期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 14, 期 43, 页码 9683-9689出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.3c02661
关键词
-
This study presents the analysis of mass-selected, cryogenically cooled molecular ions using 2D IR spectroscopy. Nonlinear response pathways were isolated and coherent coupling between vibrational modes was observed. Well-resolved 2D IR features in the congested fingerprint region were also reported. These experiments provide a more precise method for studying molecular interactions and dynamics.
Two-dimensional infrared (2D IR) spectroscopy of mass-selected, cryogenically cooled molecular ions is presented. Nonlinear response pathways, encoded in the time-domain photodissociation action response of weakly bound N-2 messenger tags, were isolated using pulse shaping techniques following excitation with four collinear ultrafast IR pulses. 2D IR spectra of Re(CO)(3)(CH3CN)(3) (+) ions capture off-diagonal cross-peak bleach signals between the asymmetric and symmetric carbonyl stretching transitions. These cross peaks display intensity variations as a function of pump-probe delay time due to coherent coupling between the vibrational modes. Well-resolved 2D IR features in the congested fingerprint region of protonated caffeine (C8H10N4O2H+) are also reported. Importantly, intense cross-peak signals were observed at 3 ps waiting time, indicating that tag-loss dynamics are not competing with the measured nonlinear signals. These demonstrations pave the way for more precise studies of molecular interactions and dynamics that are not easily obtainable with current condensed-phase methodologies.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据