperbolic and include crystalline insulators, semiconductors and artificial metamaterials. Layered anisotropic metals are also anticipated to support hyperbolic waveguiding. Yet this behavior remains elusive, primarily because interband losses arrest the propagation of infrared modes. Here, we report on the observation of propagating hyperbolic waves in a prototypical layered nodal-line semimetal ZrSiSe. The observed waveguiding originates from polaritonic hybridization between near-infrared light and nodal-line plasmons. Unique nodal electronic structures simultaneously suppress interband loss and boost the plasmonic response, ultimately enabling the propagation of infrared modes through the bulk of the crystal.

cond-mat.mes-hall↗

arXiv2021

Anti-Poiseuille Flow: Increased Vortex Velocity at Superconductor Edges

Using the time-dependent Ginzburg Landau equations we study vortex motion driven by an applied current in two dimensional superconductors in the presence of a physical boundary. At smaller sourced currents the vortex lattice moves as a whole, with each vortex moving at the same velocity. At larger sourced current, vortex motion is organized into channels, with vortices in channels nearer to the sample edges moving faster than those farther away from sample edges, opposite to the Poiseuille flow of basic hydrodynamics where the velocity is lowest at the boundaries. At intermediate currents, a stick-slip motion of the vortex lattice occurs in which vortices in the channel at the boundary break free from the Abrikosov lattice, accelerate, move past their neighbors and then slow down and reattach to the vortex lattice at which point the stick-slip process starts over. These effects could be observed experimentally, e.g. using fast scanning microscopy techniques.

cond-mat.supr-con↗

arXiv2021

Fizeau Drag in Graphene Plasmonics

Dragging of light by moving dielectrics was predicted by Fresnel and verified by Fizeau's celebrated experiments with flowing water. This momentous discovery is among the experimental cornerstones of Einstein's special relativity and is well understood in the context of relativistic kinematics. In contrast, experiments on dragging photons by an electron flow in solids are riddled with inconsistencies and so far eluded agreement with the theory. Here we report on the electron flow dragging surface plasmon polaritons (SPPs): hybrid quasiparticles of infrared photons and electrons in graphene. The drag is visualized directly through infrared nano-imaging of propagating plasmonic waves in the presence of a high-density current. The polaritons in graphene shorten their wavelength when launched against the drifting carriers. Unlike the Fizeau effect for light, the SPP drag by electrical currents defies the simple kinematics interpretation and is linked to the nonlinear electrodynamics of the Dirac electrons in graphene. The observed plasmonic Fizeau drag enables breaking of time-reversal symmetry and reciprocity at infrared frequencies without resorting to magnetic fields or chiral optical pumping.

cond-mat.mes-hall↗

arXiv2020

Influence of spin and orbital fluctuations on Mott-Hubbard exciton dynamics in LaVO${}_{3}$ Thin Films

Recent optical conductivity measurements reveal the presence of Hubbard excitons in certain Mott insulators. In light of these results, it is important to revisit the dynamics of these materials to account for excitonic correlations. We investigate time-resolved excitation and relaxation dynamics as a function of temperature in perovskite-type LaVO${}_{3}$ thin films using ultrafast optical pump-probe spectroscopy. LaVO${}_{3}$ undergoes a series of phase transitions at roughly the same critical temperature $T_C\cong 140\ K$, including a second-order magnetic phase transition (PM $\xrightarrow{}$ AFM) and a first-order structural phase transition, accompanied by \textit{C}-type spin order (SO) and \textit{G}-type orbital order (OO). Ultrafast optical pump-probe spectroscopy at 1.6 eV monitors changes in the spectral weight of the Hubbard exciton resonance which serves as a sensitive reporter of spin and orbital fluctuation dynamics. We observe dramatic slowing down of the spin, and orbital dynamics in the vicinity of $T_C\cong 140$ K, reminiscent of a second-order phase transition, despite the (weakly) first-order nature of the transition. We emphasize that since it is spectral weight changes that are probed, the measured dynamics are not reflective of conventional exciton generation and recombination, but are related to the dynamics of Hubbard exciton formation in the presence of a fluctuating many-body environment.

cond-mat.str-el↗

arXiv2020

Loschmidt-amplitude wave function spectroscopy and the physics of dynamically driven phase transitions

We introduce the Loschmidt amplitude as a powerful tool to perform spectroscopy of generic many-body wave functions and use it to interrogate the wave function obtained after ramping the transverse field quantum Ising model through its quantum critical point. Previous results are confirmed and a more complete understanding of the population of defects and of the effects of magnon-magnon interaction or finite-size corrections is obtained. The influence of quantum coherence is clarified.

