Rydberg Excitation Research Articles

Rydberg Molecules and Excitation of Lattice-Mixed Rydberg States in a Deep Ponderomotive Optical Lattice

Rydberg Molecules and Excitation of Lattice-Mixed Rydberg States in a Deep Ponderomotive Optical Lattice

Observation of collective decay dynamics of a single Rydberg superatom

The authors study the emission of single photons from a collective atomic Rydberg excitation and observe variations in its decay rate that result from the collective state's internal coherent dynamics.

From synchrotrons for XFELs: the soft x-ray near-edge spectrum of the ESCA molecule

A predictive understanding of soft x-ray near-edge absorption spectra of small molecules is an enduring theoretical challenge and of current interest for x-ray probes of molecular dynamics. We report the experimental absorption spectrum for the electron spectroscopy for chemical analysis (ESCA) molecule (ethyl trifluoroacetate) near the carbon 1s absorption edge between 285–300 eV. The ESCA molecule with four chemically distinct carbon sites has previously served as a theoretical benchmark for photoelectron spectra and now for photoabsorption spectra. We report a simple edge-specific approach for systematically expanding standard basis sets to properly describe diffuse Rydberg orbitals and the importance of triple excitations in equation-of-motion coupled-cluster calculations of the energy interval between valence and Rydberg excitations.

Stochastic switching in the Rydberg atomic ensemble.

We demonstrated stochastic switching in a bistable system implemented with the Rydberg atomic ensemble, which is realized by cascaded Rydberg excitation in a cesium vapor cell. Measurement of Rydberg state's population by means of the electromagnetically induced transparency allows us to investigate the nonlinear behavior in Rydberg atomic ensemble experimentally. The transition between the two states of the bistable system is driven by the intensity noise of the laser beams. Rydberg atomic ensemble accumulates energy in an equilibrium situation and brings the nonlinear system across the threshold, where stochastic switching occurs between the two states.

Controlling Exciton-Phonon Interactions via Electromagnetically Induced Transparency.

Highly excited Rydberg states of excitons in Cu_{2}O semiconductors provide a promising approach to explore and control strong particle interactions in a solid-state environment. A major obstacle has been the substantial absorption background that stems from exciton-phonon coupling and lies under the Rydberg excitation spectrum, weakening the effects of exciton interactions. Here, we demonstrate that two-photon excitation of Rydberg excitons under conditions of electromagnetically induced transparency (EIT) can be used to control this background. Based on a microscopic theory that describes the known single-photon absorption spectrum, we analyze the conditions under which two-photon EIT permits separating the optical Rydberg excitation from the phonon-induced absorption background, and even suppressing it entir7ely. Our findings thereby pave the way for the exploitation of Rydberg blockade with Cu_{2}O excitons in nonlinear optics and other applications.

Inelastic collision dynamics of a single cold ion immersed in a Bose-Einstein condensate

We investigate inelastic collision dynamics of a single cold ion in a Bose-Einstein condensate. We observe rapid ion-atom-atom three-body recombination leading to formation of weakly bound molecular ions followed by secondary two-body molecule-atom collisions quenching the rovibrational states towards deeper binding energies. In contrast to previous studies exploiting hybrid ion traps, we work in an effectively field-free environment and generate a free low-energy ionic impurity directly from the atomic ensemble via Rydberg excitation and ionization. This allows us to implement an energy-resolved field-dissociation technique to trace the relaxation dynamics of the recombination products. Our observations are in good agreement with numerical simulations based on Langevin capture dynamics and provide complementary means to study stability and reaction dynamics of ionic impurities in ultracold quantum gases.

Experimental and Theoretical Investigation of the 3sp(d) Rydberg States of Fenchone by Polarized Laser Resonance-Enhanced-Multiphoton-Ionization and Fourier Transform VUV Absorption Spectroscopy.

The VUV absorption spectrum of fenchone is re-examined using synchrotron radiation Fourier transform spectrometry, revealing new vibrational structure. Picosecond laser (2+1) resonance enhanced multiphoton ionization (REMPI) spectroscopy complements this, providing an alternative view of the 3spd Rydberg excitation region. These spectra display broadly similar appearance, with minor differences that are largely explained by referring to calculated one- and two-photon electronic excitation cross-sections. Both show good agreement with Franck-Condon simulations of the relevant vibrational structures. Parent ion REMPI ionization yields with both femtosecond and picosecond excitation laser pulses are studied as a function of laser polarization and intensity, the latter providing insight into the relative two-photon excitation and one-photon ionization rates. The experimental circular-linear dichroism observed in the parent ion yields varies strongly between the 3s and 3p Rydberg states, in good overall agreement with the calculated two-photon excitation circular-linear dichroism, while corroborating other evidence that the 3pz sub-state plays no more than a very minor role in the (2+1) REMPI spectrum. Vibrationally resolved photoelectron spectra are recorded with picosecond pulse duration (2+1) REMPI at selected intermediate vibrational excitations. The 3s intermediate state displays a very strong Δv=0 propensity on ionization, but the 3p intermediate evidences more complex vibronic dynamics, and we infer some 3p→3s internal conversion prior to ionization.

