Revealing ultrafast charge-carrier thermalization in tin-iodide perovskites through novel pump-push-probe terahertz spectroscopy
Tin-iodide perovskites are an important group of semiconductors for photovoltaic applications, promising higher intrinsic charge-carrier mobilities and lower toxicity than their lead-based counterparts. Controllable tin vacancy formation and the ensuing hole doping provide interesting opportunities...
| Huvudupphovsmän: | , , , |
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| Materialtyp: | Journal article |
| Språk: | English |
| Publicerad: |
American Chemical Society
2021
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| _version_ | 1826264872198864896 |
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| author | Snaith, H Johnston, M Ulatowski, A Herz, LM |
| author_facet | Snaith, H Johnston, M Ulatowski, A Herz, LM |
| author_sort | Snaith, H |
| collection | OXFORD |
| description | Tin-iodide perovskites are an important group of semiconductors for photovoltaic applications, promising higher intrinsic charge-carrier mobilities and lower toxicity than their lead-based counterparts. Controllable tin vacancy formation and the ensuing hole doping provide interesting opportunities to investigate dynamic intraband transitions of charge carriers in these materials. Here, we present for the first time an experimental implementation of a novel Optical-Pump–IR-Push–THz-Probe spectroscopic technique and demonstrate its suitability to investigate the intraband relaxation dynamics of charge carriers brought into non-equilibrium by an infrared “push” pulse. We observe a push-induced decrease of terahertz conductivity for both chemically- and photodoped FA0.83Cs0.17SnI3 thin films and show that these effects derive from stimulated THz emission. We use this technique to reveal that newly photogenerated charge carriers relax within the bands of FA0.83Cs0.17SnI3 on a sub-picosecond timescale when a large, already fully thermalized (cold) population of charge-carriers is present. Such
rapid dissipation of the initial charge-carrier energy suggests that the propensity of tin halide perovskites towards unintentional self-doping resulting from tin vacancy formation makes these materials less suited to implementation in hot-carrier solar cells than their lead-based counterparts. |
| first_indexed | 2024-03-06T20:14:49Z |
| format | Journal article |
| id | oxford-uuid:2bc5ed96-8c3c-4c3d-97d6-8d6162b2a78f |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-06T20:14:49Z |
| publishDate | 2021 |
| publisher | American Chemical Society |
| record_format | dspace |
| spelling | oxford-uuid:2bc5ed96-8c3c-4c3d-97d6-8d6162b2a78f2022-03-26T12:33:06ZRevealing ultrafast charge-carrier thermalization in tin-iodide perovskites through novel pump-push-probe terahertz spectroscopyJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:2bc5ed96-8c3c-4c3d-97d6-8d6162b2a78fEnglishSymplectic ElementsAmerican Chemical Society2021Snaith, HJohnston, MUlatowski, AHerz, LMTin-iodide perovskites are an important group of semiconductors for photovoltaic applications, promising higher intrinsic charge-carrier mobilities and lower toxicity than their lead-based counterparts. Controllable tin vacancy formation and the ensuing hole doping provide interesting opportunities to investigate dynamic intraband transitions of charge carriers in these materials. Here, we present for the first time an experimental implementation of a novel Optical-Pump–IR-Push–THz-Probe spectroscopic technique and demonstrate its suitability to investigate the intraband relaxation dynamics of charge carriers brought into non-equilibrium by an infrared “push” pulse. We observe a push-induced decrease of terahertz conductivity for both chemically- and photodoped FA0.83Cs0.17SnI3 thin films and show that these effects derive from stimulated THz emission. We use this technique to reveal that newly photogenerated charge carriers relax within the bands of FA0.83Cs0.17SnI3 on a sub-picosecond timescale when a large, already fully thermalized (cold) population of charge-carriers is present. Such rapid dissipation of the initial charge-carrier energy suggests that the propensity of tin halide perovskites towards unintentional self-doping resulting from tin vacancy formation makes these materials less suited to implementation in hot-carrier solar cells than their lead-based counterparts. |
| spellingShingle | Snaith, H Johnston, M Ulatowski, A Herz, LM Revealing ultrafast charge-carrier thermalization in tin-iodide perovskites through novel pump-push-probe terahertz spectroscopy |
| title | Revealing ultrafast charge-carrier thermalization in tin-iodide perovskites through novel pump-push-probe terahertz spectroscopy |
| title_full | Revealing ultrafast charge-carrier thermalization in tin-iodide perovskites through novel pump-push-probe terahertz spectroscopy |
| title_fullStr | Revealing ultrafast charge-carrier thermalization in tin-iodide perovskites through novel pump-push-probe terahertz spectroscopy |
| title_full_unstemmed | Revealing ultrafast charge-carrier thermalization in tin-iodide perovskites through novel pump-push-probe terahertz spectroscopy |
| title_short | Revealing ultrafast charge-carrier thermalization in tin-iodide perovskites through novel pump-push-probe terahertz spectroscopy |
| title_sort | revealing ultrafast charge carrier thermalization in tin iodide perovskites through novel pump push probe terahertz spectroscopy |
| work_keys_str_mv | AT snaithh revealingultrafastchargecarrierthermalizationintiniodideperovskitesthroughnovelpumppushprobeterahertzspectroscopy AT johnstonm revealingultrafastchargecarrierthermalizationintiniodideperovskitesthroughnovelpumppushprobeterahertzspectroscopy AT ulatowskia revealingultrafastchargecarrierthermalizationintiniodideperovskitesthroughnovelpumppushprobeterahertzspectroscopy AT herzlm revealingultrafastchargecarrierthermalizationintiniodideperovskitesthroughnovelpumppushprobeterahertzspectroscopy |