Meier Christoph, Heitz Marie-Catherine
Laboratoire Collisions, Agrégats et Réactivité, UMR 5589, Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes, Université Paul Sabatier, 118 Route de Narbonne, 31062 Toulouse, France.
J Chem Phys. 2005 Jul 22;123(4):044504. doi: 10.1063/1.1946737.
A coherent control algorithm is applied to obtain complex-shaped infrared laser pulses for the selective vibrational excitation of carbon monoxide at the active site of carbonmonoxyhemoglobin, modeled by the six-coordinated iron-porphyrin-imidazole-CO complex. The influence of the distal histidine is taken into account by an additional imidazole molecule. Density-functional theory is employed to calculate a multidimensional ground-state potential energy surface, and the vibrational dynamics as well as the laser interaction is described by quantum wave-packet calculations. At each instant in time, the optimal electric field is calculated and used for the subsequent quantum dynamics. The results presented show that the control scheme is applicable to complex systems and that it yields laser pulses with complex time-frequency structures, which, nevertheless, have a clear physical interpretation.
应用一种相干控制算法来获取复杂形状的红外激光脉冲，用于在以六配位铁 - 卟啉 - 咪唑 - 一氧化碳配合物为模型的碳氧血红蛋白活性位点上对一氧化碳进行选择性振动激发。通过一个额外的咪唑分子来考虑远端组氨酸的影响。采用密度泛函理论计算多维基态势能面，并通过量子波包计算描述振动动力学以及激光相互作用。在每个时刻，计算出最优电场并用于后续的量子动力学。给出的结果表明，该控制方案适用于复杂系统，并且能产生具有复杂时间 - 频率结构的激光脉冲，不过这些脉冲具有清晰的物理解释。
