Five-Photon Absorption and Selective Enhancement of Multiphoton Absorption Processes

摘要

We study one-, two-, three-, four- and five-photon absorption of three centrosymmetricmolecules using density functional theory. These calculations are the firstab initio calculations of five-photon absorption. Even- and odd-order absorption processesshow different trends in the absorption cross sections. The behaviour of all even-and odd-photon absorption properties shows a semi-quantitative similarity which canbe explained using few-state models. This analysis shows that odd-photon absorptionprocesses are largely determined by the one-photon absorption strength whereas alleven-photon absorption strengths are largely dominated by the two-photon absorptionstrength, in both cases modulated by powers of the polarizability of the final excitedstate. We demonstrate how to selectively enhance a specific multiphoton absorptionprocess.