TY - JOUR A1 - Klamroth, Tillmann T1 - Optimal control of ultrafast laser driven many-electron dynamics in a polyatomic molecule: N-methyl-6-quinolone N2 - We report time-dependent configuration interaction singles calculations for the ultrafast laser driven many- electron dynamics in a polyatomic molecule, N-methyl-6-quinolone. We employ optimal control theory to achieve a nearly state-selective excitation from the S-0 to the S-1 state, on a time scale of a few (approximate to 6) femtoseconds. The optimal control scheme is shown to correct for effects opposing a state-selective transition, such as multiphoton transitions and other, nonlinear phenomena, which are induced by the ultrashort and intense laser fields. In contrast, simple two-level pi pulses are not effective in state-selective excitations when very short pulses are used. Also, the dependence of multiphoton and nonlinear effects on the number of states included in the dynamical simulations is investigated. Y1 - 2006 UR - https://publishup.uni-potsdam.de/frontdoor/index/index/docId/11662 UR - http://jcp.aip.org/ SN - 0021-9606 ER -