Paulius Baronas, Justas Lekavičius, Maciej Majdecki, Jacob Lynge Elholm, Karolis Kazlauskas, Przemysław Gaweł and Kasper Moth-Poulsen*,
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Using this approach, we identify key loss mechanisms in both the established and novel TTA-UC systems. At high porphyrin-based sensitizer concentrations, upconversion quantum yield losses are attributed to sensitizer triplet self-quenching via aggregation and sensitizer triplet–triplet annihilation (sensitizer-TTA). Additionally, reverse triplet energy transfer (RTET) at elevated sensitizer levels increases the upconversion losses and excitation thresholds. Testing novel sensitizer–annihilator pairs confirms these loss mechanisms, highlighting opportunities for molecular design improvements. This automated platform offers a powerful tool for advancing TTA-UC research and other photochemical studies requiring low oxygen levels, intense laser excitation, and minimal material use.</p><p >A high-throughput concentration screening method built from commercial components for determining upconversion quantum yield and excitation threshold in sensitized triplet−triplet annihilation systems.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 3","pages":"413–421 413–421"},"PeriodicalIF":12.7000,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c02059","citationCount":"0","resultStr":"{\"title\":\"Automated Research Platform for Development of Triplet–Triplet Annihilation Photon Upconversion Systems\",\"authors\":\"Paulius Baronas, Justas Lekavičius, Maciej Majdecki, Jacob Lynge Elholm, Karolis Kazlauskas, Przemysław Gaweł and Kasper Moth-Poulsen*, \",\"doi\":\"10.1021/acscentsci.4c0205910.1021/acscentsci.4c02059\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Triplet–triplet annihilation photon upconversion (TTA-UC) systems hold great promise for applications in energy, 3D printing, and photopharmacology. However, their optimization remains challenging due to the need for precise tuning of sensitizer and annihilator concentrations under oxygen-free conditions. This study presents an automated, high-throughput platform for the discovery and optimization of TTA-UC systems. Capable of performing 100 concentration scans in just two hours, the platform generates comprehensive concentration maps of critical parameters, including quantum yield, triplet energy transfer efficiency, and threshold intensity. Using this approach, we identify key loss mechanisms in both the established and novel TTA-UC systems. At high porphyrin-based sensitizer concentrations, upconversion quantum yield losses are attributed to sensitizer triplet self-quenching via aggregation and sensitizer triplet–triplet annihilation (sensitizer-TTA). Additionally, reverse triplet energy transfer (RTET) at elevated sensitizer levels increases the upconversion losses and excitation thresholds. Testing novel sensitizer–annihilator pairs confirms these loss mechanisms, highlighting opportunities for molecular design improvements. This automated platform offers a powerful tool for advancing TTA-UC research and other photochemical studies requiring low oxygen levels, intense laser excitation, and minimal material use.</p><p >A high-throughput concentration screening method built from commercial components for determining upconversion quantum yield and excitation threshold in sensitized triplet−triplet annihilation systems.</p>\",\"PeriodicalId\":10,\"journal\":{\"name\":\"ACS Central Science\",\"volume\":\"11 3\",\"pages\":\"413–421 413–421\"},\"PeriodicalIF\":12.7000,\"publicationDate\":\"2025-02-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c02059\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Central Science\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acscentsci.4c02059\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Central Science","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acscentsci.4c02059","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Automated Research Platform for Development of Triplet–Triplet Annihilation Photon Upconversion Systems
Triplet–triplet annihilation photon upconversion (TTA-UC) systems hold great promise for applications in energy, 3D printing, and photopharmacology. However, their optimization remains challenging due to the need for precise tuning of sensitizer and annihilator concentrations under oxygen-free conditions. This study presents an automated, high-throughput platform for the discovery and optimization of TTA-UC systems. Capable of performing 100 concentration scans in just two hours, the platform generates comprehensive concentration maps of critical parameters, including quantum yield, triplet energy transfer efficiency, and threshold intensity. Using this approach, we identify key loss mechanisms in both the established and novel TTA-UC systems. At high porphyrin-based sensitizer concentrations, upconversion quantum yield losses are attributed to sensitizer triplet self-quenching via aggregation and sensitizer triplet–triplet annihilation (sensitizer-TTA). Additionally, reverse triplet energy transfer (RTET) at elevated sensitizer levels increases the upconversion losses and excitation thresholds. Testing novel sensitizer–annihilator pairs confirms these loss mechanisms, highlighting opportunities for molecular design improvements. This automated platform offers a powerful tool for advancing TTA-UC research and other photochemical studies requiring low oxygen levels, intense laser excitation, and minimal material use.
A high-throughput concentration screening method built from commercial components for determining upconversion quantum yield and excitation threshold in sensitized triplet−triplet annihilation systems.
期刊介绍:
ACS Central Science publishes significant primary reports on research in chemistry and allied fields where chemical approaches are pivotal. As the first fully open-access journal by the American Chemical Society, it covers compelling and important contributions to the broad chemistry and scientific community. "Central science," a term popularized nearly 40 years ago, emphasizes chemistry's central role in connecting physical and life sciences, and fundamental sciences with applied disciplines like medicine and engineering. The journal focuses on exceptional quality articles, addressing advances in fundamental chemistry and interdisciplinary research.