All clocks, in some form or another, use the evolution of nature toward higher entropy states to quantify the passage of time. Because of the statistical nature of the second law and corresponding entropy flows, fluctuations fundamentally limit the performance of any clock. This suggests a deep relation between the increase in entropy and the quality of clock ticks. Indeed, minimal models for autonomous clocks in the quantum realm revealed that a linear relation can be derived, where for a limited regime every bit of entropy linearly increases the accuracy of quantum clocks. But can such a linear relation persist as we move toward a more classical system? We answer this in the affirmative by presenting the first experimental investigation of this thermodynamic relation in a nanoscale clock. We stochastically drive a nanometer-thick membrane and read out its displacement with a radio-frequency cavity, allowing us to identify the ticks of a clock. We show theoretically that the maximum possible accuracy for this classical clock is proportional to the entropy created per tick, similar to the known limit for a weakly coupled quantum clock but with a different proportionality constant. We measure both the accuracy and the entropy. Once nonthermal noise is accounted for, we find that there is a linear relation between accuracy and entropy and that the clock operates within an order of magnitude of the theoretical bound.

The local number variance ${\sigma }^2(R)$ associated with a spherical sampling window of radius $R$ enables a classification of many-particle systems in $d$-dimensional Euclidean space ${\mathbb{R}}^d$ according to the degree to which large-scale density fluctuations are suppressed, resulting in a demarcation between hyperuniform and nonhyperuniform phyla. To more completely characterize density fluctuations, we carry out an extensive study of higher-order moments or cumulants, including the skewness ${\gamma }_1(R)$, excess kurtosis ${\gamma }_2(R)$, and the corresponding probability distribution function $P[N(R)]$ of a large family of models across the first three space dimensions, including both hyperuniform and nonhyperuniform systems with varying degrees of short- and long-range order. To carry out this comprehensive program, we derive new theoretical results that apply to general point processes, and we conduct high-precision numerical studies. Specifically, we derive explicit closed-form integral expressions for ${\gamma }_1(R)$ and ${\gamma }_2(R)$ that encode structural information up to three-body and four-body correlation functions, respectively. We also derive rigorous bounds on ${\gamma }_1(R)$, ${\gamma }_2(R)$, and $P[N(R)]$ for general point processes and corresponding exact results for general packings of identical spheres. High-quality simulation data for ${\gamma }_1(R)$, ${\gamma }_2(R)$, and $P[N(R)]$ are generated for each model. We also ascertain the proximity of $P[N(R)]$ to the normal distribution via a novel Gaussian “distance” metric $l_2(R)$. Among all models, the convergence to a central limit theorem (CLT) is generally fastest for the disordered hyperuniform processes in two or higher dimensions such that ${\gamma }_1(R)\sim l_2(R)\sim R^{-(d+1)/2}$ and ${\gamma }_2(R)\sim R^{-(d+1)}$ for large $R$. The convergence to a CLT is slower for standard nonhyperuniform models and slowest for the “antihyperuniform” model studied here. We prove that one-dimensional hyperuniform systems of class I or any $d$-dimensional lattice cannot obey a CLT. Remarkably, we discover a type of universality in that, for all of our models that obey a CLT, the gamma distribution provides a good approximation to $P[N(R)]$ across all dimensions for intermediate to large values of $R$, enabling us to estimate the large-$R$ scalings of ${\gamma }_1(R)$, ${\gamma }_2(R)$, and $l_2(R)$. For any $d$-dimensional model that “decorrelates” or “correlates” with $d$, we elucidate why $P[N(R)]$ increasingly moves toward or away from Gaussian-like behavior, respectively. Our work sheds light on the fundamental importance of higher-order structural information to fully characterize density fluctuations in many-body systems across length scales and dimensions, and thus has broad implications for condensed matter physics, engineering, mathematics, and biology.

