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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Vibrational Mode Coupling to Ultrafast Electron Transfer in [(CN)_5O_sCNRu(NH_3)_5]~- Studied by Femtosecond Infrared Spectroscopy
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Vibrational Mode Coupling to Ultrafast Electron Transfer in [(CN)_5O_sCNRu(NH_3)_5]~- Studied by Femtosecond Infrared Spectroscopy

机译：飞秒红外光谱研究[（CN）_5O_sCNRu（NH_3）_5]〜-中振动模式与超快电子传递的耦合

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摘要

We report studies of the coupling of vibrational excitations to photoinduced electron transfer in a mixed-valence transition metal complex [(CN)_5O_sCNRu(NH_3)_5]~-. Static metal-metal charge transfer (MMCT) spectra, infrared (IR) absorption spectra at different temperatures, resonance Raman spectra, and polarized light transient spectra were taken to reveal the solvent and vibrational coupling to reverse electron transfer. The measured reverse electron transfer rates are greater than 3 * 10~(12)s~(-1). We observed excitations in the non-totally symmetric vibrational mode accompanying the reverse electron transfer process in both formamide (FA) and deuterium oxide (D_2O) solutions. A simulation of the spectral dynamics in FA and D_2O solutions is presented using a kinetic model for vibrational excitation and relaxation. The simulation includes the effect of solvent heating through coupling a low-frequency mode to a medium-frequency oscillator. The vibrational relaxation times of trans CN obtained from the spectral fits show faster vibration relaxation in D_2O than FA,reflecting an overlap of the IR absorption spectra of the solvent and the CN vibrations.
机译：我们报道了在混合价过渡金属络合物[（CN）_5O_sCNRu（NH_3）_5]〜-中振动激发与光致电子转移的耦合研究。记录静态金属-金属电荷转移（MMCT）光谱，不同温度下的红外（IR）吸收光谱，共振拉曼光谱和偏振光瞬态光谱，以揭示溶剂和振动耦合以反向电子转移。测得的反向电子传递速率大于3 * 10〜（12）s〜（-1）。我们在非完全对称振动模式下观察到了伴随着甲酰胺（FA）和氧化氘（D_2O）溶液中的反向电子转移过程的激发。利用动力学模型进行振动激励和弛豫，对FA和D_2O溶液中的光谱动力学进行了仿真。该模拟包括通过将低频模式耦合到中频振荡器来加热溶剂的效果。由光谱拟合获得的反式CN的振动弛豫时间显示D_2O中的振动弛豫速度比FA快，反映了溶剂的IR吸收光谱和CN振动的重叠。

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