Metasurface-Based Hybrid Optical Cavities for Chiral Sensing.

Quantum metasurfaces, i.e., two-dimensional subwavelength arrays of quantum emitters, can be employed as mirrors towards the design of hybrid cavities, where the optical response is given by the interplay of a cavity-confined field and the surface modes supported by the arrays. We show that stacked layers of quantum metasurfaces with orthogonal dipole orientation can serve as helicity-preserving cavities. These structures exhibit ultranarrow resonances and can enhance the intensity of the incoming field by orders of magnitude, while simultaneously preserving the handedness of the field circulating inside the resonator, as opposed to conventional cavities. The rapid phase shift in the cavity transmission around the resonance can be exploited for the sensitive detection of chiral scatterers passing through the cavity. We discuss possible applications of these resonators as sensors for the discrimination of chiral molecules. Our approach describes a new way of chiral sensing via the measurement of particle-induced phase shifts.

Scaling Law for Kasha's Rule in Photoexcited Molecular Aggregates.

We study the photophysics of molecular aggregates from a quantum optics perspective, with emphasis on deriving scaling laws for the fast nonradiative relaxation of collective electronic excitations, referred to as Kasha's rule. Aggregates exhibit an energetically broad manifold of collective states with delocalized electronic excitations originating from near-field dipole-dipole exchanges between neighboring monomers. Photoexcitation at optical wavelengths, much larger than the monomer-monomer average separation, addresses almost exclusively symmetric collective states, which for an arrangement known as H-aggregate show an upward hypsochromic shift. The extremely fast subsequent nonradiative relaxation via intramolecular vibrational modes populates lower energy, subradiant states, resulting in effective inhibition of fluorescence. Our analytical treatment allows for the derivation of an approximate scaling law of this relaxation process, linear in the number of available low-energy vibrational modes and directly proportional to the dipole-dipole interaction strength between neighboring monomers.

Linear optical elements based on cooperative subwavelength emitter arrays.

We describe applications of two-dimensional subwavelength quantum emitter arrays as efficient optical elements in the linear regime. For normally incident light, the cooperative optical response, stemming from emitter-emitter dipole exchanges, allows the control of the array's transmission, its resonance frequency, and bandwidth. Operations on fully polarized incident light, such as generic linear and circular polarizers as well as phase retarders can be engineered and described in terms of Jones matrices. Our analytical approach and accompanying numerical simulations identify optimal regimes for such operations and reveal the importance of adjusting the array geometry and of the careful tuning of the external magnetic fields amplitude and direction.

Floquet engineering of molecular dynamics via infrared coupling.

We discuss Floquet engineering of dissipative molecular systems through periodic driving of an infrared-active vibrational transition, either directly or via a cavity mode. Following a polaron quantum Langevin equation approach, we derive correlation functions and stationary quantities showing strongly modified optical response of the infrared-dressed molecule. The coherent excitation of molecular vibrational modes in combination with the modulation of electronic degrees of freedom due to vibronic coupling can lead to both enhanced vibronic coherence and control over vibrational sideband amplitudes. The additional coupling to an infrared cavity allows for the controlled suppression of undesired sidebands, an effect stemming from the Purcell enhancement of vibrational relaxation rates.

Partial Optomechanical Refrigeration via Multimode Cold-Damping Feedback.

We provide a fully analytical treatment for the partial refrigeration of the thermal motion of a quantum mechanical resonator under the action of feedback. As opposed to standard cavity optomechanics where the aim is to isolate and cool a single mechanical mode, the aim here is to extract the thermal energy from many vibrational modes within a large frequency bandwidth. We consider a standard cold-damping technique, where homodyne readout of the cavity output field is fed into a feedback loop that provides a cooling action directly applied on the mechanical resonator. Analytical and numerical results predict that low final occupancies are achievable independent of the number of modes addressed by the feedback, as long as the cooling rate is smaller than the intermode frequency separation. For resonators exhibiting a few nearly degenerate pairs of modes, cooling is less efficient and a weak dependence on the number of modes is obtained. These scalings hint toward the design of frequency-resolved mechanical resonators, where efficient refrigeration is possible via simultaneous cold-damping feedback.

Cavity Quantum Electrodynamics with Frequency-Dependent Reflectors.

