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Annual Meeting Optical Society of America

Recent advances in single-molecule spectroscopy is solids: vibrational fingerprints and magnetic resonance of a single molecular spin

W.E. Moemer, A. B. Myers, P. Tchénio, J. Köhler, H. A. H. M. Disselhorst, M. C. J. M. Donckers, E. H. H. Groenen, H. Schmidt

Published Jan 1, 1993• 0 citations
Publisher

Abstract

The field of single-molecule spectroscopy in solids1 continues to expand beyond the spectral diffusion, hole-burning, Stark effect, and photon antibunching measurements reported earlier.
DOI
10.1364/oam.1993.ma.3

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Annual Meeting Optical Society of America•Jan 1, 1992•0 citations
Recent experimental and theoretical studies concerning single-molecule spectroscopy in solids are discussed. Pure quantum effects--such as photon bunching, antibunching, and spectral jumps--and more classical phenomena--such as near-field excitation, saturation, ac/dc Stark shifts, spectral diffusion, two-photon excitation, and customary spectroscopic analysis--are considered. The emphasis of this review is on physical results and their interpretation. This is preceded by a general introduction, where fundamentals of single-molecule spectroscopy are explained.
By severely reducing the number of molecules in the illuminated sample, the optical resonances of individual molecules can be resolved in a fluorescence excitation spectrum. Photon correlation and sudden jumps due to spectral diffusion confirm the attribution of the Lorentzian excitation peaks to single molecules. This new spectroscopy displays specific effects whith would be washed out in the average over many molecules. A single molecule is also a truly local probe of its environment, by means of which fundamental studies of the matrix dynamics as well as nanophysics experiments may be undertaken.
As was recently demonstrated1 by using highly efficient fluorescence excitation spcctroscopy with N.A. = 0.98 collection optics, single impurity molecules in both crystals and polymers may now be detected with single-to-noiseratios (SNRs) as high as 30 in a 1 Hz bandwidth at low temperatures. In essence, the solid may be regarded as a trap for the single molecule, which effectively quenches rotation. Our measurements include precise determination of the lifetime limited linewidth and the temperature dependence of the optical dephasing, as well as spectral diffusion (wandering in frequency space due to perturbations by lattice degrees of freedom). For the polymeric host, light-induced changes in resonant frequency of a single molecule can be produced, a process that is normally termed spectral hole-burning when large ensembles of molecules are probed. In recent studies, nonclassical light emission from a single molecule (photon antibunching) has been observed in a fashion analogous to that reported earlier for a single atom in a trap.