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• W4285341773 abstract "Recent experimental advances in frequency-domain spectroscopy have resulted in large increases in the quantity, quality, relative intensities, and inter-species correlated rotation-vibration population distributions. When a spectrum is recorded without scanning a laser or a monochromator, it can yield meaningful, information-rich relative intensities. We discuss a series of examples in this paper. This series culminates in two examples of multiplexed spectra: Chirped Pulse millimeter-wave Spectroscopy and Velocity Map Imaging. A few-μs duration chirped pulse of millimeter-wave radiation is generated electronically without appreciable pulse-to-pulse variation of either the pulse itself or the system to which it is applied. A velocity map image is collected event-by-event on a 2-dimensional detector, without significant variation of the laser frequencies that generate the detected species. The availability of new classes of experimental data have led to the asking and answering of previously unimaginable questions about the structure and dynamics of small molecules at high levels of internal excitation, especially in explicitly targeted regions of state-space. Spectra are assigned based on observation or reconstruction of simple patterns. These patterns are broken by spectroscopic perturbations. The broken patterns can be collected and arranged into a higher level of pattern: a pattern of broken patterns. These perturbations can be interactions of an electronic “bright state” with multiple vibrational levels of several electronic excited “dark” states or, for the 3N-6 vibrational normal modes of an N-atom polyatomic molecule, vibrational polyads. Polyads are much more robust than vibrational normal modes because, as excitation energy increases, the values of the matrix elements and the dimension of the H eff polyad matrices depend in a simple, a priori known manner on the polyad quantum numbers. At high excitation energy, the energy and structure of transition states for isomerization become encoded in a broken pattern of broken patterns, for example, the transition state for trans-cis isomerization in the S1 state of acetylene. Information about photolysis transition states comes from the vibrational population distribution of photofragments and from inter-species rotation-vibration correlated population distributions. Vibrational satellites on the J=0-1 rotational transition of HCN/HNC in the Chirped-Pulse millimeter-Wave (CPmmW) spectrum reveal the mechanism(s) of 193 nm photolysis of Vinyl Cyanide. Correlated population distributions of CO and H2, observed by Velocity Map Imaging (VMI) reveal the roaming mechanism for dissociation of H2CO via excitation of selected predissociated levels." @default.
• W4285341773 created "2022-07-14" @default.
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• W4285341773 date "2021-10-27" @default.
• W4285341773 modified "2023-09-27" @default.
• W4285341773 title "Modern Techniques, Modern Concepts, and Molecules Doing Stuff" @default.
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• W4285341773 doi "https://doi.org/10.1021/bk-2021-1398.ch015" @default.
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