journal article·2023-07-14Open access

Dissociative Host-Dopant Bonding Facilitates Molecular Doping in Halide Perovskites

Luis Lanzetta, Luca Gregori, Luis Huerta Hernandez, Anirudh Sharma, Stefanie Kern, Anna M. Kotowska, Abdul-Hamid Emwas, Luis Gutiérrez-Arzaluz, David J. Scurr, Matthew Piggott, Daniele Meggiolaro, Md Azimul Haque, Filippo De Angelis, Derya Baran

ACS Energy Letters· Volume 8· Issue 7

Abstract

Molecular doping is a promising strategy to fine-tune the electronic properties of halide perovskites and accelerate their implementation in next-generation optoelectronics. However, a deeper understanding of the role of host-dopant interactions in these systems is needed to fully exploit the potential of this avenue. Herein, we demonstrate a surface post-treatment strategy employing n-type molecular dopant n-DMBI-H to modulate free hole density in p-type CH 3 NH 3 Sn 0.75 Pb 0.25 I 3 films. We show that the adsorption of n-DMBI-H on surface Sn atoms, followed by the dissociation of an electron-donating hydride from the dopant, facilitates charge transfer to the perovskite and hole trapping at the dissociated hydride. We identify this mechanism as a key factor dictating doping compensation in perovskites, allowing carrier density control within nearly 1 order of magnitude via the dissociated molecular dopant located at film surfaces and grain boundaries. We then exploit n-DMBI-H in perovskite/transport layer junctions, achieving reduced carrier losses and improved contact selectivity and performance in p-i-n, Sn-rich perovskite solar cells. We expect this work to provide carrier density tuning guidelines for a broad range of tin-based perovskite applications.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Perovskite Materials and Applications · Chalcogenide Semiconductor Thin Films · Quantum Dots Synthesis And Properties

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Physical Science and Engineering Division (PSE), KAUST Solar Center (KSC), King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia

Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO), Istituto CNR di Scienze e Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via Elce di Sotto 8, Perugia 06123, Italy

Department of Chemistry, Biology and Biotechnology, University of Perugia, Via Elce di Sotto 8, Perugia 06123, Italy

Advanced Materials and Healthcare Technologies, School of Pharmacy, University of Nottingham, Nottingham NG7 2RD, United Kingdom

Core Laboratories, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia

Physical Science and Engineering Division (PSE), Advanced Membranes and Porous Materials and Catalysis Center, King Abdullah University of Science and Technology (KAUST), Thuwal 23955, Saudi Arabia

Department of Mechanical Engineering, College of Engineering, Prince Mohammad Bin Fahd University, P.O. Box 1664, Al Khobar 31952, Saudi Arabia

SKKU Institute of Energy Science and Technology (SIEST), Sungkyunkwan University, Suwon 440-746, Korea

Funding

Engineering and Physical Sciences Research Council · King Abdullah University of Science and Technology

References (45)

Show source-provided references
1. 10.1021/ic401215x10.1021/ic401215x ↗
2. 10.1021/acsenergylett.7b0124410.1021/acsenergylett.7b01244 ↗
3. 10.1038/s41586-021-03964-810.1038/s41586-021-03964-8 ↗
4. 10.1038/s41578-021-00286-z10.1038/s41578-021-00286-z ↗
5. 10.1021/acs.chemmater.1c0186710.1021/acs.chemmater.1c01867 ↗
6. 10.1038/s41467-018-04028-810.1038/s41467-018-04028-8 ↗
7. 10.1016/j.xcrp.2022.10081210.1016/j.xcrp.2022.100812 ↗
8. 10.1002/adfm.20220487010.1002/adfm.202204870 ↗
9. 10.1021/acs.jpclett.9b0317610.1021/acs.jpclett.9b03176 ↗
10. 10.1021/jacs.9b1163710.1021/jacs.9b11637 ↗
11. 10.1002/adma.20140199110.1002/adma.201401991 ↗
12. 10.1021/acs.jpclett.0c0104810.1021/acs.jpclett.0c01048 ↗
13. 10.1002/adfm.20200559410.1002/adfm.202005594 ↗
14. 10.1039/C9EE01773A10.1039/C9EE01773A ↗
15. 10.1002/adma.20200158110.1002/adma.202001581 ↗
16. 10.1039/D1MA00160D10.1039/D1MA00160D ↗
17. 10.1021/acs.chemrev.1c0058110.1021/acs.chemrev.1c00581 ↗
18. 10.1039/D0TC05861K10.1039/D0TC05861K ↗
19. 10.1039/D0TA01087A10.1039/D0TA01087A ↗
20. 10.1002/adfm.20200178810.1002/adfm.202001788 ↗
21. 10.1002/adfm.20201057210.1002/adfm.202010572 ↗
22. 10.1021/acs.jpclett.9b0219110.1021/acs.jpclett.9b02191 ↗
23. 10.1002/adma.20180450610.1002/adma.201804506 ↗
24. 10.1126/sciadv.abb025310.1126/sciadv.abb0253 ↗
25. 10.1038/s41928-022-00712-210.1038/s41928-022-00712-2 ↗
26. 10.1039/C9TA11794F10.1039/C9TA11794F ↗
27. 10.1021/acsenergylett.7b0063610.1021/acsenergylett.7b00636 ↗
28. 10.1021/acsenergylett.0c0144510.1021/acsenergylett.0c01445 ↗
29. 10.1021/jacs.1c0512210.1021/jacs.1c05122 ↗
30. 10.1038/s41467-021-21487-810.1038/s41467-021-21487-8 ↗
31. 10.1021/acs.chemmater.9b0115010.1021/acs.chemmater.9b01150 ↗
32. 10.1021/jacs.0c0569910.1021/jacs.0c05699 ↗
33. 10.1063/5.004763710.1063/5.0047637 ↗
34. 10.1039/C8EE02751J10.1039/C8EE02751J ↗
35. 10.1021/jacs.5b0314410.1021/jacs.5b03144 ↗
36. 10.1002/aesr.20200003310.1002/aesr.202000033 ↗
37. 10.1002/aelm.20180008710.1002/aelm.201800087 ↗
38. 10.1002/anie.20220234610.1002/anie.202202346 ↗
39. 10.1002/adma.20160474410.1002/adma.201604744 ↗
40. 10.1002/adma.20170599810.1002/adma.201705998 ↗
41. 10.1002/anie.20190241810.1002/anie.201902418 ↗
42. 10.1002/advs.20190304710.1002/advs.201903047 ↗
43. 10.1038/s41467-021-22864-z10.1038/s41467-021-22864-z ↗
44. 10.1021/acsenergylett.8b0068710.1021/acsenergylett.8b00687 ↗
45. 10.1021/jacs.1c0890510.1021/jacs.1c08905 ↗