Distinct Mechanisms of Triplet Pair Decay in Amorphous and Crystalline Heteroacene Thin Films

IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL
Brandon K. Rugg, Angana De, Sarath Santhakumar, Qiushi Ma, Brian Fluegel, Karl J. Thorley, John E. Anthony, Libai Huang, Justin C. Johnson
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Abstract

Triplet pairs (TT) in crystalline molecular semiconductors have unique spin properties of interest for quantum information or enhancing solar photoconversion. The population and diffusion dynamics of TT have been the subject of recent studies, both in covalent dimers and in crystalline systems. Here, we monitor the triplet population in neat polycrystalline and amorphous films of a heteroacene with known TT spectral properties and tunable spin polarization depending on the intermolecular geometry. Transient measurements reveal an anomalous power dependence in polycrystalline films that we attribute to the fast diffusion and interaction of dissociated triplet pairs confined to one-dimensional stacks of strongly coupled molecules. The nongeminate triplet interaction after dephasing facilitates conversion to the triplet 3TT and eventually T1+S0. Amorphous films have no power dependence and proceed directly from 1TT to 3TT and subsequently T1+S0 via state mixing facilitated by nonparallel geometries and weak exchange coupling.

Abstract Image

晶体分子半导体中的三重子对(TT)具有独特的自旋特性,可用于量子信息或增强太阳能光电转换。TT 的种群和扩散动力学是近期共价二聚体和晶体系统研究的主题。在这里,我们对具有已知 TT 光谱特性和可调自旋极化(取决于分子间几何形状)的杂芳烯的整齐多晶和无定形薄膜中的三重态种群进行了监测。瞬态测量揭示了多晶薄膜中的反常功率依赖性,我们将其归因于局限于强耦合分子一维堆栈中的解离三重子对的快速扩散和相互作用。去相后的非均相三重态相互作用促进了向三重态 3TT 的转换,并最终促进了 T1+S0 的转换。无定形薄膜没有功率依赖性,通过非平行几何结构和弱交换耦合促进的状态混合,直接从 1TT 转变为 3TT,并最终转变为 T1+S0。
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来源期刊
ChemPhotoChem
ChemPhotoChem Chemistry-Physical and Theoretical Chemistry
CiteScore
5.80
自引率
5.40%
发文量
165
期刊介绍: Light plays a crucial role in natural processes and leads to exciting phenomena in molecules and materials. ChemPhotoChem welcomes exceptional international research in the entire scope of pure and applied photochemistry, photobiology, and photophysics. Our thorough editorial practices aid us in publishing authoritative research fast. We support the photochemistry community to be a leading light in science. We understand the huge pressures the scientific community is facing every day and we want to support you. Chemistry Europe is an association of 16 chemical societies from 15 European countries. Run by chemists, for chemists—we evaluate, publish, disseminate, and amplify the scientific excellence of chemistry researchers from around the globe.
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