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Ultrafast interatomic electronic decay in multiply excited clusters.

Alexander I Kuleff1, Kirill Gokhberg, Sören Kopelke

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A new ultrafast interatomic Coulombic decay (ICD) mechanism is proposed, where energy transfer between excited species leads to ionization. This ICD process dominates ion production in large atomic clusters exposed to intense laser pulses.

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Area of Science:

  • Atomic and Molecular Physics
  • Quantum Chemistry
  • Laser Physics

Background:

  • Interatomic Coulombic decay (ICD) is a key process in atomic and molecular systems.
  • Understanding ultrafast dynamics in atomic clusters is crucial for various fields.
  • Laser-matter interactions at high intensities can lead to complex ionization pathways.

Purpose of the Study:

  • To propose and investigate a novel ultrafast interatomic Coulombic decay (ICD) mechanism.
  • To demonstrate the dominance of this ICD mechanism in large homoatomic clusters under intense laser irradiation.
  • To explore a related collective-ICD process in heteroatomic systems.

Main Methods:

  • Theoretical modeling of ultrafast energy transfer and ionization processes.
  • Simulation of large homoatomic and heteroatomic clusters exposed to intense, ultrashort laser pulses.
  • Analysis of ion production yields and comparison with alternative ionization pathways.

Main Results:

  • Proposed an ultrafast ICD mechanism involving energy transfer between two excited species.
  • Demonstrated that this ICD mechanism is the primary source of ion production in large atomic clusters under resonant laser excitation.
  • Showed that ICD significantly outcompetes direct two-photon ionization.
  • Discussed a related collective-ICD process applicable to heteroatomic systems.

Conclusions:

  • The proposed ultrafast ICD mechanism provides a new understanding of ionization dynamics in atomic clusters.
  • This ICD pathway is highly efficient and dominant under specific laser conditions.
  • The findings have implications for controlling and predicting ionization in nanoscale systems.