Strongly nonexponential time-resolved fluorescence of quantum-dot ensembles in three-dimensional photonic crystals

We observe experimentally that ensembles of quantum dots in three-dimensional (3D) photonic crystals reveal strongly nonexponential time-resolved emission. These complex emission decay curves are analyzed with a continuous distribution of decay rates. The log-normal distribution describes the decays well for all studied lattice parameters. The distribution width is identified with variations of the radiative emission rates of quantum dots with various positions and dipole orientations in the unit cell. We find a striking sixfold change of the width of the distribution by varying the lattice parameter. This interpretation qualitatively agrees with the calculations of the 3D projected local density of states. We therefore conclude that fluorescence decay of ensembles of quantum dots is highly nonexponential to an extent that is controlled by photonic crystals

Backaction in metasurface etalons

We consider the response of etalons created by a combination of a conventional mirror and a metasurface, composed of a periodic lattice of metal scatterers with a resonant response. This geometry has been used previously for perfect absorption, in so-called Salisbury screens, and for hybridization of localized plasmons with Fabry-Perot resonances. The particular aspect we address is if one can assume an environment-independent reflectivity for the metasurface when calculating the reflectivity of the composite system, as in a standard Fabry-Perot analysis, or whether the fact that the metasurface interacts with its own mirror image renormalizes its response. Using lattice sum theory, we take into account all possible retarded dipole-dipole interactions of scatterers in the metasurface amongst each other, and through the mirror. We show that while a layer-by-layer Fabry-Perot formalism captures the main qualitative features of metasurface etalons, in fact the mirror modifies both the polarizability and reflectivity of the metasurface in a fashion that is akin to Drexhage's modification of the radiative properties of a single dipole.Comment: 10 pages, 5 figure

Spontaneous radiative decay of translational levels of an atom near a dielectric surface

We study spontaneous radiative decay of translational levels of an atom in the vicinity of a semi-infinite dielectric. We systematically derive the microscopic dynamical equations for the spontaneous decay process. We calculate analytically and numerically the radiative linewidths and the spontaneous transition rates for the translational levels. The roles of the interference between the emitted and reflected fields and of the transmission into the evanescent modes are clearly identified. Our numerical calculations for the silica--cesium interaction show that the radiative linewidths of the bound excited levels with large enough but not too large vibrational quantum numbers are moderately enhanced by the emission into the evanescent modes and those for the deep bound levels are substantially reduced by the surface-induced red shift of the transition frequency

Statistical properties of spontaneous emission near a rough surface

We study the lifetime of the excited state of an atom or molecule near a plane surface with a given random surface roughness. In particular, we discuss the impact of the scattering of surface modes within the rough surface. Our study is completed by considering the lateral correlation length of the decay rate and the variance discussing its relation to the C0 correlation

Metallo-dielectric hybrid antennas for ultrastrong enhancement of spontaneous emission

We devise new optical antennas that reduce the excited-state radiative lifetimes of emitters to the order of 100 femtoseconds while maintaining quantum efficiencies of about 80% at a broadband operation. Here, we combine metallic nanoparticles with planar dielectric structures and exploit design strategies from plasmonic nanoantennas and concepts from Cavity Quantum Electrodynamics to maximize the local density of states and minimize the nonradiative losses incurred by the metallic constituents. The proposed metallo-dielectric hybrid antennas promise important impact on various fundamental and applied research fields, including photophysics, ultrafast plasmonics, bright single photon sources and Raman spectroscopy

Observation of modified radiative properties of cold atoms in vacuum near a dielectric surface

We have observed a distance-dependent absorption linewidth of cold $^{87}$Rb atoms close to a dielectric-vacuum interface. This is the first observation of modified radiative properties in vacuum near a dielectric surface. A cloud of cold atoms was created using a magneto-optical trap (MOT) and optical molasses cooling. Evanescent waves (EW) were used to observe the behavior of the atoms near the surface. We observed an increase of the absorption linewidth with up to 25% with respect to the free-space value. Approximately half the broadening can be explained by cavity-quantum electrodynamics (CQED) as an increase of the natural linewidth and inhomogeneous broadening. The remainder we attribute to local Stark shifts near the surface. By varying the characteristic EW length we have observed a distance dependence characteristic for CQED.Comment: 6 pages, 6 figures, some minor revision

Excitated state properties of 20-chloro-chlorophyll a

The excited-state and lasing properties of 20-chloro-chlorophyll a in ether solution were compared to those of chlorophyll a. Desactivation parameters and cross-sections were obtained from non-linear absorption spectroscopy in combination with a physico-mathematical methods package. The Cl substituent at C-20 (1) increases both intersystem crossing and internal conversion, (2) produces a blue-shift of the S1 absorption spectrum, and (3) leads to pronounced photochemistry