cond-mat.stat-mech↗

arXiv2019

Multi-messenger nano-probes of hidden magnetism in a strained manganite

The ground state properties of correlated electron systems can be extraordinarily sensitive to external stimuli, such as temperature, strain, and electromagnetic fields, offering abundant platforms for functional materials. We present a metastable and reversible photoinduced ferromagnetic transition in strained films of the doped manganite La(2/3)Ca(1/3)MnO3. Using the novel multi-messenger combination of atomic force microscopy, cryogenic scanning near-field optical microscopy, magnetic force microscopy, and ultrafast laser excitation, we demonstrate both "writing" and "erasing" of a metastable ferromagnetic metal phase with nanometer-resolved finesse. By tracking both optical conductivity and magnetism at the nano-scale, we reveal how spontaneous strain underlies the thermal stability, persistence, and reversal of this photoinduced metal. Our first-principles electronic structure calculations reveal how an epitaxially engineered Jahn-Teller distortion can stabilize nearly degenerate antiferromagnetic insulator and ferromagnetic metal phases. We propose a Ginzburg-Landau description to rationalize the co-active interplay of strain, lattice distortion, and magnetism we resolve in strained LCMO, thus guiding future functional engineering of epitaxial oxides like manganites into the regime of phase-programmable materials.

cond-mat.mes-hall↗

arXiv2019

Absence of dissipationless transport in clean 2D superconductors

Dissipationless charge transport is one of the defining properties of superconductors (SC). The interplay between dimensionality and disorder in determining the onset of dissipation in SCs remains an open theoretical and experimental problem. In this work, we present measurements of the dissipation phase diagrams of SCs in the two dimensional (2D) limit, layer by layer, down to a monolayer in the presence of temperature (T), magnetic field (B), and current (I) in 2H-NbSe2. Our results show that the phase-diagram strongly depends on the SC thickness even in the 2D limit. At four layers we can define a finite region in the I-B phase diagram where dissipationless transport exists at T=0. At even smaller thicknesses, this region shrinks in area. In a monolayer, we find that the region of dissipationless transport shrinks towards a single point, defined by T=B=I=0. In applied field, we show that time-dependent-Ginzburg-Landau (TDGL) simulations that describe dissipation by vortex motion, qualitatively reproduce our experimental I-B phase diagram. Last, we show that by using non-local transport and TDGL calculations that we can engineer charge flow and create phase boundaries between dissipative and dissipationless transport regions in a single sample, demonstrating control over non-equilibrium states of matter.

cond-mat.mes-hall↗

arXiv2018

Nature of the metal-insulator transition in few-unit-cell-thick LaNiO3 films

The nature of the metal insulator transition in thin films and superlattices of LaNiO3 with only few unit cells in thickness remains elusive despite tremendous effort. Quantum confinement and epitaxial strain have been evoked as the mechanisms, although other factors such as growth-induced disorder, cation non-stoichiometry, oxygen vacancies, and substrate-film interface quality may also affect the observable properties in the ultrathin films. Here we report results obtained for near-ideal LaNiO3 films with different thicknesses and terminations grown by atomic layer-by-layer laser molecular beam epitaxy on LaAlO3 substrates. We find that the room-temperature metallic behavior persists until the film thickness is reduced to an unprecedentedly small 1.5 unit cells (NiO2 termination). Electronic structure measurements using x-ray absorption spectroscopy and first-principles calculation suggest that oxygen vacancies existing in the films also contribute to the metal insulator transition.

cond-mat.mtrl-sci↗

arXiv2018

Floquet Engineering in Quantum Chains

We consider a one-dimensional interacting spinless fermion model, which displays the well-known Luttinger liquid (LL) to charge density wave (CDW) transition as a function of the ratio between the strength of the interaction, $U$, and the hopping, $J$. We subject this system to a spatially uniform drive which is ramped up over a finite time interval and becomes time-periodic in the long time limit. We show that by using a density matrix renormalization group (DMRG) approach formulated for infinite system sizes, we can access the large-time limit even when the drive induces finite heating. When both the initial and long-time states are in the gapless (LL) phase, the final state has power law correlations for all ramp speeds. However, when the initial and final state are gapped (CDW phase), we find a pseudothermal state with an effective temperature that depends on the ramp rate, both for the Magnus regime in which the drive frequency is very large compared to other scales in the system and in the opposite limit where the drive frequency is less than the gap. Remarkably, quantum defects (instantons) appear when the drive tunes the system through the quantum critical point, in a realization of the Kibble-Zurek mechanism.

cond-mat.str-el↗

arXiv2018

Evidence of an improper displacive phase transition in Cd$_2$Re$_2$O$_7$ via time-resolved coherent phonon spectroscopy

We have used a combination of ultrafast coherent phonon spectroscopy, ultrafast thermometry, and time-dependent Landau theory to study the inversion symmetry breaking phase transition at $T_c = 200$ K in the strongly spin-orbit coupled correlated metal Cd$_2$Re$_2$O$_7$. We establish that the structural distortion at $T_c$ is a secondary effect through the absence of any softening of its associated phonon mode, which supports a purely electronically driven mechanism. However, the phonon lifetime exhibits an anomalously strong temperature dependence that decreases linearly to zero near $T_c$. We show that this behavior naturally explains the spurious appearance of phonon softening in previous Raman spectroscopy experiments and should be a prevalent feature of correlated electron systems with linearly coupled order parameters.

cond-mat.str-el↗