Splitting photons: Singlet fission in nanocrystal-molecule hybrid structures
The goal of this research is to enable all the energy contained in sunlight to be harvested by making full use of the energy contained in the blue and green wavelengths of light. Current systems are unable to extract all of the energy available from photons in this wavelength range due to rapid relaxation processes that dissipate a fraction of the energy as heat. In this work, inexpensive, earth-abundant components capable of supporting multi-excitonic processes involving more than one tightly bound excited state are investigated as a way to exceed the Shockley-Queisser limit. This research will examine hybrid organic-inorganic nanostructures capable of singlet fission, a process by which one high-energy spin-singlet state is converted into two lower-energy spin-triplet states, and subsequent triplet exciton transfer. Specifically, the organic molecules diphenylhexatriene and tetracene that maximally absorb blue light and are known to exhibit singlet fission will be bound to lead chalcogenide nanocrystals. A variety of steady-state and time-resolved spectroscopic techniques will be used to study the transfer of energy from spin-triplet excitons that are created in the organic molecules to the nanoparticle acceptors. The hybrid nanostructures here will be fully characterized both in solution or thin film via electronic absorption and photoluminescence spectroscopy, nuclear magnetic resonance spectroscopy, high-resolution mass spectrometry, transmission electron microscopy, photoelectron spectroscopy, time correlated single photon counting and transient absorption experiments. The effect of molecular and nanocrystal structure on the electronic coupling between the hybrid components will be examined to establish fundamental relationships between structure and triplet energy transfer efficiency. The findings will be directly applicable to a potential tetracene-silicon platform that may ultimately enhance the power conversion efficiency of silicon solar cells.
- Research Organization:
- Univ. of California, Riverside, CA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
- DOE Contract Number:
- SC0018969
- OSTI ID:
- 1970088
- Report Number(s):
- DOE-UCR-18969
- Resource Relation:
- Related Information: List of Publications Supported by this Award1. T. Huang, T. Koh, J. Schwan, T. Tran, P. Xia, K. Wang, L. Mangolini, M. L. Tang, S. T. Roberts, " Bidirectional Triplet Exciton Transfer Between Silicon Nanocrystals and Perylene", Chem. Sci., 12, 6737, 2021.2. Z. Xu, Z. Huang, T. Jin, T. Lian, M. L. Tang "Mechanistic understanding and rational design of quantum dot/mediator interfaces for efficient photon upconversion", Acc. Chem. Res., 54, 70, 2021. (invited, selected for journal cover)3. Z. Huang, Z. Xu, T. Huang, V. Gray, K. Moth-Poulsen, T. Lian, M. L. Tang "Evolution from tunneling to hopping mediated triplet energy transfer from quantum dots to molecules", J. Am. Chem. Soc., 142, 17581, 2020.4. Z. Xu, Z. Huang, C. Li, T. Huang, F. A. Evangelista, M. L. Tang, T. Lian, " Tuning the quantum dot (QD)/mediator interface for optimal efficiency of QD-sensitized near-infrared-to-visible photon upconversion systems", ACS Appl. Mater. Interfaces, 12, 36558, 2020.5. J. De Roo, Z. Huang, N. J. Schuster, L. Hamachi, D. N. Congreve, Z. Xu, D. A. Fishman, T. Lian, J. Owen, M. L. Tang, "Anthracene Diphosphate Ligands for CdSe Nanocrystals: Molecular Design for Efficient Upconversion" Chem. Mater.,32, 1461, 2020.6. P. Xia, E. K. Raulerson, D. Coleman, C. S. Gerke, L. Mangolini, M. L. Tang, S. T. Roberts, "Achieving Spin-triplet Exciton Transfer between Silicon and Molecular Acceptors for Photon Upconversion" Nature Chem., 12, 137, 2020.7. Z. Huang, Z. Xu, M. Mahboub, Z. Liang, P. Jaimes, P. Xia, K. Graham, M. L. Tang, T. Lian, "Enhanced near-infrared-to-visible upconversion by synthetic control of PbS nanocrystal triplet photosensitizers" J. Am. Chem. Soc., 141, 9769, 2019.
- Country of Publication:
- United States
- Language:
- English
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