TY - JOUR
T1 - Orchestrating Nuclear Dynamics in a Permanganate Doped Crystal with Chirped Pump-Probe Spectroscopy
AU - Mai, Emanuele
AU - Malakar, Partha
AU - Batignani, Giovanni
AU - Martinati, Miles
AU - Ruhman, Sanford
AU - Scopigno, Tullio
N1 - Publisher Copyright:
© 2024 American Chemical Society
PY - 2024/6/27
Y1 - 2024/6/27
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85196637391&partnerID=8YFLogxK
U2 - 10.1021/acs.jpclett.4c00801
DO - 10.1021/acs.jpclett.4c00801
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C2 - 38888442
AN - SCOPUS:85196637391
SN - 1948-7185
VL - 15
SP - 6634
EP - 6646
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 25
ER -