We present a practical roadmap to achieve optical cycling and laser cooling of asymmetric top molecules (ATMs). Our theoretical analysis describes how reduced molecular symmetry, as compared to diatomic and symmetric nonlinear molecules, plays a role in photon scattering. We present methods to circumvent limitations on rapid photon cycling in these systems. We calculate vibrational branching ratios for a diverse set of asymmetric top molecules and find that many species within a broad class of molecules can be effectively cooled with a manageable number of lasers. We also describe methods to achieve rotationally closed optical cycles in ATMs. Despite significant structural complexity, laser cooling can be made effective by using extensions of the current techniques for linear molecules. Potential scientific impacts of laser-cooled ATMs span frontiers in controlled chemistry, quantum simulation, and searches for physics beyond the Standard Model.

We introduce a new approach for the robust control of quantum dynamics of strongly interacting many-body systems. Our approach involves the design of periodic global control pulse sequences to engineer desired target Hamiltonians that are robust against disorder, unwanted interactions, and pulse imperfections. It utilizes a matrix representation of the Hamiltonian engineering protocol based on time-domain transformations of the Pauli spin operator along the quantization axis. This representation allows us to derive a concise set of algebraic conditions on the sequence matrix to engineer robust target Hamiltonians, enabling the simple yet systematic design of pulse sequences. We show that this approach provides an efficient framework to (i) treat any secular many-body Hamiltonian and engineer it into a desired form, (ii) target dominant disorder and interaction characteristics of a given system, (iii) achieve robustness against imperfections, (iv) provide optimal sequence length within given constraints, and (v) substantially accelerate numerical searches of pulse sequences. Using this systematic approach, we develop novel sets of pulse sequences for the protection of quantum coherence, optimal quantum sensing, and quantum simulation. Finally, we experimentally demonstrate the robust operation of these sequences in a system with the most general interaction form.

The quantum approximate optimization algorithm (QAOA) is a hybrid quantum-classical variational algorithm designed to tackle combinatorial optimization problems. Despite its promise for near-term quantum applications, not much is currently understood about the QAOA’s performance beyond its lowest-depth variant. An essential but missing ingredient for understanding and deploying the QAOA is a constructive approach to carry out the outer-loop classical optimization. We provide an in-depth study of the performance of the QAOA on MaxCut problems by developing an efficient parameter-optimization procedure and revealing its ability to exploit nonadiabatic operations. Building on observed patterns in optimal parameters, we propose heuristic strategies for initializing optimizations to find quasioptimal $p$-level QAOA parameters in $O[\mathrm{poly}(p)]$ time, whereas the standard strategy of random initialization requires $2^{O(p)}$ optimization runs to achieve similar performance. We then benchmark the QAOA and compare it with quantum annealing, especially on difficult instances where adiabatic quantum annealing fails due to small spectral gaps. The comparison reveals that the QAOA can learn via optimization to utilize nonadiabatic mechanisms to circumvent the challenges associated with vanishing spectral gaps. Finally, we provide a realistic resource analysis on the experimental implementation of the QAOA. When quantum fluctuations in measurements are accounted for, we illustrate that optimization is important only for problem sizes beyond numerical simulations but accessible on near-term devices. We propose a feasible implementation of large MaxCut problems with a few hundred vertices in a system of 2D neutral atoms, reaching the regime to challenge the best classical algorithms.

The precise engineering of quantum states, a basic prerequisite for technologies such as quantum-enhanced sensing or quantum computing, becomes more challenging with increasing dimension of the system Hilbert space. Standard preparation techniques then require a large number of operations or slow adiabatic evolution and give access to only a limited set of states. Here, we use quantum optimal control theory to overcome this problem and derive shaped radio-frequency pulses to experimentally navigate the Stark manifold of a Rydberg atom. We demonstrate that optimal control, beyond improving the fidelity of an existing protocol, also enables us to accurately generate a nonclassical superposition state that cannot be prepared with reasonable fidelity using standard techniques. Optimal control thus substantially enlarges the range of accessible states. Our joint experimental and theoretical work establishes quantum optimal control as a key tool for quantum engineering in complex Hilbert spaces.

