The role of dissociation channels of excited electronic states in quantum optimal control of ozone isomerization: A three-state dynamical model

Yuzuru Kurosaki, Tak San Ho, Herschel Rabitz

Research output: Contribution to journalArticle

2 Scopus citations

Abstract

The prospect of performing the open → cyclic ozone isomerization has attracted much research attention. Here we explore this consideration theoretically by performing quantum optimal control calculations to demonstrate the important role that excited-state dissociation channels could play in the isomerization transformation. In the calculations we use a three-state, one-dimensional dynamical model constructed from the lowest five 1A′ potential energy curves obtained with high-level ab initio calculations. Besides the laser field-dipole couplings between all three states, this model also includes the diabatic coupling between the two excited states at an avoided crossing leading to competing dissociation channels that can further hinder the isomerization process. The present three-state optimal control simulations examine two possible control pathways previously considered in a two-state model, and reveal that only one of the pathways is viable, achieving a robust ∼95% yield to the cyclic target in the three-state model. This work represents a step towards an ultimate model for the open → cyclic ozone transformation capable of giving adequate guidance about the necessary experimental control field resources as well as an estimate of the ro-vibronic spectral character of cyclic ozone as a basis for an appropriate probe of its formation.

Original languageEnglish (US)
Pages (from-to)115-122
Number of pages8
JournalChemical Physics
Volume469-470
DOIs
StatePublished - May 1 2016

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Keywords

  • Cyclic ozone
  • Optimal control theory
  • Optimal laser pulse
  • Quantum control
  • Wave packet

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