TY  - JOUR
A1  - Schönborn, Jan Boyke
A1  - Saalfrank, Peter
A1  - Klamroth, Tillmann
T1  - Controlling the high frequency response of H-2 by ultra-short tailored laser pulses: A time-dependent configuration interaction study
JF  - The journal of chemical physics : bridges a gap between journals of physics and journals of chemistr
N2  - We combine the stochastic pulse optimization (SPO) scheme with the time-dependent configuration interaction singles method in order to control the high frequency response of a simple molecular model system to a tailored femtosecond laser pulse. For this purpose, we use H-2 treated in the fixed nuclei approximation. The SPO scheme, as similar genetic algorithms, is especially suited to control highly non-linear processes, which we consider here in the context of high harmonic generation. Here, we will demonstrate that SPO can be used to realize a "non-harmonic" response of H2 to a laser pulse. Specifically, we will show how adding low intensity side frequencies to the dominant carrier frequency of the laser pulse and stochastically optimizing their contribution can create a high-frequency spectral signal of significant intensity, not harmonic to the carrier frequency. At the same time, it is possible to suppress the harmonic signals in the same spectral region, although the carrier frequency is kept dominant during the optimization. (C) 2016 AIP Publishing LLC.
Y1  - 2016
U6  - https://doi.org/10.1063/1.4940316
SN  - 0021-9606
SN  - 1089-7690
VL  - 144
PB  - American Institute of Physics
CY  - Melville
ER  -