Photoactive High Explosives: Linear and Nonlinear Photochemistry of Petrin Tetrazine Chloride

Greenfield, Margo; McGrane, Shawn; Bolme, C. A.; Bjorgaard, Josiah; Nelson, Tammie; Tretiak, Sergei; Scharff, R. Jason

doi:10.1021/acs.jpca.5b02092

Cited by 35 publications

(43 citation statements)

References 50 publications

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“…NEXMD has been broadly used for modeling of photoinduced dynamics in a variety of molecular systems. 66,[77][78][79] As a case study for strong light-matter interaction (Fig. 2(b)), we modeled the photoisomerizaiton of stilbene (Fig 2(a)) to demonstrate the utility of the methodology.…”

Section: E Numerical Implementation and Applicationsmentioning

confidence: 99%

Non-adiabatic molecular dynamics of molecules in the presence of strong light-matter interactions

Zhang

Nelson

Tretiak

2019

The Journal of Chemical Physics

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When confined photonic modes in an optical or plasmonic cavity interact strongly with a molecule, new hybrid light-matter states, termed as polaritonic states, can form. The newly formed polaritonic states are the superpositions of electrons (excitons) of the molecules and the cavity photonic modes. It was reported that these polaritons can be employed to control photochemical reactions, charge and energy transfer, and other processes. In addition, according to recent studies, vibrational strong coupling can be employed to resonantly enhance the thermally-activated chemical reactions. In this work, a theoretical model and an efficient numerical method for studying the dynamics of molecules strongly interacting with quantum light are developed based on non-adiabatic excited-state molecular dynamics. The methodology was employed to study the cis-trans photoisomerization of a realistic molecule in a cavity. Numerical simulations demonstrate that the photochemical reactions can be controlled by tuning the properties of the cavity. In the calculated example, the isomerization is suppressed when polaritonic states develop a local minimum on the lower polaritonic state. Moreover, the observed reduction of isomerization is tunable via the photon energy and lightmolecule coupling strength. These insights suggest quantum control of photochemical reactions is possible by specially designed photonic or plasmonic cavities. arXiv:1906.11210v1 [cond-mat.mes-hall]

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Section: E Numerical Implementation and Applicationsmentioning

confidence: 99%

Non-adiabatic molecular dynamics of molecules in the presence of strong light-matter interactions

Zhang

Nelson

Tretiak

2019

The Journal of Chemical Physics

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“…Abboud et al suggests that localized surface plasmon resonance enhances heating in flash irradiated aluminum nanoparticles (nAl), which in turn leads to ignition [14]. Greenfield et al examined the photoactivity of a tetrazine derivatives of PETN known as pentaerythritol trinitrate chlorotetrazine (PetrinTzCl) [15]. The derivative PetrinTzCl exhibited a much higher level of photoactivity than PETN when irradiated with a 532 nm wavelength laser.…”

Section: Ignition By Irradiationmentioning

confidence: 99%

Photoflash and laser ignition of select high-nitrogen materials

Cummock

Gunduz

et al. 2016

Combustion and Flame

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Gas-producing energetic materials that can be readily ignited with a photoflash are typically opaque sensitive primary explosives. In this study, we explore the photoactivity of select highnitrogen (HiN) compounds that are much less sensitive than primary explosives. These HiN materials produce large amounts of gas upon decomposition and this makes them suitable for use in actuators, igniters, or micro-thrusters. This paper presents ignition experimental results using similar shaped pulses at two different wavelengths; specifically using a xenon photoflash and a single wavelength CO 2 laser. Several select HiN materials were tested for flash ignitability, and those that were found to be flash ignitable were further ignited with CO 2 laser heating. By comparing ignition behavior at various laser and flash intensities, some ignition mechanisms are suggested. Thermal heating, regardless of source, appears to be the dominant mechanism responsible for ignition and photochemical effects appear to be negligible in the ignition of the materials considered in this study. Higher laser and photoflash irradiance is shown to require less energy, and is therefore more efficient. The opacity of the material is an important consideration in ignitability, but not a sufficient criteria. We find that opaque materials that successfully propagate well in small capillary tubes are also more likely to successfully flash ignite. We suggest this is due to the higher burning rate of these materials and also in part due to the exothermic reaction occurring at or near the burning surface, allowing the reactions to proceed without quenching.

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“…Recent efforts have focused on photoactive energetic materials with absorption within the range of conventional lasers. [10][11][12][13][14][15][16][17][18][19][20][21][22][23] Introducing a fiber optic cable for direct optical initiation eliminates sensitivity to electrical insults, while replacing primary explosives with less sensitive secondary explosives reduces sensitivity to mechanical insults. A class of energetic materials that exhibit the optical, electrical, and mechanical properties suitable for this application are conjugated energetic molecules (CEMs).…”

Section: Introductionmentioning

confidence: 99%

Cooperative enhancement of the nonlinear optical response in conjugated energetic materials: A TD-DFT study

Sifain

Tadesse

Bjorgaard

et al. 2017

The Journal of Chemical Physics

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Conjugated energetic molecules (CEMs) are a class of explosives with high nitrogen content that posses both enhanced safety and energetic performance properties and are ideal for direct optical initiation. As isolated molecules, they absorb within the range of conventional lasers. Crystalline CEMs are used in practice, however, and their properties can differ due to intermolecular interaction. Herein, time-dependent density functional theory was used to investigate one-photon absorption (OPA) and two-photon absorption (TPA) of monomers and dimers obtained from experimentally determined crystal structures of CEMs. OPA scales linearly with the number of chromophore units, while TPA scales nonlinearly, where a more than 3-fold enhancement in peak intensity, per chromophore unit, is calculated. Cooperative enhancement depends on electronic delocalization spanning both chromophore units. An increase in sensitivity to nonlinear laser initiation makes these materials suitable for practical use. This is the first study predicting a cooperative enhancement of the nonlinear optical response in energetic materials composed of relatively small molecules. The proposed model quantum chemistry is validated by comparison to crystal structure geometries and the optical absorption of these materials dissolved in solution.

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Photoactive High Explosives: Linear and Nonlinear Photochemistry of Petrin Tetrazine Chloride

Cited by 35 publications

References 50 publications

Non-adiabatic molecular dynamics of molecules in the presence of strong light-matter interactions

Non-adiabatic molecular dynamics of molecules in the presence of strong light-matter interactions

Photoflash and laser ignition of select high-nitrogen materials

Cooperative enhancement of the nonlinear optical response in conjugated energetic materials: A TD-DFT study

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