Quantum-classical modeling of nonlinear pulse propagation in a dissolved two-photon active chromophore

QC 20100525
In the present work we outline the implications of a quantum-classical approach for modeling two-photon absorption of organic chromophores in solution. The approach joins many-photon absorption dynamic simulations with quantum chemical first principles calculations of corresponding excitation energies and transition matrix elements. Among a number of conclusions of the study, we highlight three: (i) The use of either short- or long-pulse excitation is demonstrated to switch the absorptive capacity of the nonlinear medium owing to enhancement of the nonlinear stepwise processes; (ii) The two-photon cross section strongly depends on the way in which the dephasing rate decays when the laser frequency is tuned off-resonant with the corresponding molecular transition; (iii) The results of the pulse propagation simulations based on electronic structure data obtained with a new Coulomb attenuated functional is shown to be in much better agreement with the experimental results than those based on data received with traditional density functionals.

Ingår i:Journal of Physical Chemistry B: American Chemical Society (ACS)110:11, s. 5379-53851520-61061520-5207

Av författaren/redakt...: Baev, A.; Salek, Pawel; Gel'mukhanov, Fa ...; Ågren, Hans

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