Electron nuclear dynamics of H++H2 collisions at Elab=30 eV

Abstract

Proton collisions with hydrogen molecules at 30 eV in the laboratory frame is a simple ion-molecule system exhibiting a number of distinct processes such as inelastic scattering, charge transfer, rearrangement, and dissociation. The electron nuclear dynamics (END) theory which allows full electron nuclear coupling and which does not restrict the system from reaching any of the possible product channels, is applied to this sytem to produce transition probabilities, differential, and integral (vibrationally resolved) cross sections. Comparisons with experiment demonstrate that END, even in its simplest implementation, with a single determinantal state for the electrons and with classical nuclei, yields results that are competitive with other theoretical approaches.

Influence of nuclear exchange on nonadiabatic electron processes in H$^+$++H$_2$2 collisions

“…21 The VCC results, which employed ab initio electronic wavefunctions, nicely coincide with previous IOSA calculations at E = 30 eV, 9 which used DIM electronic wavefunctions 22 and a small vibronic basis set, but they do not agree with END (Ref. 3) and TSH (Ref. 4) cross sections.…”

“…Among the theoretical studies of H + +H 2 collisions, only the electron nuclear dynamics (END) 3 and trajectory surface hopping (TSH) 4 calculations have simultaneously considered the nonreactive [Eqs. (1)- (5)] and reactive [Eqs.…”

New Light Shed on Charge Transfer in FundamentalH++H2Collisions

“…1. Besides intrinsically different treatments of the electron dynamics, the disagreement between our results and previous calculations (electron nuclear dynamics [14], trajectory surface hopping [13], and semiclassical IOSA [24]) also points to the necessity to quantally describe the nuclear motion for E < 200 eV.…”

“…Recommended data: (red dash-dotted line) Phelps [19]. Previous calculations: (green open upward triangle) Baer et al [9]; (green open square) Morales et al [14]; (green dashed line with open downward triangle) Ichihara et al [13]; (green solid line with open circle) Krstić [10]; (green solid line with crosses) Krstić and co-workers [24]; (green dashed line) nonreactive CT from Ref. [4].…”

“…The calculation of Errea et al [12] employed ab initio electronic wave functions and a vibronic basis set within quantal and semiclassical frameworks, covering a large energy range (10 eV < E < 10 keV). Other semiclassical methods, such as trajectory surface hopping [13], electron nuclear dynamics [14], and classical trajectory-diatomics in molecules [4], have also been applied, and the ensuing total cross sections are shown in Fig. 1.…”