Photochemistry of the α-Al2O3-PETN interface

Tsyshevsky, Roman V.; Zverev, Anton; Mitrofanov, Anatoly; Rashkeev, Sergey N.; Kuklja, Maija M.

doi:10.3390/molecules21030289

Title: Photochemistry of the α-Al₂O₃-PETN interface

Journal Article · Mon Feb 29 00:00:00 EST 2016 · Molecules

DOI:https://doi.org/10.3390/molecules21030289· OSTI ID:1264472

Tsyshevsky, Roman V. ^[1]; Zverev, Anton ^[2]; Mitrofanov, Anatoly ^[2];

^[3]; Kuklja, Maija M. ^[1]

Univ. of Maryland, College Park, MD (United States)
Kemerovo State Univ., Kemerovo (Russia); Tomsk Polytechnic Univ., Yurga (Russia)
Univ. of Maryland, College Park, MD (United States); Hamad Bin Khalifa Univ., Doha (Qatar)

Optical absorption measurements are combined with electronic structure calculations to explore photochemistry of an α-Al₂O₃-PETN interface formed by a nitroester (pentaerythritol tetranitrate, PETN, C₅H₈N₄O₁₂) and a wide band gap aluminum oxide (α-Al₂O₃) substrate. The first principles modeling is used to deconstruct and interpret the α-Al₂O₃-PETN absorption spectrum that has distinct peaks attributed to surface F⁰-centers and surfacePETN transitions. We predict the low energy α-Al₂O₃ F⁰-centerPETN transition, producing the excited triplet state, and α-Al₂O₃ F-⁰-centerPETN charge transfer, generating the PETN anion radical. This implies that irradiation by commonly used lasers can easily initiate photodecomposition of both excited and charged PETN at the interface. As a result, the feasible mechanism of the photodecomposition is proposed.

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Research Organization:: Univ. of Maryland, College Park, MD (United States)

Sponsoring Organization:: USDOE Office of Science (SC); (NERSC); US ONR; ONR Global; NSF IRD program; Ministry of Education and Science of Russian Federation; NSF XSEDE; Stampede supercomputing system at TACC/UT Austin

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1264472

Journal Information:: Molecules, Vol. 21, Issue 3; ISSN 1420-3049

Publisher:: MDPICopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 5 works

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References (55)

