Stereoselective isomerization of an ensemble of adsorbed molecules with multiple orientations: stochastic laser pulse optimization for selective switching between achiral and chiral atropisomers.
Stereoselective isomerization of an ensemble of adsorbed molecules with multiple orientations: stochastic laser pulse optimization for selective switching between achiral and chiral atropisomers.
复制标题
具有多个方向的吸附分子整体的立体选择性异构化：用于非手性和手性阻转异构体之间选择性切换的随机激光脉冲优化。
DOI：
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发表时间：
2008
影响因子：
4.4
通讯作者：
D. Kröner
中科院分区：
文献类型：
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作者：
T. Klamroth;D. Kröner
我们提出了激光驱动的多取向表面立体异构体集合异构化的量子动力学模拟。模型系统1-（2-顺式氟乙烯基）-2-氟苯在连接苯基环和乙烯的C-C单键周围扭转时支持两个手性和一个非手性对映体。红外皮秒脉冲被用来激发围绕手性轴的内部旋转，从而控制分子的手性。为了选择性地将分子（与它们在表面上的取向无关）从非手性形式切换到左手或右手形式，应用了随机脉冲优化算法。根据表面的旋转对称性，对不同的吸附取向进行了随机脉冲优化。所得到的非线性偏振激光脉冲对各取向具有高度的对映选择性。
We present quantum dynamical simulations for the laser driven isomerization of an ensemble of surface mounted stereoisomers with multiple orientations. The model system 1-(2-cis-fluoroethenyl)-2-fluorobenzene supports two chiral and one achiral atropisomers upon torsion around the C-C single bond connecting phenyl ring and ethylene group. An infrared picosecond pulse is used to excite the internal rotation around the chiral axis, thereby controlling the chirality of the molecule. In order to selectively switch the molecules--independent of their orientation on a surface--from their achiral to either their left- or right-handed form, a stochastic pulse optimization algorithm is applied. The stochastic pulse optimization is performed for different sets of defined orientations of adsorbates corresponding to the rotational symmetry of the surface. The obtained nonlinearly polarized laser pulses are highly enantioselective for each orientation.