Orchestrating Nuclear Dynamics in a Permanganate Doped Crystal with Chirped Pump-Probe Spectroscopy

Emanuele Mai, Partha Malakar, Giovanni Batignani*, Miles Martinati, Sanford Ruhman*, Tullio Scopigno*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Pump-probe spectroscopy is a powerful tool to investigate light-induced dynamical processes in molecules and solids. Targeting vibrational excitations occurring on the time scales of nuclear motions is challenging, as pulse durations shorter than a vibrational period are needed to initiate the dynamics, and complex experimental schemes are required to isolate weak signatures arising from wavepacket motion in different electronic states. Here, we demonstrate how introducing a temporal delay between the spectral components of femtosecond beams, namely a chirp resulting in the increase of their duration, can counterintuitively boost the desired signals by 2 orders of magnitude. Measuring the time-domain vibrational response of permanganate ions embedded in a KClO4 matrix, we identify an intricate dependence of the vibrational response on pulse chirps and probed wavelength that can be exploited to unveil weak signatures of the doping ions─otherwise dominated by the nonresonant matrix─or to obtain vibrational excitations pertaining only to the excited state, suppressing ground-state contributions.

Original languageEnglish
Pages (from-to)6634-6646
Number of pages13
JournalJournal of Physical Chemistry Letters
Volume15
Issue number25
DOIs
StatePublished - 27 Jun 2024

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© 2024 American Chemical Society

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