We present a general framework for cavity quantum electrodynamics with strongly frequency-dependent mirrors. The method is applicable to a variety of reflectors exhibiting sharp internal resonances as can be realized, for example, with photonic-crystal mirrors or with two-dimensional atomic arrays around subradiant points. Our approach is based on a modification of the standard input-output formalism to explicitly include the dynamics of the mirror's internal resonance. We show how to directly extract the interaction parameters from the comparison with classical transfer matrix theory and how to treat the non-Markovian dynamics of the cavity field mode introduced by the mirror's internal resonance. As an application within optomechanics, we illustrate how a non-Markovian Fano-resonance cavity with a flexible photonic-crystal mirror can provide both sideband resolution as well as strong heating suppression in optomechanical cooling. This approach, amenable to a wide range of systems, opens up possibilities for using hybrid frequency-dependent reflectors in cavity quantum electrodynamics for engineering novel forms of light-matter interactions.

Langevin Approach to Quantum Optics with Molecules.

We investigate the interaction between light and molecular systems modeled as quantum emitters coupled to a multitude of vibrational modes via a Holstein-type interaction. We follow a quantum Langevin equations approach that allows for analytical derivations of absorption and fluorescence profiles of molecules driven by classical fields or coupled to quantized optical modes. We retrieve analytical expressions for the modification of the radiative emission branching ratio in the Purcell regime and for the asymmetric cavity transmission associated with dissipative cross talk between upper and lower polaritons in the strong coupling regime. We also characterize the Förster resonance energy transfer process between donor-acceptor molecules mediated by the vacuum or by a cavity mode.

Cavity Antiresonance Spectroscopy of Dipole Coupled Subradiant Arrays.

An array of N closely spaced dipole coupled quantum emitters exhibits super- and subradiance with characteristic tailorable spatial radiation patterns. Optimizing the emitter geometry and distance with respect to the spatial profile of a near resonant optical cavity mode allows us to increase the ratio between light scattering into the cavity mode and free space emission by several orders of magnitude. This leads to distinct scaling of the collective coherent emitter-field coupling vs the free space decay as a function of the emitter number. In particular, for subradiant states, the effective cooperativity increases much faster than the typical linear ∝N scaling for independent emitters. This extraordinary collective enhancement is manifested both in the amplitude and the phase profile of narrow collective antiresonances appearing at the cavity output port in transmission spectroscopy.

Cavity-Enhanced Transport of Charge.

We theoretically investigate charge transport through electronic bands of a mesoscopic one-dimensional system, where interband transitions are coupled to a confined cavity mode, initially prepared close to its vacuum. This coupling leads to light-matter hybridization where the dressed fermionic bands interact via absorption and emission of dressed cavity photons. Using a self-consistent nonequilibrium Green's function method, we compute electronic transmissions and cavity photon spectra and demonstrate how light-matter coupling can lead to an enhancement of charge conductivity in the steady state. We find that depending on cavity loss rate, electronic bandwidth, and coupling strength, the dynamics involves either an individual or a collective response of Bloch states, and we explain how this affects the current enhancement. We show that the charge conductivity enhancement can reach orders of magnitudes under experimentally relevant conditions.

Cavity-enhanced transport of excitons.

We show that exciton-type transport in certain materials can be dramatically modified by their inclusion in an optical cavity: the modification of the electromagnetic vacuum mode structure introduced by the cavity leads to transport via delocalized polariton modes rather than through tunneling processes in the material itself. This can help overcome exponential suppression of transmission properties as a function of the system size in the case of disorder and other imperfections. We exemplify massive improvement of transmission for excitonic wave packets through a cavity, as well as enhancement of steady-state exciton currents under incoherent pumping. These results may have implications for experiments of exciton transport in disordered organic materials. We propose that the basic phenomena can be observed in quantum simulators made of Rydberg atoms, cold molecules in optical lattices, as well as in experiments with trapped ions.

Reconfigurable long-range phonon dynamics in optomechanical arrays.

We investigate periodic optomechanical arrays as reconfigurable platforms for engineering the coupling between multiple mechanical and electromagnetic modes and for exploring many-body phonon dynamics. Exploiting structural resonances in the coupling between light fields and collective motional modes of the array, we show that tunable effective long-range interactions between mechanical modes can be achieved. This paves the way towards the implementation of controlled phononic walks and heat transfer on densely connected graphs as well as the coherent transfer of excitations between distant elements of optomechanical arrays.

Hybrid architectures for terahertz molecular polaritonics.

