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Molecular crystals and liquid crystals science technology. Section A, Molecular crystals and liquid crystals/Molecular crystals and liquid crystals science and technology. Section A, Molecular crystals and liquid crystals

Spectral Hole Burning in the Single-Molecule and Few-Molecule Limit: Terrylene in p−Terphenyl

L. Kador, Andreas Müller

Published May 1, 1998• 2 citations
Publisher

Abstract

Persistent hole burning is possible in the inhomogeneous absorption bands X1 and X3 of the system terrylene in p−terphenyl. Whereas the holes are stable in X1, they decay with a time constant of a few seconds in X3. In crystals with very low dye concentration, shallow holes can be observed which consist of few (or even one single) molecular lines and can be distinctly narrower than twice the homogeneous linewidth. Monte Carlo simulations confirm the experimental findings.

DOI
10.1080/10587259808042471

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Molecular crystals and liquid crystals science technology. Section A, Molecular crystals and liquid crystals/Molecular crystals and liquid crystals science and technology. Section A, Molecular crystals and liquid crystals•Dec 1, 1996•4 citations
Persistent hole burning is possible in the inhomogeneous absorption bands X1 and X3 of the system terrylene in p−terphenyl. Whereas the holes are stable in X1, they decay with a time constant of a few seconds in X3. In crystals with very low dye concentration, shallow holes can be observed which consist of few (or even one single) molecular lines and can be distinctly narrower than twice the homogeneous linewidth. Monte Carlo simulations confirm the experimental findings.
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.
So far, persistent spectral hole-burning (PSHB) phenomenon has been observed in a number of materials. They are molecules in glasses, crystals and polymers, color centers in alkali halide crystals, and rare earth and transition metal ions in glasses and crystals. They are molecular or ionic guests embedded in glass, crystal or polymer hosts. Basic requirements for the PSHB are summarized as follows: (1) The optical absorption of guests embedded in hosts must be broadened inhomogeneously. (2) There must exist more than one ground state configurations of the total system consisting of guests and hosts. (3) The relaxation among the ground states must be slower than the decay rate of any excited state. In fact, this set of requirements is satisfied in many kinds of molecular or ionic guests in hosts, such as glasses, crystals and polymers, at low temperatures. We can naturally understand that guests consisting of small number of atoms are greatly influenced by the surrounding hosts and that the energy levels of the guests are inhomogeneously broadened.
At very low temperatures, the spread in the different environments of matrix embedded dye molecules results in an inhomogeneously broadened S1 ← S0 band. Spectroscopic techniques based on the appearence of optical zero phonon lines, such as fluorescence line narrowing, spectral hole-burning, and single molecule spectroscopy provide an experimental resolution limited by the homogeneous linewidth. From the investigation of the homogeneous line width as a function of different parameters (time, temperature) information on the guest host interactions responsible for the observed linewidth is obtained. Spectrally narrow features are extremely sensitive probes for external perturbations, such as electric fields, magnetic fields, or hydrostatic pressure.
Spectral hole-burning in the Shpol'skii system terrylene in n-octane has been investigated on the single molecule level. Fluorescence microscopy provides a link between the two methods of spectral hole-burning and single molecule spectroscopy. Information about many different individual molecules can be obtained simultaneously under identical experimental conditions allowing the determination of statistical properties. From a single frequency scan after spectral hole-burning, the ground state population function and an average hole-width, as well as the single molecule linewidth distribution of 700 molecules have been determined.