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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Optical Addressing and Switching of Water Molecules in Hole Burning Systems: A TLS Model System

K. Barth, W. Richter

Published Jan 1, 1994• 0 citations
Publisher

Abstract

The change in the profile of a spectral hole can be used to detect tunneling processes in glassy matrices as well as light-induced changes of molecular configurations. The broadening of photochemical holes as well as hole-filling processes are very sensitive probes for molecular rearrangements arround the embedded dye molecules /1/. Light-induced spectral diffusion in polymeric systems is highly selective with respect to the optical excitation of vibrational modes of the surrounding molecular groups.

DOI
10.1364/shbs.1994.wd13

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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.

Annual Meeting Optical Society of America•Jan 1, 1992•0 citations
The change in the profile of a spectral hole can be used to detect tunneling processes in glassy matrices as well as light-induced changes of molecular configurations. The broadening of photochemical holes as well as hole-filling processes are very sensitive probes for molecular rearrangements arround the embedded dye molecules /1/. Light-induced spectral diffusion in polymeric systems is highly selective with respect to the optical excitation of vibrational modes of the surrounding molecular groups.
The profile of a persistent spectral hole can be used to very sensitively detect induced broadening processes that are caused by infrared radiation absorbed in the host matrix /1,2/. Both, the hole area and the hole width are affected to an extent which depends on the frequency of the irradiated IR-light. The excitation of specific vibrations in the host matrix leads to the observed broadening and filling phenomena of a hole spectrum which are highly selective with respect to different vibrational modes.
Each dye molecule embedded in an amorphous material such as a a polymer host experiences a specific molecular environment which strongly influences its electronic transition energies. At low temperatures the different microenvironments result in an inhomogeneously broadened absorption band. The invention of the laser brought new spectroscopic techniques based on energy selection, such as fluorescence line narrowing and spectral hole-burning [1]. These techniques enable convenient addressing of thousands of molecular subsets selected by their transition energy.
Photochemically instable dye molecules in low-temperature polymers are distributed not only spatially in the medium but also spectrally along the axis of resonant optical transition frequencies and orientationally with reference to the polarization of the transition. Consequently, such composite organic materials -- spectral hole burning media1-4 -- can be considered as novel optical materials possessing not only three-dimensional photosensitivity but also sensitivity to the wavelength and polarization of the incident light.
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.
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.
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.