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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

Strong Light Extinction by a Single Molecule

Jaesuk Hwang, G. Wrigge, Ilja Gerhardt, Vahid Sandoghdar

Published Jun 1, 2007• 0 citations
Publisher

Abstract

In this paper direct measurements of light extinction by single molecules are reported. We use both near-field aperture tips and confocal microscopy at cryogenic temperature to tightly confine the excitation light to an area comparable to the absorption cross section of a single molecule, which results in directly observable 10% extinction of the laser beam. It is concluded that the access to both the incoherent and coherent emission of single molecules opens up a broad range of studies on the light-matter interaction of single solid state emitters.

DOI
10.1109/cleoe-iqec.2007.4386906

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In this paper direct measurements of light extinction by single molecules are reported. We use both near-field aperture tips and confocal microscopy at cryogenic temperature to tightly confine the excitation light to an area comparable to the absorption cross section of a single molecule, which results in directly observable 10% extinction of the laser beam. It is concluded that the access to both the incoherent and coherent emission of single molecules opens up a broad range of studies on the light-matter interaction of single solid state emitters.
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Simultaneous detection of single molecules by absorption and fluorescence is demonstrated using confocal microscopy at cryogenic temperature. Dynamical processes such as blinking and spectral jumping of single emitters are observed in both detection channels. The relative magnitude of fluorescence and absorption varies between molecules. In particular, we observe molecules that do not emit detectable Stokes-shifted fluorescence but show a strong absorption signal. The fact that coherent resonant scattering underlies the absorption process is demonstrated by a correlation between small linewidth and large absorption amplitude.
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 built an interferometer where one of the two slits of a classical Young's setup is replaced by a single molecule embedded in a solid matrix. This enabled direct measurement of the first order coherence of the 0-0 single-molecule emission, which at high excitation powers proves to be split in coherent and incoherent parts. We demonstrate an order of magnitude higher precision in axial localization of single molecules in comparison with that of confocal microscopy. These experiments open a possibility for single-molecule holography. Detection of single molecules with low luminescence quantum yields could be another application of this technique.
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