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How to Find Molecules with Long-lasting Charge Migration?

Alan Scheidegger1, Nikolay V Golubev2, Jiří Vaníček3

  • 1Laboratory of Theoretical Physical Chemistry, Institut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), Av. F.-A. Forel 2, CH-1015 Lausanne. alan.scheidegger@epfl.ch.

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Summary
This summary is machine-generated.

Researchers identified molecules with long-lasting electronic coherence after ionization, crucial for attochemistry applications. But-3-ynal shows promise, while 3-oxopropanenitrile highlights necessary properties for controlling ultrafast electron dynamics.

Keywords:
AttochemistryFirst-principles calculationsSemiclassical methodsUltrafast electron dynamics

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Area of Science:

  • Physical Chemistry
  • Quantum Dynamics
  • Molecular Physics

Background:

  • Ionization can induce superposition of electronic states, leading to ultrafast electron dynamics.
  • Nuclear motion typically causes decoherence in femtoseconds, limiting attochemistry applications.
  • Controlling electron motion is key for attochemistry, but challenging due to decoherence.

Purpose of the Study:

  • To identify molecules exhibiting long-lasting electronic coherence and charge migration after valence ionization.
  • To explain why but-3-ynal is a promising candidate for studying ultrafast electron dynamics.
  • To demonstrate the necessary properties for successful attochemistry applications using 3-oxopropanenitrile as a counterexample.

Main Methods:

  • Development of an efficient algorithm to find molecules with specific electronic properties.
  • Computational analysis of but-3-ynal to assess its potential for long-lasting coherence.
  • Investigation of 3-oxopropanenitrile under various ionization scenarios to understand limitations.

Main Results:

  • But-3-ynal identified as a promising molecule for sustained electronic coherence and charge migration.
  • 3-oxopropanenitrile demonstrated a lack of long-lasting charge migration in multiple ionization scenarios.
  • The study highlights that multiple specific molecular properties are required for attochemistry.

Conclusions:

  • Long-lasting electronic coherence and charge migration are achievable in specific molecular systems.
  • But-3-ynal serves as a key example for exploring ultrafast electron dynamics.
  • Achieving attochemistry applications requires a precise combination of molecular characteristics to overcome decoherence.