Automated Research Platform for Development of Triplet–Triplet Annihilation Photon Upconversion Systems

IF 12.7 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Central Science Pub Date : 2025-02-21 DOI:10.1021/acscentsci.4c0205910.1021/acscentsci.4c02059

Paulius Baronas, Justas Lekavičius, Maciej Majdecki, Jacob Lynge Elholm, Karolis Kazlauskas, Przemysław Gaweł and Kasper Moth-Poulsen*,

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引用次数: 0

Abstract

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.

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三重态-三重态湮灭光子上转换系统开发的自动化研究平台

三重态-三重态湮灭光子上转换（TTA-UC）系统在能源、3D打印和光药理学等领域有着巨大的应用前景。然而，由于需要在无氧条件下精确调整敏化剂和湮灭剂浓度，它们的优化仍然具有挑战性。本研究提出了一个自动化的高通量平台，用于发现和优化ta - uc系统。该平台能够在短短两小时内进行100次浓度扫描，生成关键参数的综合浓度图，包括量子产率、三重态能量传递效率和阈值强度。使用这种方法，我们确定了现有和新的ta - uc系统中的关键损失机制。在高卟啉基敏化剂浓度下，上转换量子产率损失归因于敏化剂三重态通过聚集自猝灭和敏化剂三重态-三重态湮灭（敏化剂- tta）。此外，在敏化剂水平升高时，反向三重态能量转移（RTET）会增加上转换损失和激发阈值。测试新的敏化剂-湮灭剂对证实了这些损失机制，突出了分子设计改进的机会。这个自动化平台为推进TTA-UC研究和其他需要低氧水平、强激光激发和最小材料使用的光化学研究提供了强大的工具。一种高通量浓度筛选方法，用于确定敏化三重态-三重态湮灭系统的上转换量子产率和激发阈值。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Central Science Chemical Engineering-General Chemical Engineering

CiteScore

25.50

自引率

0.50%

发文量

194

审稿时长

10 weeks

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.