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Title: Photodissociation transition states characterized by chirped pulse millimeter wave spectroscopy

Abstract

The 193-nm photolysis of CH 2 CHCN illustrates the capability of chirped-pulse Fourier transform millimeter-wave spectroscopy to characterize transition states. We investigate the HCN, HNC photofragments in highly excited vibrational states using both frequency and intensity information. Measured relative intensities of J = 1–0 rotational transition lines yield vibrational-level population distributions (VPD). These VPDs encode the properties of the parent molecule transition state at which the fragment molecule was born. A Poisson distribution formalism, based on the generalized Franck–Condon principle, is proposed as a framework for extracting information about the transition-state structure from the observed VPD. We employ the isotopologue CH 2 CDCN to disentangle the unimolecular 3-center DCN elimination mechanism from other pathways to HCN. Our experimental results reveal a previously unknown transition state that we tentatively associate with the HCN eliminated via a secondary, bimolecular reaction.

Authors:
; ORCiD logo; ORCiD logo; ; ; ; ORCiD logo; ; ORCiD logo
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1579963
Grant/Contract Number:  
DEFG0287ER; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 117 Journal Issue: 1; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English

Citation Formats

Prozument, Kirill, Baraban, Joshua H., Changala, P. Bryan, Park, G. Barratt, Shaver, Rachel G., Muenter, John S., Klippenstein, Stephen J., Chernyak, Vladimir Y., and Field, Robert W. Photodissociation transition states characterized by chirped pulse millimeter wave spectroscopy. United States: N. p., 2019. Web. doi:10.1073/pnas.1911326116.
Prozument, Kirill, Baraban, Joshua H., Changala, P. Bryan, Park, G. Barratt, Shaver, Rachel G., Muenter, John S., Klippenstein, Stephen J., Chernyak, Vladimir Y., & Field, Robert W. Photodissociation transition states characterized by chirped pulse millimeter wave spectroscopy. United States. doi:10.1073/pnas.1911326116.
Prozument, Kirill, Baraban, Joshua H., Changala, P. Bryan, Park, G. Barratt, Shaver, Rachel G., Muenter, John S., Klippenstein, Stephen J., Chernyak, Vladimir Y., and Field, Robert W. Wed . "Photodissociation transition states characterized by chirped pulse millimeter wave spectroscopy". United States. doi:10.1073/pnas.1911326116.
@article{osti_1579963,
title = {Photodissociation transition states characterized by chirped pulse millimeter wave spectroscopy},
author = {Prozument, Kirill and Baraban, Joshua H. and Changala, P. Bryan and Park, G. Barratt and Shaver, Rachel G. and Muenter, John S. and Klippenstein, Stephen J. and Chernyak, Vladimir Y. and Field, Robert W.},
abstractNote = {The 193-nm photolysis of CH 2 CHCN illustrates the capability of chirped-pulse Fourier transform millimeter-wave spectroscopy to characterize transition states. We investigate the HCN, HNC photofragments in highly excited vibrational states using both frequency and intensity information. Measured relative intensities of J = 1–0 rotational transition lines yield vibrational-level population distributions (VPD). These VPDs encode the properties of the parent molecule transition state at which the fragment molecule was born. A Poisson distribution formalism, based on the generalized Franck–Condon principle, is proposed as a framework for extracting information about the transition-state structure from the observed VPD. We employ the isotopologue CH 2 CDCN to disentangle the unimolecular 3-center DCN elimination mechanism from other pathways to HCN. Our experimental results reveal a previously unknown transition state that we tentatively associate with the HCN eliminated via a secondary, bimolecular reaction.},
doi = {10.1073/pnas.1911326116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 1,
volume = 117,
place = {United States},
year = {2019},
month = {12}
}

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