Quantum Dot-Induced Kinetic Bottleneck in Singlet Exciton Relaxation of Conjugated Polymer Aggregates
Abstract We designed hybrid aggregate model systems with cascade energy alignment from conjugated polymers (CPs) to quantum dots (QDs) to investigate the effects of QDs on CP singlet (S1) excitons. Radiative recombination of S1 excitons occurs within 1 ps in the chlorinated CP/QD hybrid system, indicating an enhanced emissive pathway in an early-time regime. Optimized CP/QD phase separation induces end-on chain orientation and strengthens intrachain excitonic coupling, generating a vertical driving force for intrachain-mediated S1 dissociation along the z-axis. This force interacts with a lateral driving force in the xy-plane—stemming from the conduction-band offset—that biases CP electron density toward QD domains. The interplay between the two forces introduces a kinetic bottleneck that delays exciton relaxation and polaron formation, thereby increasing the probability of radiative recombination and the photoluminescence quantum yield. Our findings provide a strategy to regulate exciton decay pathways and improve CP-based device efficiency.
Authors
- Hyunjin Cho (ORCID: https://orcid.org/0000-0002-2161-4891)
- Jun Sang Cho
- Jaekak Yoo (ORCID: https://orcid.org/0000-0002-8080-8362)
- Jungho Mun (ORCID: https://orcid.org/0000-0002-7290-6253)
- Kyu Young Kim
- Joon I. Jang (ORCID: https://orcid.org/0000-0002-1608-8321)
- Yeon Gyu Kim
- Gui‐Min Kim (ORCID: https://orcid.org/0009-0009-7513-6109)
- Jieun Bang (ORCID: https://orcid.org/0000-0003-1933-5209)
- Boseok Kang (ORCID: https://orcid.org/0000-0003-4295-3881)
- Minyoung Jeong
- Junsuk Rho (ORCID: https://orcid.org/0000-0002-2179-2890)
- Taeyong Ha
- Kilwon Cho (ORCID: https://orcid.org/0000-0003-0321-3629)
- Sein Chung (ORCID: https://orcid.org/0000-0003-3953-5208)
- Mun Seok Jeong (ORCID: https://orcid.org/0000-0002-7019-8089)
- Se Gyo Han
- Kyeong‐Hyeon Lee
- Sungjee Kim (ORCID: https://orcid.org/0000-0002-1289-1926)
- Young Jin Choi (ORCID: https://orcid.org/0000-0002-2604-9051)
- Jaehong Park (ORCID: https://orcid.org/0000-0002-0509-3934)
- Doh C. Lee (ORCID: https://orcid.org/0000-0002-3489-6189)
- Dong Hyeon Kim (ORCID: https://orcid.org/0000-0002-5953-8433)
- Seung Mi Lee (ORCID: https://orcid.org/0000-0002-5956-5853)
- Dongki Lee (ORCID: https://orcid.org/0000-0002-4294-091X)
- Hyuk Gu Yun
- Tae Rim Ko
Institutions
- Pohang University of Science and Technology (KR)
- Georgia Institute of Technology (US)
- Ewha Womans University (KR)
- Sogang University (KR)
- Korea Advanced Institute of Science and Technology (KR)
- Chulalongkorn University (TH)
- Purdue University West Lafayette (US)
- Korea Research Institute of Standards and Science (KR)
- Sejong University (KR)
- University of Illinois Chicago (US)
- University of Chicago (US)
- Ewha Womans University Medical Center (KR)
- Hanyang University Medical Center (KR)
- Hanyang University (KR)
- Sungkyunkwan University (KR)
Publication Details
- Journal
- Macromolecules
- Published
- 2026-09-20
- DOI
- https://doi.org/10.1021/acs.macromol.6c01207
- Primary Topic
- Organic Electronics and Photovoltaics
- Type
- article
- Field-Weighted Citation Impact
- 0.00