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Understanding and controlling the efficiency of Au24M(SR)18 nanoclusters as singlet-oxygen photosensitizers
Chemical Science ( IF 7.6 ) Pub Date : 2020/02/19 , DOI: 10.1039/d0sc00520g Mikhail Agrachev 1 , Wenwen Fei 1 , Sabrina Antonello 1 , Sara Bonacchi 1 , Tiziano Dainese 1 , Alfonso Zoleo 1 , Marco Ruzzi 1 , Flavio Maran 1, 2
Chemical Science ( IF 7.6 ) Pub Date : 2020/02/19 , DOI: 10.1039/d0sc00520g Mikhail Agrachev 1 , Wenwen Fei 1 , Sabrina Antonello 1 , Sara Bonacchi 1 , Tiziano Dainese 1 , Alfonso Zoleo 1 , Marco Ruzzi 1 , Flavio Maran 1, 2
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Singlet oxygen, 1O2, can be generated by molecules that upon photoexcitation enable the 3O2 → 1O2 transition. We used a series of atomically precise Au24M(SR)18 clusters, with different R groups and doping metal atoms M. Upon nanosecond photoexcitation of the cluster, 1O2 was efficiently generated. Detection was carried out by time-resolved electron paramagnetic resonance (TREPR) spectroscopy. The resulting TREPR transient yielded the 1O2 lifetime as a function of the nature of the cluster. We found that: these clusters indeed generate 1O2 by forming a triplet state; a more positive oxidation potential of the molecular cluster corresponds to a longer 1O2 lifetime; proper design of the cluster yields results analogous to those of a well-known reference photosensitizer, although more effectively. Comprehensive kinetic analysis provided important insights into the mechanism and driving-force dependence of the quenching of 1O2 by gold nanoclusters. Understanding on a molecular basis why these molecules may perform so well in 1O2 photosensitization is instrumental to controlling their performance.
中文翻译：
了解和控制 Au24M(SR)18 纳米团簇作为单线态氧光敏剂的效率
单线态氧1 O 2可由在光激发下实现3 O 2 → 1 O 2跃迁的分子产生。我们使用了一系列原子级精确的Au 24 M(SR) 18簇，具有不同的R基团和掺杂金属原子M。在簇的纳秒光激发下，有效地生成了1 O 2 。通过时间分辨电子顺磁共振（TREPR）光谱进行检测。由此产生的 TREPR 瞬态产生了1 O 2寿命作为团簇性质的函数。我们发现：这些团簇确实通过形成三重态产生了1 O 2 ；分子簇的氧化电位越正，对应的1 O 2寿命越长；簇的正确设计产生了与众所周知的参考光敏剂类似的结果，尽管更有效。全面的动力学分析为金纳米团簇猝灭1 O 2的机制和驱动力依赖性提供了重要的见解。 在分子基础上理解为什么这些分子在1 O 2光敏化中表现如此良好有助于控制它们的性能。
更新日期：2020-04-01
中文翻译：
了解和控制 Au24M(SR)18 纳米团簇作为单线态氧光敏剂的效率
单线态氧1 O 2可由在光激发下实现3 O 2 → 1 O 2跃迁的分子产生。我们使用了一系列原子级精确的Au 24 M(SR) 18簇，具有不同的R基团和掺杂金属原子M。在簇的纳秒光激发下，有效地生成了1 O 2 。通过时间分辨电子顺磁共振（TREPR）光谱进行检测。由此产生的 TREPR 瞬态产生了1 O 2寿命作为团簇性质的函数。我们发现：这些团簇确实通过形成三重态产生了1 O 2 ；分子簇的氧化电位越正，对应的1 O 2寿命越长；簇的正确设计产生了与众所周知的参考光敏剂类似的结果，尽管更有效。全面的动力学分析为金纳米团簇猝灭1 O 2的机制和驱动力依赖性提供了重要的见解。 在分子基础上理解为什么这些分子在1 O 2光敏化中表现如此良好有助于控制它们的性能。
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