Light-matter interaction based on strong laser fields enables probing the structure and dynamics of atomic and molecular systems with unprecedented resolutions, through high-order harmonic spectroscopy, laser-induced electron diffraction, and holography. All strong-field processes rely on a primary ionization mechanism where electrons tunnel through the target potential barrier lowered by the laser field. Tunnel ionization is, thus, of paramount importance in strong-field physics and attoscience. However, the tunneling dynamics and properties of the outgoing electronic wave packets often remain hidden beneath the influence of the subsequent scattering of the released electron onto the ionic potential. Here, we present a joint experimental-theoretical endeavor to characterize the influence of sub-barrier dynamics on the amplitude and phase of the wave packets emerging from the tunnel. We use chiral molecules, whose photoionization by circularly polarized light produces forward-backward asymmetric electron distributions with respect to the light propagation direction. These asymmetric patterns provide a background-free signature of the chiral potential in the ionization process. We first implement the attoclock technique, using bicircular two-color fields. We find that, in the tunnel-ionization process, molecular chirality induces a strong forward-backward asymmetry in the electron yield, while the subsequent scattering of the freed electron onto the chiral potential leads to an asymmetric angular streaking of the electron momentum distribution. In order to access the phase of the tunneling wave packets, we introduce subcycle gated chiral interferometry. We employ an orthogonally polarized two-color laser field whose optical chirality is manipulated on a sub-laser-cycle timescale. Numerical simulations are used to interpret the electron interference patterns inherent to this interaction scheme. They show that the combined action of the chiral potential and rotating laser field not only imprints asymmetric ionization amplitudes during the tunneling process, but also induces a forward-backward asymmetric phase profile onto the outgoing electron wave packets. Chiral light-matter interaction thus induces subtle angular-dependent shaping of both the amplitude and the phase of tunneling wave packets.

We study ultrafast magnetization quenching of ferromagnetic iron following excitation by an optical versus a terahertz pump pulse. While the optical pump (photon energy of 3.1 eV) induces a strongly nonthermal electron distribution, terahertz excitation (4.1 meV) results in a quasithermal perturbation of the electron population. The pump-induced spin and electron dynamics are interrogated by the magneto-optic Kerr effect (MOKE). A deconvolution procedure allows us to push the time resolution down to 130 fs, even though the driving terahertz pulse is about 500 fs long. Remarkably, the MOKE signals exhibit an almost identical time evolution for both optical and terahertz pump pulses, despite the 3 orders of magnitude different number of excited electrons. We are able to quantitatively explain our results using a nonthermal model based on quasielastic spin-flip scattering. It shows that, in the small-perturbation limit, the rate of demagnetization of a metallic ferromagnet is proportional to the excess energy of the electrons, independent of the precise shape of their distribution. Our results reveal that, for simple metallic ferromagnets, the dynamics of ultrafast demagnetization and of the closely related terahertz spin transport do not depend on the pump photon energy.

In Heisenberg models with exchange anisotropy, transverse spin components are not conserved and can decay not only by transport, but also by dephasing. Here, we utilize ultracold atoms to simulate the dynamics of 1D Heisenberg spin chains and observe fast, local spin decay controlled by the anisotropy. However, even for isotropic interactions, we observe dephasing due to a new effect: an effective magnetic field created by superexchange. If spatially uniform, it leads only to uniform spin precession and is, therefore, typically ignored. However, we show through experimental studies and extensive numerical simulations how this superexchange-generated field is relevant and leads to additional dephasing mechanisms over the exchange anisotropy: There is dephasing due to (i) inhomogeneity of the effective field from variations of lattice depth between chains; (ii) a twofold reduction of the field at the edges of finite chains; and (iii) fluctuations of the effective field due to the presence of mobile holes in the system. The latter is a new coupling mechanism between holes and magnons. All these dephasing mechanisms have not been observed before with ultracold atoms and illustrate basic properties of the underlying Hubbard model.

