We develop a unified many-body theory of two-photon dark-state laser cooling, the workhorse for preparing trapped ions close to their motional quantum ground state. For ions with a Λ level structure, driven by Raman lasers, we identify an ion-number-dependent crossover between weak and strong coupling where both the cooling rate and final temperature are simultaneously optimized. We obtain simple analytic results in both extremes: In the weak coupling limit, we show a Lorentzian spin-absorption spectrum determines the cooling rate and final occupation of the motional state, which are both independent of the number of ions. We also highlight the benefit of including an additional spin dependent force in this case. In the strong coupling regime, our theory reveals the role of collective dynamics arising from phonon exchange between dark and bright states, allowing us to explain the enhancement of the cooling rate with increasing ion number. Our analytic results agree closely with exact numerical simulations and provide experimentally accessible guidelines for optimizing cooling in large ion crystals, a key step toward scalable, high-fidelity trapped-ion quantum technologies.
Polar molecules are a promising platform for quantum-enhanced sensing and precision tests of fundamental physics, owing to their strong long-range dipolar interactions, broad sensitivity to electromagnetic fields, and sensitivity to potential physics beyond the Standard Model. However, the creation of metrologically useful entangled states in molecular systems has remained elusive. Here, we report the first observation of a class of metrologically useful entangled states - spin-squeezed states - in polar CaF molecules trapped in an optical tweezer array. The spin degree of freedom is encoded in rotational levels which are directly coupled by dipolar exchange interactions. By harnessing appropriate dynamical decoupling schemes we observe up to 3.0(3)dB of metrological gain, (2.2(3)dB without measurement correction) from direct exchange interactions. Using Floquet engineering, we further realize richer Hamiltonians that preserve spin squeezing while enabling the development of longer-range quantum correlations. Using site- and spin-resolved measurements we demonstrate that these entangled states enhance sensitivity to both homogeneous and spatially varying fields, and reveal strong non-classical correlations, including bipartite entanglement and Einstein-Podolsky-Rosen steering. Finally, we transfer the spin-squeezed states into long-lived and non-interacting hyperfine states, where the metrological enhancement persists for up to 100ms. Our results establish molecular optical tweezer arrays as a scalable platform for generating, controlling, characterizing, and storing entangled states of molecules, opening new opportunities for quantum-enhanced sensing and precision tests of fundamental physics.
Using a strontium cavity-QED apparatus, we first explore dynamical phases of BCS superconductors and perform time-resolved spectral gap spectroscopy. We also observe the continuous dissipation-induced superradiant transition in the cooperative resonance fluorescence (CRF) model.
We investigate the quantum many-body dynamics of bosonic atoms hopping in a two-leg ladder with strong on-site contact interactions. We observe that when the atoms are prepared in a staggered pattern with pairs of atoms on every other rung, singlon defects, i.e. rungs with only one atom, can localize due to an emergent topological model, even though the underlying model in the absence of interactions admits only topologically trivial states. This emergent topological localization results from the formation of a zero-energy edge mode in an effective lattice formed by two adjacent chains with alternating strong and weak hoping links (Su-Schrieffer-Heeger chains) and opposite staggering which interface at the defect position. Our findings open the opportunity to dynamically generate non-trivial topological behaviors without the need for complex Hamiltonian engineering.
Long-range and anisotropic dipolar interactions profoundly modify the dynamics of particles hopping in a periodic lattice potential. We report the realization of a generalized t-J model with dipolar interactions using a system of ultracold fermionic molecules with spin encoded in the two lowest rotational states. We independently tuned the dipolar Ising and spin-exchange couplings and the molecular motion and studied their interplay on coherent spin dynamics. Using Ramsey spectroscopy, we observed and modeled interaction-driven contrast decay that depends strongly both on the strength of the anisotropy between Ising and spin-exchange couplings and on motion. This study paves the way for future exploration of kinetic spin dynamics and quantum magnetism with highly tunable molecular platforms in regimes that are challenging for existing numerical and analytical methods.
Entangled spin squeezed states generated via dipolar interactions in lattice models provide unique opportunities for quantum enhanced sensing and are now within reach of current experiments. A critical question in this context is which parameter regimes offer the best prospects under realistic conditions. Light scattering in deep lattices can induce significant decoherence and strong Stark shifts, while shallow lattices face motional decoherence as a fundamental obstacle. Here we analyze the interplay between motion and spin squeezing in itinerant fermionic dipoles in one dimensional chains using exact matrix product state simulations. We demonstrate that shallow lattices can achieve more than 5dB of squeezing, outperforming deep lattices by up to more than 3dB, even in the presence of low filling, loss and decoherence. We relate this finding to SU(2)-symmetric superexchange interactions, which keep spins aligned and protect collective correlations. We show that the optimal regime is achieved for small repulsive off-site interactions, with a trade-off between maximal squeezing and optimal squeezing time.
