Temperature dependence of Coherent versus spontaneous Raman Scattering

Due to their sub picosecond temporal resolution, coherent Raman spectroscopies have been proposed as a viable extension of Spontaneous Raman (SR) thermometry, to determine dynamics of mode specific vibrational energy content during out of equilibrium molecular processes. Here we show that the presen...

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Bibliographic Details
Main Authors Batignani, Giovanni, Mai, Emanuele, Martinati, Miles, Neethish, Mohanan M, Mukamel, Shaul, Scopigno, Tullio
Format Journal Article
LanguageEnglish
Published 01.05.2024
Subjects
Physics - Chemical Physics
Physics - Optics
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Summary:Due to their sub picosecond temporal resolution, coherent Raman spectroscopies have been proposed as a viable extension of Spontaneous Raman (SR) thermometry, to determine dynamics of mode specific vibrational energy content during out of equilibrium molecular processes. Here we show that the presence of multiple laser fields stimulating the vibrational coherences introduces additional quantum pathways, resulting in destructive interference. This ultimately reduces the thermal sensitivity of single spectral lines, nullifying it for harmonic vibrations and temperature independent polarizability. We demonstrate how harnessing anharmonic signatures such as vibrational hot bands enables coherent Raman thermometry.
DOI:10.48550/arxiv.2405.00521