Single fluorescent molecules provide useful nanometer-sized absorbers and sources of light, which enable superresolution imaging, trapping, and nanometer-scale probing of optical fields in nanophotonic structures. Fundamentals of these effects will be described.
Experiments with single quantum systems are at the frontier of modern physics. Probing single molecules allows for very precise control of light-matter interaction and for quantum optical studies. Moreover, a single guest molecule in a solid host matrix is a very sensitive probe of local dynamics in its nano-environment. Fluorescence excitation spectroscopy on single molecules is a powerful tool for spectroscopic characterizations at highest resolution, as information can be revealed that is not accessible in experiments on ensembles of molecules. The detection of the fluorescence signal of a single absorber is achieved by exploiting the high spectral selectivity given by the ratio (10 10) of homogeneous to inhomogeneous linewidths of optical transitions at cryogenic temperatures (zero-phonon transitions). Two-photon fluorescence excitation, a fundamental nonlinear optical process, was observed on a single quantum system [1]. Single diphenyl-octatetraene molecules trapped in an n-tetradecane matrix were excited from the 1Ag ground to the lowest excited singlet state by simultaneous absorption of two photons using a single-mode cw laser. Excited molecules were observed through weak one-photon emission resulting from a symmetry breaking induced by the crystal field. The fundamental principles and the experimental technique of single molecule spectroscopy will be introduced briefly and some particular single molecule experiments presented. This work was done in collaboration with T. Plakhotnik, A. Renn and U.P. Wild
The advent of single molecule optics has had a profound impact in fields ranging from biophysics to material science, photophysics, and quantum optics. However, all existing room-temperature single molecule methods have been based on fluorescence detection of highly efficient emitters. Here we demonstrate that standard, modulation-free measurements known from conventional absorption spectrometers can indeed detect single molecules. We report on quantitative measurements of the absorption cross section of single molecules under ambient condition even in their dark state, for example during photoblinking or strong quenching. Our work extends single-molecule microscopy and spectroscopy to a huge class of materials that absorb light but do not fluoresce efficiently.
We propose a novel, to the best of our knowledge, approach to superresolution optical imaging by combining quantum optics and near-field optics. Our concept involves the utilization of single-photon quantum emitters to generate a standalone evanescent wave. We demonstrate that the quantum interference effects of single-photon emitters, in conjunction with their near-field, result in a higher resolution of subwavelength structures than systems that are only quantum enhanced or only near-field enhanced. We believe that nano-sized emitters could be employed to accomplish the goals of this research, taking into account the current progress in nanophotonics and quantum optics technology.
Single particle-resolved fluorescence imaging is an enabling technology in cold-atom physics. However, so far, this technique has not been available for nanophotonic atom-light interfaces. Here, we image single atoms that are trapped and optically interfaced using an optical nanofiber. Near-resonant light is scattered off the atoms and imaged while counteracting heating mechanisms via degenerate Raman cooling. We detect trapped atoms within 150 ms and record image sequences of given atoms. Building on our technique, we perform two experiments which are conditioned on the number and position of the nanofiber-trapped atoms. We measure the transmission of nanofiber-guided resonant light and verify its exponential scaling in the few-atom limit, in accordance with Beer-Lambert's law. Moreover, depending on the interatomic distance, we observe interference of the fields that two simultaneously trapped atoms emit into the nanofiber. The demonstrated technique enables postselection and possible feedback schemes and thereby opens the road toward a new generation of experiments in quantum nanophotonics.