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Title: Photoactive High Explosives: Substituents Effects on Tetrazine Photochemistry and Photophysics

Abstract

High explosives that are photoactive, i.e., can be initiated with light, offer significant advantages in reduced potential for accidental electrical initiation. In this study, we examined a series of structurally related tetrazine based photoactive high explosive materials to detail their photochemical and photophysical properties. Using photobleaching infrared absorption, we determined quantum yields of photochemistry for nanosecond pulsed excitation at 355 and 532 nm. Changes in mass spectrometry during laser irradiation in vacuum measured the evolution of gaseous products. Fluorescence spectra, quantum yields, and lifetimes were measured to observe radiative channels of energy decay that compete with photochemistry. For the 6 materials studied, quantum yields of photochemistry ranged from <10 –5 to 0.03 and quantum yield of fluorescence ranged from <10 –3 to 0.33. In all cases, the photoexcitation nonradiatively relaxed primarily to heat, appropriate for supporting photothermal initiation processes. Lastly, the photochemistry observed was dominated by ring scission of the tetrazine, but there was evidence of more extensive multistep reactions as well.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (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:
1337091
Report Number(s):
LA-UR-15-29258
Journal ID: ISSN 1089-5639
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 120; Journal Issue: 6; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; explosives, photoactive

Citation Formats

McGrane, Shawn David, Bolme, Cynthia Anne, Greenfield, Margo Torello, Chavez, David E., Hanson, Susan Kloek, and Scharff, Robert Jason. Photoactive High Explosives: Substituents Effects on Tetrazine Photochemistry and Photophysics. United States: N. p., 2016. Web. doi:10.1021/acs.jpca.5b11851.
McGrane, Shawn David, Bolme, Cynthia Anne, Greenfield, Margo Torello, Chavez, David E., Hanson, Susan Kloek, & Scharff, Robert Jason. Photoactive High Explosives: Substituents Effects on Tetrazine Photochemistry and Photophysics. United States. doi:10.1021/acs.jpca.5b11851.
McGrane, Shawn David, Bolme, Cynthia Anne, Greenfield, Margo Torello, Chavez, David E., Hanson, Susan Kloek, and Scharff, Robert Jason. Thu . "Photoactive High Explosives: Substituents Effects on Tetrazine Photochemistry and Photophysics". United States. doi:10.1021/acs.jpca.5b11851. https://www.osti.gov/servlets/purl/1337091.
@article{osti_1337091,
title = {Photoactive High Explosives: Substituents Effects on Tetrazine Photochemistry and Photophysics},
author = {McGrane, Shawn David and Bolme, Cynthia Anne and Greenfield, Margo Torello and Chavez, David E. and Hanson, Susan Kloek and Scharff, Robert Jason},
abstractNote = {High explosives that are photoactive, i.e., can be initiated with light, offer significant advantages in reduced potential for accidental electrical initiation. In this study, we examined a series of structurally related tetrazine based photoactive high explosive materials to detail their photochemical and photophysical properties. Using photobleaching infrared absorption, we determined quantum yields of photochemistry for nanosecond pulsed excitation at 355 and 532 nm. Changes in mass spectrometry during laser irradiation in vacuum measured the evolution of gaseous products. Fluorescence spectra, quantum yields, and lifetimes were measured to observe radiative channels of energy decay that compete with photochemistry. For the 6 materials studied, quantum yields of photochemistry ranged from <10–5 to 0.03 and quantum yield of fluorescence ranged from <10–3 to 0.33. In all cases, the photoexcitation nonradiatively relaxed primarily to heat, appropriate for supporting photothermal initiation processes. Lastly, the photochemistry observed was dominated by ring scission of the tetrazine, but there was evidence of more extensive multistep reactions as well.},
doi = {10.1021/acs.jpca.5b11851},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 6,
volume = 120,
place = {United States},
year = {2016},
month = {1}
}

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