Adsorption of Small Palladium Clusters on the Relaxed α-Al₂O₃(0001) Surface Gomes, J. R. B.; Lodziana, Z.; Illas, F. The Journal of Physical Chemistry B, Vol. 107, Issue 26 https://doi.org/10.1021/jp022520h	journal	June 2003
Nitroaromatic Actuation of Mitochondrial Bioelectrocatalysis for Self-Powered Explosive Sensors Germain, Marguerite N.; Arechederra, Robert L.; Minteer, Shelley D. Journal of the American Chemical Society, Vol. 130, Issue 46 https://doi.org/10.1021/ja807250b	journal	November 2008
Electronic Band Structure of Al2O3, with Comparison to Alon and AIN French, Roger H. Journal of the American Ceramic Society, Vol. 73, Issue 3 https://doi.org/10.1111/j.1151-2916.1990.tb06541.x	journal	March 1990
Adsorption of Cu and Pd on α-Al2O3(0001) surfaces with different stoichiometries Łodziana, Z.; Nørskov, J. K. The Journal of Chemical Physics, Vol. 115, Issue 24 https://doi.org/10.1063/1.1421107	journal	December 2001
Van der Waals Density Functional for General Geometries Dion, M.; Rydberg, H.; Schroder, E. arXiv https://doi.org/10.48550/arxiv.cond-mat/0402105	text	January 2004
Defect states at organic–inorganic interfaces: Insight from first principles calculations for pentaerythritol tetranitrate on MgO surface Tsyshevsky, Roman V.; Rashkeev, Sergey N.; Kuklja, Maija M. Surface Science, Vol. 637-638 https://doi.org/10.1016/j.susc.2015.01.021	journal	July 2015
Thermal Decomposition Mechanisms of Nitroesters: Ab Initio Modeling of Pentaerythritol Tetranitrate Tsyshevsky, Roman V.; Sharia, Onise; Kuklja, Maija M. The Journal of Physical Chemistry C, Vol. 117, Issue 35 https://doi.org/10.1021/jp407754q	journal	August 2013
Interfacial processes in the dye-sensitized solar cell Gregg, Brian A. Coordination Chemistry Reviews, Vol. 248, Issue 13-14 https://doi.org/10.1016/j.ccr.2004.02.009	journal	July 2004
Toward reliable density functional methods without adjustable parameters: The PBE0 model Adamo, Carlo; Barone, Vincenzo The Journal of Chemical Physics, Vol. 110, Issue 13 https://doi.org/10.1063/1.478522	journal	April 1999
Detection of Explosives with a Fluorescent Nanofibril Film Naddo, Tammene; Che, Yanke; Zhang, Wei Journal of the American Chemical Society, Vol. 129, Issue 22 https://doi.org/10.1021/ja070747q	journal	May 2007
Sensitivity gains in chemosensing by lasing action in organic polymers Rose, Aimée; Zhu, Zhengguo; Madigan, Conor F. Nature, Vol. 434, Issue 7035 https://doi.org/10.1038/nature03438	journal	April 2005
A Fluorescence Turn-On Mechanism to Detect High Explosives RDX and PETN Andrew, Trisha L.; Swager, Timothy M. Journal of the American Chemical Society, Vol. 129, Issue 23 https://doi.org/10.1021/ja071911c	journal	June 2007
Attogram Sensing of Trinitrotoluene with a Self-Assembled Molecular Gelator Kartha, Kalathil K.; Babu, Sukumaran S.; Srinivasan, Sampath Journal of the American Chemical Society, Vol. 134, Issue 10 https://doi.org/10.1021/ja210728c	journal	March 2012
Electron paramagnetic resonance of porous silicon: Observation and identification of conduction-band electrons Young, C. F.; Poindexter, E. H.; Gerardi, G. J. Journal of Applied Physics, Vol. 81, Issue 11 https://doi.org/10.1063/1.365289	journal	June 1997
Van der Waals density functional: Self-consistent potential and the nature of the van der Waals bond Thonhauser, T.; Cooper, Valentino R.; Li, Shen Physical Review B, Vol. 76, Issue 12 https://doi.org/10.1103/physrevb.76.125112	journal	September 2007
Nitrogen-Doped Titanium Dioxide as Visible-Light-Sensitive Photocatalyst: Designs, Developments, and Prospects Asahi, Ryoji; Morikawa, Takeshi; Irie, Hiroshi Chemical Reviews, Vol. 114, Issue 19 https://doi.org/10.1021/cr5000738	journal	May 2014
Theoretical Studies of Photoinduced Electron Transfer in Dye-Sensitized TiO ₂ Duncan, Walter R.; Prezhdo, Oleg V. Annual Review of Physical Chemistry, Vol. 58, Issue 1 https://doi.org/10.1146/annurev.physchem.58.052306.144054	journal	May 2007
Size and habit evolution of PETN crystals—a lattice Monte Carlo study Zepeda-Ruiz, Luis A.; Maiti, Amitesh; Gee, Richard Journal of Crystal Growth, Vol. 291, Issue 2 https://doi.org/10.1016/j.jcrysgro.2006.02.052	journal	June 2006
Theoretical Insights into Photoinduced Charge Transfer and Catalysis at Oxide Interfaces Akimov, Alexey V.; Neukirch, Amanda J.; Prezhdo, Oleg V. Chemical Reviews, Vol. 113, Issue 6 https://doi.org/10.1021/cr3004899	journal	December 2012
