Optimal control of ultrafast cis-trans photoisomerization of retinal in rhodopsin via a conical intersection -: art. no. 144508

被引:76
作者
Abe, M
Ohtsuki, Y [1 ]
Fujimura, Y
Domcke, W
机构
[1] Tohoku Univ, Dept Chem, Grad Sch Sci, Sendai, Miyagi 9808578, Japan
[2] JST, CREST, Kawaguchi, Saitama 3320012, Japan
基金
日本学术振兴会;
关键词
D O I
10.1063/1.2034488
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
Optimal control simulation is applied to the cis-trans photoisomerization of retinal in rhodopsin within a two-dimensional, two-electronic-state model with a conical intersection [S. Hahn and G. Stock, J. Phys. Chem. B 104, 1146 (2000)]. For this case study, we investigate coherent control mechanisms, in which laser pulses work cooperatively with a conical intersection that acts as a "wave-packet cannon." Optimally designed pulses largely consist of shaping subpulses that prepare a wave packet, which is localized along a reaction coordinate and has little energy in the coupling mode, through multiple electronic transitions. This shaping process is shown to be essential for achieving a high target yield although the envelopes of the calculated pulses depend on the local topography of the potential-energy surfaces around the conical intersection and the choice of target. The control mechanisms are analyzed by considering the motion of reduced wave packets in a nuclear configuration space as well as by snapshots of probability current-density maps. (c) 2005 American Institute of Physics.
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页数:10
相关论文
共 41 条
[1]  
Abe M, 2005, SPRINGER SERIES CHEM, V79, P613
[2]   Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses [J].
Assion, A ;
Baumert, T ;
Bergt, M ;
Brixner, T ;
Kiefer, B ;
Seyfried, V ;
Strehle, M ;
Gerber, G .
SCIENCE, 1998, 282 (5390) :919-922
[3]   PREDICTION OF STRUCTURAL AND ENVIRONMENTAL-EFFECTS ON THE S1-S0 ENERGY-GAP AND JUMP PROBABILITY IN DOUBLE-BOND CIS TRANS PHOTOISOMERIZATION - A GENERAL RULE [J].
BONACICKOUTECKY, V ;
KOHLER, J ;
MICHL, J .
CHEMICAL PHYSICS LETTERS, 1984, 104 (05) :440-443
[4]   Quantum control by ultrafast polarization shaping [J].
Brixner, T ;
Krampert, G ;
Pfeifer, T ;
Selle, R ;
Gerber, G ;
Wollenhaupt, M ;
Graefe, O ;
Horn, C ;
Liese, D ;
Baumert, T .
PHYSICAL REVIEW LETTERS, 2004, 92 (20) :208301-1
[5]  
COHENTANNOUDJI C, 1977, QUANTUM MECH, pCH3
[6]   Deciphering the reaction dynamics underlying optimal control laser fields [J].
Daniel, C ;
Full, J ;
González, L ;
Lupulescu, C ;
Manz, J ;
Merli, A ;
Vajda, S ;
Wöste, L .
SCIENCE, 2003, 299 (5606) :536-539
[7]  
Domcke W., 2004, Conical Intersections: Electronic Structure, Dynamics and Spectroscopy
[8]  
Advanced Series in Physical Chemistry
[9]   The C5H6NH2+ protonated Shiff base: An ab initio minimal model for retinal photoisomerization [J].
Garavelli, M ;
Celani, P ;
Bernardi, F ;
Robb, MA ;
Olivucci, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1997, 119 (29) :6891-6901
[10]   Photoisomerization path for a realistic retinal chromophore model: The nonatetraeniminium cation [J].
Garavelli, M ;
Vreven, T ;
Celani, P ;
Bernardi, F ;
Robb, MA ;
Olivucci, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1998, 120 (06) :1285-1288