Thanks to the nearsightedness principle, the low-energy electronic structure of solids can be represented by localized states such as the Wannier functions. Wannier functions are actively being applied to a wide range of phenomena in condensed matter systems. However, the Wannier-function-based representation is limited to a small number of bands and thus cannot describe the change of wave functions due to various kinds of perturbations, which require sums over an infinite number of bands. Here, we introduce the concept of the Wannier function perturbation, which provides a localized representation of wave function perturbations. Wannier function perturbation theory allows efficient calculation of numerous quantities involving wave function perturbation, among which we provide three applications. First, we calculate the temperature-dependent indirect optical absorption spectra of silicon near the absorption edge nonadiabatically, i.e., differentiating phonon-absorption and phonon-emission processes, and without arbitrary temperature-dependent shifts in energy. Second, we establish a theory to calculate the shift spin conductivity without any band-truncation error. Unlike the shift charge conductivity, an exact calculation of the shift spin conductivity is not possible within the conventional Wannier function methods because it cannot be obtained from geometric quantities for low-energy bands. We apply the theory to monolayer ${\mathrm{WTe}}_2$. Third, we calculate the spin Hall conductivity of the same material again without any band-truncation error. Wannier function perturbation theory is a versatile method that can be readily applied to calculate a wide range of quantities related to various kinds of perturbations.

Interactions between electrons and lattice vibrations are responsible for a wide range of material properties and applications. Recently, there has been considerable interest in the development of resonant inelastic x-ray scattering (RIXS) as a tool for measuring electron-phonon ($e$-ph) interactions. Here, we demonstrate the ability of RIXS to probe the interaction between phonons and specific electronic states both near to, and away from, the Fermi level. We perform carbon $K$-edge RIXS measurements on graphite, tuning the incident x-ray energy to separately probe the interactions of the ${\pi }^{*}$ and ${\sigma }^{*}$ electronic states. Our high-resolution data reveal detailed structure in the multiphonon RIXS features that directly encodes the momentum dependence of the $e$-ph interaction strength. We develop a Green’s-function method to model this structure, which naturally accounts for the phonon and interaction-strength dispersions, as well as the mixing of phonon momenta in the intermediate state. This model shows that the differences between the spectra can be fully explained by contrasting trends of the $e$-ph interaction through the Brillouin zone, being concentrated at the $\mathrm{\Gamma }$ and $K$ points for the ${\pi }^{*}$ states while being significant at all momenta for the ${\sigma }^{*}$ states. Our results advance the interpretation of phonon excitations in RIXS and extend its applicability as a probe of $e$-ph interactions to a new range of out-of-equilibrium situations.

In this paper, we characterize quasicrystalline interacting topological phases of matter, i.e., phases protected by some quasicrystalline structure. We show that the elasticity theory of quasicrystals, which accounts for both “phonon” and “phason” modes, admits nontrivial quantized topological terms with far richer structure than their crystalline counterparts. We show that these terms correspond to distinct phases of matter and also uncover intrinsically quasicrystalline phases, which have no crystalline analogs. For quasicrystals with internal U(1) symmetry, we discuss a number of interpretations and physical implications of the topological terms, including constraints on the mobility of dislocations in $d=2$ quasicrystals and a quasicrystalline generalization of the Lieb-Schultz-Mattis-Oshikawa-Hastings theorem. We then extend these ideas much further and address the complete classification of quasicrystalline topological phases, including systems with point-group symmetry as well as noninvertible phases. We hence obtain the “quasicrystalline equivalence principle,” which generalizes the classification of crystalline topological phases to the quasicrystalline setting.

Continued timing observations of the double pulsar PSR J0737–3039A/B, which consists of two active radio pulsars (A and B) that orbit each other with a period of 2.45 h in a mildly eccentric ($e=0.088$) binary system, have led to large improvements in the measurement of relativistic effects in this system. With a 16-yr data span, the results enable precision tests of theories of gravity for strongly self-gravitating bodies and also reveal new relativistic effects that have been expected but are now observed for the first time. These include effects of light propagation in strong gravitational fields which are currently not testable by any other method. In particular, we observe the effects of retardation and aberrational light bending that allow determination of the spin direction of the pulsar. In total, we detect seven post-Keplerian parameters in this system, more than for any other known binary pulsar. For some of these effects, the measurement precision is now so high that for the first time we have to take higher-order contributions into account. These include the contribution of the A pulsar’s effective mass loss (due to spin-down) to the observed orbital period decay, a relativistic deformation of the orbit, and the effects of the equation of state of superdense matter on the observed post-Keplerian parameters via relativistic spin-orbit coupling. We discuss the implications of our findings, including those for the moment of inertia of neutron stars, and present the currently most precise test of general relativity’s quadrupolar description of gravitational waves, validating the prediction of general relativity at a level of $1.3\times {10}^{-4}$ with 95% confidence. We demonstrate the utility of the double pulsar for tests of alternative theories of gravity by focusing on two specific examples and also discuss some implications of the observations for studies of the interstellar medium and models for the formation of the double pulsar system. Finally, we provide context to other types of related experiments and prospects for the future.