We propose to simulate dynamical phases of a BCS superconductor using an ensemble of cold atoms trapped in an optical cavity. Effective Cooper pairs are encoded via internal states of the atoms and attractive interactions are realized via the exchange of virtual photons between atoms coupled to a common cavity mode. Control of the interaction strength combined with a tunable dispersion relation of the effective Cooper pairs allows exploration of the full dynamical phase diagram of the BCS model, as a function of system parameters and the prepared initial state. Our proposal paves the way for the study of non-equilibrium features of quantum magnetism and superconductivity by harnessing atom-light interactions in cold atomic gases.
Ultracold dipolar particles pinned in optical lattices or tweezers provide an excellent platform for studying out-of-equilibrium quantum magnetism with dipole-mediated couplings. Starting with an initial state with spins of opposite orientation in each of the legs of a ladder lattice, we show that spin relaxation displays an unexpected dependence on inter-leg distance and dipole orientation. This intricate dependence, stemming from the interplay between intra- and inter-leg interactions, results in three distinct dynamical regimes: (i) ergodic, characterized by the fast relaxation towards equilibrium of correlated pairs of excitations generated at exponentially fast rates from the initial state; (ii) metastable, in which the state is quasi-localized in the initial state and only decays at exceedingly long timescales, resembling false vacuum decay; and, surprisingly, (iii) partially-relaxed, with coexisting fast partial relaxation and very long-lived partial quasi-localization. Realizing these intriguing dynamics is within reach of current state-of-the-art experiments in dipolar gases.
Quantum computation (QC) and simulation rely on long-lived qubits with controllable interactions. Early work in quantum computing made use of molecules because of their readily available intramolecular nuclear spin coupling and chemical shifts, along with mature nuclear magnetic resonance techniques. Subsequently, the pursuit of many physical platforms has flourished. Trapped polar molecules have been proposed as a promising quantum computing platform, offering scalability and single-particle addressability while still leveraging inherent complexity and strong couplings of molecules. Recent progress in the single quantum state preparation and coherence of the hyperfine-rotational states of individually trapped molecules allows them to serve as promising qubits, with intermolecular dipolar interactions creating entanglement. However, universal two-qubit gates have not been demonstrated with molecules. Here, we harness intrinsic molecular resources to implement a two-qubit iSWAP gate using individually trapped $X^{1}\Sigma^{+}$ NaCs molecules. We characterize the innate dipolar interaction between rotational states and control its strength by tuning the polarization of the traps. By allowing the molecules to interact for 664 $\mu$s at a distance of 1.9 $\mu$m, we create a maximally entangled Bell state with a fidelity of 94(3)\%, following postselection to remove trials with empty traps. Using motion-rotation coupling, we measure residual excitation of the lowest few motional states along the axial trapping direction and find them to be the primary source of decoherence. Finally, we identify two non-interacting hyperfine states within the ground rotational level in which we encode a qubit. The interaction is toggled by transferring between interacting and non-interacting states to realize an iSWAP gate. We verify the gate performance by measuring its logical truth table.
We simulate out-of-equilibrium dynamics in Bardeen-Cooper-Schrieffer model of superconductivity using ~106 Sr atoms coupled via cavity-mediated spin-exchange inter-actions. In doing so, we observe three theoretically-predicted dynamical phases and identify corresponding phase transitions.
The dynamics of one-dimensional quantum many-body systems is often numerically simulated with matrix-product states (MPSs). The computational complexity of MPS methods is known to be related to the growth of entropies of reduced density matrices for bipartitions of the chain. While for closed systems the entropy relevant for the complexity is uniquely defined by the entanglement entropy, for open systems it depends on the choice of the representation. Here, we systematically compare the growth of different entropies relevant to the complexity of matrix-product representations in open-system simulations. We simulate an XXZ spin-1/2 chain in the presence of spontaneous emission and absorption, and dephasing. We compare simulations using a representation of the full density matrix as a matrix-product density operator (MPDO) with a quantum trajectory unraveling, where each trajectory is itself represented by an MPS (QT+MPS). We show that the bipartite entropy in the MPDO description (operator entanglement, OE) generally scales more favorably with time than the entropy in QT+MPS (trajectory entanglement, TE): i) For spontaneous emission and absorption the OE vanishes while the TE grows and reaches a constant value for large dissipative rates and sufficiently long times; ii) for dephasing the OE exhibits only logarithmic growth while the TE grows polynomially. Although QT+MPS requires a smaller local state space, the more favorable entropy growth can thus make MPDO simulations fundamentally more efficient than QT+MPS. Furthermore, MPDO simulations allow for easier exploitation of higher-order Trotter decompositions and translational invariance, allowing for larger time steps and system sizes.
