Laser-Induced Electron Symmetry Restoration in Oriented Molecules Made Simple

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Abstract
Electron symmetry determines many important properties of molecules, from selection rules for photoelectron spectroscopy to symmetry selection rules for chemical reactions. The original electron symmetry is broken if a laser pulse changes the initial state, typically the ground state g, to a superposition of g and an excited state e with different irreducible representations (IRREPs). Quantum dynamics simulations for two examples, the oriented benzene and LiCN molecules, show that the original electron symmetry can be restored by means of a reoptimized π-laser pulse which transfers the component in the excited state e to another state e′, or to several others with the same IRREP as the ground state. This method lends itself to much easier experimental applications than all previous ones because it allows the healing of electron symmetry immediately, without any attosecond constraint on the timing of the second pulse.
Funding Information
  • Fund for Shanxi Key Subjects Construction
  • National Natural Science Foundation of China (11904215)
  • Higher Education Discipline Innovation Project (D18001)
  • Hundred Talent Program of Shanxi Province
  • National Key Research and Development Program of China (12004193, 2017YFA0304203)
  • program for Changjiang Scholars and Innovative Research Team (IRT_17R70)

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