The majority of ions and other charged particles of spectroscopic interest lack the fast, cycling transitions that are necessary for direct laser cooling. In most cases, they can still be cooled sympathetically through their Coulomb interaction with a second, coolable ion species confined in the same potential. If the charge-to-mass ratios of the two ion types are too mismatched, the cooling of certain motional degrees of freedom becomes difficult. This limits both the achievable fidelity of quantum gates and the spectroscopic accuracy. Here, we introduce a novel algorithmic cooling protocol for transferring phonons from poorly to efficiently cooled modes. We demonstrate it experimentally by simultaneously bringing two motional modes of a ${\mathrm{Be}}^{+}\text{−}{\mathrm{Ar}}^{13+}$ mixed Coulomb crystal close to their zero-point energies, despite the weak coupling between the ions. We reach the lowest temperature reported for a highly charged ion, with a residual temperature of only $T\lesssim 200\mu \mathrm{K}$ in each of the two modes, corresponding to a residual mean motional phonon number of $⟨n⟩\lesssim 0.4$. Combined with the lowest observed electric-field noise in a radio-frequency ion trap, these values enable an optical clock based on a highly charged ion with fractional systematic uncertainty below the ${10}^{-18}$ level. Our scheme is also applicable to (anti)protons, molecular ions, macroscopic charged particles, and other highly charged ion species, enabling reliable preparation of their motional quantum ground states in traps.

In superconductors, electrons with spin $s=1/2$ form Cooper pairs whose spin structure is usually singlet ($S=0$) or triplet ($S=1$). When the electronic structure near the Fermi level is characterized by fermions with angular momentum $j=3/2$ due to strong spin-orbit interactions, novel pairing states such as even-parity quintet ($J=2$) and odd-parity septet ($J=3$) states are allowed. Prime candidates for such exotic states are half-Heusler superconductors, which exhibit unconventional superconducting properties, but their pairing nature remains unsettled. Here, we show that the superconductivity in the noncentrosymmetric half-Heusler LuPdBi can be consistently described by the admixture of isotropic even-parity singlet and anisotropic odd-parity septet pairing, whose ratio can be tuned by electron irradiation. From magnetotransport and penetration depth measurements, we find that carrier concentrations and impurity scattering both increase with irradiation, resulting in a nonmonotonic change of the superconducting gap structure. Our findings shed new light on our fundamental understanding of unconventional superconducting states in topological materials.

Stochastic network dynamics are typically assumed to be memoryless. Involving prolonged dwells interrupted by instantaneous transitions between nodes, such Markov networks stand as a coarse-graining paradigm for chemical reactions, gene expression, molecular machines, spreading of diseases, protein dynamics, diffusion in energy landscapes, epigenetics, and many others. However, as soon as transitions cease to be negligibly short, as often observed in experiments, the dynamics develops a memory. That is, state changes depend not only on the present state but also on the past. Here, we establish the first thermodynamically consistent—dissipation-preserving—mapping of continuous dynamics onto a network, which reveals ingrained dynamical symmetries and an unforeseen kinetic hysteresis. These symmetries impose three independent sources of fluctuations in state-to-state kinetics that determine the “flavor of memory.” The hysteresis between the forward- or backward-in-time coarse graining of continuous trajectories implies a new paradigm for the thermodynamics of active molecular processes in the presence of memory, that is, beyond the assumption of local detailed balance. Our results provide a new understanding of fluctuations in the operation of molecular machines as well as catch bonds involved in cellular adhesion.

Exposing a many-body system to external drives and losses can transform the nature of its phases and opens perspectives for engineering new properties of matter. How such characteristics are related to the underlying microscopic processes of the driven and dissipative system is a fundamental question. Here, we address this point in a quantum gas that is strongly coupled to a lossy optical cavity mode using two independent Raman drives, which act on the spin and motional degrees of freedom of the atoms. This setting allows us to control the competition between coherent dynamics and dissipation by adjusting the imbalance between the drives. For strong enough coupling, the transition to a superradiant phase occurs, as is the case for a closed system. Yet, by imbalancing the drives, we can enter a dissipation-stabilized normal phase and a region of multistability. Measuring the properties of excitations on top of the out-of-equilibrium phases reveals the microscopic elementary processes in the open system. Our findings provide prospects for studying squeezing in non-Hermitian systems, quantum jumps in superradiance, and dynamical spin-orbit coupling in a dissipative setting.

