Physics

Absolute excited state molecular geometries revealed by resonance Raman signals

G. Batignani, E. Mai, et al.

Discover groundbreaking insights into excited-state potential energy surfaces and their role in ultrafast light-activated reactions. This innovative two-color broadband impulsive Raman experimental scheme, led by Giovanni Batignani and colleagues, reveals the direction and magnitude of excited-state displacements, providing a new understanding of stimulated vibrational coherences.

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Abstract

Excited-state (ES) potential energy surfaces (PESs) govern ultrafast light-activated reactions. Conventional spectroscopy only reveals the absolute value of ES displacements, not their direction. This paper introduces a two-color broadband impulsive Raman experimental scheme to directly measure complex Raman excitation profiles, revealing the magnitude and direction of ES displacements relative to the ground state. This is achieved through non-degenerate resonant probe and off-resonant pump pulses, providing time-domain sensitivity to the phase of stimulated vibrational coherences.

Publisher

Nature Communications

Published On

Dec 15, 2022

Authors

Giovanni Batignani, Emanuele Mai, Giuseppe Fumero, Shaul Mukamel, Tullio Scopigno

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