[1] Max Planck Inst Quantum Opt, D-85748 Garching, Germany
来源:
FARADAY DISCUSSIONS
|
1999年
/
113卷
关键词:
D O I:
10.1039/a901657k
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
We present schemes for the laser pulse control of bimolecular reactions. As a model system we treat the collision complex Na-H-2, which is unbound in the electronic ground state X(2)A(1) and weakly bound in the electronic excited state A(2)B(2). This system decays non-adiabatically from the excited state via a conical intersection back to the ground state. The objective of the laser controls presented is the excitation of the collision pair with simultaneous focusing of the wavepacket towards the conical intersection. In the first step an optimal laser pulse is derived by optimal control theory over the expectation values for semi-positive definite operators. In the second step chirped laser pulses are fitted to the optimal one. For the chirped laser pulses the influences of the chirp is discussed. Special emphasis is placed on the excitation of vibrations of the H-2 compound, which are considered to be important for the passage through the conical intersection.