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Quantum Electronics and Laser Science Conference

OPTICAL DETECTION AND SPECTROSCOPY OF SINGLE MOLECULES IN SOLIDS

W. E. Moerner, L. Kador

Published Apr 24, 1989• 4 citations
OpenAlex

Abstract

Optical detection and spectroscopy of single ions in vacuum confined in electromagnetic traps1 has led to novel measurements that test our understanding of quantum physics. The detection and spectroscopy of a single absorber in a solid (single-molecule detection, or SMD) would provide a useful tool for the study of local host-absorber interactions where the absorbing center is at rest, confined by the host lattice, and where the norn1al averaging over many equivalent centers is removed.

Related papers

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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

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Th. Basché, Christoph Bräuchle

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.

Berichte der Bunsengesellschaft für physikalische Chemie•Aug 1, 1996•11 citations
Optical detection and spectroscopy of single ions in vacuum confined in electromagnetic traps1 has led to novel measurements that test our understanding of quantum physics. The detection and spectroscopy of a single absorber in a solid (single-molecule detection, or SMD) would provide a useful tool for the study of local host-absorber interactions where the absorbing center is at rest, confined by the host lattice, and where the norn1al averaging over many equivalent centers is removed.
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
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.
Optical spectroscopy provides a useful tool for probing the structure and dynamics of solids. Over the years, optical methods have evolved from absorption spectroscopy to more complex methods such as spectral hole burning, photon echoes, and luminescence line narrowing. The absorption spectrum provides information about inhomogeneous broadening, while the latter approaches provide information about the systematics of the homogeneous line shape information that is often obscured by inhomogeneous broadening. When external perturbations such as strain or electric fields are applied, details of the local site can be obtained. Recently, the ultimate limit of optical spectroscopy has been attained, in which the spectral properties of individual single impurity molecules in a solid can be measured, with all ensemble averaging removed. This novel regime has provided additional, previously unobtainable, information on a highly local scale, such as the direct observation of the spectral shifting of a single molecule produced by configurational transitions of the host. It is to be expected that further surprises await us in this new frontier of single-molecule spectroscopy in solids.
Abstract Optical spectroscopy of a single impurity molecule provides the first truly local probe of host–guest interactions in doped solids. In conventional optical high‐resolution experiments with many molecules only ensemble averages of the microscopic parameters can be obtained. In the single‐molecule regime, the exquisite sensitivity of an individual dopant molecule to both the local environment and to external perturbations has been exploited in recent experiments to reveal a wealth of fascinating novel phenomena such as spectral diffusion in crystals and polymers, optical modification of a single impurity molecule (spectral hole‐burning), local field measurements at the site of a single impurity molecule, and quantum optics in a solid.
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.