Probing plasmon-NV0 coupling at the nanometer scale with photons and fast electrons

• Main Authors: Lourenço-Martins, Hugo, Kociak, Mathieu, Meuret, Sophie, Treussart, François, Lee, Yih Hong, Ling, Xing Yi, Chang, Huan-Cheng, Galvão Tizei, Luiz Henrique
• Other Authors: School of Physical and Mathematical Sciences
• Format: Article
• Language: English
• Published: 2019
• Subjects: Lifetime Measurement; Science::Chemistry::Biochemistry; Purcell Effect
• Online Access: https://hdl.handle.net/10356/104415; http://hdl.handle.net/10220/50010
• Institution: Nanyang Technological University

The local density of optical states governs an emitters’ lifetime and quantum yield through the Purcell effect. It can be modified by a surface plasmon electromagnetic field, but such a field has a spatial extension limited to a few hundreds of nanometers, complicating the use of optical methods to spatially probe emitter–plasmon coupling. Here we show that a combination of electron-based imaging, spectroscopies, and photon-based correlation spectroscopy enables measurement of the Purcell effect with nanometer and nanosecond spatiotemporal resolutions. Due to the large variability of radiative lifetimes of emitters in nanoparticles we relied on a statistical approach to probe the coupling between nitrogen-vacancy centers in nanodiamonds and surface plasmons in silver nanocubes. We quantified the Purcell effect by measuring the nitrogen-vacancy excited state lifetimes in a large number of either isolated nanodiamonds or nanodiamond-nanocube dimers and demonstrated a significant lifetime reduction for dimers.