First-Principles Calculations of the Adsorption of Nitromethane and 1,1-Diamino-2,2-dinitroethylene (FOX-7) Molecules on the Al(111) Surface Sorescu, Dan C.; Boatz, Jerry A.; Thompson, Donald L. The Journal of Physical Chemistry B, Vol. 107, Issue 34 https://doi.org/10.1021/jp030258m	journal	July 2003
Structure and function of a novel antioxidant peptide from the skin of tropical frogs Barbosa, Eder Alves; Oliveira, Ana; Plácido, Alexandra Free Radical Biology and Medicine, Vol. 115 https://doi.org/10.1016/j.freeradbiomed.2017.11.001	journal	February 2018
Selective Response of Mesoporous Silicon to Adsorbants with Nitro Groups McLeod, John A.; Kurmaev, Ernst Z.; Sushko, Peter V. Chemistry - A European Journal, Vol. 18, Issue 10 https://doi.org/10.1002/chem.201102084	journal	January 2012
New Microporous Metal−Organic Framework Demonstrating Unique Selectivity for Detection of High Explosives and Aromatic Compounds Pramanik, Sanhita; Zheng, Chong; Zhang, Xiao Journal of the American Chemical Society, Vol. 133, Issue 12 https://doi.org/10.1021/ja106851d	journal	March 2011
Experimental and TD-DFT Study of Optical Absorption of Six Explosive Molecules: RDX, HMX, PETN, TNT, TATP, and HMTD Cooper, Jason K.; Grant, Christian D.; Zhang, Jin Z. The Journal of Physical Chemistry A, Vol. 117, Issue 29 https://doi.org/10.1021/jp312492v	journal	March 2013
Amine-Capped ZnS−Mn ²⁺ Nanocrystals for Fluorescence Detection of Trace TNT Explosive Tu, Renyong; Liu, Bianhua; Wang, Zhenyang Analytical Chemistry, Vol. 80, Issue 9 https://doi.org/10.1021/ac800060f	journal	May 2008
Porous Shape Persistent Fluorescent Polymer Films: An Approach to TNT Sensory Materials Yang, Jye-Shane; Swager, Timothy M. Journal of the American Chemical Society, Vol. 120, Issue 21 https://doi.org/10.1021/ja9742996	journal	June 1998
Detection of Nitroaromatic Explosives Based on Photoluminescent Polymers Containing Metalloles Sohn, Honglae; Sailor, Michael J.; Magde, Douglas Journal of the American Chemical Society, Vol. 125, Issue 13 https://doi.org/10.1021/ja021214e	journal	April 2003
Discrimination of Nitroaromatics and Explosives Mimics by a Fluorescent Zn(salicylaldimine) Sensor Array Germain, Meaghan E.; Knapp, Michael J. Journal of the American Chemical Society, Vol. 130, Issue 16 https://doi.org/10.1021/ja800403k	journal	April 2008
Development of a New s-Tetrazine-Based Copolymer for Efficient Solar Cells ^§ Li, Zhao; Ding, Jianfu; Song, Naiheng Journal of the American Chemical Society, Vol. 132, Issue 38 https://doi.org/10.1021/ja106052e	journal	September 2010
A microsensor for trinitrotoluene vapour Pinnaduwage, L. A.; Gehl, A.; Hedden, D. L. Nature, Vol. 425, Issue 6957 https://doi.org/10.1038/425474a	journal	October 2003
Recent Advances in Trace Explosives Detection Instrumentation Moore, David S. Sensing and Imaging: An International Journal, Vol. 8, Issue 1 https://doi.org/10.1007/s11220-007-0029-8	journal	March 2007
Model of the photostimulated fragmentation of PETN molecules in selective photoinitiation Aluker, E. D.; Krechetov, A. G.; Mitrofanov, A. Yu. Russian Journal of Physical Chemistry B, Vol. 5, Issue 5 https://doi.org/10.1134/S1990793111090156	journal	October 2011
Laser Initiation of Energetic Materials: Selective Photoinitiation Regime in Pentaerythritol Tetranitrate Aluker, Edward D.; Krechetov, Alexander G.; Mitrofanov, Anatoliy Y. The Journal of Physical Chemistry C, Vol. 115, Issue 14 https://doi.org/10.1021/jp1089195	journal	March 2011
Understanding Limits of the Thermal Mechanism of Laser Initiation of Energetic Materials Aluker, Edward D.; Krechetov, Alexander G.; Mitrofanov, Anatoliy Y. The Journal of Physical Chemistry C, Vol. 116, Issue 46 https://doi.org/10.1021/jp308633y	journal	November 2012
Topography of Photochemical Initiation in Molecular Materials Aluker, Edward; Krechetov, Alexander; Mitrofanov, Anatoly Molecules, Vol. 18, Issue 11 https://doi.org/10.3390/molecules181114148	journal	November 2013
Energies of Electronic Transitions of Pentaerythritol Tetranitrate Molecules and Crystals Tsyshevsky, Roman V.; Sharia, Onise; Kuklja, Maija M. The Journal of Physical Chemistry C, Vol. 118, Issue 18 https://doi.org/10.1021/jp500011a	journal	April 2014
