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Breaking the Selection Rules of Spin-Forbidden Molecular Absorption in Plasmonic Nanocavities
ACS Photonics ( IF 6.5 ) Pub Date : 2020-08-12 , DOI: 10.1021/acsphotonics.0c00732 Oluwafemi S. Ojambati 1 , William M. Deacon 1 , Rohit Chikkaraddy 1 , Charlie Readman 1, 2 , Qianqi Lin 1 , Zsuzsanna Koczor-Benda 3 , Edina Rosta 3, 4 , Oren A. Scherman 2 , Jeremy J. Baumberg 1
ACS Photonics ( IF 6.5 ) Pub Date : 2020-08-12 , DOI: 10.1021/acsphotonics.0c00732 Oluwafemi S. Ojambati 1 , William M. Deacon 1 , Rohit Chikkaraddy 1 , Charlie Readman 1, 2 , Qianqi Lin 1 , Zsuzsanna Koczor-Benda 3 , Edina Rosta 3, 4 , Oren A. Scherman 2 , Jeremy J. Baumberg 1
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Controlling absorption and emission of organic molecules is crucial for efficient light-emitting diodes, organic solar cells, and single-molecule spectroscopy. Here, a new molecular absorption is activated inside a gold plasmonic nanocavity and found to break selection rules via spin–orbit coupling. Photoluminescence excitation scans reveal absorption from a normally spin-forbidden singlet to triplet state transition, while drastically enhancing the emission rate by several thousand fold. The experimental results are supported by density functional theory, revealing the manipulation of molecular absorption by nearby metallic gold atoms.
中文翻译：
打破等离子纳米腔中自旋禁止分子吸收的选择规则
控制有机分子的吸收和发射对于有效的发光二极管，有机太阳能电池和单分子光谱学至关重要。在这里，一种新的分子吸收在金等离激元纳米腔体内被激活，并通过自旋轨道耦合破坏了选择规则。光致发光激发扫描揭示了从正常自旋禁止的单重态到三重态转变的吸收，同时将发射速率大大提高了数千倍。实验结果得到密度泛函理论的支持，揭示了附近金属金原子对分子吸收的操纵。
更新日期：2020-09-16
中文翻译：
打破等离子纳米腔中自旋禁止分子吸收的选择规则
控制有机分子的吸收和发射对于有效的发光二极管，有机太阳能电池和单分子光谱学至关重要。在这里，一种新的分子吸收在金等离激元纳米腔体内被激活，并通过自旋轨道耦合破坏了选择规则。光致发光激发扫描揭示了从正常自旋禁止的单重态到三重态转变的吸收，同时将发射速率大大提高了数千倍。实验结果得到密度泛函理论的支持，揭示了附近金属金原子对分子吸收的操纵。
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