Hannes Hempel, Martin Stolterfoht, Orestis Karalis, Thomas Unold
{"title":"通过时间分辨光致发光揭示卤化铅包晶中双星对的潜力","authors":"Hannes Hempel, Martin Stolterfoht, Orestis Karalis, Thomas Unold","doi":"arxiv-2409.06382","DOIUrl":null,"url":null,"abstract":"Photoluminescence (PL) under continuous illumination is commonly employed to\nassess voltage losses in solar energy conversion materials. However, the early\ntemporal evolution of these losses remains poorly understood. Therefore, we\nextend the methodology to time-resolved PL, introducing the concepts of\ngeminate PL, doping PL, and sibling PL to quantify the transient chemical\npotential of photogenerated electron-hole pairs and key optoelectronic\nproperties. Analyzing the initial PL amplitudes reveals hot charge carrier\nseparation for around 100 nm and is likely limited by the grain size of the\ntriple cation perovskite. The following PL decay is caused by the diffusive\nseparation of non-excitonic geminate pairs and time-resolves a fundamental yet\noften overlooked energy loss by increasing entropy. For triple-cation halide\nperovskite, we measure a \"geminate correlation energy\" of up to 90 meV,\npersisting for ~ten nanoseconds. This energy is unutilized in standard solar\ncells and is considered lost in the Shockley-Queisser model. Therefore, this\ngeminate energy could substantially enhance the device's efficiency,\nparticularly under maximum power point and low-illumination conditions.","PeriodicalId":501083,"journal":{"name":"arXiv - PHYS - Applied Physics","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"The Potential of Geminate Pairs in Lead Halide Perovskite revealed via Time-resolved Photoluminescence\",\"authors\":\"Hannes Hempel, Martin Stolterfoht, Orestis Karalis, Thomas Unold\",\"doi\":\"arxiv-2409.06382\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Photoluminescence (PL) under continuous illumination is commonly employed to\\nassess voltage losses in solar energy conversion materials. However, the early\\ntemporal evolution of these losses remains poorly understood. Therefore, we\\nextend the methodology to time-resolved PL, introducing the concepts of\\ngeminate PL, doping PL, and sibling PL to quantify the transient chemical\\npotential of photogenerated electron-hole pairs and key optoelectronic\\nproperties. Analyzing the initial PL amplitudes reveals hot charge carrier\\nseparation for around 100 nm and is likely limited by the grain size of the\\ntriple cation perovskite. The following PL decay is caused by the diffusive\\nseparation of non-excitonic geminate pairs and time-resolves a fundamental yet\\noften overlooked energy loss by increasing entropy. For triple-cation halide\\nperovskite, we measure a \\\"geminate correlation energy\\\" of up to 90 meV,\\npersisting for ~ten nanoseconds. This energy is unutilized in standard solar\\ncells and is considered lost in the Shockley-Queisser model. Therefore, this\\ngeminate energy could substantially enhance the device's efficiency,\\nparticularly under maximum power point and low-illumination conditions.\",\"PeriodicalId\":501083,\"journal\":{\"name\":\"arXiv - PHYS - Applied Physics\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-09-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"arXiv - PHYS - Applied Physics\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/arxiv-2409.06382\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"arXiv - PHYS - Applied Physics","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/arxiv-2409.06382","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
The Potential of Geminate Pairs in Lead Halide Perovskite revealed via Time-resolved Photoluminescence
Photoluminescence (PL) under continuous illumination is commonly employed to
assess voltage losses in solar energy conversion materials. However, the early
temporal evolution of these losses remains poorly understood. Therefore, we
extend the methodology to time-resolved PL, introducing the concepts of
geminate PL, doping PL, and sibling PL to quantify the transient chemical
potential of photogenerated electron-hole pairs and key optoelectronic
properties. Analyzing the initial PL amplitudes reveals hot charge carrier
separation for around 100 nm and is likely limited by the grain size of the
triple cation perovskite. The following PL decay is caused by the diffusive
separation of non-excitonic geminate pairs and time-resolves a fundamental yet
often overlooked energy loss by increasing entropy. For triple-cation halide
perovskite, we measure a "geminate correlation energy" of up to 90 meV,
persisting for ~ten nanoseconds. This energy is unutilized in standard solar
cells and is considered lost in the Shockley-Queisser model. Therefore, this
geminate energy could substantially enhance the device's efficiency,
particularly under maximum power point and low-illumination conditions.