ABSTRACT
Detection of the extremely weak signals in spectroscopy over an extremely wide frequency region is central to diverse sciences, including materials science, biology, astronomy and chemistry. Here we show a new type of atomic-scale spectroscopy, heterodyne scanning tunnelling spectroscopy (HSTS), which is based on the innovative application of the nonlinear heterodyne-mixing detection at the metal-insulator-metal (MIM) heterojunction of STM tip-vacuum-sample. The principle of HSTS is identical to that of the Atacama Large Millimeter Array (ALMA) space telescope in terms of using heterojunction for detecting extremely weak signals by converting from terahertz region to lower frequency regions. The MIM detector of ALMA, which is composed of niobium-titanium-nitride (NbTiN) tip-insulator-NbTiN, is very similar in shape and size to that of HSTS. We successfully detect a heterodyne beat signal f3(= |f2- f1) and intermodulation distortion via tunnelling current by superimposing two different AC signals, f1 and f2, onto the DC tunnelling current at a highly oriented pyrolytic graphite (HOPG) surface. We then obtain spectra of the localized electronic states of HOPG by using f3. HSTS can be performed with a high resolution and over a wide energy range, including the terahertz range.
ABSTRACT
Studies of spin dynamics in low-dimensional systems are important from both fundamental and practical points of view. Spin-polarized scanning tunnelling microscopy allows localized spin dynamics to be characterized and plays important roles in nanoscale science and technology. However, nanoscale analysis of the ultrafast dynamics of itinerant magnetism, as well as its localized characteristics, should be pursued to advance further the investigation of quantum dynamics in functional structures of small systems. Here, we demonstrate the optical pump-probe scanning tunnelling microscopy technique, which enables the nanoscale probing of spin dynamics with the temporal resolution corresponding, in principle, to the optical pulse width. Spins are optically oriented using circularly polarized light, and their dynamics are probed by scanning tunnelling microscopy based on the optical pump-probe method. Spin relaxation in a single quantum well with a width of 6 nm was observed with a spatial resolution of â¼ 1 nm. In addition to spin relaxation dynamics, spin precession, which provides an estimation of the Landé g factor, was observed successfully.
ABSTRACT
The tangled mechanism that produces optical pump-probe scanning tunneling microscopy spectra from semiconductors was analyzed by comparing model simulation data with experimental data. The nonlinearities reflected in the spectra, namely, the excitations generated by paired laser pulses with a delay time, the logarithmic relationship between carrier density and surface photovoltage (SPV), and the effect of the change in tunneling barrier height depending on SPV, were examined along with the delay-time-dependent integration process used in measurement. The optimum conditions required to realize reliable measurement, as well as the validity of the microscopy technique, were demonstrated for the first time.