The elementary optical excitations in two-dimensional semiconductors hosting itinerant electrons are attractive and repulsive polarons—excitons that are dynamically screened by electrons. Exciton polarons have hitherto been studied in translationally invariant degenerate Fermi systems. Here, we show that periodic distribution of electrons breaks the excitonic translational invariance and leads to a direct optical signature in the exciton-polaron spectrum. Specifically, we demonstrate that new optical resonances appear due to spatially modulated interactions between excitons and electrons in an incompressible Mott-like correlated state. Our observations demonstrate that resonant optical spectroscopy provides an invaluable tool for studying strongly correlated states, such as Wigner crystals and density waves, where exciton-electron interactions are modified by the emergence of charge order.

Recently, moiré superlattices have been found on the surface of topological insulators due to the rotational misalignment of topmost layers. In this work, we study the effects of moiré superlattices on the topological surface states using a continuum model of Dirac electrons moving in a periodic potential. Unlike twisted bilayer graphene, moiré surface states cannot host isolated bands due to their topological nature. Instead, we find (high-order) van Hove singularities (VHS) in the moiré band structure that give rise to divergent density of states (DOS) and enhance interaction effects. Because of spin-momentum locking in moiré surface states, possible interaction channels are limited. In the presence of phonon mediated attraction, superconductivity is strongly enhanced by the power-law divergent DOS at high-order VHS. The transition temperature $T_c$ exhibits a power-law dependence on the retarded electron-phonon interaction strength ${\lambda }^{*}$. This enhancement is found to be robust under various perturbations from the high-order VHS.

Soft modes are intimately linked to structural instabilities and are key for the understanding of phase transitions. The soft modes in ferroelectrics, for example, map directly the polar order parameter of a crystal lattice. Driving these modes into the nonlinear, frequency-changing regime with intense terahertz (THz) light fields is an efficient way to alter the lattice and, with it, the physical properties. However, recent studies show that the THz electric-field amplitudes triggering a nonlinear soft-mode response are surprisingly low, which raises the question on the microscopic picture behind the origin of this nonlinear response. Here, we use linear and two-dimensional terahertz (2D THz) spectroscopy to unravel the origin of the soft-mode nonlinearities in a strain-engineered epitaxial ferroelectric ${\mathrm{SrTiO}}_3$ thin film. We find that the linear dielectric function of this mode is quantitatively incompatible with pure ionic or pure electronic motions. Instead, 2D THz spectroscopy reveals a pronounced coupling of electronic and ionic-displacement dipoles. Hence, the soft mode is a hybrid mode of lattice (ionic) motions and electronic interband transitions. We confirm this conclusion with model calculations based on a simplified pseudopotential concept of the electronic band structure. It reveals that the entire THz nonlinearity is caused by the off-resonant nonlinear response of the electronic interband transitions of the lattice-electronic hybrid mode. With this work, we provide fundamental insights into the microscopic processes that govern the softness that any material assumes near a ferroic phase transition. This knowledge will allow us to gain an efficient all-optical control over the associated large nonlinear effects.

The evolution between Fermi-liquid and non-Fermi-liquid states in correlated electron systems has been a central subject in condensed matter physics because of the coupled intriguing magnetic and electronic states. An effective pathway to explore the nature of non-Fermi-liquid behavior is to approach its phase boundary. Here we report a crossover from non-Fermi-liquid to Fermi-liquid state in metallic ${\mathrm{CaRuO}}_3$ through ionic liquid gating induced protonation with electric field. This electronic transition subsequently triggers a reversible magnetic transition with the emergence of an exotic ferromagnetic state from this paramagnetic compound. Our theoretical analysis reveals that hydrogen incorporation plays a critical role in both the electronic and magnetic phase transitions via structural distortion and electron doping. These observations not only help understand the correlated magnetic and electronic transitions in perovskite ruthenate systems, but also provide novel pathways to design electronic phases in correlated materials.

