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<p>Symmetry-breaking charge separation (SB-CS) processes hold significant importance during natural light harvesting and exhibit potential application in the field of organic semiconductors. However, the impact of SB-CS on the excited-state chirality has not yet been fully investigated. Herein, we combine femtosecond time-resolved circularly polarized luminescence (TRCPL) and transient absorption (TA) spectroscopy to study the excited state chirality dynamics of a chiral perylenediimide (Cy-PDI<sub>2</sub>). The extracted time-dependent emission dissymmetry factor <i>g</i><sub>lum</sub>(<i>t</i>) indicates that there is a one order of magnitude enhancement of its CPL emission after the SB-CS process. For the first time, the impact of SB-CS on the generation and evolution of excited state dynamics is revealed, and the underlying mechanism is proposed.</p>

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Unravel excited state chirality dynamics during symmetry-breaking charge separation

  • 期刊论文

  • 发表日期：

    2026年1月5日

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  • Tong Cui,
  • Xueli Wang,
  • Haifeng Pan,
  • Jinquan Chen

摘要

Symmetry-breaking charge separation (SB-CS) processes hold significant importance during natural light harvesting and exhibit potential application in the field of organic semiconductors. However, the impact of SB-CS on the excited-state chirality has not yet been fully investigated. Herein, we combine femtosecond time-resolved circularly polarized luminescence (TRCPL) and transient absorption (TA) spectroscopy to study the excited state chirality dynamics of a chiral perylenediimide (Cy-PDI2). The extracted time-dependent emission dissymmetry factor glum(t) indicates that there is a one order of magnitude enhancement of its CPL emission after the SB-CS process. For the first time, the impact of SB-CS on the generation and evolution of excited state dynamics is revealed, and the underlying mechanism is proposed.