Abstract
The introduction of a self-adaptive molecular switch is an appealing strategy to achieve complete charge separation (CS) in donor-acceptor (D-A) systems. Here, we designed donor-switch-acceptor (D-S-A) systems using a platinum(II) terpyridyl complex as the acceptor, dimethyldihydropyrene/cyclophanediene (DHP/CPD) as the bridge, and methoxybenzene, thieno[3,2-b]thiophene, 2,2'-bifuran, and 4,8-dimethoxybenzo[1,2-b:4,5-b']difuran as donors, respectively. We then systematically studied the whole opto-electronic conversion process of the donor-DHP/CPD-acceptor (D-DHP/CPD-A) systems based on time-dependent density functional theory, time-dependent ultrafast electron evolution, and electron transport property calculations. We first found that the substitution of -CH3 by -H and -CN groups in DHP/CPD can enlarge the range of the adsorption wavenumber in opto-electric conversion. Then the light absorption induces the cationization of DHP switch, largely accelerating the forth-isomerization to CPD form. Once the D-CPD-A molecule is formed, the poor conjugation can realize the complete CS state by inhibiting the radiative and nonradiative charge recombinations. Finally, the repeatable and complete CS can be achieved through the automatic back-isomerization of CPD to DHP. The present work provides valuable insights into design of D-S-A systems for practical utilization of molecule-based solar harvesting.
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