The interplay between time-reversal symmetry (TRS) and band topology plays a crucial role in topological states of quantum matter. In time-reversal-invariant (TRI) systems, the inversion of spin-degenerate bands with opposite parity leads to nontrivial topological states, such as topological insulators and Dirac semimetals. When the TRS is broken, the exchange field induces spin splitting of the bands. The inversion of a pair of spin-splitting subbands can generate more exotic topological states, such as quantum anomalous Hall insulators and magnetic Weyl semimetals. So far, such topological phase transitions driven by the TRS breaking have not been visualized. In this work, using angle-resolved photoemission spectroscopy, we have demonstrated that the TRS breaking induces a band inversion of a pair of spin-splitting subbands at the TRI points of Brillouin zone in ${\mathrm{EuB}}_6$, when a long-range ferromagnetic order is developed. The dramatic changes in the electronic structure result in a topological phase transition from a TRI ordinary insulator state to a TRS-broken topological semimetal (TSM) state. Remarkably, the magnetic TSM state has an ideal electronic structure, in which the band crossings are located at the Fermi level without any interference from other bands. Our findings not only reveal the topological phase transition driven by the TRS breaking, but also provide an excellent platform to explore novel physical behavior in the magnetic topological states of quantum matter.

The Dzyaloshinskii-Moriya interaction (DMI) has drawn much attention, as it stabilizes magnetic chirality, with important implications in fundamental and applied research. This antisymmetric exchange interaction is induced by the broken inversion symmetry at interfaces or in noncentrosymmetric lattices. Significant interfacial DMIs are often found at magnetic/heavy-metal interfaces with large spin-orbit coupling. Recent studies have shown promise for induced DMI at interfaces involving light elements such as carbon (graphene) or oxygen. Here, we report direct observation of induced DMI by chemisorption of the lightest element, hydrogen, on a ferromagnetic layer at room temperature, which is supported by density functional theory calculations. We further demonstrate a reversible chirality transition of the magnetic domain walls due to the induced DMI via hydrogen chemisorption and desorption. These results shed new light on the understanding of DMI in low atomic number materials and the design of novel chiral spintronics and magneto-ionic devices.

Periodically driven coherent conductors provide a universal platform for the development of quantum transport devices. Here, we lay down a comprehensive theory to describe the thermodynamics of these systems. We first focus on moderate thermoelectrical biases and low driving frequencies. For this linear response regime, we establish generalized Onsager-Casimir relations and an extended fluctuation-dissipation theorem. Furthermore, we derive a family of thermodynamic bounds proving that any local matter or heat current puts a nontrivial lower limit on the overall dissipation rate of a coherent transport process. These bounds do not depend on system-specific parameters, are robust against dephasing, and involve only experimentally accessible quantities. They thus provide powerful tools to optimize the performance of mesoscopic devices and for thermodynamic inference, as we demonstrate by working out three specific applications. We then show that physically transparent extensions of our bounds hold also for strong biases and high frequencies. These generalized bounds imply a thermodynamic uncertainty relation that fully accounts for quantum effects and periodic driving. Moreover, they lead to a universal and operationally accessible bound on entropy production that can be readily used for thermodynamic inference and device engineering far from equilibrium. Connecting a broad variety of topics that range from thermodynamic geometry over thermodynamic uncertainty relations to quantum engineering, our work provides a unifying thermodynamic theory of coherent transport that can be tested and utilized with current technologies.

