Optical control on the nanoscale via photoresponsive compounds

通过光响应化合物进行纳米级光学控制

• 批准号: 236629596
• 负责人: Professor Dr. Josef Wachtveitl
• 金额: --
• 依托单位: Institut für Physikalische und Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/236629596?language=en
• 关键词: Optical; control; nanoscale; via; photoresponsive

Molecular photoswitches undergo a light-triggered transformation between states with different physicochemical properties, which offers a highly selective, spatiotemporally precise and non-invasive way of nanoscale control. Therefore, photoswitches have become extremely attractive for various applications in chemistry and biotechnology. Nevertheless, the application of photoswitches is relatively rudimentary. Selectivity and efficiency are typically achieved via exhaustive search of appropriate substituents, and photoswitches are triggered via simple excitation fields. Moreover, the application of photoswitches is generally unidimensional, i.e. photoswitches are implemented to control single reactions or properties.Previously, we studied the photochromism of various photoswitches and large photoresponsive constructs and investigated their potential for control at the molecular level. Particularly intriguing aspects of our research are i) the observation of coherent wavepacket motion during the excited state dynamics of photoswitches and ii) the detection of different interactions between the subunits of multiphotochromic compounds (excitonic coupling, steric hindrance, etc.). To address these phenomena, we built a transient absorption set-up for pump-dump/repump-probe and coherent control experiments.Within the new project we will employ our new set-up to investigate the role of coherent vibrational motions in the photochemistry of photoswitches. The experiments will reveal the reactive vibrational modes which will aid the rational design of tailored photoswitches. Further, using multipulse experiments we will study the presence of reactive and non-reactive pathways to gain insight into the complex reaction mechanisms of photoresponsive systems. With the help of multipulse excitation schemes, we will also investigate the intricate molecular interactions between the constituents of multiphotochromic system. Moreover, such excitation schemes will allow us to perform optical programming of the state of multiphotochromic compounds to demonstrate their potential as molecular logics. These type of molecular logics would afford control in multiple dimensions to achieve complex control scenarios.In addition to these projects, we will continue with the development of novel photoswitch designs. We will explore the properties of azoheteroarenes and hydrazones as ultrafast photochromic oscillators, which are of interest for various applications ranging from nanoscale muscles and motors, through information processors, to photopharmacology. We have also initiated work on chiral photoswitches to exploit this molecular property for exerting optical control. Finally, we are working on combining ultrafast spectroscopy and time-resolved crystallography to reach in-depth understanding of the dynamics and the mechanism of operation of photoswitchable biomimetic protein ligands.

分子光开关在不同物理化学性质的状态之间进行光触发转换，提供了一种高选择性、时空精确和非侵入性的纳米尺度控制方式。因此，光开关在化学和生物技术中的各种应用都变得非常有吸引力。尽管如此，光开关的应用还是相对初级的。选择性和效率通常是通过穷尽地寻找合适的取代基来实现的，而光开关是通过简单的激发场来触发的。此外，光开关的应用通常是一维的，即光开关是用来控制单个反应或性质的。在此之前，我们研究了各种光开关和大型光响应结构的光致变色，并在分子水平上研究了它们的控制潜力。我们的研究特别有趣的方面是：i)在光开关的激发态动力学过程中观察到相干波包运动；ii)检测到多个光致变色化合物亚单位之间的不同相互作用(激子耦合、空间位阻等)。为了解决这些现象，我们建立了一个用于泵浦-倾倒/再泵浦-探测和相干控制实验的瞬时吸收装置。在这个新的项目中，我们将使用我们的新装置来研究相干振动运动在光开关的光化学中的作用。实验将揭示反应振动模式，这将有助于合理设计定制的光开关。此外，利用多脉冲实验，我们将研究反应和非反应途径的存在，以深入了解光响应系统的复杂反应机制。在多脉冲激发方案的帮助下，我们还将研究多光致变色体系各组分之间复杂的分子相互作用。此外，这种激发方案将允许我们对多光致变色化合物的状态进行光学编程，以展示它们作为分子逻辑的潜力。这些类型的分子逻辑将提供多个维度的控制，以实现复杂的控制场景。除了这些项目，我们还将继续开发新的光开关设计。我们将探索偶氮杂芳烃和肼类化合物作为超快光致变色振荡器的性质，这对从纳米级肌肉和马达到信息处理器到光药学的各种应用都很有意义。我们还开始了手性光开关的研究工作，以利用这一分子特性来施加光学控制。最后，我们正致力于将超快光谱和时间分辨结晶学相结合，以深入了解可光切换的仿生蛋白质配体的动力学和操作机制。