Search

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, under external magnetic field control, stacked layers of quantum metasurfaces 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., Comment: 6+11 pages, 2+3 figures

We study the photophysics of molecular aggregates from a quantum optics perspective, with emphasis on deriving scaling laws for the fast non-radiative 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. Photo-excitation 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 non-radiative relaxation via intramolecular vibrational modes populates lower energy, subradiant states, resulting in an 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 neighbouring monomers.

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., Comment: 12 pages main text + 4 Appendix, 8 figures

Dipole-coupled subwavelength quantum emitter arrays respond cooperatively to external light fields as they may host collective delocalized excitations (a form of excitons) with super- or subradiant character. Deeply subwavelength separations typically occur in molecular ensembles, where in addition to photon-electron interactions, electron-vibron couplings and vibrational relaxation processes play an important role. We provide analytical and numerical results on the modification of super- and subradiance in molecular rings of dipoles including excitations of the vibrational degrees of freedom. While vibrations are typically considered detrimental to coherent dynamics, we show that molecular dimers or rings can be operated as platforms for the preparation of long-lived dark superposition states aided by vibrational relaxation. In closed ring configurations, we extend previous predictions for the generation of coherent light from ideal quantum emitters to molecular emitters, quantifying the role of vibronic coupling onto the output intensity and coherence., Comment: 16 pages, 8 figures

Quantum cooperativity is evident in light-matter platforms where quantum emitter ensembles are interfaced with confined optical modes and are coupled via the ubiquitous electromagnetic quantum vacuum. Cooperative effects can find applications, among other areas, in topological quantum optics, in quantum metrology or in quantum information. This tutorial provides a set of theoretical tools to tackle the behavior responsible for the onset of cooperativity by extending open quantum system dynamics methods, such as the master equation and quantum Langevin equations, to electron-photon interactions in strongly coupled and correlated quantum emitter ensembles. The methods are illustrated on a wide range of current research topics such as the design of nanoscale coherent light sources, highly-reflective quantum metasurfaces or low intracavity power superradiant lasers. The analytical approaches are developed for ensembles of identical two-level quantum emitters and then extended to more complex systems where frequency disorder or vibronic couplings are taken into account. The relevance of the approach ranges from atoms in optical lattices to quantum dots or molecular systems in solid-state environments., Comment: 43 pages, 18 figures; revised version; contains some additional material w.r.t. published version

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 equations 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 as well as 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., Comment: [v4]: minor updates to published version

We study the dependence of the vacuum Rabi splitting (VRS) on frequency disorder, vibrations, near-field effects and density in molecular polaritonics. In the mesoscopic limit, static frequency disorder alone can already introduce a loss mechanism from polaritonic states into a dark state reservoir, which we quantitatively describe, providing an analytical scaling of the VRS with the level of disorder. Disorder additionally can split a molecular ensemble into donor-type and acceptor-type molecules and the combination of vibronic coupling, dipole-dipole interactions and vibrational relaxation induces an incoherent FRET (F\"{o}rster resonance energy transfer) migration of excitations within the collective molecular state. This is equivalent to a dissipative disorder and has the effect of saturating and even reducing the VRS in the mesoscopic, high-density limit. Overall, this analysis allows to quantify the crucial role played by dark states in cavity quantum electrodynamics with mesoscopic, disordered ensembles.

Molecules constitute compact hybrid quantum optical systems that can interface photons, electronic degrees of freedom, localized mechanical vibrations and phonons. In particular, the strong vibronic interaction between electrons and nuclear motion in a molecule resembles the optomechanical radiation pressure Hamiltonian. While molecular vibrations are often in the ground state even at elevated temperatures, one still needs to get a handle on decoherence channels associated with phonons before an efficient quantum optical network based on opto-vibrational interactions in solid-state molecular systems could be realized. As a step towards a better understanding of decoherence in phononic environments, we take here an open quantum system approach to the non-equilibrium dynamics of guest molecules embedded in a crystal, identifying regimes of Markovian versus non-Markovian vibrational relaxation. A stochastic treatment based on quantum Langevin equations predicts collective vibron-vibron dynamics that resembles processes of sub- and superradiance for radiative transitions. This in turn leads to the possibility of decoupling intramolecular vibrations from the phononic bath, allowing for enhanced coherence times of collective vibrations. For molecular polaritonics in strongly confined geometries, we also show that the imprint of opto-vibrational couplings onto the emerging output field results in effective polariton cross-talk rates for finite bath occupancies., Comment: [v2]: revised abstract and introduction, [v3]: corrected rotating frame in Eqs. (31)

