State-to-state reactive scattering using reactant–product decoupling

Cvitaš, Marko T.; Althorpe, Stuart C.

doi:10.1088/0031-8949/80/04/048115

Cited by 19 publications

(4 citation statements)

References 57 publications

(89 reference statements)

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“…Our starting point towards development of a computational method for problems such as that described in Fig. 1 is through a connection to the reactant product decoupling (RPD) method popular in quantum scattering theory [151][152][153][154][155][156][157][158][159][160][161][162] . However, it is important to note that while in RPD, absorbing and emitting potentials are applied in configurational space to partition the global potential surface, in our case, the absorbing and emitting potentials are applied in real space to partition the system into multiple portions (or stages, as discussed below) to facilitate an efficient and accurate treatment.…”

Section: A Multi-stage Ab Initio Wavepacket Dynamical (Ms-aiwd) Formamentioning

confidence: 99%

A multistage ab initio quantum wavepacket dynamics formalism for electronic structure and dynamics in open systems

Pacheco

Iyengar

2010

The Journal of Chemical Physics

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We propose a multistage quantum wavepacket dynamical treatment for the study of delocalized electronic systems as well as electron transport through donor-bridge-acceptor systems such as those found in molecular-wire/electrode networks. The full donor-bridge-acceptor system is treated through a rigorous partitioning scheme that utilizes judiciously placed offsetting absorbing and emitting boundary conditions. These facilitate a computationally efficient and potentially accurate treatment of the long-range coupling interactions between the bridge and donor/acceptor systems and the associated open system boundary conditions. Time-independent forms of the associated, partitioned equations are also derived. In the time-independent form corresponding to the bridge system, coupling to donor and acceptor, that is long-range interactions, is completely accounted. For the time-dependent study, the quantum dynamics of the electronic flux through the bridge-donor/acceptor interface is constructed using an accurate and efficient representation of the discretized quantum-mechanical free-propagator. A model for an electrode-molecular wire-electrode system is used to test the accuracy of the scheme proposed. Transmission probability is obtained directly from the probability density of the electronic flux in the acceptor region. Conductivity through the molecular wire is computed using a wavepacket flux correlation function.

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Section: A Multi-stage Ab Initio Wavepacket Dynamical (Ms-aiwd) Formamentioning

confidence: 99%

A multistage ab initio quantum wavepacket dynamics formalism for electronic structure and dynamics in open systems

Pacheco

Iyengar

2010

The Journal of Chemical Physics

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“…The RPD method was first proposed by Peng and Zhang for state‐to‐state studies of triatomic reaction systems and further developed by Althorpe and coworkers . The RPD method has been widely used for computing the S ‐matrix elements.…”

Section: State‐to‐state Quantum Reactive Scatteringmentioning

confidence: 99%

State‐to‐state quantum reactive scattering in four‐atom systems

Zhao

Guo

2017

WIREs Comput Mol Sci

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The recent advances in quantum mechanical studies of four-atom reactions at the state-to-state level are reviewed. With six internal degrees of freedom, such reactions offer richer chemistry than the much studied atom-diatom reactions, but also pose challenges to the quantum mechanical treatment of the state-tostate scattering process. Several approaches that are capable of providing a complete solution to the problem have recently been suggested and a brief description and comparison of these approaches are given here. In addition, recent quantum mechanical state-to-state results for tetratomic reactions are discussed and a simple transition-state-based model is shown to provide useful insights into the correlation between reactant and product quantum states during a reaction. , for useful discussions. FIGURE 7 | Three-dimensional polar plots of differential cross sections (DCSs) for the D 2 + OH(v) ! D + DOH(v OD v b v OH ) reaction with the OH reactant in the v = 0 (a) and v = 1 (b) vibrational states at the collision energies of E c = 0.25 eV. The 3D DCSs show the product angular distributions with respect to the incoming direction of the OH reactant, i.e., the forward direction of DOH product corresponds to 0 while backward direction to 180 . The radius of the plot represents the product translational energy and arcs with shorter radius correspond to product states with higher internal energies and vice versa. Reproduced from Ref 46 with permission. WIREs Computational Molecular ScienceState-to-state quantum reactive scattering in four-atom systems Volume 7,

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“…An extensive overview of scattering theories and results in the E-and T-domains, up to 2006, has been provided by Hu and Schatz 1 (some more recent reviews are Refs. [2][3][4][5][6].…”

Section: Introductionmentioning

confidence: 99%

Semiclassical glory analyses in the time domain for the H + D2(vi = 0, ji = 0) → HD(vf = 3, jf = 0) + D reaction

Xiao

Connor

2012

The Journal of Chemical Physics

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We make the first application of semiclassical (SC) techniques to the plane-wavepacket formulation of time-domain (T-domain) scattering. The angular scattering of the state-to-state reaction, H + D(2)(v(i) = 0, j(i) = 0) → HD(v(f) = 3, j(f) = 0) + D, is analysed, where v and j are vibrational and rotational quantum numbers, respectively. It is proved that the forward-angle scattering in the T-domain, which arises from a delayed mechanism, is an example of a glory. The SC techniques used in the T-domain are: An integral transitional approximation, a semiclassical transitional approximation, a uniform semiclassical approximation (USA), a primitive semiclassical approximation and a classical semiclassical approximation. Nearside-farside (NF) scattering theory is also employed, both partial wave and SC, since a NF analysis provides valuable insights into oscillatory structures present in the full scattering pattern. In addition, we incorporate techniques into the SC theory called "one linear fit" and "two linear fits", which allow the derivative of the quantum deflection function, Θ̃(')(J), to be estimated when Θ̃J exhibits undulations as a function of J, the total angular momentum variable. The input to our SC analyses is numerical scattering (S) matrix data, calculated from accurate quantum collisional calculations for the Boothroyd-Keogh-Martin-Peterson potential energy surface No. 2, in the energy domain (E-domain), from which accurate S matrix elements in the T-domain are generated. In the E-domain, we introduce a new technique, called "T-to-E domain SC analysis." It half-Fourier transforms the E-domain accurate quantum scattering amplitude to the T-domain, where we carry out a SC analysis; this is followed by an inverse half-Fourier transform of the T-domain SC scattering amplitude back to the E-domain. We demonstrate that T-to-E USA differential cross sections (DCSs) agree well with exact quantum DCSs at forward angles, for energies where a direct USA analysis in the E-domain fails.

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State-to-state reactive scattering using reactant–product decoupling

Cited by 19 publications

References 57 publications

A multistage ab initio quantum wavepacket dynamics formalism for electronic structure and dynamics in open systems

A multistage ab initio quantum wavepacket dynamics formalism for electronic structure and dynamics in open systems

State‐to‐state quantum reactive scattering in four‐atom systems

Semiclassical glory analyses in the time domain for the H + D2(vi = 0, ji = 0) → HD(vf = 3, jf = 0) + D reaction

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