Solving strongly coupled gauge theories in two or three spatial dimensions is of fundamental importance in several areas of physics ranging from high-energy physics to condensed matter. On a lattice, gauge invariance and gauge-invariant (plaquette) interactions involve (at least) four-body interactions that are challenging to realize. Here, we show that Rydberg atoms in configurable arrays realized in current tweezer experiments are the natural platform to realize scalable simulators of the Rokhsar-Kivelson Hamiltonian—a 2D U(1) lattice gauge theory that describes quantum dimer and spin-ice dynamics. Using an electromagnetic duality, we implement the plaquette interactions as Rabi oscillations subject to Rydberg blockade. Remarkably, we show that by controlling the atom arrangement in the array we can engineer anisotropic interactions and generalized blockade conditions for spins built of atom pairs. We describe how to prepare the resonating valence bond and the crystal phases of the Rokhsar-Kivelson Hamiltonian adiabatically and probe them and their quench dynamics by on-site measurements of their quantum correlations. We discuss the potential applications of our Rydberg simulator to lattice gauge theory and exotic spin models.

Quantum computing and quantum simulation can be implemented by concatenation of one- and two-qubit gates and interactions. For most physical implementations, however, it may be advantageous to explore state components and interactions that depart from this universal paradigm and offer faster or more robust access to more advanced operations on the system. In this article, we show that adiabatic passage along the dark eigenstate of excitation exchange interactions can be used to implement fast multiqubit Toffoli (${\mathrm{C}}_k$-NOT) and fan-out (C-${\text{NOT}}^k$) gates. This mechanism can be realized by simultaneous excitation of atoms to Rydberg levels, featuring resonant exchange interaction. Our theoretical estimates and numerical simulations show that these multiqubit Rydberg gates are possible with errors below 1% for up to 20 qubits. The excitation exchange mechanism is ubiquitous across experimental platforms, and we show that similar multiqubit gates can be implemented in superconducting circuits.

A central motivation for the development of x-ray free-electron lasers has been the prospect of time-resolved single-molecule imaging with atomic resolution. Here, we show that x-ray photoelectron diffraction—where a photoelectron emitted after x-ray absorption illuminates the molecular structure from within—can be used to image the increase of the internuclear distance during the x-ray-induced fragmentation of an ${\mathrm{O}}_2$ molecule. By measuring the molecular-frame photoelectron emission patterns for a two-photon sequential $K$-shell ionization in coincidence with the fragment ions, and by sorting the data as a function of the measured kinetic energy release, we can resolve the elongation of the molecular bond by approximately 1.2 a.u. within the duration of the x-ray pulse. The experiment paves the road toward time-resolved pump-probe photoelectron diffraction imaging at high-repetition-rate x-ray free-electron lasers.

Complex molecular structure demands customized solutions to laser cooling by extending its general set of principles and practices. Compared with other laser-cooled molecules, yttrium monoxide (YO) exhibits a large electron-nucleus interaction, resulting in a dominant hyperfine interaction over the electron spin-rotation coupling. The YO ground state is thus comprised of two manifolds of closely spaced states, with one of them possessing a negligible Landé $g$ factor. This unique energy level structure favors dual-frequency dc magneto-optical trapping (MOT) and gray molasses cooling (GMC). We report exceptionally robust cooling of YO at $4\mu \mathrm{K}$ over a wide range of laser intensity, detunings (one- and two-photon), and magnetic field. The magnetic insensitivity enables the spatial compression of the molecular cloud by alternating GMC and MOT under the continuous operation of the quadrupole magnetic field. A combination of these techniques produces a laser-cooled molecular sample with the highest phase space density in free space.

