A scanning tunneling microscope capable of electron spin resonance and pump-probe spectroscopy at mK temperature and in vector magnetic field
Werner M. J. van Weerdenburg, Manuel Steinbrecher, Niels P. E. van Mullekom, Jan W. Gerritsen, Henning von Allwörden, Fabian D. Natterer, Alexander A. Khajetoorians
在过去十年中，通过将电子自旋共振（ESR）或泵浦-探测光谱等技术与扫描隧道显微镜（STM）相结合，原子尺度上的自旋动力学探测已成为可能。在此，我们展示了一台可在 milliKelvin（mK）温度和矢量磁场下运行、并兼具 ESR 与泵浦-探测光谱能力的超高真空（UHV）STM。通过采用兼容 GHz 的布线，我们在维持 mK 基础温度的同时，在结处获得了可观的 RF 振幅。我们利用 MgO/Ag(100) 上单个 TiH 分子的两种实验 ESR 模式（频率扫描和磁场扫描）证明了装置的成功运行，并提取了有效 g 因子。借助 mK 基础温度，我们将 ESR 跃迁追踪到低至 MHz 的前所未有的低频段。我们还实现了一种基于波形序列的全电学泵浦-探测方案，适合研究低至纳秒范围的动力学。我们通过探测 MgO/Ag(100) 上单个 Fe 原子的自旋弛豫时间 T1 对系统进行了基准测试，并注意到弛豫时间依赖于磁场强度和方向。
英文摘要：
In the last decade, detecting spin dynamics at the atomic scale has been enabled by combining techniques like electron spin resonance (ESR) or pump-probe spectroscopy with scanning tunneling microscopy (STM). Here, we demonstrate an ultra-high vacuum (UHV) STM operational at milliKelvin (mK) and in a vector magnetic field capable of both ESR and pump-probe spectroscopy. By implementing GHz compatible cabling, we achieve appreciable RF amplitudes at the junction while maintaining mK base temperature. We demonstrate the successful operation of our setup by utilizing two experimental ESR modes (frequency sweep and magnetic field sweep) on an individual TiH molecule on MgO/Ag(100) and extract the effective g-factor. We trace the ESR transitions down to MHz into an unprecedented low frequency band enabled by the mK base temperature. We also implement an all-electrical pump-probe scheme based on waveform sequencing suited for studying dynamics down to the nanoseconds range. We benchmark our system by detecting the spin relaxation time T1 of individual Fe atoms on MgO/Ag(100) and note a field strength and orientation dependent relaxation time.
Probing Dirac Fermion Dynamics in Topological Insulator Bi$_2$Se$_3$ Films with Scanning Tunneling Microscope
利用扫描隧道显微镜和光谱学研究了拓扑绝缘体Bi $_2$ Se $_3$薄膜中狄拉克费米子的飞秒动力学.在二维极限下，体电子被量子化，量子化可以通过薄膜厚度控制。通过研究驻波（准粒子干涉图样）的空间衰减，直接测量了拓扑表面态电子的相位弛豫长度$l_ϕ$和非弹性散射寿命$τ$与能量和膜厚的关系.我们发现，$τ$表现出显着的$(E-E_F)^{-2}$能量依赖性，并增加与膜厚度。我们发现，所揭示的功能是典型的表面和体状态之间的电子-电子散射。
Silicon can be isotopically enriched, allowing for the fabrication of highly coherent semiconductor spin qubits. However, the conduction band of bulk Si exhibits a six-fold valley degeneracy, which may adversely impact the performance of silicon quantum devices. To date, the spatial characterization of valley states in Si remains limited. Moreover, techniques for probing valley states in functional electronic devices are needed. We describe here a cryogen-free scanning gate microscope for the characterization of Si/Si$_{0.7}$Ge$_{0.3}$ quantum devices at mK temperatures. The microscope is base…
Electron paramagnetic resonance (EPR) spectroscopy is widely employed to characterize paramagnetic complexes. Recently, EPR combined with scanning tunneling microscopy (STM) achieved single-spin sensitivity with sub-angstrom spatial resolution. The excitation mechanism of EPR in STM, however, is broadly debated, raising concerns about widespread application of this technique. Here, we present an extensive experimental study and modelling of EPR-STM of Fe and hydrogenated Ti atoms on an MgO surface. Our results support a piezoelectric coupling mechanism, in which the EPR species oscillate adiab…
Multi-tip scanning tunneling microscopy (STM) is a powerful method to perform charge transport measurements at the nanoscale. With four STM tips positioned on the surface of a sample, four-point resistance measurements can be performed in dedicated geometric configurations. Here, we present an alternative to the most often used scanning electron microscope (SEM) imaging to infer the corresponding tip positions. After initial coarse positioning monitored by an optical microscope, STM scanning itself is used to determine the inter-tip distances. A large STM overview scan serves as a reference ma…
