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Advances in coherent light sources and development of pump–probe techniques in recent decades have opened the way to study electronic motion in its natural time scale. When an ultrashort laser pulse interacts with a molecular target, a coherent superposition of electronic states is created and the triggered electron dynamics is coupled to the nuclear motion. A natural and computationally efficient choice to simulate this correlated dynamics is a trajectory-based method where the quantum-mechanical electronic evolution is coupled to a classical-like nuclear dynamics. These methods must approximate the initial correlated electron–nuclear state by associating an initial electronic wavefunction to each classical trajectory in the ensemble. Different possibilities exist that reproduce the initial populations of the exact molecular wavefunction when represented in a basis. We show that different choices yield different dynamics and explore the effect of this choice in Ehrenfest, surface hopping, and exact-factorization-based coupled-trajectory schemes in a one-dimensional two-electronic-state model system that can be solved numerically exactly. This work aims to clarify the problems that standard trajectory-based techniques might have when a coherent superposition of electronic states is created to initialize the dynamics, to discuss what properties and observables are affected by different choices of electronic initial conditions and to point out the importance of quantum-momentum-induced electronic transitions in coupled-trajectory schemes.
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Asymmetries in ionization of atomic superposition states by ultrashort laser pulses
Abstract Progress in ultrafast science allows for probing quantum superposition states with ultrashort laser pulses in the new regime where several linear and nonlinear ionization pathways compete. Interferences of pathways can be observed in the photoelectron angular distribution and in the past they have been analyzed for atoms and molecules in a single quantum state via anisotropy and asymmetry parameters. Those conventional parameters, however, do not provide comprehensive tools for probing superposition states in the emerging research area of bright and ultrashort light sources, such as free-electron lasers and high-order harmonic generation. We propose a new set of generalized asymmetry parameters which are sensitive to interference effects in the photoionization and the interplay of competing pathways as the laser pulse duration is shortened and the laser intensity is increased. The relevance of the parameters is demonstrated using results of state-of-the-art numerical solutions of the time-dependent Schrödinger equation for ionization of helium atom and neon atom.
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- Award ID(s):
- 1734006
- PAR ID:
- 10231201
- Date Published:
- Journal Name:
- Scientific Reports
- Volume:
- 10
- Issue:
- 1
- ISSN:
- 2045-2322
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1038/s41598-020-73196-9
