石墨烯- ptcdi - tiopc三层异质结构中的长寿命电荷转移激子

IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL
Ryan J. Scott, Neno Fuller, Adithya Sadanandan, Pavel Valencia-Acuna, Wai-Lun Chan, Qunfei Zhou* and Hui Zhao*, 
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引用次数: 0

摘要

利用瞬态吸收和光致发光光谱技术研究了石墨烯、苝四羧基二亚胺(PTCDI)和酞菁钛(TiOPc)之间的界面激发转移。光致发光猝灭和瞬态吸收测量均证实PTCDI和TiOPc之间存在ii型界面。虽然石墨烯/PTCDI界面有望表现出i型行为,但瞬态吸收测量表明,只有电子从PTCDI转移到石墨烯,没有空穴转移的证据。密度函数理论计算揭示了从石墨烯到PTCDI的显著基态电子转移,导致能带弯曲,阻止了激发空穴从PTCDI转移到石墨烯。在石墨烯/PTCDI/TiOPc的三层异质结构中利用了这一特征,其中石墨烯和TiOPc中光激发电子和空穴的空间分离分别导致形成寿命约为500 ps的长寿命光激发。此外,空间分辨的瞬态吸收测量揭示了这些激发的不动性质,证实它们是电荷转移激子,而不是自由电子和空穴。这些结果为复杂的层间光激发转移特性提供了有价值的见解,并证明了对这种杂化异质结构中层数和光载流子的复合寿命的精确控制。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Long-Lived Charge-Transfer Excitons in a Graphene–PTCDI–TiOPc Trilayer Heterostructure

Long-Lived Charge-Transfer Excitons in a Graphene–PTCDI–TiOPc Trilayer Heterostructure

Excitation transfer across the interfaces between graphene, perylenetetracarboxylic diimide (PTCDI), and titanyl phthalocyanine (TiOPc) was studied by using transient absorption and photoluminescence spectroscopy. Both photoluminescence quenching and transient absorption measurements confirm the presence of a type-II interface between PTCDI and TiOPc. While the graphene/PTCDI interface is expected to exhibit type-I behavior, transient absorption measurements indicate that only electrons transfer from PTCDI to graphene, with no evidence of hole transfer. Density functional theory calculations reveal significant ground-state electron transfer from graphene to PTCDI, resulting in band bending that prevents excited holes from transferring from PTCDI to graphene. This feature is exploited in a trilayer heterostructure of graphene/PTCDI/TiOPc, where the spatial separation of photoexcited electrons and holes in graphene and TiOPc, respectively, leads to the formation of long-lived photoexcitations with a lifetime of approximately 500 ps. Furthermore, spatially resolved transient absorption measurements reveal the immobile nature of these excitations, confirming that they are charge-transfer excitons rather than free electrons and holes. These results provide valuable insights into the complex interlayer photoexcitation transfer properties and demonstrate precise control over the layer population and the recombination lifetime of photocarriers in such hybrid heterostructures.

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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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