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High Resolution Spectroscopy

High Resolution Spectroscopy on Single Molecules

Jerzy Sepioł, Frank Güttler, Marco Pirotta, Alois Renn, Urs P. Wild

Published Jan 1, 1993• 0 citations
Publisher

Abstract

Single particle spectroscopy has become a source of valuable information on fundamental interactions between light and matter. Whereas trapping and cooling of ions and atoms has been sucessfully achieved, single molecules, because of their multilevel structure (high number of internal degrees of freedom) have not been observed in electromagnetic traps so far. However due to the presence of zero phonon lines in conjunction with inhomogeneous broadening the spectroscopic isolation and detection of single molecules ‘trapped in solids at very low temperatures' is made feasible [1,2]. Single molecule spectroscopy allows to study the distribution of molecular properties and not only the statistical average which is generally observed.

DOI
10.1364/hrs.1993.wa5

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Single particle spectroscopy has become a source of valuable information on fundamental interactions between light and matter. Whereas trapping and cooling of ions and atoms has been sucessfully achieved, single molecules, because of their multilevel structure (high number of internal degrees of freedom) have not been observed in electromagnetic traps so far. However due to the presence of zero phonon lines in conjunction with inhomogeneous broadening the spectroscopic isolation and detection of single molecules ‘trapped in solids at very low temperatures' is made feasible [1,2]. Single molecule spectroscopy allows to study the distribution of molecular properties and not only the statistical average which is generally observed.
Single-particle spectroscopy has become a source of valuable information on fundamental interactions between light and mat- ter. Whereas trapping and cooling of ions and atoms has been successfully achieved, single molecules, because of their multilevel structure (high number of internal degrees of freedom) have not to date been observed in electromagnetic traps. However, because of the presence of zero phonon lines in conjunction with inhomogeneous broadening, the spectroscopic isolation and detection of single molecules trapped in solids at very low temperatures has been made feasible.1,2 Single-molecule spectroscopy permits the study of the distribution of molecular properties in addition to the statistical average that is generally observed.
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.
Recent advances in absorption1 and fluorescence2 detection now allow high-quality measurement of the optical absorption spectrum of individual single-impurity molecules in both crystals and polymers at liquid-helium temperatures. Here, the solid may be viewed as a trap for the defect center similar to the well-known electromagnetic single-ion traps, except that Doppler and recoil effects are replaced by (static) inhomogeneous broadening and host-guest interactions. Most importantly, molecular rotation is absent because of steric effects at low temperatures.