Abstract
The rapid ionization of D2 in a short and intense laser pulse generates a rotational–vibrational (RV) nuclear wave packet in D2+. By solving the time-dependent Schrödinger equation in full dimensionality, we simulate the coherent evolution of such wave packets and discuss their ro-vibrational dynamics. Within a harmonic time-series analysis of the evolving nuclear probability density, we characterize the RV dynamics in D2+ in an external intense linearly polarized infrared laser field in terms of quantum-beat (QB) spectra in which both internuclear distance and molecular orientation relative to the linearly polarized laser field are resolved. Based on numerical examples for the nuclear dynamics without and under the influence of pulsed and continuum-wave (cw) laser light, we discuss and quantify the signature of RV couplings in QB spectra and the extent to which the QB analysis of measured time-dependent fragment kinetic energy release spectra is expected to image the laser-dressed RV structure of D2+.
Highlights
Formal solution of the time-dependent Schrödinger equationAfter separating the center-of-mass motion, the TDSE of the D+2 molecular ion in a laser field is given by i
The distribution of internuclear distances R in the excited molecule. This promotes our understanding of the evolution of a variety of molecular phenomena that are triggered by intense laser pulses, such as vibrational-state-resolved dissociation, ionization followed by fragmentation, the decoherence and dephasing of nuclear wave packets, and the transient formation of laser-induced bound molecular states ([10, 21, 22] and references therein)
As was shown previously in numerical simulations that neglect molecular rotation, Fourier analysis of a time series of spectral data over a finite interval of pump–probe delays τ [0, T ] yields R-dependent quantum-beat (QB) spectra that reveal the nodal structure of bound vibrational states of the lowest adiabatic potential curve of the molecular ion, together with the corresponding vibrational transition energies
Summary
After separating the center-of-mass motion, the TDSE of the D+2 molecular ion in a laser field is given by i. Separately for a large number of fixed internuclear distances, in order to obtain the adiabatic electronic wave functions {φi } and the corresponding energy surfaces, {Ei (R)}. The expansion of the total wave function in (1) in terms of the complete set of electronic wave functions, ψ(R,r, t) =. I defines the nuclear wave functions { i (R, t)} Inserting this Born–Oppenheimer (BO) expansion into (1), followed by projection on to individual adiabatic electronic states, leads to a set of coupled differential equations for the nuclear wave functions. Allows the set of differential equations for the components of the nuclear wave function (R, θ, t) = ( 1(R, θ, t), 2(R, θ, t), .
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