论文标题
激光诱导的傅立叶限制单分子发射器的频率调整
Laser-induced frequency tuning of Fourier-limited single-molecule emitters
论文作者
论文摘要
有机固体中电荷和光的局部相互作用是独特和基本效果的基础。我们在这里观察到单分子尺度,聚焦激光束如何在自然宽度上局部移动数百次,并以持久的方式在不同宿主矩阵的液体温度下冷却有机发色团的过渡频率。在量子化学计算的支持下,结果被解释为光电级联的效果,导致稳定的电场,从而使分子电子水平急切。然后将实验方法应用于量子光子学中的共同挑战,即近量子发射器的独立调整和同步,这对于多光子实验是可取的。五个在空间分离约50微米且最初分开20 GHz的分子在其线宽的两倍之内引起共振。将这种能力与仅受自发衰减限制的发射线宽相结合,该系统可以使集成在同一光子芯片上的多个分子进行无制造,独立调整。
The local interaction of charges and light in organic solids is the basis of distinct and fundamental effects. We here observe, at the single molecule scale, how a focused laser beam can locally shift by hundreds-time their natural linewidth and in a persistent way the transition frequency of organic chromophores, cooled at liquid helium temperatures in different host matrices. Supported by quantum chemistry calculations, the results are interpreted as effects of a photo-ionization cascade, leading to a stable electric field, which Stark-shifts the molecular electronic levels. The experimental method is then applied to a common challenge in quantum photonics, i.e. the independent tuning and synchronization of close-by quantum emitters, which is desirable for multi-photon experiments. Five molecules that are spatially separated by about 50 microns and originally 20 GHz apart are brought into resonance within twice their linewidth. Combining this ability with an emission linewidth that is only limited by the spontaneous decay, the system enables fabrication-free, independent tuning of multiple molecules integrated on the same photonic chip.