论文标题

六角硼表面上的单个有机分子的尖锐零孔线

Sharp zero-phonon lines of single organic molecules on a hexagonal boron-nitride surface

论文作者

Smit, Robert, Tebyani, Arash, Hameury, Jil, van der Molen, Sense Jan, Orrit, Michel

论文摘要

由于它们在低温温度下,嵌入了大部分宿主晶体中的单个荧光分子已被证明是其纳米环境中动力学的极好探针。然而,由于单分子位于表面或界面靠近,但已经发现0-0 ZPL的光线宽度显着增加,而在任何表面上的有机分子中都未检测到0-0 ZPL。在这里,我们研究了吸附在六角硼硝酸盐(HBN)底物表面上的单个荧光扭转分子。我们的低温结果首次显示了表面上荧光分子0-0 ZPL的观察。通过共振激发,我们发现0-0 ZPL线宽,低于45 +/- 3 MHz的傅立叶极限约10倍,该值由荧光寿命决定。我们比较了沉积在退火和非退缩HBN薄片表面上的分子的结果,我们看到退火后发射器的光谱稳定性有明显的改善。我们在扭转上获得的高分辨率光谱表明,有可能将HBN与多种单分子发射器结合使用,以研究表面上的物理现象或用于纳米光子设备。

Single fluorescent molecules embedded in the bulk of host crystals have proven to be excellent probes of the dynamics in their nano environment, thanks to their narrow (about 0.1 μeV) optical linewidth of the 0-0 zero-phonon line (0-0 ZPL) at cryogenic temperatures. However, the optical linewidths of the 0-0 ZPL have been found to increase dramatically as the single molecules are located closer to a surface or interface, while no 0-0 ZPL has been detected for organic molecules on any surface. Here, we study single fluorescent terrylene molecules adsorbed on the surface of hexagonal boron-nitride (hBN) substrates. Our low-temperature results show for the first time the observation of the 0-0 ZPL of fluorescent molecules on a surface. With resonant excitation, we find 0-0 ZPL linewidths down to values that are about 10 times larger than the Fourier limit of 45 +/- 3 MHz, dictated by the fluorescence lifetime. We compare our results for molecules deposited on the surfaces of annealed and non-annealed hBN flakes and we see a marked improvement in the spectral stability of the emitters after annealing. Our high-resolution spectra obtained on terrylene suggest the possibility of employing hBN in combination with a wide variety of single molecule emitters for investigation of physical phenomena at surfaces or for use in nanophotonic devices.

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