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

被引:1
作者
Mai, Emanuele [1 ,2 ]
Malakar, Partha [3 ]
Batignani, Giovanni [1 ,2 ]
Martinati, Miles [1 ]
Ruhman, Sanford [3 ]
Scopigno, Tullio [1 ,4 ]
机构
[1] Sapienza Univ Roma, Dipartimento Fis, I-00185 Rome, Italy
[2] Ist Italiano Tecnol, Ctr Life Nano Sci Sapienza, I-00161 Rome, Italy
[3] Hebrew Univ Jerusalem, Inst Chem, IL-9190401 Jerusalem, Israel
[4] Ist Italiano Tecnol, Graphene Labs, I-16163 Genoa, Italy
基金
欧盟地平线“2020”;
关键词
STIMULATED RAMAN-SPECTROSCOPY; CONICAL INTERSECTION DYNAMICS; MOLECULAR VIBRATIONAL MOTION; EXCITED-STATE DYNAMICS; RESONANCE RAMAN; TIME-DOMAIN; ABSORPTION; EXCITATION; SCATTERING; SPECTRA;
D O I
10.1021/acs.jpclett.4c00801
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:6634 / 6646
页数:13
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