In the Landau levels of a two-dimensional electron system or when flat bands are present, e.g., in twisted van der Waals bilayers, strong electron-electron interaction gives rise to quantum Hall ferromagnetism with spontaneously broken symmetries in the spin and isospin sectors. Quantum Hall ferromagnets support a rich variety of low-energy collective excitations that are instrumental to understand the nature of the magnetic ground states and are also potentially useful as carriers of quantum information. Probing such collective excitations, especially their dispersion $\omega (k)$, is experimentally challenging due to small sample size and measurement constraints. In this work, we demonstrate an all-electrical approach that integrates a Fabry-Pérot cavity with nonequilibrium transport to achieve the excitation, wave vector selection, and detection of spin waves in graphene heterostructures. Our experiments reveal gapless, linearly dispersed spin wave excitations in the $E=0$ Landau level of bilayer graphene, thus providing direct experimental evidence for a predicted canted antiferromagnetic order. We show that the gapless spin wave mode propagates with a high group velocity of several tens of kilometers per second and maintains phase coherence over a distance of many micrometers. Its dependence on the magnetic field and temperature agree well with the hydrodynamic theory of spin waves. These results lay the foundation for the quest of spin superfluidity in this high-quality material. The resonant cavity technique we develop offers a powerful and timely method to explore the collective excitation of many spin- and isospin-ordered many-body ground states in van der Waals heterostructures and opens the possibility of engineering magnonic devices.

We consider a clean quantum system subject to strong periodic driving. The existence of a dominant energy scale, $h_D^x$, can generate considerable structure in an effective description of a system that, in the absence of the drive, is nonintegrable and interacting, and does not host localization. In particular, we uncover points of freezing in the space of drive parameters (frequency and amplitude). At those points, the dynamics is severely constrained due to the emergence of an almost exact, local conserved quantity, which scars the entire Floquet spectrum by preventing the system from heating up ergodically, starting from any generic state, even though it delocalizes over an appropriate subspace. At large drive frequencies, where a naïve Magnus expansion would predict a vanishing effective (average) drive, we devise instead a strong-drive Magnus expansion in a moving frame. There, the emergent conservation law is reflected in the appearance of the “integrability” of an effective Hamiltonian. These results hold for a wide variety of Hamiltonians, including the Ising model in a transverse field in any dimension and for any form of Ising interaction. The phenomenon is also shown to be robust in the presence of two-body Heisenberg interactions with any arbitrary choice of couplings. Furthermore, we construct a real-time perturbation theory that captures resonance phenomena where the conservation breaks down, giving way to unbounded heating. This approach opens a window on the low-frequency regime where the Magnus expansion fails.

The quantitative prediction of electronic properties in correlated materials requires simulations without empirical truncations and parameters. We present a method to achieve this goal through a new ab initio formulation of dynamical mean-field theory (DMFT). Instead of using small impurities defined in a low-energy subspace, which require complicated downfolded interactions which are often approximated, we describe a full cell $GW+\mathrm{DMFT}$ approach, where the impurities comprise all atoms in a unit cell or supercell of the crystal. Our formulation results in large impurity problems, which we treat here with efficient quantum chemistry impurity solvers that work on the real-frequency axis, combined with a one-shot $G_0{W}_0$ treatment of long-range interactions. We apply our full cell approach to bulk Si, two antiferromagnetic correlated insulators NiO and $\alpha \text{−}{\mathrm{Fe}}_2{\mathrm{O}}_3$, and the paramagnetic correlated metal ${\mathrm{SrMoO}}_3$, with impurities containing up to ten atoms and 124 orbitals. We find that spectral properties, magnetic moments, and two-particle spin correlation functions are obtained in good agreement with experiment. In addition, in the metal oxide insulators, the balanced treatment of correlations involving all orbitals in the cell leads to new insights into the orbital character around the insulating gap.

A system with charge conservation and lattice translation symmetry has a well-defined filling $\nu$, which is a real number representing the average charge per unit cell. We show that if $\nu$ is fractional (i.e., not an integer), this imposes very strong constraints on the low-energy theory of the system and give a framework to understand such constraints in great generality, vastly generalizing the Luttinger and Lieb-Schultz-Mattis theorems. The most powerful constraint comes about if $\nu$ is continuously tunable (i.e., the system is charge compressible), in which case, we show that the low-energy theory must have a very large emergent symmetry group—larger than any compact Lie group. An example is the Fermi surface of a Fermi liquid, where the charge at every point on the Fermi surface is conserved. We expect that in many, if not all, cases, even exotic non-Fermi liquids will have the same emergent symmetry group as a Fermi liquid, even though they could have very different dynamics. We call a system with this property an ersatz Fermi liquid. We show that ersatz Fermi liquids share a number of properties in common with Fermi liquids, including Luttinger’s theorem (which is thus extended to a large class of non-Fermi liquids) and periodic “quantum oscillations” in the response to an applied magnetic field. We also establish versions of Luttinger’s theorem for the composite Fermi liquid in quantum Hall systems and for spinon Fermi surfaces in Mott insulators. Our work makes a connection between filling constraints and the theory of symmetry-protected topological phases, in particular through the concept of “’t Hooft anomalies.”