Controlling the Dipole Blockade and Ionization Rate of Rydberg Atoms in Strong Electric Fields.

We study a hitherto unexplored regime of the Rydberg excitation blockade using highly Stark-shifted, yet long-living, states of Rb atoms subject to electric fields above the classical ionization limit. Such states allow tuning the dipole-dipole interaction strength while their ionization rate can be changed over 2 orders of magnitude by small variations of the electric field. We demonstrate laser excitation of the interacting Rydberg states followed by their detection using controlled ionization and magnified imaging with high spatial and temporal resolution. Our work reveals new possibilities to engineer the interaction strength and dynamically control the ionization and detection of Rydberg atoms, which can be useful for realizing and assessing quantum simulators that vary in space and time.

Rydberg Composites

We introduce the Rydberg Composite, a new class of Rydberg matter where a single Rydberg atom is interfaced with a dense environment of neutral ground state atoms. The properties of the Composite depend on both the Rydberg excitation, which provides the gross energetic and spatial scales, and on the distribution of ground state atoms within the volume of the Rydberg wave function, which sculpt the electronic states. The latter range from the "trilobites", for small numbers of scatterers, to delocalized and chaotic eigenstates for disordered scatterer arrays, culminating in the dense scatterer limit in symmetry-dominated wave functions which promise good control in future experiments. We characterize these scenarios with different theoretical methods, enabling us to obtain scaling behavior for the regular spectrum and measures of chaos and delocalization in the disordered regime. Thus, we obtain a systematic description of the Composite states. The 2D monolayer Composite possesses the richest spectrum with an intricate band structure in the limit of homogeneous scatterers.

Dynamics of Rydberg excitations and quantum correlations in an atomic array coupled to a photonic crystal waveguide

We study the dynamics of up to two Rydberg excitations and the correlation growth in a chain of atoms coupled to a photonic crystal waveguide. In this setup, an excitation can hop from one atom to another via exponentially decaying exchange interactions mediated by the waveguide. An initially localized excitation undergoes a continuous-time quantum walk for short-range hopping, and for long-range, it experiences quasi-localization. Besides that, the inverse participation ratio reveals a super-ballistic diffusion of the excitation in short times, whereas, at a long time, it becomes ballistic. For two initially localized excitations, intriguing, and complex dynamical scenarios emerge for different initial separations due to the competition between the Rydberg-Rydberg and exchange interactions. In particular, the two-point correlation reveals a light-cone behavior even for sufficiently long-range exchange interactions. Additionally, we characterize the growth of bipartite entanglement entropy, which exhibits a global bound if only one excitation is present in the dynamics. Finally, we analyze the effect of imperfections due to spontaneous emission from the Rydberg state into photons outside the waveguide and show that all physical phenomena we predict are well within experimental reach.

Dynamics of the vacuum state in a periodically driven Rydberg chain

We study the dynamics of the periodically driven Rydberg chain starting from the state with zero Rydberg excitations (vacuum state denoted by $|0\rangle$) using a square pulse protocol in the high drive amplitude limit. We show, using exact diagonalization for finite system sizes ($L\le 26$), that the Floquet Hamiltonian of the system, within a range of drive frequencies which we chart out, hosts a set of quantum scars which have large overlap with the $|0\rangle$ state. These scars are distinct from their counterparts having high overlap with the maximal Rydberg excitation state ($|\mathbb{Z}_2\rangle$); they coexist with the latter class of scars and lead to persistent coherent oscillations of the density-density correlator starting from the $|0\rangle$ state. We also identify special drive frequencies at which the system undergoes perfect dynamic freezing and provide an analytic explanation for this phenomenon. Finally, we demonstrate that for a wide range of drive frequencies, the system reaches a steady state with sub-thermal values of the density-density correlator. The presence of such sub-thermal steady states, which are absent for dynamics starting from the $|\mathbb{Z}_2\rangle$ state, imply a weak violation of the eigenstate thermalization hypothesis in finite sized Rydberg chains distinct from that due to the scar-induced persistent oscillations reported earlier. We conjecture that in the thermodynamic limit such states may exist as pre-thermal steady states that show anomalously slow relaxation. We supplement our numerical results by deriving an analytic expression for the Floquet Hamiltonian using a Floquet perturbation theory in the high amplitude limit which provides an analytic, albeit qualitative, understanding of these phenomena at arbitrary drive frequencies. We discuss experiments which can test our theory.

