Donostia International Physics Center (DIPC) , 20018 San Sebastián-Donostia , Spain.
IKERBASQUE, Basque Foundation for Science , Maria Diaz de Haro 3 , 48013 Bilbao , Spain.
Nano Lett. 2018 Apr 11;18(4):2358-2364. doi: 10.1021/acs.nanolett.7b05297. Epub 2018 Mar 23.
As the size of a molecular emitter becomes comparable to the dimensions of a nearby optical resonator, the standard approach that considers the emitter to be a point-like dipole breaks down. By adoption of a quantum description of the electronic transitions of organic molecular emitters, coupled to a plasmonic electromagnetic field, we are able to accurately calculate the position-dependent coupling strength between a plasmon and an emitter. The spatial distribution of excitonic and photonic quantum states is found to be a key aspect in determining the dynamics of molecular emission in ultrasmall cavities both in the weak and strong coupling regimes. Moreover, we show that the extreme localization of plasmonic fields leads to the selection rule breaking of molecular excitations.
随着分子发射器的尺寸变得与附近的光学谐振器的尺寸相当，标准的将发射器视为点状偶极子的方法就不再适用了。通过采用有机分子发射器的电子跃迁的量子描述，并与等离子体电磁波场相结合，我们能够准确地计算等离子体与发射器之间的位置相关耦合强度。发现激子和光子量子态的空间分布是确定在弱耦合和强耦合两种情况下超小腔中分子发射动力学的关键方面。此外，我们还表明，等离子体场的极端局域化导致分子激发的选择定则被打破。
