Temperature Dependence of Coherent versus Spontaneous Raman Scattering

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

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Bibliographic Details
Published in:Physical review letters 2024-11, Vol.133 (20), p.206902, Article 206902
Main Authors: Batignani, Giovanni, Mai, Emanuele, Martinati, Miles, Neethish, Mohanan M, Mukamel, Shaul, Scopigno, Tullio
Format: Article
Language:English
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Summary:Because of their sub picosecond temporal resolution, coherent Raman spectroscopies have been proposed as a viable extension of spontaneous Raman 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.
ISSN:0031-9007
1079-7114
1079-7114
DOI:10.1103/PhysRevLett.133.206902