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Optical-field driven charge-transfer modulations near composite nanostructures
Nature Communications ( IF 14.7 ) Pub Date : 2020-12-01 , DOI: 10.1038/s41467-020-19423-3
Kwang Jin Lee , Elke Beyreuther , Sohail A. Jalil , Sang Jun Kim , Lukas M. Eng , Chunlei Guo , Pascal André

Optical activation of material properties illustrates the potentials held by tuning light-matter interactions with impacts ranging from basic science to technological applications. Here, we demonstrate for the first time that composite nanostructures providing nonlocal environments can be engineered to optically trigger photoinduced charge-transfer-dynamic modulations in the solid state. The nanostructures explored herein lead to out-of-phase behavior between charge separation and recombination dynamics, along with linear charge-transfer-dynamic variations with the optical-field intensity. Using transient absorption spectroscopy, up to 270% increase in charge separation rate is obtained in organic semiconductor thin films. We provide evidence that composite nanostructures allow for surface photovoltages to be created, which kinetics vary with the composite architecture and last beyond optical pulse temporal characteristics. Furthermore, by generalizing Marcus theory framework, we explain why charge-transfer-dynamic modulations can only be unveiled when optic-field effects are enhanced by nonlocal image-dipole interactions. Our demonstration, that composite nanostructures can be designed to take advantage of optical fields for tuneable charge-transfer-dynamic remote actuators, opens the path for their use in practical applications ranging from photochemistry to optoelectronics.



中文翻译:

复合纳米结构附近的光场驱动电荷转移调制

材料特性的光学活化说明了通过调节光与物质相互作用所具有的潜力,其影响范围从基础科学到技术应用。在这里,我们首次证明了提供非局部环境的复合纳米结构可以被设计为以光学方式触发固态的光致电荷转移动态调制。本文探讨的纳米结构导致电荷分离和复合动力学之间的异相行为,以及线性电荷转移动力学随光场强度的变化。使用瞬态吸收光谱法,有机半导体薄膜中的电荷分离率提高了270%。我们提供的证据表明,复合纳米结构可以产生表面光电压,哪些动力学随复合材料结构而变化,并且超出了光脉冲的时间特性。此外,通过推广马库斯理论框架,我们解释了为什么仅当通过非局部图像-偶极子相互作用增强光场效应时才能揭示电荷转移动态调制的原因。我们的演示表明,可以设计复合纳米结构以利用可调谐电荷转移动态远程执行器的光场,为它们在从光化学到光电的实际应用中的使用开辟了道路。

更新日期:2020-12-01
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