Subradiant states in a finite chain of two-level quantum emitters coupled to a one-dimensional reservoir are a resource for superior photon storage and their controlled release. As one can maximally store one energy quantum per emitter, storing multiple excitations requires delocalized states, which typically exhibit fermionic correlations and antisymmetric wave functions, thus making them hard to access experimentally. Here we identify a new class of quasilocalized dark states with up to half of the qubits excited, which only appear for lattice constants of an integer multiple of the wavelength. These states allow for a high-fidelity preparation and minimally invasive readout in state-of-the-art setups. In particular, we suggest an experimental implementation using a coplanar waveguide coupled to superconducting transmon qubits on a chip. With minimal free space and intrinsic losses, virtually perfect dark states can be achieved for a low number of qubits featuring fast preparation and precise manipulation.
A laser is composed of an optical resonator and a gain medium. When stimulated emission dominates mirror losses, the emitted light becomes coherent. We propose a new class of coherent light sources based on wavelength sized regular structures of quantum emitters whose eigenmodes form high- resonators. Incoherent pumping of few atoms induces light emission with spatial and temporal coherence. We show that an atomic nanoring with a single gain atom at the center behaves like a thresholdless laser, featuring a narrow linewidth. Symmetric subradiant excitations provide optimal operating conditions.
Regular arrays of two-level emitters at distances smaller than that of the transition wavelength collectively scatter, absorb, and emit photons. The strong inter-particle dipole coupling creates large energy shifts of the collective delocalized excitations, which generates a highly nonlinear response at the single and few photon level. This should allow us to implement nanoscale non-classical light sources via weak coherent illumination. At the generic tailored examples of regular chains or polygons, we show that the fields emitted perpendicular to the illumination direction exhibit a strong directional confinement with genuine quantum properties as antibunching. For short interparticle distances, superradiant directional emission can enhance the radiated intensity by an order of magnitude compared to a single atom focused to a strongly confined solid angle but still keeping the anti-bunching parameter at the level of .
Efficient transport and harvesting of excitation energy under low light conditions is an important process in nature and quantum technologies alike. Here we formulate a quantum optics perspective to excitation energy transport in configurations of two-level quantum emitters with a particular emphasis on efficiency and robustness against disorder. We study a periodic geometry of emitter rings with subwavelength spacing, where collective electronic states emerge due to near-field dipole–dipole interactions. The system gives rise to collective subradiant states that are particularly suited to excitation transport and are protected from energy disorder and radiative decoherence. Comparing ring geometries with other configurations shows that the former are more efficient in absorbing, transporting, and trapping incident light. Because our findings are agnostic as to the specific choice of quantum emitters, they indicate general design principles for quantum technologies with superior photon transport properties and may elucidate potential mechanisms resulting in the highly efficient energy transport efficiencies in natural light-harvesting systems.
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.
3 April 2024 in The Journal of Physical Chemistry A
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.