2024/01/02 by Alejandro R. Ramos Ramos, E. Fischer, Ramos, A. R. Ramos +5
Chemistry · Materials Science · Physics and Astronomy · #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Laser-Matter Interactions and Applications #Photochemistry and Electron Transfer Studies #Porphyrin and Phthalocyanine Chemistry #Quantum Physics (quant-ph)
paper · pdf · doi:10.48550/arxiv.2401.01138
openalex publication_date 2024/01/02 · openalex created_date 2024/01/04 · openalex updated_date 2026/07/31
Controlling molecular reactivity by shaped laser pulses is a long-standing goal in chemistry. Here we suggest a direct optimal control approach which combines external pulse optimization with other control parameters arising in the upcoming field of vibro-polaritonic chemistry, for enhanced controllability The direct optimal control approach is characterized by a simultaneous simulation and optimization paradigm, meaning that the equations of motion are discretized and converted into a set of holonomic constraints for a nonlinear optimization problem given by the control functional. Compared with indirect optimal control this procedure offers great flexibility such as final time or Hamiltonian parameter optimization. Simultaneous direct optimal control (SimDOC) theory will be applied to a model system describing H-atom transfer in a lossy Fabry-Pérot cavity under vibrational strong coupling conditions. Specifically, optimization of the cavity coupling strength and thus of the control landscape will be demonstrated.