Ab initio study of coherent anti-Stokes Raman scattering (CARS) of the 1,3,5-trinitro-1,3,5-triazacyclohexane (RDX) explosive

Mohammed, Abdelsalam; Ågren, Hans; Thorvaldsen, Andreas J.; Ruud, Kenneth

doi:10.1016/j.cplett.2009.12.061

Cited by 6 publications

(14 citation statements)

References 28 publications

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“…13,14 HF theory's neglect of electron-electron interaction is especially unphysical for systems with sig-nificant correlation, like metals. For this reason, we replace HF for the calculation of CARS on metal cluster models.…”

mentioning

confidence: 99%

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

Parkhill

Rappoport

Aspuru‐Guzik

2011

J. Phys. Chem. Lett.

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We present the first density functional simulations of coherent anti-Stokes Raman scattering (CARS) and an analysis of the chemical effects upon binding to a metal surface. Spectra are obtained from first-principles electronic structure calculations and are compared with available experiments and previously available theoretical results following from Hartree–Fock polarizability derivatives. A first approximation to the nonresonant portion of the CARS signal is also explored. We examine the silver pyridine cluster models of the surface chemical signal enhancement, previously introduced for surface-enhanced Raman scattering. Chemical resonant intensity enhancements of roughly 102 are found for several model clusters. The prospects of realizing further enhancement of CARS signal with metal surfaces is discussed in light of the predicted chemical enhancements.

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mentioning

confidence: 99%

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

Parkhill

Rappoport

Aspuru‐Guzik

2011

J. Phys. Chem. Lett.

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“…The theoretical harmonic frequencies of the C-H stretch, C-N stretch, C-C stretch, C-H bend and C arom breathing modes are 3052, 2280, 1590, 1200 and 967 cm À1 , respectively (see Figure 2). These important calculated harmonic frequency modes, which are also active in CARS and NRS spectra, have been presented and discussed in our previous work [11] and compared there with the corresponding experimental fundamental frequencies.…”

Section: Results and Discussion 41 Bn And Rdxmentioning

confidence: 92%

“…The procedure is analogous to that employed in previous papers studying coherent anti-Stokes Raman Scattering (CARS) [10,11], and vibrational contributions to the hyperpolarizability [16].…”

Section: Hyperpolarizability Gradientmentioning

confidence: 94%

“…In our previous work [11], we studied CARS and NRS spectra for two molecules, namely benzonitrile C 7 H 5 N (BN) and 1,3,5-trinitro-1,3,5-triazacyclohexane (RDX) C 3 H 6 N 6 O 6 . In the present work we will use the same test molecules and apply the same basic theoretical approach to investigate HRS.…”

Section: Computational Detailsmentioning

confidence: 99%

“…In the present work we advocate that a most effective approach to accomplish this is by means of the matrix-based analytic technique recently developed by Thorvaldsen et al [10]. This technology is applicable for properties of any order, and was employed to study normal Raman (NRS) and CARS in our earlier work [11], where the first, respectively, the third polarizability is involved. The present work thus offers the possibility to test its efficiency also for the second polarizability and so to provide a comprehensive comparison of the three Raman techniques, NRS, HRS and CARS, for the same molecules.…”

Section: Introductionmentioning

confidence: 98%

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Hyper Raman spectra calculated in a time-dependent Hartree–Fock method

et al. 2012

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Hyper Raman scattering (HRS) of the benzonitrile (BN) and 1,3,5-trinitro-1,3,5-triazacyclohexane (RDX) molecules is studied by means of ab initio calculations. The computational procedure employs a recently developed methodology for the analytic calculations of frequency-dependent polarizability gradients of arbitrary order, including perturbation dependent basis sets. The result are compared to normal Raman scattering (NRS) and coherent anti-Stokes Raman scattering (CARS) that previously have been studied using the same technology. It is found that some suppressed or silent modes in CARS and NRS spectra are clearly seen in HRS, and that although under general excitation conditions the HRS intensities are much lower than for CARS and NRS, HRS provides complementary information useful for target identification.

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Response Function Theory Computational Approaches to Linear and Nonlinear Optical Spectroscopy

Rizzo

Coriani

Ruud

2011

Computational Strategies for Spectroscopy

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Ab initio study of coherent anti-Stokes Raman scattering (CARS) of the 1,3,5-trinitro-1,3,5-triazacyclohexane (RDX) explosive

Cited by 6 publications

References 28 publications

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

Hyper Raman spectra calculated in a time-dependent Hartree–Fock method

Response Function Theory Computational Approaches to Linear and Nonlinear Optical Spectroscopy

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