Mechanochemical Tuning of Pyrene Absorption Spectrum Using Force Probes
Mechanochemical Tuning of Pyrene Absorption Spectrum Using Force Probes
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DOI：
10.1021/acs.jctc.6b01020
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发表时间：
2017-02-01
影响因子：
5.5
通讯作者：
Manuel Frutos, Luis
中科院分区：
文献类型：
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作者：
Angel Fernandez-Gonzalez, Miguel;Rivero, Daniel;Manuel Frutos, Luis
发色团吸收光谱的控制是许多光化学和光物理过程的一个基本方面，因为它构成了全球光诱导过程的第一步。在这里，我们探索使用机械力来调制光吸收过程。具体而言，我们开发了一个计算形式主义，用于确定允许的吸收光谱的全局调谐的机械力的类型。这种控制延伸到激发波长、吸收带重叠和振荡器强度。这些最佳力的确定使我们能够合理地指导新的机械响应生色团的设计。芘已被选为应用这些计算工具的案例研究，因为显着的吸收光谱信息是可用于发色团以及不同的应变衍生物。此外，芘具有很大的灵活性，这使得它成为一个很好的系统来测试包括力探针作为对系统施加力的策略。
Control of absorption spectra in chromophores is a fundamental aspect of many photochemical and photophysical processes as it constitutes the first step of the global photoinduced process. Here we explore the use of mechanical forces to modulate the light absorption process. Specifically, we develop a computational formalism for determining the type of mechanical forces permitting a global tuning of the absorption spectrum. This control extends to the excitation wavelength, absorption bands overlap, and oscillator strength. The determination of these optimal forces permits us to rationally guide the design of new mechano-responsive chromophores. Pyrene has been chosen as the case study for applying these computational tools because significant absorption spectra information is available for the chromophore as well as for different strained derivatives. Additionally, pyrene presents a large flexibility, which makes it a good system to test the inclusion of force probes as the strategy to exert forces on the system.