Atoms and their different arrangements into molecules are nature's building blocks. In a regime of strong coupling, matter hybridizes with light to modify physical and chemical properties, hence creating new building blocks that can be used for avant-garde technologies. However, this regime relies on the strong confinement of the optical field, which is technically challenging to achieve, especially at terahertz frequencies in the far-infrared region. Here we demonstrate several schemes of electromagnetic field confinement aimed at facilitating the collective coupling of a localized terahertz photonic mode to molecular vibrations. We observe an enhanced vacuum Rabi splitting of 200 GHz from a hybrid cavity architecture consisting of a plasmonic metasurface, coupled to glucose, and interfaced with a planar mirror. This enhanced light-matter interaction is found to emerge from the modified intracavity field of the cavity, leading to an enhanced zero-point electric field amplitude. Our study provides key insight into the design of polaritonic platforms with organic molecules to harvest the unique properties of hybrid light-matter states.

Protected state enhanced quantum metrology with interacting two-level ensembles.

Ramsey interferometry is routinely used in quantum metrology for the most sensitive measurements of optical clock frequencies. Spontaneous decay to the electromagnetic vacuum ultimately limits the interrogation time and thus sets a lower bound to the optimal frequency sensitivity. In dense ensembles of two-level systems, the presence of collective effects such as superradiance and dipole-dipole interaction tends to decrease the sensitivity even further. We show that by a redesign of the Ramsey-pulse sequence to include different rotations of individual spins that effectively fold the collective state onto a state close to the center of the Bloch sphere, partial protection from collective decoherence is possible. This allows a significant improvement in the sensitivity limit of a clock transition detection scheme over the conventional Ramsey method for interacting systems and even for noninteracting decaying atoms.

Strong coupling and long-range collective interactions in optomechanical arrays.

We investigate the collective optomechanics of an ensemble of scatterers inside a Fabry-Pérot resonator and identify an optimized configuration where the ensemble is transmissive, in contrast to the usual reflective optomechanics approach. In this configuration, the optomechanical coupling of a specific collective mechanical mode can be several orders of magnitude larger than the single-element case, and long-range interactions can be generated between the different elements since light permeates throughout the array. This new regime should realistically allow for achieving strong single-photon optomechanical coupling with massive resonators, realizing hybrid quantum interfaces, and exploiting collective long-range interactions in arrays of atoms or mechanical oscillators.

Prospects of reinforcement learning for the simultaneous damping of many mechanical modes.

We apply adaptive feedback for the partial refrigeration of a mechanical resonator, i.e. with the aim to simultaneously cool the classical thermal motion of more than one vibrational degree of freedom. The feedback is obtained from a neural network parametrized policy trained via a reinforcement learning strategy to choose the correct sequence of actions from a finite set in order to simultaneously reduce the energy of many modes of vibration. The actions are realized either as optical modulations of the spring constants in the so-called quadratic optomechanical coupling regime or as radiation pressure induced momentum kicks in the linear coupling regime. As a proof of principle we numerically illustrate efficient simultaneous cooling of four independent modes with an overall strong reduction of the total system temperature.

Energy transfer and correlations in cavity-embedded donor-acceptor configurations.

The rate of energy transfer in donor-acceptor systems can be manipulated via the common interaction with the confined electromagnetic modes of a micro-cavity. We analyze the competition between the near-field short range dipole-dipole energy exchange processes and the cavity mediated long-range interactions in a simplified model consisting of effective two-level quantum emitters that could be relevant for molecules in experiments under cryogenic conditions. We find that free-space collective incoherent interactions, typically associated with sub- and superradiance, can modify the traditional resonant energy transfer scaling with distance. The same holds true for cavity-mediated collective incoherent interactions in a weak-coupling but strong-cooperativity regime. In the strong coupling regime, we elucidate the effect of pumping into cavity polaritons and analytically identify an optimal energy flow regime characterized by equal donor/acceptor Hopfield coefficients in the middle polariton. Finally we quantify the build-up of quantum correlations in the donor-acceptor system via the two-qubit concurrence as a measure of entanglement.

Direct observation of ultrafast many-body electron dynamics in an ultracold Rydberg gas.

Many-body correlations govern a variety of important quantum phenomena such as the emergence of superconductivity and magnetism. Understanding quantum many-body systems is thus one of the central goals of modern sciences. Here we demonstrate an experimental approach towards this goal by utilizing an ultracold Rydberg gas generated with a broadband picosecond laser pulse. We follow the ultrafast evolution of its electronic coherence by time-domain Ramsey interferometry with attosecond precision. The observed electronic coherence shows an ultrafast oscillation with a period of 1 femtosecond, whose phase shift on the attosecond timescale is consistent with many-body correlations among Rydberg atoms beyond mean-field approximations. This coherent and ultrafast many-body dynamics is actively controlled by tuning the orbital size and population of the Rydberg state, as well as the mean atomic distance. Our approach will offer a versatile platform to observe and manipulate non-equilibrium dynamics of quantum many-body systems on the ultrafast timescale.