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Chemical Physics Letters

Persistent spectral hole burning in the few-molecule limit: terrylene in p-terphenyl

A. Müller, W. Richter, L. Kador

Published Mar 1, 1998• 9 citations
Publisher
DOI
10.1016/s0009-2614(98)00007-4

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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.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1991•0 citations
Fluorescence excitation spectra of single terrylene molecules in p-terphenyl crystals were investigated at low temperatures. The line shifts due to hydrostatic pressure and external electric fields were measured, with the electric field strength oriented either parallel or perpendicular to the k vector of the laser light. A linear Stark effect was found for most molecules, indicating local environments of low symmetry. In sites X1 and X3 (and XY, a photoproduct state), spectral hole burning was observed. Whereas the holes are stable in sites X1 and XY, they decay with a time constant of some minutes in X3. Pressure experiments were performed on the stable hole spectra in sites X1 and XY. In weakly doped samples, holes composed of very few molecular lines were generated with halfwidths distinctly narrower than twice the homogeneous linewidth.
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.