We study the interplay between charge transport and light-matter interactions in a confined geometry, by considering an open, mesoscopic chain of two-orbital systems resonantly coupled to a single bosonic mode close to its vacuum state. We introduce and benchmark different methods based on self-consistent solutions of non-equilibrium Green's functions and numerical simulations of the quantum master equation, and derive both analytical and numerical results. It is shown that in the dissipative regime where the cavity photon decay rate is the largest parameter, the light-matter coupling is responsible for a steady-state current enhancement scaling with the cooperativity parameter. We further identify different regimes of interest depending on the ratio between the cavity decay rate and the electronic bandwidth. Considering the situation where the lower band has a vanishing bandwidth, we show that for a high-finesse cavity, the properties of the resonant Bloch state in the upper band are transfered to the lower one, giving rise to a delocalized state along the chain. Conversely, in the dissipative regime with low cavity quality factors, we find that the current enhancement is due to a collective decay of populations from the upper to the lower band., Comment: 52 pages, 11 figures

We theoretically investigate charge transport through electronic bands of a mesoscopic one-dimensional system, where inter-band 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 non-equilibrium 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 explain how this affects the current enhancement. We show that the charge conductivity enhancement can reach orders of magnitudes under experimentally relevant conditions.

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., Comment: 10 pages, 7 figures, [v2]: Updated reference to complementary work arXiv:1409.2514, [v3]: Update to version accepted for publication

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., Comment: 11 pages, 7 figures

This book chapter reports on theoretical protocols for generating nonclassical states of light and mechanics. Nonclassical states are understood as squeezed states, entangled states or states with negative Wigner function, and the nonclassicality can refer either to light, to mechanics, or to both, light and mechanics. In all protocols nonclassicallity arises from a strong optomechanical coupling. Some protocols rely in addition on homodyne detection or photon counting of light., Comment: 31 page review paper; to be pulished as a chapter in the forthcoming Springer textbook "Cavity Optomechanics", edited by M. Aspelmeyer, T. Kippenberg, and F. Marquardt. Comments are welcome!

We discuss hybrid systems in which a mechanical oscillator is coupled to another (microscopic) quantum system, such as trapped atoms or ions, solid-state spin qubits, or superconducting devices. We summarize and compare different coupling schemes and describe first experimental implementations. Hybrid mechanical systems enable new approaches to quantum control of mechanical objects, precision sensing, and quantum information processing., Comment: To cite this review, please refer to the published book chapter (see Journal-ref and DOI). This v2 corresponds to the published version

We investigate the collective optomechanics of an ensemble of scatterers inside a Fabry-Perot resonator and identify an optimized configuration where the ensemble is transmissive, in contrast with 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., Comment: 11 pages, 12 figures

We provide a general framework to describe cooling of a micromechanical oscillator to its quantum ground state by means of radiation-pressure coupling with a driven optical cavity. We apply it to two experimentally realized schemes, back-action cooling via a detuned cavity and cold-damping quantum-feedback cooling, and we determine the ultimate quantum limits of both schemes for the full parameter range of a stable cavity. While both allow to reach the oscillator's quantum ground state, we find that back-action cooling is more efficient in the good cavity limit, i.e. when the cavity bandwidth is smaller than the mechanical frequency, while cold damping is more suitable for the bad cavity limit. The results of previous treatments are recovered as limiting cases of specific parameter regimes., Comment: 10 pages, 4 figures. Erratum of the published version included