Work

Temperature Dependence of Coherent versus Spontaneous Raman Scattering

Year: 2024

Type: article

Abstract: 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.

Source: Physical Review Letters

DOI: 10.1103/physrevlett.133.206902

Authors: Giovanni Batignani, Emanuele Mai, Miles Martinati, Mohanan M. Neethish, Shaul Mukamel, Tullio Scopigno

Institutions: Italian Institute of Technology, Sapienza University of Rome, University of California, Irvine

Language: English

Topic: Spectroscopy Techniques in Biomedical and Chemical Research

Subfield: Biophysics

Field: Biochemistry, Genetics and Molecular Biology

Domain: Life Sciences

Open Access status: green

Funders: National Science Foundation, European Commission, Sapienza Università di Roma, Division of Chemistry