2026-09-19T06:49:01Zhttps://dspace.mit.edu/server/oai/requestoai:dspace.mit.edu:1721.1/794962022-01-13T07:54:01Zcom_1721.1_7582com_1721.1_7581col_1721.1_131022
Marc A. Baldo.
Lee, Jiye
Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science.
Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science
2013-07-10T14:49:28Z
2013-07-10T14:49:28Z
2013
2013
http://hdl.handle.net/1721.1/79496
849650026
Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Electrical Engineering and Computer Science, 2013.
Cataloged from PDF version of thesis.
Includes bibliographical references (p. 131-151).
The efficiency of a solar cell is restricted by the "single junction limit," whereby photons with energy higher than the bandgap lose energy by thermalization. Singlet exciton fission splits a high-energy molecular excitation ("singlet" exciton) into a pair of lowenergy ones ("triplet" excitons). In solar cells, it promises to generate two electrons per photon, potentially overcoming the singlet junction efficiency limit. In this thesis, we present singlet-fission-based photovoltaic cells that generate more than one electron per photon. We first demonstrate organic photodetectors with quantum efficiencies reaching 100% by exploiting singlet exciton fission. Through study of the magnetic field dependence of the fission process, we find an optimum thickness of singlet fission layers that guarantees the nearly 100% conversion of a singlet into two triplets. By employing an exciton blocking layer and a light trapping scheme to the solar cell, we demonstrate the peak external quantum efficiency exceeding 100% in the visible spectrum. It is the first time that any solar cell has generated more than one electron per photon outside the UV spectrum. We also build a simple model that predicts the rate of singlet fission through intermolecular coupling, enabling rational designs of singlet fission molecules and devices. Finally, we propose a future direction-generating three electrons per photon. As a step toward this goal, we demonstrate singlet exciton fission in hexacene, whose energetics may allow a singlet to split into three triplets.
by Jiye Lee.
Ph.D.
151 p.
eng
Massachusetts Institute of Technology
M.I.T. theses are protected by
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http://dspace.mit.edu/handle/1721.1/7582
Electrical Engineering and Computer Science.
Singlet fission photovoltaics
Thesis
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Publication
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<Abstract>The efficiency of a solar cell is restricted by the "single junction limit," whereby photons with energy higher than the bandgap lose energy by thermalization. Singlet exciton fission splits a high-energy molecular excitation ("singlet" exciton) into a pair of lowenergy ones ("triplet" excitons). In solar cells, it promises to generate two electrons per photon, potentially overcoming the singlet junction efficiency limit. In this thesis, we present singlet-fission-based photovoltaic cells that generate more than one electron per photon. We first demonstrate organic photodetectors with quantum efficiencies reaching 100% by exploiting singlet exciton fission. Through study of the magnetic field dependence of the fission process, we find an optimum thickness of singlet fission layers that guarantees the nearly 100% conversion of a singlet into two triplets. By employing an exciton blocking layer and a light trapping scheme to the solar cell, we demonstrate the peak external quantum efficiency exceeding 100% in the visible spectrum. It is the first time that any solar cell has generated more than one electron per photon outside the UV spectrum. We also build a simple model that predicts the rate of singlet fission through intermolecular coupling, enabling rational designs of singlet fission molecules and devices. Finally, we propose a future direction-generating three electrons per photon. As a step toward this goal, we demonstrate singlet exciton fission in hexacene, whose energetics may allow a singlet to split into three triplets.</Abstract>
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