Long-Lived Electronic Coherences in Molecules

Phys Rev Lett. 2023 Dec 29;131(26):263202. doi: 10.1103/PhysRevLett.131.263202.

Abstract

We demonstrate long-lived electronic coherences in molecules using a combination of measurements with shaped octave spanning ultrafast laser pulses and calculations of the light matter interaction. Our pump-probe measurements prepare and interrogate entangled nuclear-electronic wave packets whose electronic phase remains well defined despite vibrational motion along many degrees of freedom. The experiments and calculations illustrate how coherences between excited states can survive, even when coherence with the ground state is lost, and may have important implications for many areas of attosecond science and photochemistry.