We discuss quantum variational optimization of Ramsey interferometry with ensembles of $N$ entangled atoms, and its application to atomic clocks based on a Bayesian approach to phase estimation. We identify best input states and generalized measurements within a variational approximation for the corresponding entangling and decoding quantum circuits. These circuits are built from basic quantum operations available for the particular sensor platform, such as one-axis twisting, or finite range interactions. Optimization is defined relative to a cost function, which in the present study is the Bayesian mean squared error of the estimated phase for a given prior distribution; i.e., we optimize for a finite dynamic range of the interferometer. In analogous variational optimizations of optical atomic clocks, we use the Allan deviation for a given Ramsey interrogation time as the relevant cost function for the long-term instability. Remarkably, even low-depth quantum circuits yield excellent results that closely approach the fundamental quantum limits for optimal Ramsey interferometry and atomic clocks. The quantum metrological schemes identified here are readily applicable to atomic clocks based on optical lattices, tweezer arrays, or trapped ions. While in the present work variationally optimized circuits are found with classical simulations, optimization can also be performed “on” the (physical) quantum sensor, also in regimes not accessible to classical computations and in the presence of imperfections.

The ultrafast structural dynamics of water following inner-shell ionization is a crucial issue in high-energy radiation chemistry. We have exposed isolated water molecules to a short x-ray pulse from a free-electron laser and detected momenta of all produced ions in coincidence. By combining experimental results and theoretical modeling, we can image dissociation dynamics of individual molecules in unprecedented detail. We reveal significant molecular structural dynamics in ${\mathrm{H}}_2{\mathrm{O}}^{2+}$, such as asymmetric deformation and bond-angle opening, leading to two-body or three-body fragmentation on a timescale of a few femtoseconds. We thus reconstruct several snapshots of structural dynamics at different time intervals, which highlight dynamical patterns that are relevant as initiating steps of subsequent radiation-damage processes.

Quantum emitters in the presence of an electromagnetic reservoir with varying density of states, or structure, can undergo a rich set of dynamical behavior. In particular, the reservoir can be tailored to have a memory of past interactions with emitters, in contrast to memoryless Markovian dynamics of typical open systems. In this article, we investigate the non-Markovian dynamics of a superconducting qubit strongly coupled to a superconducting waveguide engineered to have both a sharp spectral variation in its transmission properties and a slowing of light by a factor of 650. Tuning the qubit into the spectral vicinity of the passband of this slow-light waveguide reservoir, we observe a 400-fold change in the emission rate of the qubit, along with oscillatory energy relaxation of the qubit resulting from the beating of bound and radiative dressed qubit-photon states. Furthermore, upon addition of a reflective boundary to one end of the waveguide, we observe revivals in the qubit population on a timescale 30 times longer than the inverse of the qubit’s emission rate, corresponding to the round-trip travel time of an emitted photon. By in situ tuning of the qubit-waveguide interaction strength, we also probe a crossover between Markovian and non-Markovian qubit emission dynamics in the presence of feedback from waveguide reflections. With this superconducting circuit platform, future studies of multiqubit interactions via highly structured reservoirs and the generation of multiphoton highly entangled states are possible.

Dielectric laser accelerators (DLAs) hold great promise for producing economic and compact on-chip radiation sources. On-chip DLAs benefit from fabrication capabilities of the silicon industry and from breakthroughs in silicon-photonic nanostructures to enhance the interaction between particles and laser fields. Seemingly unrelated recent advances in the quantum interactions of electrons and light have raised interest in the underlying classical-quantum correspondence principle at the foundations of electron acceleration. Here, we present the observation of the underlying quantum nature of DLAs: observing quantized peaks in the electron-energy spectra. Our findings demonstrate quasi-phase-matching between an electron wave function and a light wave, which also demonstrates the role of the quantum wave function in the inverse Smith-Purcell effect. We harness the capabilities of an ultrafast transmission electron microscope (UTEM) to maintain a long electron-light interaction length extending over hundreds of periods of the laser pulse, mediated by a silicon-photonic nanograting DLA. The UTEM is shown as a new platform for characterization of future DLA concepts. The results raise fundamental questions regarding the role of quantum mechanics in DLA design, and more generally about the prospects of manipulating particles’ quantum wave functions in accelerator physics.

