Photodriven Dipole Reordering: Key to Carrier Separation in Metalorganic Halide Perovskites.

Photodriven dipole reordering of the intercalated organic molecules in halide perovskites has been suggested to be a critical degree of freedom, potentially affecting physical properties, device performance, and stability of hybrid perovskite-based optoelectronic devices. However, thus far a direct atomically resolved dipole mapping under device operation condition, that is, illumination, is lacking. Here, we map simultaneously the molecule dipole orientation pattern and the electrostatic potential with atomic resolution using photoexcited cross-sectional scanning tunneling microscopy and spectroscopy. Our experimental observations demonstrate that a photodriven molecule dipole reordering, initiated by a photoexcited separation of electron-hole pairs in spatially displaced orbitals, leads to a fundamental reshaping of the potential landscape in halide perovskites, creating separate one-dimensional transport channels for holes and electrons. We anticipate that analogous light-induced polarization order transitions occur in bulk and are at the origin of the extraordinary efficiencies of organometal halide perovskite-based solar cells as well as could reconcile apparently contradictory materials' properties.

The design and the performance of an ultrahigh vacuum 3He fridge-based scanning tunneling microscope with a double deck sample stage for in-situ tip treatment.

Scanning tunneling microscope (STM) is a powerful tool for studying the structural and electronic properties of materials at the atomic scale. The combination of low temperature and high magnetic field for STM and related spectroscopy techniques allows us to investigate the novel physical properties of materials at these extreme conditions with high energy resolution. Here, we present the construction and the performance of an ultrahigh vacuum 3He fridge-based STM system with a 7 Tesla superconducting magnet. It features a double deck sample stage on the STM head so we can clean the tip by field emission or prepare a spin-polarized tip in situ without removing the sample from the STM. It is also capable of in situ sample and tip exchange and preparation. The energy resolution of scanning tunneling spectroscopy at T = 310 mK is determined to be 400 mK by measuring the superconducting gap with a niobium tip on a gold surface. We demonstrate the performance of this STM system by imaging the bicollinear magnetic order of Fe1+xTe at T = 5 K.

Lattice-resolved frictional pattern probed by tailored carbon nanotubes.

In this study, we demonstrate a high-resolution friction profiling technique using synchronous atomic/lateral force microscopy (AFM/LFM). The atomic resolution is achieved by our special carbon nanotube (CNT) probes made via in situ tailoring and manipulation inside an ultra-high vacuum transmission electron microscope (UHV TEM). The frictional pattern mapped on graphite displays a periodic distribution similar to the atomic (0001)-oriented graphite lattice structure. Furthermore, the electrothermal process in the UHV TEM renders a graphite-capped CNT tip, which delivers the nanotribology study within two graphite layers by the LFM measurement on graphite. The synchronous AFM and LFM images can discern a spatial shift between the atomic points and local friction maxima. We further interpret this shift as caused by the lattice distortion, which in turn induces irreversible energy dissipation. We believe this is the origin of atomic friction on the sub-nanonewton scale.

The fabrication of carbon nanotube probes utilizing ultra-high vacuum transmission electron microscopy.

An application of ultra-high vacuum transmission electron microscopy (UHV TEM) is demonstrated for the fabrication of carbon nanotube (CNT) probes. In this study, all the fabrication processes -- such as CNT attachment, CNT orientation manipulation, and apex trimming -- are integrated into a single UHV TEM system. The in situ work under UHV conditions (<5 x 10(-10) mbar) allows us to clean the tip surface at the start of the fabrication process to ensure a good contact between the tip and CNT. Furthermore, the CNT size can be user-selected to meet the various needs for scanning probe microscopy (SPM). Most importantly, the in situ trimming enables a multi-walled CNT to have the sharpness of a single-walled CNT. The three advantages mentioned above are designed to improve conventional methods and will be shown in detail as the procedures of CNT probe fabrication by a series of high-resolution TEM images. Finally, we compare the scanned image via our CNT probes and conventional probes, where the typical artefacts coming from the conventional ones are addressed. We believe the technique we have developed here will further enhance the resolution of SPM measurements.

Specular scattering probability of acoustic phonons in atomically flat interfaces.

We report a direct determination of the specular scattering probability of acoustic phonons at a crystal boundary by observing the escape of incident coherent phonons from the coherent state during reflection. In the sub-THz frequency range where the phonon wavelength is much longer than the lattice constant, the acoustic phonon-interface interaction is found to agree well with the macroscopic theory on wave scattering from rough surfaces. This examination thus quantitatively verifies the dominant role of atomic-scale corrugations in the Kapitza anomaly observed at 1-10 K and further opens a new path to nondestructively estimate subnanoscale roughness of buried interfaces.

Two-dimensional dopant profiling by electrostatic force microscopy using carbon nanotube modified cantilevers.

A two-dimensional (2D) dopant profiling technique is demonstrated in this work. We apply a unique cantilever probe in electrostatic force microscopy (EFM) modified by the attachment of a multiwalled carbon nanotube (MWNT). Furthermore, the tip apex of the MWNT was trimmed to the sharpness of a single-walled carbon nanotube (SWNT). This ultra-sharp MWNT tip helps us to resolve dopant features to within 10 nm in air, which approaches the resolution achieved by ultra-high vacuum scanning tunnelling microscopy (UHV STM). In this study, the CNT-probed EFM is used to profile 2D buried dopant distribution under a nano-scale device structure and shows the feasibility of device characterization for sub-45 nm complementary metal-oxide-semiconductor (CMOS) field-effect transistors.

Non-degenerate fs pump-probe study on InGaN with multi-wavelength second-harmonic generation.

Non-degenerate fs pump-probe experiments in the UV-visible range for ultrafast carrier dynamics study of InGaN with adjustable pump and probe photon energies are implemented with simultaneously multiwavelength second-harmonic generation (SHG) of a 10 fs Ti:sapphire laser. The multi-wavelength SHG is realized with two beta-barium borate crystals of different cutting angles. The full-widths at half-maximum of the SHG pulses are around 150 fs, which are obtained from the cross-correlation measurement with a reverse-biased 280-nm light-emitting diode as the twophoton absorption photo-detector. Such pulses are used to perform nondegenerate pump-probe experiments on an InGaN thin film, in which indium-rich nano-clusters and compositional fluctuations have been identified. Relaxation of carriers from the pump level to the probe one through the scattering-induced local thermalization (<1 ps) and then the carrier-transport-dominating global thermalization (in several ps) processes is observed.