Pathways to New Applications for Quantum Control.
Pathways to New Applications for Quantum Control.
复制标题
量子控制新应用的途径。
DOI：
10.1021/acs.accounts.8b00244
复制
发表时间：
2018
影响因子：
18.3
通讯作者：
R. de Vivie
中科院分区：
文献类型：
--
作者：
D. Keefer;R. de Vivie
1998年，利用整形激光脉冲进行了首次成功应用于分子框架的量子控制实验，优化了不同有机金属反应通道之间的支化比。这项工作在接下来的十年里引发了量子控制领域的巨大活动，并且在气相、液相，甚至在光捕获复合物等生物相关分子中实现了不同的优化目标。伴随和领先这一发展的是理论量子控制模拟的重要进展。他们预测了几种控制场景，并解释了量子控制实验如何以及为何进行。在分子科学中多次成功地证明概念之后，最大的挑战是扩展其巨大的概念潜力，即能够直接引导核和/或电子运动到更多的应用中。在本报告中，根据最近的几项进展，我们对分子量子控制领域目前的发展状况，特别是我们认为在不久的将来有希望的应用领域进行了个人评估。 One of these paths leads to synthetic chemistry.新型药物化合物或天然产物的合成通常涉及许多合成步骤，每一步都会消耗资源并降低产品收率。整形激光脉冲可能充当光子试剂并缩短所需产品的合成路线。化学合成通常在溶液中进行，通过在我们的量子控制模拟中包含显式溶剂分子，我们能够确定它们对化学反应的高度不均匀影响以及这如何影响潜在的量子控制。更重要的是，我们通过一个综合相关的例子证明，这些复杂性在理论上是可以克服的，并且可以优化激光脉冲以引发所需的碳-碳键形成。将这一点与最近出现的流动化学概念结合起来，为激光脉冲的应用带来了一些实际优势，我们希望鼓励实验小组利用这一概念。另一条道路是通过对常用激光脉冲优化算法（最优控制理论，OCT）的一些补充而开辟的，其中一些是我们小组开发的。 OCT 算法本身是一个纯粹的数学优化过程，与实验要求没有直接关系。这意味着通常通过 OCT 优化获得的电场与可以通过实验实现的激光脉冲不同。然而，前面提到的补充旨在缩小与实验的差距。在我们小组最近的一项量子控制研究中，这些算法的发展取得了成果。我们能够提出一种成形激光脉冲，它可以在尿嘧啶的激发态下诱导出长寿命的波包。这可能为致力于研究 DNA 和 RNA 生物光损伤形成的新实验铺平道路。由于扩展的 OCT 算法，我们建议的脉冲非常简单，并且满足实验上可访问的所有标准。
In 1998, the first successful quantum control experiment with application to a molecular framework was conducted with a shaped laser pulse, optimizing the branching ratio between different organometallic reaction channels. This work induced a vast activity in quantum control during the next 10 years, and different optimization aims were achieved in the gas phase, liquid phase, and even in biologically relevant molecules like light-harvesting complexes. Accompanying and preceding this development were important advances in theoretical quantum control simulations. They predicted several control scenarios and explained how and why quantum control experiments work. After many successful proofs of concept in molecular science, the big challenge is to expand its huge conceptual potential of directly being able to steer nuclear and/or electronic motion to more applied implementations. In this Account, based on several recent advances, we give a personal evaluation of where the field of molecular quantum control is at the moment and especially where we think promising applications can be in the near future. One of these paths leads to synthetic chemistry. The synthesis of novel pharmaceutical compounds or natural products often involves many synthetic steps, each one devouring resources and lowering the product yield. Shaped laser pulses can possibly act as photonic reagents and shorten the synthetic route toward the desired product. Chemical synthesis usually takes place in solution, and by including explicit solvent molecules in our quantum control simulations, we were able to identify their highly inhomogeneous influence on chemical reactions and how this affects potential quantum control. More important, we demonstrated for a synthetically relevant example that these complications can be overcome in theory, and laser pulses can be optimized to initiate the desired carbon-carbon bond formation. Putting this into context with the recently emerging concept of flow chemistry, which brings several practical advantages to the application of laser pulses, we want to encourage experimental groups to exploit this concept. Another path was opened by several additions to the commonly used laser pulse optimization algorithm (optimal control theory, OCT), several of which were developed in our group. The OCT algorithm as such is a purely mathematical optimization procedure, with no direct relation to experimental requirements. This means that usually the electric fields obtained out of OCT optimizations do not resemble laser pulses that can be achieved experimentally. However, the previously mentioned additions are aimed at closing the gap toward the experiment. In a recent quantum control study of our group, these algorithmic developments came to fruition. We were able to suggest a shaped laser pulse which can induce a long-living wave packet in the excited state of uracil. This might pave the way for novel experiments dedicated to investigating the formation of biological photodamage in DNA and RNA. The pulse we suggest is surprisingly simple because of the extended OCT algorithm and fulfills all criteria to be experimentally accessible.