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Title: Probing ultrafast shock-induced chemistry in liquids using broad-band mid-infrared absorption spectroscopy

Abstract

We probe shock-induced chemistry in two organic liquids by measuring broadband, midinfrared absorption in the 800–1400 cm –1 frequency range. To test this new method and understand the signatures of chemical reactions in time resolved vibrational spectra, we compared liquid benzene shocked to unreactive conditions (shocked to a pressure of 18 GPa for a duration of 300 ps) to nitromethane under reactive conditions (25 GPa). We see clear signatures of shock-induced chemistry that are distinguishable from the pressure- and temperature-induced changes in vibrational mode shapes. While shocked benzene shows primarily a broadening and shifting of the vibrational modes, the nitromethane vibrational modes vanish once the shock wave enters the liquid and simultaneously, a spectrally broad feature appears that we interpret as the infrared spectrum of the complex mixture of product and intermediate species. To further interpret these measurements, we compare them to reactive quantum molecular dynamics simulations, which gives qualitatively consistent results. As a result, this work demonstrates a promising method for time resolving shock-induced chemistry, illustrating that chemical reactions produce distinct changes in the vibrational spectra.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Purdue Univ., West Lafayette, IN (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1532719
Alternate Identifier(s):
OSTI ID: 1515577
Report Number(s):
LA-UR-19-20976
Journal ID: ISSN 0021-9606
Grant/Contract Number:  
89233218CNA000001; 20170070DR
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 150; Journal Issue: 20; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; mid-infrared; time-resolved chemistry; explosives; ultrafast spectroscopy; nitromethane

Citation Formats

Bowlan, Pamela Renee, Powell, Michael Stephan, Perriot, Romain Thibault, Martinez, Enrique Saez, Kober, Edward Martin, Cawkwell, Marc Jon, and McGrane, Shawn David. Probing ultrafast shock-induced chemistry in liquids using broad-band mid-infrared absorption spectroscopy. United States: N. p., 2019. Web. doi:10.1063/1.5092242.
Bowlan, Pamela Renee, Powell, Michael Stephan, Perriot, Romain Thibault, Martinez, Enrique Saez, Kober, Edward Martin, Cawkwell, Marc Jon, & McGrane, Shawn David. Probing ultrafast shock-induced chemistry in liquids using broad-band mid-infrared absorption spectroscopy. United States. doi:10.1063/1.5092242.
Bowlan, Pamela Renee, Powell, Michael Stephan, Perriot, Romain Thibault, Martinez, Enrique Saez, Kober, Edward Martin, Cawkwell, Marc Jon, and McGrane, Shawn David. Thu . "Probing ultrafast shock-induced chemistry in liquids using broad-band mid-infrared absorption spectroscopy". United States. doi:10.1063/1.5092242.
@article{osti_1532719,
title = {Probing ultrafast shock-induced chemistry in liquids using broad-band mid-infrared absorption spectroscopy},
author = {Bowlan, Pamela Renee and Powell, Michael Stephan and Perriot, Romain Thibault and Martinez, Enrique Saez and Kober, Edward Martin and Cawkwell, Marc Jon and McGrane, Shawn David},
abstractNote = {We probe shock-induced chemistry in two organic liquids by measuring broadband, midinfrared absorption in the 800–1400 cm–1 frequency range. To test this new method and understand the signatures of chemical reactions in time resolved vibrational spectra, we compared liquid benzene shocked to unreactive conditions (shocked to a pressure of 18 GPa for a duration of 300 ps) to nitromethane under reactive conditions (25 GPa). We see clear signatures of shock-induced chemistry that are distinguishable from the pressure- and temperature-induced changes in vibrational mode shapes. While shocked benzene shows primarily a broadening and shifting of the vibrational modes, the nitromethane vibrational modes vanish once the shock wave enters the liquid and simultaneously, a spectrally broad feature appears that we interpret as the infrared spectrum of the complex mixture of product and intermediate species. To further interpret these measurements, we compare them to reactive quantum molecular dynamics simulations, which gives qualitatively consistent results. As a result, this work demonstrates a promising method for time resolving shock-induced chemistry, illustrating that chemical reactions produce distinct changes in the vibrational spectra.},
doi = {10.1063/1.5092242},
journal = {Journal of Chemical Physics},
number = 20,
volume = 150,
place = {United States},
year = {2019},
month = {5}
}

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This content will become publicly available on May 23, 2020
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