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Dimers of Plasmonic Nanocubes to Reach Single-Molecule Strong Coupling with High Emission Yields
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2022-12-20 , DOI: 10.1021/acs.jpclett.2c02872
Jeanne Heintz 1 , Francesca Legittimo 1 , Sébastien Bidault 1
Affiliation  

Reaching reproducible strong coupling between a quantum emitter and a plasmonic resonator at room temperature, while maintaining high emission yields, would make quantum information processing with light possible outside of cryogenic conditions. We theoretically propose to exploit the high local curvatures at the tips of plasmonic nanocubes to reach Purcell factors of >106 at visible frequencies, rendering single-molecule strong coupling more easily accessible than with the faceted spherical nanoparticles used in recent experimental demonstrations. In the case of gold nanocube dimers, we highlight a trade-off between coupling strength and emission yield that depends on the nanocube size. Electrodynamic simulations on silver nanostructures are performed using a realistic dielectric constant, as confirmed by scattering spectroscopy performed on single nanocubes. Dimers of silver nanocubes feature Purcell factors similar to those of gold while allowing emission yields of >60%, thus providing design rules for efficient strongly coupled hybrid nanostructures at room temperature.

中文翻译:

等离子体纳米立方体的二聚体可实现具有高发射率的单分子强耦合

在室温下实现量子发射器和等离子体共振器之间可重现的强耦合,同时保持高发射产率,将使在低温条件之外使用光进行量子信息处理成为可能。我们理论上建议利用等离子体纳米立方体尖端的高局部曲率来达到 >10 6的珀塞尔因子在可见频率下,与最近的实验演示中使用的多面球形纳米粒子相比,使单分子强耦合更容易获得。在金纳米立方体二聚体的情况下,我们强调了取决于纳米立方体尺寸的耦合强度和发射产率之间的权衡。银纳米结构的电动力学模拟是使用真实的介电常数进行的,正如在单个纳米立方体上进行的散射光谱所证实的那样。银纳米立方体的二聚体具有与金相似的珀塞尔因子,同时允许 >60% 的发射产率,从而为室温下高效强耦合混合纳米结构提供设计规则。
更新日期:2022-12-20
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