Quantum Interference Paves the Way for Long-Lived Electronic Coherences.

Area of Science:

• Quantum dynamics
• Molecular physics
• Attosecond science

Background:

• Broadband ionization with extreme ultraviolet (XUV) pulses creates coherent superpositions of electronic states in polyatomic molecules.
• Electronic coherence between hole states is typically short-lived, decaying due to nuclear dynamics (decoherence).
• Attosecond science aims to control and extend electronic coherence for novel applications.

Purpose of the Study:

• Investigate methods to prolong electronic coherence in molecules after XUV ionization.
• Explore the potential of using time-delayed pulses for coherent control of electronic motion.
• Demonstrate the feasibility of controlling charge migration phenomena through extended electronic coherence.

Main Methods:

• Employed the multiconfiguration time-dependent Hartree (MCTDH) method.
• Incorporated an ionization continuum model Hamiltonian.
• Simulated the dynamical fate of coherent electronic states generated by broadband XUV pulses.

Main Results:

• Electronic coherence persists until nuclear dynamics induce decoherence.
• Time-delayed pulses were shown to be a viable strategy for retaining electronic coherence.
• The study demonstrates the prospect of coherent control over charge migration.

Conclusions:

• Controlling electronic coherence is achievable using tailored laser pulse schemes.
• Extended electronic coherence opens pathways for manipulating charge migration dynamics.
• This work advances the understanding and control capabilities within attosecond molecular science.