Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
Publication date: 16th December 2024
Over the past decade, metal halide semiconductors have emerged as promising materials for solar cell applications. While lead halide semiconductors have achieved remarkable power conversion efficiencies, now exceeding 26%, Pb(II) toxicity and alloying-stability issues have raised the urgency of developing nontoxic, stable, and environmentally friendly alternatives. As a result, a catalogue of bismuth-based semiconductors (e.g., double perovskites, rudorffites, and others) has been the subject of intense investigation.[1] However, record power conversion efficiencies for this new class of materials are currently limited at around ~6%, thus prompting new research efforts to explore and eliminate current limitations to performance. This poster will delve deeper into how ultrafast charge-carrier localisation processes fundamentally limit charge-carrier transport in several bismuth-based halides and chalcogenides, and will present possible strategies to overcome this issue.[2-7]
Focusing on the archetypal silver-bismuth based double perovskite Cs2AgBiBr6, we will show how the rapid decays in terahertz photoconductivity and their temperature dependence reveal an ultrafast localization of free charge-carriers to a small polaronic state. The implications of the resulting hopping-like transport regime on charge-carrier transport will be further discussed. For instance, alloying Cs2AgBiBr6 with Cs2AgSbBr6 on the trivalent metal site interestingly leads to significantly stronger self-localisation.4 This effect results from the more local probing of the energetic landscape by small polarons, which turns alloyed low-energy sites – in this case, Sb (III) sites – effectively into traps, and significantly hinders charge-carrier transport. Delving deeper into the causes of this localisation process, I will discuss the role of the electronic structure and the electronic dimensionality. To do so, the role of Ag and Bi cation-ordering in AgBiS2 nanocrystals thin films will be examined.[5] By tuning the Ag/Bi cation arrangement via cation-disorder engineering, the combination of a higher electronic dimensionality and a more ordered electronic landscape will be shown to assist in mitigating the effect of this localisation in silver-bismuth semiconductors.
Overall, the ultrafast localisation of charge carriers emerges as a formidable challenge for the new class of bismuth-based semiconductors and their application in renewable energy applications. The findings presented in this post explore the underlying causes of such localization and its effects on charge-carrier transport. Furthermore, possible strategies to overcome the charge-carrier localisation issue are presented.
(1) Huang et al. Nanotechnology 2021, 32, 132004.
(2) Huang, Kavanagh, Righetto et al. Nature Communications 2022, 13, 4960.
(3) Jia*, Righetto* et al. ACS Energy Letters 2023, 8, 1485-1492.
(4) Righetto et al. The Journal of Physical Chemistry Letters 2023, 14, 10340-10347.
(5) Righetto et al. Advanced Materials 2023, 35, 2305009.
(6) Lal, Righetto et al. Films. The Journal of Physical Chemistry Letters 2023, 14, 6620-6629.
(7) Putland, Righetto et al. Advanced Energy Materials 2024, 2303313.
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