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Quantum optimal control for the full ensemble of randomly oriented molecules having different field-free Hamiltonians

Kurosaki, Yuzuru; Ichihara, Akira; Yokoyama, Keiichi

We have presented the OCT formulation to calculate optimal fields that can control the full ensemble of randomly-oriented molecules having different field-free Hamiltonians. The theory is applied to the fifty-fifty mixture of randomly-oriented $$^{133}$$CsI and $$^{135}$$CsI isotopomers and an optimal field is sought to achieve isotope-selective vibrational excitations with high efficiency. Rotational motion is frozen and two total times $$T$$'s of electric field duration, 460000 and 920000 au (11.1 and 22.2 ps), are chosen in the present calculation. As a result, the final yields for $$T$$ = 460000 and 920000 a.u. are calculated to be 0.706 and 0.815, respectively. The relatively high final yield obtained for $$T$$ = 920000 a.u. strongly suggests that a single laser pulse can control the full ensemble of randomly-oriented non-identical molecules. The result is quite encouraging in terms of the application to isotope-separation processes.

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Category:Chemistry, Physical

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