Externally-triggerable optical pump-probe scanning tunneling microscopy with a time resoloution of tens-picosecond.

Photoinduced carrier dynamics of nanostructures play a crucial role in developing novel functionalities in advanced materials. Optical pump-probe scanning tunneling microscopy (OPP-STM) represents distinctive capabilities of real-space imaging of such carrier dynamics with nanoscale spatial resolution. However, combining the advanced technology of ultrafast pulsed lasers with STM for stable time-resolved measurements has remained challenging. The recent OPP-STM system, whose laser-pulse timing is electrically controlled by external triggers, has significantly simplified this combination but limited its application due to nanosecond temporal resolution. Here we report an externally-triggerable OPP-STM system with a temporal resolution in the tens-picosecond range. We also realize the stable laser illumination of the tip-sample junction by placing a position-movable aspheric lens driven by piezo actuators directly on the STM stage and by employing an optical beam stabilization system. We demonstrate the OPP-STM measurements on GaAs(110) surfaces, observing carrier dynamics with a decay time of [Formula: see text] ps and revealing local carrier dynamics at features including a step edge and a nanoscale defect. The stable OPP-STM measurements with the tens-picosecond resolution by the electrical control of laser pulses highlight the potential capabilities of this system for investigating nanoscale carrier dynamics of a wide range of functional materials.

Development of a near-5-Kelvin, cryogen-free, pulse-tube refrigerator-based scanning probe microscope.

We report the design and performance of a cryogen-free, pulse-tube refrigerator (PTR)-based scanning probe microscopy (SPM) system capable of operating at a base temperature of near 5 K. We achieve this by combining a home-made interface design between the PTR cold head and the SPM head, with an automatic gas-handling system. The interface design isolates the PTR vibrations by a combination of polytetrafluoroethylene and stainless-steel bellows and by placing the SPM head on a passive vibration isolation table via two cold stages that are connected to thermal radiation shields using copper heat links. The gas-handling system regulates the helium heat-exchange gas pressures, facilitating both the cooldown to and maintenance of the base temperature. We discuss the effects of each component using measured vibration, current-noise, temperature, and pressure data. We demonstrate that our SPM system performance is comparable to known liquid-helium-based systems with the measurements of the superconducting gap spectrum of Pb, atomic-resolution scanning tunneling microscopy image and quasiparticle interference pattern of Au(111) surface, and non-contact atomic force microscopy image of NaCl(100) surface. Without the need for cryogen refills, the present SPM system enables uninterrupted low-temperature measurements.

Bases for time-resolved probing of transient carrier dynamics by optical pump-probe scanning tunneling microscopy.

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.