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Quantum Electronics and Laser Science Conference

A solid as a single-molecule trap: observation of spectral diffusion and hole-burning on the single-center level

W. E. Moerner, Th. Basché, W. Patrick Ambrose

Published May 10, 1992• 0 citations
OpenAlex

Abstract

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.

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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.

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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.
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.
Recent advances in the optical detection and spectroscopy of single impurity centers in crystals has provided the possibility of obtaining information about defect-solid interactions on a truly local level. For the system composed of pentacene impurity molecules in the crystal p-terphenyl, single molecules have been studied using both absorption1 and fluorescence excitation2 techniques at liquid helium temperatures. The superior signal-to-noise of the latter technique has led to direct observations of the lifetime-limited Lorentzian homogeneous profile of a single pentacene impurity3 as well as the surprising observation of spontaneous spectral diffusion4. Spectral diffusion, or changes in the resonance frequency of an impurity molecule with time as a result of low-energy excitations (two-level system transitions (TLS)),5 is generally expected in amorphous hosts. Indeed, the presence of TLSs in amorphous solids is intimately connected with nonphotochemical mechanisms for persistent spectral hole-burning (PSHB) in amorphous materials6-8. Using perylene impurity molecules in poly(ethylene), we have observed the optical spectra of single molecules in a polymeric host for the first time. At 1.5K, individual perylene molecules show the expected spectral diffusion; moreover, we observe light-induced changes in resonance frequency, i.e., persistent spectral hole-burning, which allows one to envision optical storage on the single-molecule level.
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.
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.
Single-molecule detection and spectroscopy in solids has the potential for direct observation of the microscopic physics and chemistry of defects without multicenter averaging. Initial observations of the optical absorption spectra of a single pentacene molecule in p-terphenyl crystals achieved signal-to-noise ratios (SNR's) of 3-5 in a 1-Hz bandwidth and required intensities at the sample above the saturation intensity. Careful noise analysis of our detectors showed that little improvement in SNR could be expected with an absorption technique unless simple and reliable sources of squeezed light were available. Recent advances in fluorescence- excitation spectroscopy have removed this SNR limitation.3
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.