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Optics and Spectroscopy

On the radiative linewidth in single molecule spectroscopy

Inna Rebane

Published Oct 1, 1999• 2 citations
OpenAlex

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Quantum tunneling of the magnetization in a single molecule magnet has been studied in experiments that combine microwave spectroscopy with high sensitivity magnetic measurements. By monitoring spin-state populations in the presence of microwave radiation, the energy splittings between low lying superpositions of high-spin states of single molecule magnet Ni4 (S=4) have been measured. Absorption linewidths give an upper bound on the rate of decoherence. Pulsed microwave experiments provide a measure of energy relaxation time, which is found to increase with frequency.
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.