Periodic driving has emerged as a powerful tool in the quest to engineer new and exotic quantum phases. While driven many-body systems are generically expected to absorb energy indefinitely and reach an infinite-temperature state, the rate of heating can be exponentially suppressed when the drive frequency is large compared to the local energy scales of the system—leading to long-lived “prethermal” regimes. In this work, we experimentally study a bosonic cloud of ultracold atoms in a driven optical lattice and identify such a prethermal regime in the Bose-Hubbard model. By measuring the energy absorption of the cloud as the driving frequency is increased, we observe an exponential-in-frequency reduction of the heating rate persisting over more than 2 orders of magnitude. The tunability of the lattice potentials allows us to explore one- and two-dimensional systems in a range of different interacting regimes. Alongside the exponential decrease, the dependence of the heating rate on the frequency displays features characteristic of the phase diagram of the Bose-Hubbard model, whose understanding is additionally supported by numerical simulations in one dimension. Our results show experimental evidence of the phenomenon of Floquet prethermalization and provide insight into the characterization of heating for driven bosonic systems.

Gauge theories are the cornerstone of our understanding of fundamental interactions among elementary particles. Their properties are often probed in dynamical experiments, such as those performed at ion colliders and high-intensity laser facilities. Describing the evolution of these strongly coupled systems is a formidable challenge for classical computers and represents one of the key open quests for quantum simulation approaches to particle physics phenomena. In this work, we show how recent experiments done on Rydberg atom chains naturally realize the real-time dynamics of a lattice gauge theory at system sizes at the boundary of classical computational methods. We prove that the constrained Hamiltonian dynamics induced by strong Rydberg interactions maps exactly onto the one of a U(1) lattice gauge theory. Building on this correspondence, we show that the recently observed anomalously slow dynamics corresponds to a string-inversion mechanism, reminiscent of the string breaking typically observed in gauge theories. This underlies the generality of this slow dynamics, which we illustrate in the context of one-dimensional quantum electrodynamics on the lattice. Within the same platform, we propose a set of experiments that generically show long-lived oscillations, including the evolution of particle-antiparticle pairs, and discuss how a tunable topological angle can be realized, further affecting the dynamics following a quench. Our work shows that the state of the art for quantum simulation of lattice gauge theories is at 51 qubits and connects the recently observed slow dynamics in atomic systems to archetypal phenomena in particle physics.

We show how a large family of interacting nonequilibrium phases of matter can arise from the presence of multiple time-translation symmetries, which occur by quasiperiodically driving an isolated, quantum many-body system with two or more incommensurate frequencies. These phases are fundamentally different from those realizable in time-independent or periodically driven (Floquet) settings. Focusing on high-frequency drives with smooth time dependence, we rigorously establish general conditions for which these phases are stable in a parametrically long-lived “preheating” regime. We develop a formalism to analyze the effect of the multiple time-translation symmetries on the dynamics of the system, which we use to classify and construct explicit examples of the emergent phases. In particular, we discuss time quasicrystals which spontaneously break the time-translation symmetries, as well as time-translation symmetry-protected topological phases.

We experimentally realize a Peierls phase in the hopping amplitude of excitations carried by Rydberg atoms, and observe the resulting characteristic chiral motion in a minimal setup of three sites. Our demonstration relies on the intrinsic spin-orbit coupling of the dipolar exchange interaction combined with time-reversal symmetry breaking by a homogeneous external magnetic field. Remarkably, the phase of the hopping amplitude between two sites strongly depends on the occupancy of the third site, thus leading to a correlated hopping associated with a density-dependent Peierls phase. We experimentally observe this density-dependent hopping and show that the excitations behave as anyonic particles with a nontrivial phase under exchange. Finally, we confirm the dependence of the Peierls phase on the geometrical arrangement of the Rydberg atoms.

