Nanosecond Dynamics of Single-Molecule Fluorescence Resonance Energy Transfer

光子泵浦、光解离与耗散在腔中分子荧光中的相互作用

Photon pumping, photodissociation and dissipation at interplay for the fluorescence of a molecule in a cavity

本文提出光学腔中双原子分子的精确模型，同等处理电子与核运动，涵盖莫洛谱、谐波产生与解离竞争及荧光对泵浦和耗散的依赖，为相关实验提供通用模板。

IDTBT单分子荧光的频率和时间分辨二级量子相干函数

Frequency- and time-resolved second order quantum coherence function of IDTBT single-molecule fluorescence

本研究开发了一种单分子荧光量子光谱学技术，用于研究IDTBT单分子的量子相干特性，揭示其激发态动力学和量子相干性。

Entangled-Photon Coincidence Fluorescence Imaging

We extend entangled coincidence (ghost) imaging to fluorescent samples. Given the entangled photon correlation, one photon of the pair carries information on where the other photon has been absorbed and has produced fluorescence in a sample. Fluorescent molecules serve as ''detectors breaking'' the entanglement.

Fast recognition of single molecules based on single event photon statistics

Mandel Q-parameter, which is determined from single event photon statistics, provides an alternative to differentiate single-molecule with fluorescence detection. In this work, by using the Q-parameter of the sample fluorescence compared to that of an ideal double-molecule system with the same average photon number, we present a novel and fast approach for identifying single molecules based on single event photon statistics analyses, compared with commonly used two-time correlation measurements. The error estimates for critical values of photon statistics are also presented for single-molecule…

Spontaneous emission enhancement of a single molecule by a double-sphere nanoantenna across an interface

We report on two orders of magnitude reduction in the fluorescence lifetime when a single molecule placed in a thin film is surrounded by two gold nanospheres across the film interface. By attaching one of the gold particles to the end of a glass fiber tip, we could control the modification of the molecular fluorescence at will. We find a good agreement between our experimental data and the outcome of numerical calculations.

Radiative and non-radiative photokinetics alteration inside a single metallic nanometric aperture

We resolve the photokinetic rates enhancement of Rhodamine 6G molecules diffusing in a water-glycerol mixture within a single nanometric aperture milled in an opaque aluminium film. Combining fluorescence correlation spectroscopy and lifetime measurements, we report the relative influence of excitation, radiative and non-radiative decay in the fluorescence process, giving a detailed description of the physics behind the overall 15 fold enhancement of the average fluorescence rate per molecule. This procedure is broadly adaptable to a wide range of nanostructures.

Coherent Interaction of Light and Single Molecules in a Dielectric Nanoguide

We present a new scheme for performing optical spectroscopy on single molecules. A glass capillary with a diameter of 600 nm filled with an organic crystal tightly guides the excitation light and provides a maximum spontaneous emission coupling factor ($β$) of 18% for the dye molecules doped in the organic crystal. Combination of extinction, fluorescence excitation and resonance fluorescence spectroscopy with microscopy provides high-resolution spatio-spectral access to a very large number of single molecules in a linear geometry. We discuss strategies for exploring a range of quantum optical …

Making the best of mixed-field orientation of polar molecules: A recipe for achieving adiabatic dynamics in an electrostatic field combined with laser pulses

We have experimentally and theoretically investigated the mixed-field orientation of rotational-state-selected OCS molecules and we achieve strong degrees of alignment and orientation. The applied moderately intense nanosecond laser pulses are long enough to adiabatically align molecules. However, in combination with a weak dc electric field, the same laser pulses result in nonadiabatic dynamics in the mixed-field orientation. These observations are fully explained by calculations employing, both, adiabatic and non-adiabatic time-dependent models.

Exciton-spin memory with a semiconductor quantum dot molecule

We report on a single photon and spin storage device based on a semiconductor quantum dot molecule. Optically excited single electron-hole pairs are trapped within the molecule and their recombination rate is electrically controlled over three orders of magnitude. Single photons are stored up to 1 microsecond and read out on a sub-nanosecond timescale. Using resonant excitation, the circular polarisation of individual photons is transferred into the spin state of electron-hole pairs with a fidelity above 80%, which does not degrade for storage times up to the 12.5ns repetition period of the ex…

Efficiently tunable photon emission from an optically driven artificial molecule

In this work, we investigate the emission properties of double quantum dot driven by a monochromatic electromagnetic field, while undergoing resonant tunneling and dissipation by phonons. We found emission spectra for both cases, with and without phonons, whose comparison allows to determine the dissipative effects. On the basis of the obtained results we propose efficient control of the resonance fluorescence of an artificial molecule, suitable for optoelectronic applications.