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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Main Authors | , , , , , |
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Format | Journal Article |
Language | English |
Published |
01.05.2024
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Subjects | |
Online Access | Get full text |
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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. |
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DOI: | 10.48550/arxiv.2405.00521 |