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The Journal of Physical Chemistry

Saturation of Depth and Polarization of Resonant and Satellite Spectral Holes Generated with Pulsed Laser Excitation

Wolfgang Drescher, Bernhard Dick

Published Mar 1, 1994• 3 citations
Publisher

Abstract

The authors consider photochem. hole burning of an inhomogeneous and isotropic ensemble of chromophores through excitation with a narrow-bandwidth source of polarized light. The authors derive expressions for the depth and anisotropy of resonant and vibronic satellite spectral holes with increasing fluence. A fit of these satn. curves to exptl. data yields the Debye-Waller factor of the system. A simple rate equation model predicts that the anisotropy of a spectral hole depends only on the angle between the transition dipoles of the burnt and the probed transitions. In expts. with pulsed lasers strong deviations from this ideal behavior are obsd. An extended theory including satn. gives a satisfactory description of this phenomenon and provides a new method for the detn. of photochem. quantum yields.

DOI
10.1021/j100062a028

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The authors consider photochem. hole burning of an inhomogeneous and isotropic ensemble of chromophores through excitation with a narrow-bandwidth source of polarized light. The authors derive expressions for the depth and anisotropy of resonant and vibronic satellite spectral holes with increasing fluence. A fit of these satn. curves to exptl. data yields the Debye-Waller factor of the system. A simple rate equation model predicts that the anisotropy of a spectral hole depends only on the angle between the transition dipoles of the burnt and the probed transitions. In expts. with pulsed lasers strong deviations from this ideal behavior are obsd. An extended theory including satn. gives a satisfactory description of this phenomenon and provides a new method for the detn. of photochem. quantum yields.
Abstract A two‐step spectral hole burning (SHB) is considered, where the selective excitation of the first step is fixed by a photochemical transformation through the second excitation step. It is shown that in a three‐level system excited by two consecutive pulses, the kinetics of the forming spectral hole differs essentially from the one on stationary irradiation. In the case of a short second pulse the shape of the hole in the inhomogeneous distribution function (IDF) of the purely electronic line frequency Ω01 is dependent on the time interval T between the first and second excitation steps and under certain conditions a hole can be obtained which is narrower than in the one‐step SHB with monochromatic light. It is considered how the hole in IDF is manifested in the absorption and two‐step pulse excitation spectra. It is shown that the hole in the absorption spectrum may be narrower than 2γ1 and in the two‐step pulse excitation, −γ1 (γ1 is the energy relaxation constant of the first excited level).
Photochemical hole burning (PHB) is a topic of attracting increasing interest from spectroscopic viewpoints as well as from the practical prospects for ultra-high-density frequency-domain optical storage. Recent advances in PHB study are reviewed mainly focusing on the effects of chemical structure of guest ions and molecules as well as host matrices on the efficiency of hole formation and its temperature dependence, low energy excitation modes and Debye-Waller factors in amorphous matrices, and the mechanism of photon-gated PHB.
One-step (0 to 1) spectral hole burning (SHB) is widely used as a method of eliminating inhomogeneous broadening of spectra: the minimal width of the hole in the inhomogeneous distribution function (IDF) of the transition frequency Omega 01 is obtained by SHB with monochromatic light and is determined by the homogeneous linewidth sigma 0 = gamma 1 + Gamma (where gamma 1 and Gamma are the constants of the energetic and the phase relaxation of the (first) excited level respectively). Two-step (0 to 1 to 2) SHB is considered where the selective excitation of the first step is fixed by a photochemical transformation through the second excitation step. If the selective pulse is a coherent and single-sided exponential then, in the case of an extremely short fixing pulse ( delta pulse), on the increase of the time delay T between the selective and fixing pulses, a monotonic narrowing of the spectral hole in the IDF of the frequency Omega 01 takes place up to the limit width Gamma + mod gamma 1 - Delta mod (where Delta is the spectral width of the selective pulse).
Spectral hole burning in solids is a selective bleaching of a small portion of an inhomogeneously broadened optical transition by a laser. In the photon gated holeburning process spectral holes are burned in two steps. The first is provided by a narrow band laser resonant with the inhomogeneously broadened transition and the second (gating) can be initiated by a broad band light source. Photon gated spectral hole burning was reported recently in 7F0→5D0 and 7F0→5D1 absorption lines of Sm2+ in BaClF(1). In this poster we report on the spectral holeburning behaviour of 1F0→5D2 transition. We found that even in absence of additional light source for gating, permanent holes can be burned. This self gating behaviour is consistent with the observation that the optimum frequency following 5D0 excitation is ≈ 22 000cm-1 so that two photons of energy 5D2 - 7F0 are sufficient to produce photoionisation. We have analysed the light intensity dependance of hole area and a simple model indicate that the electron transfer following the photoionisation is strongly dependant on the ion - electron trap distance.
In inhomogeneously broadened lines, selective photochemistry with narrow band lasers leads to photochemical hole burning. We describe this phenomenon with particular reference to free-base porphyrin (H2P) and chlorin molecules in n-alkane matrices at low temperatures. It is shown that hole burning, which is permanent at low temperatures, can be used to study homogeneous optical dephasing processes as a function of temperature, to measure fast vibronic relaxation, and to assign complex vibronic spectra. Some of the parameters that are important to the potential use of photochemical hole burning for information storage in inhomogeneously broadened lines are measured and discussed.