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Colloidal quantum dots (CQDs) are of interest for photovoltaic applications such as flexible and multijunction solar cells, where solution processability and infrared absorption are crucial; however, current CQD solar cell performance is limited by the hole transport layers (HTLs) used in the cells. We report on a method to develop new HTLs for the highest-performing PbS CQD solar cell architecture by tuning the stoichiometry via sulfur infiltration of the p-type CQD HTL to increase its doping density and carrier mobility. Using SCAPS simulations, we predict that increased doping density and mobility should improve the performance of the solar cells. We show that sulfur doping of the current HTL is a facile and effective method to boost the performance of CQD photovoltaics.
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Structurally Driven Ultrafast Charge Funneling in Organic Bulk Heterojunction Hole Transport Layer for Efficient Colloidal Quantum Dot Photovoltaics
Abstract Nanoscopic packing structures crucially determine the charge conduction and the consequent functionalities of organic semiconductors including bulk heterojunctions (BHJs), which are dependent on various processing parameters. Today's high‐performance colloidal quantum dot photovoltaics (CQDPVs) employ functional organic semiconductors as a hole transport layer (HTL). However, the processing of those films replicates a protocol dedicated to high‐performance organic PVs, and thus little is known about how to control the molecular packing structures to maximize the hole extraction function of the HTLs. Herein, it is uncovered that the random‐oriented, but closer‐packed BHJ crystallites, constructed by 1,2‐dichlorobenzene (o‐DCB) as a solvent, allow exceptional charge conduction vertically across the film and restrict diffusion‐driven charge transfer process, enabling ultrafast hole funneling from CQD to BHJ to be extracted. As a result, a power conversion efficiency of 13.66% with high photocurrent >34 mA cm−2is achieved by employingo‐DCB‐processed BHJ HTL, far exceeding the performance of the CQDPV solely employing neat polymer HTL. A charge conduction mechanism associated with the BHJ HTL structure suppressing the bimolecular recombination is proposed. This works not only suggests key principles to control the packing structures of organic HTLs but also opens a new avenue to boost optoelectronic performance.
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- Award ID(s):
- 2043205
- PAR ID:
- 10415921
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Energy Materials
- Volume:
- 13
- Issue:
- 20
- ISSN:
- 1614-6832
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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