Photoselective adaptive femtosecond quantum control in the liquid phase
Photoselective adaptive femtosecond quantum control in the liquid phase
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DOI：
10.1038/35102037
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发表时间：
2001-11-01
期刊：
影响因子：
64.8
通讯作者：
Gerber, G
中科院分区：
文献类型：
--
作者：
Brixner, T;Damrauer, NH;Gerber, G
相干光源可以利用时域和频域的干涉现象来操纵光-物质相互作用的结果。在这个新兴的“量子控制”领域（1-6），一个强大的工具是飞秒激光脉冲的自适应成形（7-10），例如，导致选择性分子激发。这种方法的基础是，被研究的量子系统本身通过迭代循环引导自动搜索最适合完成实验者设计的控制任务的相干光场（11）。因此，该方法是控制复杂实验的理想方法（7,12-20）。迄今为止，该技术在分子系统上的所有演示都集中在控制相同分子中光诱导反应的结果，而很少关注选择性地控制不同分子的混合物。在这里，我们报道了溶液中两种不同的电子和结构复杂的染料分子同时但选择性的多光子激发。尽管单参数变化（波长，强度或线性啁啾控制）失败，自适应飞秒脉冲整形可以揭示复杂的激光场，以实现化学选择性分子激发。此外，我们的结果证明了溶质分子的相相干性在溶剂环境中持续超过100 fs。
Coherent light sources can be used to manipulate the outcome of light-matter interactions by exploiting interference phenomena in the time and frequency domain. A powerful tool in this emerging field of 'quantum control'(1-6) is the adaptive shaping of femtosecond laser pulses(7-10), resulting, for instance, in selective molecular excitation. The basis of this method is that the quantum system under investigation itself guides an automated search, via iteration loops, for coherent light fields best suited for achieving a control task designed by the experimenter(11). The method is therefore ideal for the control of complex experiments(7,12-20). To date, all demonstrations of this technique on molecular systems have focused on controlling the outcome of photo-induced reactions in identical molecules, and little attention has been paid to selectively controlling mixtures of different molecules. Here we report simultaneous but selective multi-photon excitation of two distinct electronically and structurally complex dye molecules in solution. Despite the failure of single parameter variations (wavelength, intensity, or linear chirp control), adaptive femtosecond pulse shaping can reveal complex laser fields to achieve chemically selective molecular excitation. Furthermore, our results prove that phase coherences of the solute molecule persist for more than 100 fs in the solvent environment.