Assessing the Tamm-Dancoff approximation, singlet-singlet, and singlet-triplet excitations with the latest long-range corrected double-hybrid density functionals.

We continue our work on the long-range corrected double-hybrid density functionals (LC-DHDFs) ωB2PLYP and ωB2GP-PLYP that we developed in the context of time-dependent (TD) Density Functional Theory (DFT) to enable the robust description of singlet-singlet excitations [M. Casanova-Páez, M. B. Dardis, and L. Goerigk, J. Chem. Theory Comput. 15, 4735 (2019)]. In our initial study, we only assessed the impact of a LC on BLYP-based DHDFs, and herein, we extend our understanding by providing the first test of PBE-based LC-DHDFs within the established TD-DHDF scheme. Moreover, this study is one of few that provides a direct comparison between TD-DHDFs and their faster Tamm-Dancoff-approximation variants (TDA-DHDFs). Most importantly, this is the first TDA-DHDF study since Grimme and Neese's TDA-B2PLYP [J. Chem. Phys. 127, 154116 (2007)] and the first work on TD-DHDFs that addresses singlet-triplet excitations. We show how the difference between TD-DHDFs and TDA-DHDFs is often negligible for singlet-singlet excitations, but how one has to apply TDA-DHDFs for triplet excitations. For both excitation types, the LC is beneficial to the BLYP-based DHDFs, but detrimental to the PBE-based ones. For local-valence and Rydberg excitations, ωB2PLYP and ωB2GP-PLYP as well as the global DHDF PBE-QIDH can be recommended. If a transition exhibits charge-transfer character, ωB2PLYP and ωB2GP-PLYP should be applied. An analysis of the gaps between the first singlet and triplet excited states of our systems revealed that there is room for further improvements to reach better robustness. Until that goal has been achieved, we recommend ωB2PLYP and ωB2GP-PLYP as some of the currently best TDA-DFT methods.

Observation of Double Excitations in the Resonant Inelastic X-ray Scattering of Nitric Oxide.

The nitrogen K-edge resonant inelastic X-ray scattering (RIXS) map of nitric oxide (NO) has been measured and simulated to provide a detailed analysis of the observed features. High-resolution experimental RIXS maps were collected using an in situ gas flow cell and a high-transmission soft X-ray spectrometer. Accurate descriptions of the ground, excited, and core-excited states are based upon restricted active space self-consistent-field calculations using second order multiconfigurational perturbation theory. The nitrogen K-edge RIXS map of NO shows a range of features that can be assigned to intermediate states arising from 1s → π* and 1s → Rydberg excitations; additional bands are attributed to doubly excited intermediate states comprising 1s → π* and π → π* excitations. These results provide a detailed picture of RIXS for an open-shell molecule and an extensive description of the core-excited electronic structure of NO, an important molecule in many chemical and biological processes.

On-demand indistinguishable single photons from an efficient and pure source based on a Rydberg ensemble

Single photons coupled to atomic systems have shown to be a promising platform for developing quantum technologies. Yet a bright on-demand, highly pure, and highly indistinguishable single-photon source compatible with atomic platforms is lacking. In this work, we demonstrate such a source based on a strongly interacting Rydberg system. The large optical nonlinearities in a blockaded Rydberg ensemble convert coherent light into a single collective excitation that can be coherently retrieved as a quantum field. We simultaneously observe a fully single-mode (spectral, temporal, spatial, and polarization) efficiency up to 0.098(2), a detector-background-subtracted g ( 2 ) = 5.0 ( 1.6 ) × 10 − 4 , and indistinguishability of 0.980(7), at an average photon production rate of 1.18 ( 2 ) × 10 4 s − 1 . All of these make this system promising for scalable quantum information applications. Furthermore, we investigate the effects of contaminant Rydberg excitations on the source efficiency and observed single-mode efficiencies up to 0.18(2) for lower photon rates. Finally, recognizing that many quantum information protocols require a single photon in a fully single mode, we introduce metrics that take into account all degrees of freedom to benchmark the performance of on-demand sources.

