论文标题

具有扫描力显微镜的单分子中的原子尺度访问单分子中的长旋连贯性

Atomic-scale access to long spin coherence in single molecules with scanning force microscopy

论文作者

Sellies, Lisanne, Spachtholz, Raffael, Scheuerer, Philipp, Repp, Jascha

论文摘要

在开放量子系统中理解和控制破坏性是科学的基本兴趣,而实现较长连贯的时间对于量子信息处理至关重要。尽管已经证明了具有纳米级分辨率的单旋转的个体,孤立系统和电子自旋共振(ESR)取得的巨大进展,但已经证明了复杂的固态量子设备的构建最终需要最终控制原子尺度的环境,这可能通过扫描具有其原子和分子表征和manipluction和Manippulation和Manippulation和Manippulation和Manippulation Clissipers扫描探针来实现。因此,最近在扫描隧道显微镜(STM)中实施了ESR代表了实现这一目标的里程碑,随后迅速证明了相干振荡,可调偶极和交换耦合以及与真实空间原子分辨率的核自旋的访问。原子操纵甚至助长了雄心壮志,以实现第一个人工原子尺度量子设备。但是,此方法固有的基于当前的传感限制了相干时间。在这里,我们证明了泵浦探针ESR原子力显微镜检测到单个五苯分子的非平衡三重态之间的电子自旋跃迁。这些过渡的光谱表现出亚纳米电伏能的分辨率,从而允许对它们的同位素构型的局部歧视分子。此外,电子旋转可以在数十微秒内连贯地操纵,这可能不受检测方法的限制,而是通过分子特性来限制。单分子ESR原子力显微镜可以与原子的操纵和表征结合使用,从而为原子良好定义的量子成分铺平了道路,具有较长的相干时间和局部量子感应实验。

Understanding and controlling decoherence in open quantum systems is of fundamental interest in science, while achieving long coherence times is critical for quantum information processing. Although great progress was made for individual, isolated systems, and electron spin resonance (ESR) of single spins with nanoscale resolution has been demonstrated, the construction of complex solid-state quantum devices requires ultimately controlling the environment down to atomic scales, as potentially enabled by scanning probe microscopy with its atomic and molecular characterization and manipulation capabilities. Consequently, the recent implementation of ESR in scanning tunneling microscopy (STM) represents a milestone towards this goal and was quickly followed by the demonstration of coherent oscillations, tunable dipolar and exchange couplings and access to nuclear spins with real-space atomic resolution. Atomic manipulation even fueled the ambition to realize first artificial atomic-scale quantum devices. However, the current-based sensing inherent to this method limits coherence times. Here, we demonstrate pump-probe ESR atomic force microscopy detection of electron spin transitions between non-equilibrium triplet states of individual pentacene molecules. Spectra of these transitions exhibit sub-nanoelectronvolt energy resolution, allowing local discrimination of molecules that only differ in their isotopic configuration. Furthermore, the electron spins can be coherently manipulated over tens of microseconds, likely not limited by the detection method but by the molecular properties. Single-molecule ESR atomic force microscopy can be combined with atomic manipulation and characterization, and thereby paves the way for atomically well-defined quantum components with long coherence times and local quantum-sensing experiments.

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