First-Principles Calculations of the Adsorption of Nitromethane and 1,1-Diamino-2,2-dinitroethylene (FOX-7) Molecules on the α-Al₂O₃(0001) Surface Sorescu, Dan C.; Boatz, Jerry A.; Thompson, Donald L. The Journal of Physical Chemistry B, Vol. 109, Issue 4 https://doi.org/10.1021/jp046193k	journal	January 2005
Electronic structure of molecular crystals containing edge dislocations Kuklja, Maija M.; Kunz, A. Barry Journal of Applied Physics, Vol. 89, Issue 9 https://doi.org/10.1063/1.1359171	journal	May 2001
Radiation-induced point defects in simple oxides Kotomin, E. A.; Popov, A. I. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 141, Issue 1-4 https://doi.org/10.1016/S0168-583X(98)00079-2	journal	May 1998
Theoretical study of bulk and surface oxygen and aluminum vacancies in $α - {Al}_{2} O_{3}$ Carrasco, Javier; Gomes, José R. B.; Illas, Francesc Physical Review B, Vol. 69, Issue 6 https://doi.org/10.1103/PhysRevB.69.064116	journal	February 2004
The kinetics and mechanism of doped corundum structure formation in an water fluid Ivakin, Yu. D.; Danchevskaya, M. N.; Ovchinnikova, O. G. Russian Journal of Physical Chemistry B, Vol. 3, Issue 7 https://doi.org/10.1134/S199079310907001X	journal	December 2009
Ultraviolet absorption spectrum of pentaerythritol tetranitrate Mullen, P. A.; Orloff, M. K. The Journal of Physical Chemistry, Vol. 77, Issue 7 https://doi.org/10.1021/j100626a011	journal	March 1973
First-principles study of the optical transitions ofFcenters in the bulk and on the (0001) surface ofα−Al2O3 Carrasco, Javier; Lopez, Nuria; Sousa, Carmen Physical Review B, Vol. 72, Issue 5 https://doi.org/10.1103/PhysRevB.72.054109	journal	August 2005
Optical Absorption Energies of Molecular Defects in Pentaerythritol Tetranitrate Crystals: Quantum Chemical Modeling Tsyshevsky, Roman V.; Sharia, Onise; Kuklja, Maija M. The Journal of Physical Chemistry C, Vol. 118, Issue 46 https://doi.org/10.1021/jp508271k	journal	November 2014
Inhomogeneous Electron Gas Hohenberg, P.; Kohn, W. Physical Review, Vol. 136, Issue 3B, p. B864-B871 https://doi.org/10.1103/PhysRev.136.B864	journal	November 1964
Self-Consistent Equations Including Exchange and Correlation Effects Kohn, W.; Sham, L. J. Physical Review, Vol. 140, Issue 4A, p. A1133-A1138 https://doi.org/10.1103/PhysRev.140.A1133	journal	November 1965
Van der Waals Density Functional for General Geometries Dion, M.; Rydberg, H.; Schröder, E. Physical Review Letters, Vol. 92, Issue 24 https://doi.org/10.1103/PhysRevLett.92.246401	journal	June 2004
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Ab initio molecular dynamics for liquid metals Kresse, G. Journal of Non-Crystalline Solids, Vol. 192-193 https://doi.org/10.1016/0022-3093(95)00355-X	journal	December 1995
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Accurate structure analysis with synchrotron radiation. The electron density in Al2O3 and Cu2O Kirfel, A.; Eichhorn, K. Acta Crystallographica Section A Foundations of Crystallography, Vol. 46, Issue 4 https://doi.org/10.1107/S0108767389012596	journal	April 1990
Linear optical properties in the projector-augmented wave methodology Gajdoš, M.; Hummer, K.; Kresse, G. Physical Review B, Vol. 73, Issue 4 https://doi.org/10.1103/PhysRevB.73.045112	journal	January 2006
Density‐functional thermochemistry. III. The role of exact exchange Becke, Axel D. The Journal of Chemical Physics, Vol. 98, Issue 7, p. 5648-5652 https://doi.org/10.1063/1.464913	journal	April 1993
Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density Lee, Chengteh; Yang, Weitao; Parr, Robert G. Physical Review B, Vol. 37, Issue 2 https://doi.org/10.1103/PhysRevB.37.785	journal	January 1988

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
36 MATERIALS SCIENCE
1
1-diamino-2
2-dinitroethylene fox-7 molecules
total-energy calculations
wave basis-set
pentaerythritol tetranitrate
1st-principles calculations
selective photoinitiation
optical-absorption
laser initiation
electron-density
explosives
singlet-triplet exciton
electronically excited and charged state
decomposition barrier
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Title: Photochemistry of the α-Al2O3-PETN interface

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Title: Photochemistry of the α-Al₂O₃-PETN interface