Polarized neutron diffraction (PND) is a powerful technique to distinguish a weak magnetic contribution from the total scattering intensity. It can provide a detailed insight into the microscopic spin ordering at the unit cell level, but also into the mesoscopic magnetic ordering, like different types of domain populations. Here we report on the application of this technique to the long-standing problem of determining the absolute direction of the Dzyaloshinskii-Moriya vector in relation to the crystal structure. The proposed PND method, based on the measurement of one representative reflection, is easy to perform and straightforward to interpret. The absolute sign of the Dzyaloshinskii-Moriya interaction (DMI) in ${\mathrm{MnCO}}_3$ has been independently determined by PND and found to be in agreement with recent results obtained by resonant magnetic synchrotron scattering. This validates the method. In addition, the absolute DMI vector direction in the prototypical room-temperature weak ferromagnet $\alpha \text{−}{\mathrm{Fe}}_2{\mathrm{O}}_3$ (hematite) has been determined for the first time. To demonstrate the generality of our method, further examples with different symmetries are also presented. Ab initio calculations of the resulting weak noncollinear magnetization using the quantum espresso package, considering DMI in addition to the symmetric magnetic exchange interaction, were also conducted and found to be in agreement with the experimental results from PND.

Electron-phonon-driven charge-density waves can in some circumstances allow electronic correlations to become predominant, driving a system into a Mott insulating state. New insight into both the Mott state and preceding charge-density wave may result from observations of the coupled dynamics of their underlying degrees of freedom. Here, tunneling injection of single electrons into the upper Hubbard band of the Mott charge-density-wave material $1T\text{−}{\mathrm{TaS}}_2$ reveals extraordinarily narrow electronic excitations which couple to amplitude mode phonons associated with the charge-density wave’s periodic lattice distortion. This gives a vivid microscopic view of the interplay between excitations of the Mott state and the lattice dynamics of its charge-density wave precursor.

The Hubbard model represents the fundamental model for interacting quantum systems and electronic correlations. Using the two-dimensional half-filled Hubbard model at weak coupling as a testing ground, we perform a comparative study of a comprehensive set of state-of-the-art quantum many-body methods. Upon cooling into its insulating antiferromagnetic ground state, the model hosts a rich sequence of distinct physical regimes with crossovers between a high-temperature incoherent regime, an intermediate-temperature metallic regime, and a low-temperature insulating regime with a pseudogap created by antiferromagnetic fluctuations. We assess the ability of each method to properly address these physical regimes and crossovers through the computation of several observables probing both quasiparticle properties and magnetic correlations, with two numerically exact methods (diagrammatic and determinantal quantum Monte Carlo methods) serving as a benchmark. By combining computational results and analytical insights, we elucidate the nature and role of spin fluctuations in each of these regimes. Based on this analysis, we explain how quasiparticles can coexist with increasingly long-range antiferromagnetic correlations and why dynamical mean-field theory is found to provide a remarkably accurate approximation of local quantities in the metallic regime. We also critically discuss whether imaginary-time methods are able to capture the non-Fermi-liquid singularities of this fully nested system.

