利用光子关联阴极荧光揭示纳米金刚石中氮-空位中心耦合至传播和局域表面等离激元的Purcell效应
Purcell effect of nitrogen-vacancy centers in nanodiamond coupled to propagating and localized surface plasmons revealed by photon-correlation cathodoluminescence
AI总结：
本研究结合扫描电子显微镜阴极荧光与干涉测量法，利用纳米金刚石氮-空位中心作为量子发射体，首次在纳米分辨率下实验揭示了其与表面等离极化激元耦合产生的Purcell效应及寿命缩短现象。
摘要：
我们测量了阴极荧光强度的二阶关联函数，并通过比较有和没有金属结构的量子发射体的寿命研究了Purcell效应。由于量子发射体与等离激元结构耦合导致的电磁局域态密度增加，会引起发射体寿命的缩短，这被称为Purcell效应。由于等离激元增强的电场被限制在远小于光波长的范围内，量子发射体的寿命在纳米尺度范围内发生改变。在本研究中，我们将扫描（透射）电子显微镜中的阴极荧光与Hanbury Brown-Twiss干涉测量法相结合，以纳米和纳秒分辨率测量了Purcell效应。我们使用包含在纳米金刚石中的氮-空位中心作为量子发射体，并比较了它们在不同环境中的寿命：在薄SiO2膜上、在厚平坦银膜上以及嵌入银膜中。在带有银的样品中清楚地观察到了氮-空位中心的寿命缩短。我们通过解析计算和数值模拟评估了寿命，并揭示了发射体耦合到传播和局域表面等离激元的Purcell效应。这是首个展示纳米金刚石中氮-空位中心与表面等离极化激元之间耦合导致Purcell效应的具有纳米分辨率的实验结果。
英文摘要：
We measured the second-order correlation function of the cathodoluminescence intensity and investigated the Purcell effect by comparing the lifetimes of quantum emitters with and without metal structure. The increase in the electromagnetic local density of state due to the coupling of a quantum emitter with a plasmonic structure causes a shortening of the emitter lifetime, which is called the Purcell effect. Since the plasmon-enhanced electric field is confined well below the wavelength of light, the quantum emitter lifetime is changed in the nanoscale range. In this study, we combined cathodoluminescence in scanning (transmission) electron microscopy with Hanbury Brown-Twiss interferometry to measure the Purcell effect with nanometer and nanosecond resolutions. We used nitrogen-vacancy centers contained in nanodiamonds as quantum emitters and compared their lifetime in different environments: on a thin SiO2 membrane, on a thick flat silver film, and embedded in a silver film. The lifetime reductions of nitrogen-vacancy centers were clearly observed in the samples with silver. We evaluated the lifetime by analytical calculation and numerical simulations and revealed the Purcell effects of emitters coupled to propagating and localized surface plasmons. This is the first experimental result showing the Purcell effect due to the coupling between nitrogen-vacancy centers in nanodiamonds and surface plasmon polaritons with nanometer resolution.
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