Contrasting Ultra-Low Frequency Raman and Infrared Modes in Emerging Metal Halides for Photovoltaics
Lattice dynamics are critical to photovoltaic material performance, governing dynamic disorder, hot-carrier cooling, charge-carrier recombination, and transport. Soft metal-halide perovskites exhibit particularly intriguing dynamics, with Raman spectra exhibiting an unusually broad low-frequency res...
| Main Authors: | , , , , , , , , , , , , , , , |
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| Format: | Journal article |
| Language: | English |
| Published: |
American Chemical Society
2024
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| _version_ | 1826314842731970560 |
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| author | Lim, VJ Righetto, M Yan, S Patel, JB Siday, T Putland, B McCall, KM Sirtl, MT Kominko, Y Peng, J Lin, Q Bein, T Kovalenko, M Snaith, HJ Johnston, MB Herz, LM |
| author_facet | Lim, VJ Righetto, M Yan, S Patel, JB Siday, T Putland, B McCall, KM Sirtl, MT Kominko, Y Peng, J Lin, Q Bein, T Kovalenko, M Snaith, HJ Johnston, MB Herz, LM |
| author_sort | Lim, VJ |
| collection | OXFORD |
| description | Lattice dynamics are critical to photovoltaic material performance, governing dynamic disorder, hot-carrier cooling, charge-carrier recombination, and transport. Soft metal-halide perovskites exhibit particularly intriguing dynamics, with Raman spectra exhibiting an unusually broad low-frequency response whose origin is still much debated. Here, we utilize ultra-low frequency Raman and infrared terahertz time-domain spectroscopies to provide a systematic examination of the vibrational response for a wide range of metal-halide semiconductors: FAPbI3, MAPbI x Br3–x , CsPbBr3, PbI2, Cs2AgBiBr6, Cu2AgBiI6, and AgI. We rule out extrinsic defects, octahedral tilting, cation lone pairs, and “liquid-like” Boson peaks as causes of the debated central Raman peak. Instead, we propose that the central Raman response results from an interplay of the significant broadening of Raman-active, low-energy phonon modes that are strongly amplified by a population component from Bose–Einstein statistics toward low frequency. These findings elucidate the complexities of light interactions with low-energy lattice vibrations in soft metal-halide semiconductors emerging for photovoltaic applications. |
| first_indexed | 2024-09-25T04:21:43Z |
| format | Journal article |
| id | oxford-uuid:3301ec65-b683-4289-9050-2a35b7d15d96 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-12-09T03:14:33Z |
| publishDate | 2024 |
| publisher | American Chemical Society |
| record_format | dspace |
| spelling | oxford-uuid:3301ec65-b683-4289-9050-2a35b7d15d962024-10-16T09:39:52ZContrasting Ultra-Low Frequency Raman and Infrared Modes in Emerging Metal Halides for PhotovoltaicsJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:3301ec65-b683-4289-9050-2a35b7d15d96EnglishJisc Publications RouterAmerican Chemical Society2024Lim, VJRighetto, MYan, SPatel, JBSiday, TPutland, BMcCall, KMSirtl, MTKominko, YPeng, JLin, QBein, TKovalenko, MSnaith, HJJohnston, MBHerz, LMLattice dynamics are critical to photovoltaic material performance, governing dynamic disorder, hot-carrier cooling, charge-carrier recombination, and transport. Soft metal-halide perovskites exhibit particularly intriguing dynamics, with Raman spectra exhibiting an unusually broad low-frequency response whose origin is still much debated. Here, we utilize ultra-low frequency Raman and infrared terahertz time-domain spectroscopies to provide a systematic examination of the vibrational response for a wide range of metal-halide semiconductors: FAPbI3, MAPbI x Br3–x , CsPbBr3, PbI2, Cs2AgBiBr6, Cu2AgBiI6, and AgI. We rule out extrinsic defects, octahedral tilting, cation lone pairs, and “liquid-like” Boson peaks as causes of the debated central Raman peak. Instead, we propose that the central Raman response results from an interplay of the significant broadening of Raman-active, low-energy phonon modes that are strongly amplified by a population component from Bose–Einstein statistics toward low frequency. These findings elucidate the complexities of light interactions with low-energy lattice vibrations in soft metal-halide semiconductors emerging for photovoltaic applications. |
| spellingShingle | Lim, VJ Righetto, M Yan, S Patel, JB Siday, T Putland, B McCall, KM Sirtl, MT Kominko, Y Peng, J Lin, Q Bein, T Kovalenko, M Snaith, HJ Johnston, MB Herz, LM Contrasting Ultra-Low Frequency Raman and Infrared Modes in Emerging Metal Halides for Photovoltaics |
| title | Contrasting Ultra-Low Frequency Raman and Infrared Modes in Emerging Metal Halides for Photovoltaics |
| title_full | Contrasting Ultra-Low Frequency Raman and Infrared Modes in Emerging Metal Halides for Photovoltaics |
| title_fullStr | Contrasting Ultra-Low Frequency Raman and Infrared Modes in Emerging Metal Halides for Photovoltaics |
| title_full_unstemmed | Contrasting Ultra-Low Frequency Raman and Infrared Modes in Emerging Metal Halides for Photovoltaics |
| title_short | Contrasting Ultra-Low Frequency Raman and Infrared Modes in Emerging Metal Halides for Photovoltaics |
| title_sort | contrasting ultra low frequency raman and infrared modes in emerging metal halides for photovoltaics |
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