The Scanning Quantum Cryogenic Atom Microscope (SQCRAMscope) is a quantum sensor in which a quasi-1D quantum gas images electromagnetic fields emitted from a nearby sample. We report improvements to the microscope. Cryogen usage is reduced by replacing the liquid cryostat with a closed-cycle system and modified cold finger, and cryogenic cooling is enhanced by adding a radiation shield. The minimum accessible sample temperature is reduced from 35 K to 5.8 K while maintaining low sample vibrations. A new sample mount is easier to exchange, and quantum gas preparation is streamlined.
The molecular dark state participates in many important photon-induced processes, yet is typically beyond the optical-spectroscopic measurement due to the forbidden transition dictated by the selection rule. In this work, we propose to use the scanning tunneling microscope (STM) as an incisive tool to directly profile the dark-state transition density of a single molecule, taking advantage of the localized static electronic field near the metal tip. The detection of dark state is achieved by measuring the fluorescence from a higher bright state to the ground state with assistant optical pumpin…
The quantitative characterization of the degree of randomness and aggregation of surface micro and nanostructures is critical to evaluate their effects on targeted functionalities. To this end, the methods of Point Pattern Analysis (PPA), largely used in ecology and medical imaging, seem to provide a powerful toolset. However, the application of these techniques requires the extraction of the point pattern of nanostructures from their microscope images. In this work, we address the issue of the impact that Scanning Electron Microscope (SEM) image processing may have on the fundamental metric o…
Ultrafast supercontinuum fiber-laser based pump-probe scanning MOKE microscope for the investigation of electron spin dynamics in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution
Inelastic electron tunneling in a scanning tunneling microscope (STM) is used to generate excitons in monolayer tungsten disulfide (WS$_2$). Excitonic electroluminescence is measured both at positive and negative sample bias. Using optical spectroscopy and Fourier-space optical microscopy, we show that the bias polarity of the tunnel junction determines the spectral and angular distribution of the emitted light. At positive sample bias, only emission from excitonic species featuring an in-plane transition dipole moment is detected. Based on the spectral distribution of the emitted light, we in…
A scanning tunneling microscope for spectroscopic imaging below 90 mK in magnetic fields up to 17.5 T
我们描述了超高真空扫描隧道显微镜的发展和性能的组合极端条件下的超低温和高磁场。我们结合了顶部加载稀释制冷机和标准桶杜瓦瓶与底部加载超导磁体，以实现4.5天的运行时间，这是足够长的时间来执行各种光谱成像测量。为了使有效电子温度更接近混合室温度，我们特别注意滤除射频噪声，以及增强显微镜单元和混合室之间的热连接。通过测量铝的超导能隙谱，我们估计最低有效电子温度在90 mK以下。我们证实了长期稳定的光谱成像测量可视化超导涡旋的铜酸盐超导体Bi $_{2}$ Sr $_{2}$ CaCu $_{2}$ O $_{8+δ}$。
We report a scanning superconducting quantum interference device (SQUID) microscope in a cryogen-free dilution refrigerator with a base temperature at the sample stage of at least 30 mK. The microscope is rigidly mounted to the mixing chamber plate to optimize thermal anchoring of the sample. The microscope housing fits into the bore of a superconducting vector magnet, and our design accommodates a large number of wires connecting the sample and sensor. Through a combination of vibration isolation in the cryostat and a rigid microscope housing, we achieve relative vibrations between the SQUID …
