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

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

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

Measuring the quantum efficiency of single radiating dipoles using a scanning mirror

Using scanning probe techniques, we show the controlled manipulation of the radiation from single dipoles. In one experiment we study the modification of the fluorescence lifetime of a single molecular dipole in front of a movable silver mirror. A second experiment demonstrates the changing plasmon spectrum of a gold nanoparticle in front of a dielectric mirror. Comparison of our data with theoretical models allows determination of the quantum efficiency of each radiating dipole.Comment: 4 pages, 4 figure

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

Strongly Coupled Matter-Field and Non-Analytic Decay Rate of Dipole Molecules in a Waveguide

The decay rate \gam of an excited dipole molecule inside a waveguide is evaluated for the strongly coupled matter-field case near a cutoff frequency \ome_c without using perturbation analysis. Due to the singularity in the density of photon states at the cutoff frequency, we find that \gam depends non-analytically on the coupling constant $\ggg$ as $\ggg^{4/3}$. In contrast to the ordinary evaluation of \gam which relies on the Fermi golden rule (itself based on perturbation analysis), \gam has an upper bound and does not diverge at \ome_c even if we assume perfect conductance in the waveguide walls. As a result, again in contrast to the statement found in the literature, the speed of emitted light from the molecule does not vanish at \ome_c and is proportional to $c\ggg^{2/3}$ which is on the order of $10^3 \sim 10^4$ m/s for typical dipole molecules.Comment: 4 pages, 2 figure

Photonic mode density effects on single-molecule fluorescence blinking

We investigated the influence of the photonic mode density (PMD) on the triplet dynamics of individual chromophores on a dielectric interface by comparing their response in the presence and absence of a nearby gold film. Lifetimes of the excited singlet state were evaluated in ordet to measure directly the PMD at the molecules position. Triplet state lifetimes were simultaneously determined by statistical analysis of the detection time of the fluorescence photons. The observed singlet decay rates are in agreement with the predicted PMD for molecules with different orientations. The triplet decay rate is modified in a fashion correlated to the singlet decay rate. These results show that PMD engineering can lead to an important suppression of the fluorescence, introducing a novel aspect of the physical mechanism to enhance fluorescence intensity in PMD-enhancing systems such as plasmonic devices

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

Size-Dependence of the Wavefunction of Self-Assembled Quantum Dots

The radiative and non-radiative decay rates of InAs quantum dots are measured by controlling the local density of optical states near an interface. From time-resolved measurements we extract the oscillator strength and the quantum efficiency and their dependence on emission energy. From our results and a theoretical model we determine the striking dependence of the overlap of the electron and hole wavefunctions on the quantum dot size. We conclude that the optical quality is best for large quantum dots, which is important in order to optimally tailor quantum dot emitters for, e.g., quantum electrodynamics experiments.Comment: 5 pages, 3 figure