TY  - JOUR
A1  - Kroener, Dominik
A1  - Schimka, Selina
A1  - Klamroth, Tillmann
T1  - Laser control for coupled torsions in chiroptical switches: a combined quantum and classical dynamics approach
JF  - The journal of physical chemistry : C, Nanomaterials and interfaces
N2  - We present a novel laser pulse control for the chiroptical switch 1-(2-cis-fluoroethenyl)-2-fluoro-3,5-dibromobenzene mounted on adamantane, where the latter imitates a linker group or part of a solid surface. This molecular device offers three switching states: a true achiral "off"-state and two chiral "on"-states of opposite handedness. Due to the alignment of its chiral axis along the surface normal several defined orientations of the switch have to be considered for an efficient stereocontrol strategy. In addition to these different initial conditions, coupled torsional degrees of freedom around the chiral axis make the quest for highly stereoselective laser pulses a challenge. The necessary flexibility in pulse accomplished by employing the iterative stochastic pulse optimization method we presented recently. Still, the complexity of the system dictates a combined treatment by fast molecular dynamics and computationally intensive quantum dynamics. Although quantum effects are found to be of importance, the pulses optimized within the classical treatment allow us to turn on the chirality of the switch, achieving high enantioselectivity in the quantum treatment for all orientations at the same time.
Y1  - 2014
U6  - https://doi.org/10.1021/jp410342a
SN  - 1932-7447
VL  - 118
IS  - 2
SP  - 1322
EP  - 1331
PB  - American Chemical Society
CY  - Washington
ER  -