Michalchuk, A.A.L., Trestman, M., Rudic, S. et al. (4 more authors) (2019) Predicting the reactivity of energetic materials : an ab initio multi-phonon approach. Journal of Materials Chemistry A, 7 (33). pp. 19539-19553. ISSN 2050-7488
Abstract
The ease with which an energetic material (explosives, propellants, and pyrotechnics) can be initiated is a critical parameter to as-sess their safety and application. Impact sensitivity parameters are traditionally derived experimentally, at great cost and risk to safety. In this work we explore a fully ab initio approach based on concepts of vibrational energy transfer to predict impact sensi-tivities for a series of chemically, structurally and energetically diverse molecular materials. The quality of DFT calculations is as-sessed for a subset of the materials by comparison with experimental inelastic neutron scattering spectra (INS). A variety of mod-els are considered, including both qualitative and quantitative analysis of the vibrational spectra. Excellent agreement against ex-perimental impact sensitivity is achieved by consideration of a multi-phonon ladder-type up-pumping mechanism that includes both overtone and combination pathways, and is improved further by the added consideration of temperature. This fully ab initio approach not only permits ranking of energetic materials in terms of their impact sensitivity but also provides a tool to guide the targeted design of advanced energetic compounds with tailored properties.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | © 2019 Royal Society of Chemistry. This is an Open Access article distributed under the terms of the Creative Commons Attribution Unported Licence (http://creativecommons.org/licenses/by/3.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. |
Keywords: | energetic materials; impact sensitivity prediction; vibrational up-pumping; DFT |
Dates: |
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Institution: | The University of Sheffield |
Academic Units: | The University of Sheffield > Faculty of Science (Sheffield) > Department of Chemistry (Sheffield) |
Funding Information: | Funder Grant number Defence Science and Technology Laboratory DSTLX-1000112699 |
Depositing User: | Symplectic Sheffield |
Date Deposited: | 08 Aug 2019 11:26 |
Last Modified: | 09 Dec 2021 14:39 |
Status: | Published |
Publisher: | Royal Society of Chemistry (RSC) |
Refereed: | Yes |
Identification Number: | 10.1039/c9ta06209b |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:149486 |