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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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Critical role of parallel momentum in quantum well state couplings in multi-stacked nanofilms: An angle resolved photoemission study
We use angle resolved photoemission spectroscopy to investigate the coupling of electron quantum well states (QWSs) in epitaxial thin Pb and Ag films. More specifically, we investigate the Ag/Si, Pb/Si, and Pb/Ag/Si systems. We found that the parallel momentum plays a very profound role in determining how two adjacent quantum wells are coupled electronically across the interface. We revealed that in the Pb/Ag bimetallic system, there exist two distinctly different regimes in the energy vs momentum (E vs k) space. In one regime, the electronic states in Ag and Pb are strongly coupled, resulting in a new set of QWSs for the bi-metallic system. In the other regime, the electronic states in individual metallic layers are retained in their respective regions, as if they are totally decoupled. This result is corroborated by calculations using density functional theory. We further unravel the underlying mechanism associated with the electron refraction and total internal reflection across the interface.
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- PAR ID:
- 10596944
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- AIP Advances
- Volume:
- 10
- Issue:
- 12
- ISSN:
- 2158-3226
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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