Manipulating Triplet Yield through Control of Symmetry-Breaking Charge Transfer

被引：57

作者：

Das, Saptaparna ^{[1
]}

Thornbury, William G. ^{[2
]}

Bartynski, Andrew N. ^{[2
]}

Thompson, Mark E. ^{[1
]}

Bradforth, Stephen E. ^{[1
]}

机构：

[1] Univ Southern Calif, Dept Chem, Los Angeles, CA 90089 USA

[2] Univ Southern Calif, Dept Chem Engn, Los Angeles, CA 90089 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2018年 / 9卷 / 12期

基金：

美国国家科学基金会;

关键词：

OPEN-CIRCUIT VOLTAGE; ANNIHILATION UP-CONVERSION; SINGLET OXYGEN GENERATION; EXCITON BINDING-ENERGY; ORGANIC SOLAR-CELLS; CONJUGATED POLYMERS; TRANSFER STATES; BODIPY-DIMERS; RADICAL-PAIR; DESIGN RULES;

D O I：

10.1021/acs.jpclett.8b01237

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The efficiency of an organic solar cell depends on the efficacy of exciton diffusion and dissociation processes, and this can be enhanced by reducing the exciton binding energy and increasing the exciton lifetime. Zinc chlorodipyrrin (ZCl) complexes exhibit reduced exciton binding energy due to ultrafast generation of intramolecular charge transfer (ICT) states via symmetry-breaking charge transfer in polar media. This Letter explores the fate of the ICT states using nanosecond transient absorption. In cyclohexane, ZCl undergoes intersystem crossing to produce triplets with similar to 8 ns time constant (similar to 30% yield), and no ICT states are generated. However, in more polar solvents, triplets are generated within 1 ns via ICT state recombination with similar to 3 times higher yield than produced via ISC. This high triplet yield in toluene (89%) and acetonitrile (76%) via ICT state recombination is a beneficial pathway to spin-protect the excited state decay for additional charge generation from triplet excited states.

引用

页码：3264 / 3270

页数：13

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