Ultrafast two-photon absorption in organic molecules : quantitative spectroscopy and applications
Makarov, Nikolay Sergeevich.
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This dissertation explores quantitative two-photon absorption spectroscopy to relate molecular structure with optical properties of organic chromophores. The dissertation describes an advanced fluorescence-based technique for reliable measurements of the two-photon spectra and cross sections. To facilitate the measurements it establishes a set of reference compounds measured with a 15% absolute accuracy covering a broad range of excitation and fluorescence wavelengths. The dissertation shows that in many cases the few-essential-levels model can be successfully applied for the description and interpretation of two-photon absorption spectra and cross sections, at least for the low-energy transitions. The dissertation presents examples of applications of two-photon absorption for volumetric optical storage and cancer tumor detection. It describes the basic principles of the two-photon absorption-based optical memory and limitations imposed on two-photon sensitivity of photochromic materials by a necessity of fast access to the data. It also proposes a novel technique for sensitive detection of cancer cells by using two-photon excitation of near-IR fluorescence of a commercial dye and discusses the mechanisms responsible for differentiation between the normal and the cancer cells. The methods described in this dissertation can be applied to understanding the relations between structure and two-photon absorption strength of individual transitions of organic and biological chromophores, which can be used for design of new materials, maximally adapted for particular applications.