Group-IV color centers in diamond are a promising light-matter interface for quantum networking devices. The negatively charged tin-vacancy center ($\mathrm{Sn}\mathrm{V}$) is particularly interesting, as its large spin-orbit coupling offers strong protection against phonon dephasing and robust cyclicity of its optical transitions toward spin-photon-entanglement schemes. Here, we demonstrate multiaxis coherent control of the $\mathrm{Sn}\mathrm{V}$ spin qubit via an all-optical stimulated Raman drive between the ground and excited states. We use coherent population trapping and optically driven electronic spin resonance to confirm coherent access to the qubit at 1.7 K and obtain spin Rabi oscillations at a rate of $\mathrm{\Omega }/2\pi =19.0(1)\mathrm{MHz}$. All-optical Ramsey interferometry reveals a spin dephasing time of $T_2^{*}=1.3(3)\mu \mathrm{s}$, and four-pulse dynamical decoupling already extends the spin-coherence time to $T_2=0.30(8)\mathrm{ms}$. Combined with transform-limited photons and integration into photonic nanostructures, our results make the $\mathrm{Sn}\mathrm{V}$ a competitive spin-photon building block for quantum networks.

We develop an efficient approach for computing two-particle response functions and interaction vertices for multiorbital strongly correlated systems based on the rotationally invariant slave-boson framework. The method is applied to the degenerate three-orbital Hubbard-Kanamori model for investigating the origin of the $s$-wave orbital antisymmetric spin-triplet superconductivity in Hund’s metal regime, previously found in the dynamical mean-field theory studies. By computing the pairing interaction considering the particle-particle and the particle-hole scattering channels, we identify the mechanism leading to the pairing instability around Hund’s metal crossover arises from the particle-particle channel, which contains the local electron pair fluctuation between different particle-number sectors of the atomic Hilbert space. On the other hand, the particle-hole spin fluctuations induce the $s$-wave pairing instability before entering Hund’s regime. Our approach paves the way for investigating the pairing mechanism in realistic correlated materials.

The successful implementation of algorithms on quantum processors relies on the accurate control of quantum bits (qubits) to perform logic gate operations. In this era of noisy intermediate-scale quantum (NISQ) computing, systematic miscalibrations, drift, and crosstalk in the control of qubits can lead to a coherent form of error that has no classical analog. Coherent errors severely limit the performance of quantum algorithms in an unpredictable manner, and mitigating their impact is necessary for realizing reliable quantum computations. Moreover, the average error rates measured by randomized benchmarking and related protocols are not sensitive to the full impact of coherent errors and therefore do not reliably predict the global performance of quantum algorithms, leaving us unprepared to validate the accuracy of future large-scale quantum computations. Randomized compiling is a protocol designed to overcome these performance limitations by converting coherent errors into stochastic noise, dramatically reducing unpredictable errors in quantum algorithms and enabling accurate predictions of algorithmic performance from error rates measured via cycle benchmarking. In this work, we demonstrate significant performance gains under randomized compiling for the four-qubit quantum Fourier transform algorithm and for random circuits of variable depth on a superconducting quantum processor. Additionally, we accurately predict algorithm performance using experimentally measured error rates. Our results demonstrate that randomized compiling can be utilized to leverage and predict the capabilities of modern-day noisy quantum processors, paving the way forward for scalable quantum computing.

Quantum phase transitions play an important role in shaping the phase diagram of high-temperature cuprate superconductors. These cuprates possess intertwined orders which interact strongly with superconductivity. However, the evidence for the quantum critical point associated with the charge order in the superconducting phase remains elusive. Here, we reveal the short-range charge orders and the spectral signature of the quantum fluctuations in ${\mathrm{La}}_{2-x}{\mathrm{Sr}}_x{\mathrm{CuO}}_4$ (LSCO) near the optimal doping using high-resolution resonant inelastic x-ray scattering. On performing calculations through a diagrammatic framework, we discover that the charge correlations significantly soften several branches of phonons. These results elucidate the role of charge order in the LSCO compound, providing evidence for quantum critical scaling and discommensurations associated with charge order.

Cell neighbor exchanges are integral to tissue rearrangements in biology, including development and repair. Often, these processes occur via topological T1 transitions analogous to those observed in foams, grains, and colloids. However, in contrast to those in nonliving materials, the T1 transitions in biological tissues are rate limited and cannot occur instantaneously due to the finite time required to remodel complex structures at cell-cell junctions. Here, we study how this rate-limiting process affects the mechanics and collective behavior of cells in a tissue by introducing this important biological constraint in a theoretical vertex-based model as an intrinsic single-cell property. We report that, in the absence of this time constraint, the tissue undergoes a glass transition with lowering of cell motility characterized by a sharp increase in the intermittency of cell-cell rearrangements. Remarkably, this glass transition disappears, as T1 transitions are temporally limited. As a unique consequence of limited rearrangements, we also find that the tissue develops spatially correlated populations of fast and slow cells, in which the fast cells organize into streamlike patterns and maintain optimally stable cell-cell contacts. The predictions of this work are compared with existing in vivo experiments in Drosophila pupal development.