Two-photon absorption in conjugated energetic molecule
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Univ. of Southern California, Los Angeles, CA (United States)
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.
- Research Organization:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Organization:
- USDOE Laboratory Directed Research and Development (LDRD) Program
- Grant/Contract Number:
- AC52-06NA25396
- OSTI ID:
- 1338766
- Report Number(s):
- LA-UR-16-20834
- Journal Information:
- Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Vol. 120, Issue 26; ISSN 1089-5639
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
Monocationic Iridium(III) Complexes with Far-Red Charge-Transfer Absorption and Near-IR Emission: Synthesis, Photophysics, and Reverse Saturable Absorption: Monocationic Iridium(III) Complexes with Far-Red Charge-Transfer Absorption and Near-IR Emission: Synthesis, Photophysics, and Reverse Saturable Absor
|
journal | April 2019 |
Azido and Tetrazolo 1,2,4,5-Tetrazine N-Oxides
|
journal | February 2017 |
Similar Records
Site-Specific Photodecomposition in Conjugated Energetic Materials
Comparison of the resonance-enhanced multiphoton ionization spectra of pyrrole and 2,5-dimethylpyrrole: Building toward an understanding of the electronic structure and photochemistry of porphyrins