Far-from-equilibrium dynamics that lead to self-organization are highly relevant to complex dynamical systems not only in physics but also in life, earth, and social sciences. However, it is challenging to find systems with sufficiently controllable parameters that allow quantitatively modeling of emergent properties. Here, we study a nonequilibrium phase transition and observe signatures of self-organized criticality in a dilute thermal vapor of atoms optically excited to strongly interacting Rydberg states. Electromagnetically induced transparency provides excellent control over the population dynamics and enables high-resolution probing of the driven-dissipative dynamics, which also exhibits phase bistability. Increased sensitivity compared to previous work allows us to reconstruct the complete phase diagram, including in the vicinity of the critical point. We observe that interaction-induced energy shifts and enhanced decay only occur in one of the phases above a critical Rydberg population. This case limits the application of generic mean-field models; however, a modified, threshold-dependent approach is in qualitative agreement with experimental data. Near threshold, we observe self-organized dynamics in the form of population jumps that return the density to a critical value.

We present a new approach for deriving exact closed-form solutions for the steady state of a wide class of driven-dissipative nonlinear resonators that is distinct from more common complex-$P$-function methods. Our method generalizes the coherent quantum-absorber approach of Stannigel et al. [New J. Phys. 14, 063014 (2012)] to include nonlinear driving and dissipation and relies crucially on exploiting the Segal-Bargmann representation of Fock space. Our solutions and method reveal a wealth of previously unexplored observable phenomena in these systems, including new generalized photon-blockade and antiblockade effects and an infinite number of new parameter choices that yield quantum bistability.

Pump-probe measurements aim to capture the motion of electrons and nuclei on their natural timescales (femtoseconds to attoseconds) as chemical and physical transformations take place, effectively making “molecular movies” with short light pulses. However, the quantum dynamics of interest are filtered by the coordinate-dependent matrix elements of the chosen experimental observable. Thus, it is only through a combination of experimental measurements and theoretical calculations that one can gain insight into the internal dynamics. Here, we report on a combination of structural (relativistic ultrafast electron diffraction, or UED) and spectroscopic (time-resolved photoelectron spectroscopy, or TRPES) measurements to follow the coupled electronic and nuclear dynamics involved in the internal conversion and photodissociation of the polyatomic molecule, diiodomethane (${\mathrm{CH}}_2{\mathrm{I}}_2$). While UED directly probes the 3D nuclear dynamics, TRPES only serves as an indirect probe of nuclear dynamics via Franck-Condon factors, but it is sensitive to electronic energies and configurations, via Koopmans’ correlations and photoelectron angular distributions. These two measurements are interpreted with trajectory surface hopping calculations, which are capable of simulating the observables for both measurements from the same dynamics calculations. The measurements highlight the nonlocal dynamics captured by different groups of trajectories in the calculations. For the first time, both UED and TRPES are combined with theory capable of calculating the observables in both cases, yielding a direct view of the structural and nonadiabatic dynamics involved.

The creation of delocalized coherent superpositions of quantum systems experiencing different relativistic effects is an important milestone in future research at the interface of gravity and quantum mechanics. This milestone could be achieved by generating a superposition of quantum clocks that follow paths with different gravitational time dilation and investigating the consequences on the interference signal when they are eventually recombined. Light-pulse atom interferometry with elements employed in optical atomic clocks is a promising candidate for that purpose, but it suffers from major challenges including its insensitivity to the gravitational redshift in a uniform field. All of these difficulties can be overcome with the novel scheme presented here, which is based on initializing the clock when the spatially separate superposition has already been generated and performing a doubly differential measurement where the differential phase shift between the two internal states is compared for different initialization times. This scheme can be exploited to test the universality of the gravitational redshift with delocalized coherent superpositions of quantum clocks, and it is argued that its experimental implementation should be feasible with a new generation of 10-meter atomic fountains that will soon become available. Interestingly, the approach also offers significant advantages for more compact setups based on guided interferometry or hybrid configurations. Furthermore, in order to provide a solid foundation for the analysis of the various interferometry schemes and the effects that can be measured with them, a general formalism for a relativistic description of atom interferometry in curved spacetime is developed. It can describe freely falling atoms as well as the effects of external forces and guiding potentials, and it can be applied to a very wide range of situations. As an important ingredient for quantum-clock interferometry, suitable diffraction mechanisms for atoms in internal-state superpositions are investigated too. Finally, the relation of the proposed doubly differential measurement scheme to other experimental approaches and to tests of the universality of free fall is discussed in detail.

