Two-photon absorption in conjugated energetic molecule [electronic resource].
- Washington, D.C. : United States. Dept. of Energy, 2016.
Oak Ridge, Tenn. : Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy
- Physical Description:
- pages 4,455-4,464 : digital, PDF file
- Additional Creators:
- Los Alamos National Laboratory
United States. Department of Energy
United States. Department of Energy. Office of Scientific and Technical Information
- Time-dependent density functional theory (TD-DFT) is used to investigate the relationship between molecular structure and one- and two-photon absorption (OPA and TPA, respectively) properties in novel and recently synthesized conjugated energetic molecules (CEMs). The molecular structure of CEMs can be strategically altered to influence the heat of formation and oxygen balance, two factors that can contribute to the sensitivity and strength of an explosive material. OPA and TPA are sensitive to changes in molecular structure as well, influencing optical range of excitation. We find calculated vertical excitation energies in good agreement with experiment for most molecules. Peak TPA intensities are significant and on the order of 102 GM. Natural transition orbitals for essential electronic states defining TPA peaks of relatively large intensity to examine the character of relevant transitions. Minor modification of molecular substituents, such as additional oxygen and other functional groups, produces significant changes in electronic structure, OPA, TPA, and improves the oxygen balance. Results show that select molecules are apt to nonlinear absorption, opening the possibility for controlled, direct optical initiation of CEMs through photochemical pathways.
- Published through SciTech Connect.
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory 120 26 ISSN 1089-5639 AM
Josiah August Bjorgaard; Andrew Sifain; Tammie Renee Nelson; Thomas Winfield Myers; Jacqueline Marie Veauthier; David E. Chavez; Robert Jason Scharff; Sergei Tretiak.
- Funding Information:
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