The concept of “Floquet engineering” relies on an external periodic drive to realize novel, effectively static Hamiltonians. This technique is being explored in experimental platforms across physics, including ultracold atoms, laser-driven electron systems, nuclear magnetic resonance, and trapped ions. The key challenge in Floquet engineering is to avoid the uncontrolled absorption of photons from the drive, especially in interacting systems in which the excitation spectrum becomes effectively dense. The resulting dissipative coupling to higher-lying modes, such as the excited bands of an optical lattice, has been explored in recent experimental and theoretical works, but the demonstration of a broadly applicable method to mitigate this effect is lacking. Here, we show how two-path quantum interference applied to strongly correlated fermions in a driven optical lattice suppresses dissipative coupling to higher bands and increases the lifetime of double occupancies and spin correlations by 2 to 3 orders of magnitude. Interference is achieved by introducing a weak second modulation at twice the fundamental driving frequency with a definite relative phase. This technique is shown to suppress dissipation in both weakly and strongly interacting regimes of an off-resonantly driven Hubbard system, opening an avenue to realizing low-temperature phases of matter in interacting Floquet systems.

We propose a novel nonequilibrium phenomenon, through which a prompt quench from a metal to a transient superconducting state can induce large oscillations of the order parameter amplitude. We argue that this oscillating mode acts as a source of parametric amplification of the incident radiation. We report experimental results on optically driven ${\mathrm{K}}_3{\mathrm{C}}_{60}$ that are consistent with these predictions. The effect is found to disappear when the onset of the excitation becomes slower than the Higgs-mode period, consistent with the theory proposed here. These results open new possibilities for the use of collective modes in many-body systems to induce nonlinear optical effects.

The recent discovery of superconductivity in oxygen-reduced monovalent nickelates has raised a new platform for the study of unconventional superconductivity, with similarities to and differences from the cuprate high-temperature superconductors. In this paper, we investigate the family of infinite-layer nickelates $R{\mathrm{NiO}}_2$ with rare-earth $R$ spanning across the lanthanide series, introducing a new and nontrivial “knob” with which to tune nickelate superconductivity. When traversing from La to Lu, the out-of-plane lattice constant decreases dramatically with an accompanying increase of Ni $d_{x^2-y^2}$ bandwidth; however, surprisingly, the role of oxygen charge transfer diminishes. In contrast, the magnetic exchange grows across the lanthanides, which may be favorable to superconductivity. Moreover, compensation effects from the itinerant $5d$ electrons present a closer analogy to Kondo lattices, indicating a stronger interplay between charge transfer, bandwidth renormalization, compensation, and magnetic exchange. We also obtain the microscopic Hamiltonian using the Wannier downfolding technique, which will provide the starting point for further many-body theoretical studies.

An accurate description of the optical response of subwavelength metallic particles and nanogap structures is a key problem of plasmonics. Quantum hydrodynamic theory (QHT) has emerged as a powerful method to calculate the optical response of metallic nanoparticles (NPs) since it takes into account nonlocality and spill-out effects. Nevertheless, the absorption spectra of metallic NPs obtained with conventional QHT, i.e., incorporating Thomas-Fermi (TF) and von Weizsäcker (vW) kinetic energy (KE) contributions, can be affected by several spurious resonances at energies higher than the main localized surface plasmon (LSP). These peaks are not present in reference time-dependent density-functional-theory spectra, where, instead, only a broad shoulder exists. Moreover, we show here that these peaks incorrectly reduce the LSP peak intensity and have a strong dependence on the simulation domain size so that a proper calculation of QHT absorption spectra can be problematic. In this article, we introduce a more general QHT method accounting for KE contributions depending on the Laplacian of the electronic density ($q$), thus, beyond the gradient-only dependence of the TFvW functional. We show that employing a KE functional with a term proportional to $q^2$ results in an absorption spectrum free of spurious peaks, with LSP resonance of correct intensity and numerically stable Bennett state. Finally, we present a novel Laplacian-level KE functional that is very accurate for the description of the optical properties of NPs of different sizes as well as for dimers. Thus, the Laplacian-level QHT represents a novel, efficient, and accurate platform to study plasmonic systems.