A mixed-species geometric phase gate has been proposed for implementing quantum logic spectroscopy on trapped ions, which combines probe and information transfer from the spectroscopy to the logic ion in a single pulse. We experimentally realize this method, show how it can be applied as a technique for identifying transitions in currently intractable atoms or molecules, demonstrate its reduced temperature sensitivity, and observe quantum-enhanced frequency sensitivity when it is applied to multi-ion chains. Potential applications include improved readout of trapped-ion clocks and simplified error syndrome measurements for quantum error correction.

Molecular iodine is photoexcited by a strong 800-nm laser driving several channels of multiphoton excitation. The motion following photoexcitation is probed using time-resolved x-ray scattering, which produces a scattering map $S(Q,\tau )$. Temporal Fourier-transform methods are employed to obtain a frequency-resolved x-ray-scattering signal $\tilde{S}(Q,\omega )$. Taken together, $S(Q,\tau )$ and $\tilde{S}(Q,\omega )$ separate different modes of motion so that mode-specific nuclear oscillatory positions, oscillation amplitudes, directions of motion, and times may be measured accurately. Molecular dissociations likewise have a distinct signature, which may be used to identify both velocities and dissociation time shifts and also can reveal laser-induced couplings among the molecular potentials.

Measuring the magnetic response of matter relies acutely on the degree to which a magnetic field source’s amplitude, spatial, and temporal character can be tailored. Magnetic fields are inseparable from light-matter interaction, yet due to the dominance of electric-field-induced effects in many systems, laser pulses have heretofore provided comparatively limited insight into the high-frequency magnetic response of matter. Conductors or superconductors arranged in a solenoidal configuration embody the state-of-the-art apparatus for generating spatially isolated magnetic fields, but the reliance on electrical circuitry limits the field amplitude, pulse brevity, and absolute timing of the generated fields. We transfer the concept of solenoidal currents commonly leveraged in electromagnets to photo-ionized electrons driven by moderately intense vector laser beams, in a scheme that does not require the laser mode to carry orbital angular momentum. We predict that this all-optical approach will enable magnetic fields exceeding 8 Tesla to be turned on within 50 femtoseconds using moderate laser intensities, an unprecedented combination of parameters that will open the possibility for ultrafast metrological techniques to be combined with intense, spatially isolated, magnetic fields.

The relaxation of few-body quantum systems can strongly depend on the initial state when the system’s semiclassical phase space is mixed; i.e., regions of chaotic motion coexist with regular islands. In recent years, there has been much effort to understand the process of thermalization in strongly interacting quantum systems that often lack an obvious semiclassical limit. The time-dependent variational principle (TDVP) allows one to systematically derive an effective classical (nonlinear) dynamical system by projecting unitary many-body dynamics onto a manifold of weakly entangled variational states. We demonstrate that such dynamical systems generally possess mixed phase space. When TDVP errors are small, the mixed phase space leaves a footprint on the exact dynamics of the quantum model. For example, when the system is initialized in a state belonging to a stable periodic orbit or the surrounding regular region, it exhibits persistent many-body quantum revivals. As a proof of principle, we identify new types of “quantum many-body scars,” i.e., initial states that lead to long-time oscillations in a model of interacting Rydberg atoms in one and two dimensions. Intriguingly, the initial states that give rise to most robust revivals are typically entangled states. On the other hand, even when TDVP errors are large, as in the thermalizing tilted-field Ising model, initializing the system in a regular region of phase space leads to a surprising slowdown of thermalization. Our work establishes TDVP as a method for identifying interacting quantum systems with anomalous dynamics in arbitrary dimensions. Moreover, the mixed phase space classical variational equations allow one to find slowly thermalizing initial conditions in interacting models. Our results shed light on a link between classical and quantum chaos, pointing toward possible extensions of the classical Kolmogorov-Arnold-Moser theorem to quantum systems.