Excited states of molecular and crystalline acetylene: application of TDHF and BSE via density fitting methods

Low-lying states in small, multiply bonded hydrocarbon molecules may be divided into valence and Rydberg excitations. Excited states of the cubic phase of the acetylene molecular crystal are calculated using the time-dependent Hartree–Fock (TDHF) method. TDHF and Bethe–Salpeter equation (BSE) calculations are performed on molecular CH in order to interpret these excited states. Computationally inexpensive TDHF and BSE methods are compared to previous CASPT2, MRCI and EOM-CCSD calculations and experiment. Localised, lowest energy excited states in the CH molecular crystal mirror those in the gas phase. In the next lowest excitations the electron and hole separate over one or two shells of molecular neighbours. A density fitting method for calculating the Coulomb matrix elements which arise in time-dependent Hartree Fock theory (TDHF) in periodic systems is implemented in the Exciton code and described briefly.

Experimental creation of single Rydberg excitations via adiabatic passage

In an atomic ensemble, quantum information is typically carried as single collective excitations. It is very advantageous if the creation of single excitations is efficient and robust. Rydberg blockade enables deterministic creation of single excitations via collective Rabi oscillation by precisely controlling the pulse area, being sensitive to many experimental parameters. In this paper, we implement the adiabatic rapid passage technique to the Rydberg excitation process in a mesoscopic atomic ensemble. We make use of a two-photon excitation scheme with an intermediate state off-resonant and sweep the laser frequency of one excitation laser. We find the chirped scheme preserves internal phases of the collective Rydberg excitation and be more robust against variance of laser intensity and frequency detuning.

Quantum many-body scar states in two-dimensional Rydberg atom arrays

We find exponentially many exact quantum many-body scar states in a two-dimensional PXP model---an effective model for a two-dimensional Rydberg atom array in the nearest-neighbor blockade regime. Such scar states are remarkably simple valence bond solids despite being at an effectively infinite temperature, and thus strongly violate the eigenstate thermalization hypothesis. For a particular boundary condition, such eigenstates have integer-valued energies. Moreover, certain charge-density-wave initial states give rise to strong oscillations in the Rydberg excitation density after a quantum quench and towerlike structures in their overlaps with eigenstates.

Assembled arrays of Rydberg-interacting atoms

Assembled arrays of individual atoms with Rydberg-mediated interactions provide a powerful platform for the simulation of many-body spin Hamiltonians as well as the implementation of universal gate-based quantum information processing. We demonstrate the first realization of Rydberg excitations and controlled interactions in microlens-generated multisite trap arrays of reconfigurable geometry. We utilize atom-by-atom assembly for the deterministic preparation of pre-defined 2D structures of rubidium Rydberg atoms with exactly known mutual separations and selectable interaction strength. By adapting the geometry and the addressed Rydberg state, a parameter regime spanning from weak interactions to strong coupling can be accessed. We characterize the simultaneous coherent excitation of non-interacting atom clusters for the state 57D5/2 and analyze the experimental parameters and limitations. For configurations optimized for Rydberg blockade utilizing the state 87D5/2, we observe collectively enhanced Rabi oscillations.

Observation of Laughlin states made of light.

Much of the richness in nature emerges because simple constituents form an endless variety of ordered states1. Whereas many such states are fully characterized by symmetries2, interacting quantum systems can exhibit topological order and are instead characterized by intricate patterns of entanglement3,4. A paradigmatic example of topological order is the Laughlin state5, which minimizes the interaction energy of charged particles in a magnetic field and underlies the fractional quantum Hall effect6. Efforts have been made to enhance our understanding of topological order by forming Laughlin states in synthetic systems of ultracold atoms7,8 or photons9-11. Nonetheless, electron gases remain the only systems in which such topological states have been definitively observed6,12-14. Here we create Laughlin-ordered photon pairs using a gas of strongly interacting, lowest-Landau-level polaritons as a photon collider. Initially uncorrelated photons enter a cavity and hybridize with atomic Rydberg excitations to form polaritons15-17, quasiparticles that here behave like electrons in the lowest Landau level owing to a synthetic magnetic field created by Floquet engineering18 a twisted cavity11,19 and by Rydberg-mediated interactions between them16,17,20,21. Polariton pairs collide and self-organize to avoid each other while conserving angular momentum. Our finite-lifetime polaritons only weakly prefer such organization. Therefore, we harness the unique tunability of Floquet polaritons to distil high-fidelity Laughlin states of photons outside the cavity. Particle-resolved measurements show that these photons avoid each other and exhibit angular momentum correlations, the hallmarks of Laughlin physics. This work provides broad prospects for the study of topological quantum light22.

Quantifying the impact of state mixing on the Rydberg excitation blockade

This paper demonstrates a new technique to quantify the negative impact of state-mixing interactions on the Rydberg excitation blockade near the Forster resonance. By observing state-mixing events on a shot-by-shot basis, the authors identify the mechanisms responsible for large rates of mixing, and determine the extent to which mixing breaks the blockade in a mesoscopic ensemble.