Network science provides a universal framework for modeling complex systems, contrasting the reductionist approach generally adopted in physics. In a prototypical study, we utilize network models created from spectroscopic data of atoms to predict microscopic properties of the underlying physical system. For simple atoms such as helium, an a posteriori inspection of spectroscopic network communities reveals the emergence of quantum numbers and symmetries. For more complex atoms such as thorium, finer network hierarchies suggest additional microscopic symmetries or configurations. Furthermore, link prediction in spectroscopic networks yields a quantitative ranking of yet unknown atomic transitions, offering opportunities to discover new spectral lines in a well-controlled manner. Our work promotes a genuine bi-directional exchange of methodology between network science and physics, and presents new perspectives for the study of atomic spectra.
We experimentally demonstrate all three predicted dynamical phases of quenched superconductors using strontium atoms coupled to a high-finesse cavity. We show that this rich phenomenology can also be observed with a similar but different Hamiltonian.
We study the temporal growth and spatial propagation of quantum correlations in a two-dimensional bilayer realising a spin-1/2 quantum XXZ model with couplings mediated by long-range and anisotropic dipolar interactions. Starting with an initial state consisting of spins with opposite magnetization in each of the layers, we predict the emergence of a momentum-dependent dynamic instability in the spin structure factor that results, at short times, in the creation of pairs of excitations at exponentially fast rates. The created pairs present a characteristic momentum distribution that can be tuned by controlling the dipolar orientation, the layer separation or the dipolar couplings. The predicted behavior remains observable at very low filling fractions, making it accessible in state-of-the-art experiments with Rydberg atoms, magnetic atoms, and polar molecule arrays.
Collectively coupling molecular ensembles to a cavity has been demonstrated to modify chemical reactions akin to catalysis. Theoretically understanding this experimental finding remains an important challenge. In particular the role of quantum effects in such setups is an open question of fundamental and practical interest. Theoretical descriptions often neglect quantum entanglement between nuclear and electro-photonic degrees of freedom, e.g., by computing Ehrenfest dynamics. Here we discover that disorder can strongly enhance the build-up of this entanglement on short timescales after incoherent photo-excitation. We find that this can have direct consequences for nuclear coordinate dynamics. We analyze this phenomenon in a disordered Holstein-Tavis-Cummings model, a minimal toy model that includes all fundamental degrees of freedom. Using a numerical technique based on matrix product states we simulate the exact quantum dynamics of more than 100 molecules. Our results highlight the importance of beyond Born-Oppenheimer theories in polaritonic chemistry.
The operator space entanglement entropy, or simply "operator entanglement" (OE), is an indicator of the complexity of quantum operators and of their approximability by matrix product operators (MPOs). We study the OE of the density matrix of 1D many-body models undergoing dissipative evolution. It is expected that, after an initial linear growth reminiscent of unitary quench dynamics, the OE should be suppressed by dissipative processes as the system evolves to a simple stationary state. Surprisingly, we find that this scenario breaks down for one of the most fundamental dissipative mechanisms: dephasing. Under dephasing, after the initial "rise and fall," the OE can rise again, increasing logarithmically at long times. Using a combination of MPO simulations for chains of infinite length and analytical arguments valid for strong dephasing, we demonstrate that this growth is inherent to a U(1) conservation law. We argue that in an XXZ spin model and a Bose-Hubbard model the OE grows universally as 1/4log_{2}t at long times and as 1/2log_{2}t for a Fermi-Hubbard model. We trace this behavior back to anomalous classical diffusion processes.
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We study a simple model for photoinduced electron transfer reactions for the case of many donor-acceptor pairs that are collectively and homogeneously coupled to a photon mode of a cavity. We describe both coherent and dissipative collective effects resulting from this coupling within the framework of a quantum optics Lindblad master equation. We introduce a method to derive an effective rate equation for electron transfer by adiabatically eliminating donor and acceptor states and the cavity mode. The resulting rate equation is valid for both weak and strong coupling to the cavity mode and describes electronic transfer through both the cavity-coupled bright states and the uncoupled dark states. We derive an analytic expression for the instantaneous electron transfer rate that depends non-trivially on the time-varying number of pairs in the ground state. We find that under proper resonance conditions, and in the presence of an incoherent drive, reaction rates can be enhanced by the cavity. This enhancement persists, and can even be largest, in the weak light-matter coupling regime. We discuss how the cavity effect is relevant for realistic experiments.
We propose a mechanism to realize high-yield molecular formation from ultracold atoms. Atom pairs are continuously excited by a laser, and a collective decay into the molecular ground state is induced by a coupling to a lossy cavity mode. Using a combination of analytical and numerical techniques, we demonstrate that the molecular yield can be improved by simply increasing the number of atoms, and can overcome efficiencies of state-of-the-art association schemes. We discuss realistic experimental setups for diatomic polar and nonpolar molecules, opening up collective light matter interactions as a tool for quantum state engineering, enhanced molecule formation, collective dynamics, and cavity mediated chemistry.