Preparing Superposition States to Modify the Spectra and to Achieve Complete Selectivity in Photodissociation Reactions
Ignacio R. Sola, Alberto García-Vela
TL;DR
This paper shows how to use superposition states to control and enhance chemical reactions with high selectivity using light pulses.
Contribution
A new geometric optimization methodology is introduced to prepare superposition states for complete selectivity in photodissociation reactions.
Findings
Using weak ultrashort pulses, reaction efficiency toward desired products can be increased by 100–200%.
High selectivity can be achieved by suppressing the most dominant reaction channel to less than one part in a million.
Preparing superpositions of vibrational states allows precise control over reaction outcomes.
Abstract
We derive and apply the geometric optimization methodology to modify the photodissociation spectra of CH3I in the A band. For this purpose, we prepare optimized initial wave functions that maximally exploit interference-induced coherent control to drive a reaction mediated by nonadiabatic couplings in a polyatomic molecule essentially from the beginning. By designing functionals that maximize the output of the products, or that imply competition between the products, or discrimination of one of them, we test the performance of the methods and the effect of preparing initial vibrational coherences among CH3–I stretching vibrational states, CH3 vibrational states, or both. Our results show that using weak ultrashort pulses, one can easily increase the efficiency of the reaction toward any of the products by 100–200% using vibrational states related to the reaction coordinate; that one can…
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Taxonomy
TopicsMass Spectrometry Techniques and Applications · Advanced Chemical Physics Studies · Laser-Matter Interactions and Applications