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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Excitation spectroscopy on single molecules in solids at low temperatures

L. Fleury, H. Talon, J. Bernard, Michel Orrit

Published Sep 24, 1993• 0 citations
Publisher

Abstract

By severely reducing the number of solute molecules in the illuminated sample, the optical resonances of individual molecules can be resolved in a fluorescence excitation spectrum. Single molecule lines can be studied as a function of time and temperature: sudden jumps of their resonance frequencies are due to spectral diffusion processes. The signal from a single molecule displays specific correlations which makes time-resolved studies possible. Here, emphasis is put on photon-bunching arising from intersystem crossing (ISC). ISC rates are deduced from the observed decay rates of the correlation and are found to differ from molecule to molecule. A single molecule is 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.

DOI
10.1117/12.155640

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By severely reducing the number of solute molecules in the illuminated sample, the optical resonances of individual molecules can be resolved in a fluorescence excitation spectrum. Single molecule lines can be studied as a function of time and temperature: sudden jumps of their resonance frequencies are due to spectral diffusion processes. The signal from a single molecule displays specific correlations which makes time-resolved studies possible. Here, emphasis is put on photon-bunching arising from intersystem crossing (ISC). ISC rates are deduced from the observed decay rates of the correlation and are found to differ from molecule to molecule. A single molecule is 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.
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.
Fluorescence photons emitted by a single molecule trapped in a solid at low temperature are correlated in time. A simple theory of the correlation pattern is presented, including in the same formalism photon antibunching from coherent Rabi oscillations and photon bunching due to incoherent quantum transitions between electronic levels. The correlation method is applied to single pentacene molecules in a para-terphenyl crystal. A clear photon bunching allows us to determine the ISC rates for each molecule. We attribute the scatter of our results for the transition rate between excited singlet and triplet states, and the difference with the average value taken from the literature, to molecular distortions induced by crystal defects in our small sample. We conclude that the correlation method associated to single molecule spectroscopy has a great potential to study dynamical processes on intermediate time scales in condensed matter.
Optical spectroscopy of single impurity molecules in low-temperature solids provides an exquisitely sensitive probe of the structure and dynamics of the specific local environment around the single molecule, unobscured by ensemble averaging. Effects such as spectral diffusion, perturbations by external fields, changes in molecular photophysics, optical switching, dynamics due to amorphous system physics, magnetic resonance of a single molecular spin, and perturbations due to nearby charge transport have all been observed. Because properly chosen single molecules act as two- and three-level quantum systems, a variety of quantum optical effects may be observed, such as photon antibunching, optical Stark effect, and single-photon emission on command. When they carry spin in their ground and excited states, single molecules and other nano-objects open many more experiments in quantum optics and nanophysics, because they are sensitive to magnetic interactions and can serve as readouts for spin systems with long coherence times. As a new class of nanoscale experiments, the ability to optically pump and probe single 2–3-nm-sized molecules in complex systems provides a new window into the local dynamics and heterogeneity of solids.
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
Abstract In recent years different microscopic and spectroscopic techniques were successfully employed to detect the fluorescence signals of single dye molecules in the condensed phase. In low temperature solids the fluorescence excitation line of a single dopant molecule is a high resolution optical probe of its local nanoenvironment. As inhomogeneous contributions and ensemble averaging are absent, many effects hidden when looking at large populations of molecules become observable. Two important research areas in single molecule spectroscopy deal with the investigation of quantum optical effects and the spectral jumping behaviour of single molecule excitation lines caused by fluctuations of two‐level systems inherent to disordered solids. Rather than delivering a complete presentation, we will focus on some selected examples which emphasize the unique features of spectroscopy with a single absorber.
Optical spectroscopy of single impurity molecules in solids can be used as an exquisitely sensitive probe of the structure and dynamics of the specific local environment around the single molecule (the “nanoenvironment”. Some phenomena that have been studied are the spectral diffusion dynamics of a single molecule, perturbations by external fields, changes in molecular photophysics, shifts in vibrational modes, optical modification of the absorption spectrum, dynamics due to amorphous system physics, and magnetic resonance of a single molecular spin. This demonstrates the vitality of and growing interest in this new field, which may in the future lead to optical storage on the single‐molecule level.