Control of Surface Plasmon Propagation and Terahertz Near-Field Waveforms in a Scanning Tunneling Microscope.

Coupling subcycle THz pulses to a scanning tunneling microscope (STM) enables ultrafast spectroscopy at the atomic scale. This technique critically depends on the shape of the THz near-field waveform in the tunnel junction. We characterize the THz electric field waveform in the STM junction by electro-optic sampling of tip-scattered THz light (-EOS) and pulse correlation using the THz-induced current.

Terahertz spectroscopy of collective charge density wave dynamics at the atomic scale.

Charge density waves are wave-like modulations of a material's electron density that display collective amplitude and phase dynamics. The interaction with atomic impurities induces strong spatial heterogeneity of the charge-ordered phase. Direct real-space observation of phase excitation dynamics of such defect-induced charge modulation is absent.

Selective excitation of vibrations in a single molecule.

The capability to excite, probe, and manipulate vibrational modes is essential for understanding and controlling chemical reactions at the molecular level. Recent advancements in tip-enhanced Raman spectroscopies have enabled the probing of vibrational fingerprints in a single molecule with Ångström-scale spatial resolution. However, achieving controllable excitation of specific vibrational modes in individual molecules remains challenging.

Launching Coherent Acoustic Phonon Wave Packets with Local Femtosecond Coulomb Forces.

Generation and manipulation of coherent acoustic phonons enables ultrafast control of solids and has been exploited for applications in various acoustic devices. We show that localized coherent acoustic phonon wave packets can be launched by ultrafast Coulomb forces in a scanning tunneling microscope (STM) using tip-enhanced terahertz electric fields. The wave packets propagate at the speed of the longitudinal acoustic phonon, creating standing waves up to 0.

Melamine self-assembly and dehydrogenation on Ag(111) studied by tip-enhanced Raman spectroscopy.

The adsorption and self-assembly structures of melamine molecules on an Ag(111) surface are studied by low temperature scanning tunneling microscopy (STM) combined with tip-enhanced Raman spectroscopy (TERS). Two ordered self-assembly phases of melamine molecules on Ag(111) were studied by STM and TERS, combining with first-principles simulations. The α-phase consists of flat-lying melamine molecules, while the β-phase consists of mixed up-standing/tilted melamine molecules.

Vibrational Property of α-Borophene Determined by Tip-Enhanced Raman Spectroscopy.

We report a Raman characterization of the α borophene polymorph by scanning tunneling microscopy combined with tip-enhanced Raman spectroscopy. A series of Raman peaks were discovered, which can be well related with the phonon modes calculated based on an asymmetric buckled α structure. The unusual enhancement of high-frequency Raman peaks in TERS spectra of α borophene is found and associated with its unique buckling when landed on the Ag(111) surface.

Variable Repetition Rate THz Source for Ultrafast Scanning Tunneling Microscopy.

Broadband THz pulses enable ultrafast electronic transport experiments on the nanoscale by coupling THz electric fields into the devices with antennas, asperities, or scanning probe tips. Here, we design a versatile THz source optimized for driving the highly resistive tunnel junction of a scanning tunneling microscope. The source uses optical rectification in lithium niobate to generate arbitrary THz pulse trains with freely adjustable repetition rates between 0.

Raman Spectroscopy of Two-Dimensional Borophene Sheets.

The successful fabrication of a two-dimensional boron sheet, which features a triangular lattice with periodic hole arrays, has stimulated great interest in its specific structure as well as properties such as possible superconductivity. Here, we report a study on the vibrational spectra and electron-phonon coupling (EPC) in monolayer boron sheets by in situ Raman and tip-enhanced Raman spectroscopy (TERS) at low temperature and ultrahigh vacuum. The gap-mode TERS gives a 3 × 10 selective enhancement on vertical vibrational Raman modes.

Scanning tunneling microscopy investigations of unoccupied surface states in two-dimensional semiconducting β-√3 × √3-Bi/Si(111) surface.

Two-dimensional surface structures often host a surface state in the bulk gap, which plays a crucial role in the surface electron transport. The diversity of in-gap surface states extends the category of two-dimensional systems and gives us more choices in material applications. In this article, we investigated the surface states of β-√3 × √3-Bi/Si(111) surface by scanning tunneling microscopy.

Low-temperature, ultrahigh-vacuum tip-enhanced Raman spectroscopy combined with molecular beam epitaxy for in situ two-dimensional materials' studies.

Tip-enhanced Raman spectroscopy (TERS), which combines scanning probe microscopy with the Raman spectroscopy, is capable to access the local structure and chemical information simultaneously. However, the application of ambient TERS is limited by the unstable and poorly controllable experimental conditions. Here, we designed a high performance TERS system based on a low-temperature ultrahigh-vacuum scanning tunneling microscope (LT-UHV-STM) and combined with a molecular beam epitaxy (MBE) system.

The Pentagonal Nature of Self-Assembled Silicon Chains and Magic Clusters on Ag(110).

The atomic structures of self-assembled silicon nanoribbons and magic clusters on Ag(110) substrate have been studied by high-resolution noncontact atomic force microscopy (nc-AFM) and tip-enhanced Raman spectroscopy (TERS). Pentagon-ring structures in Si nanoribbons and clusters have been directly visualized. Moreover, the vibrational fingerprints of individual Si nanoribbon and cluster retrieved by subnanometer resolution TERS confirm the pentagonal nature of both Si nanoribbons and clusters.

Experimental realization of honeycomb borophene.

We report the successful preparation of a purely honeycomb, graphene-like borophene, by using an Al(1 1 1) surface as the substrate and molecular beam epitaxy (MBE) growth in ultrahigh vacuum. Scanning tunneling microscopy (STM) images reveal perfect monolayer borophene with planar, non-buckled honeycomb lattice similar as graphene. Theoretical calculations show that the honeycomb borophene on Al(1 1 1) is energetically stable.

Vibrational Properties of a Monolayer Silicene Sheet Studied by Tip-Enhanced Raman Spectroscopy.

Combining ultrahigh sensitivity, spatial resolution, and the capability to resolve chemical information, tip-enhanced Raman spectroscopy (TERS) is a powerful tool to study molecules or nanoscale objects. Here we show that TERS can also be a powerful tool in studying two-dimensional materials. We have achieved a 10^{9} Raman signal enhancement and a 0.

Metastable phases of 2D boron sheets on Ag(1 1 1).

Two reproducible new phases of 2D boron sheets have been found on Ag(1 1 1). One of them shares the identical atomic structure of the previously reported S1 phase (β sheet) but has a different rotational relationship with the substrate, and thus exhibits very different features in scanning tunneling microscopy (STM) images. The other new phase has a hexagonal symmetry and is proposed to be the long-expected α-sheet.

Tip-Enhanced Raman Spectroscopy.

Tip-enhanced Raman spectroscopy (TERS), a combination of Raman spectroscopy and apertureless near-field scanning optical microscopy using a metallic tip which resonates with the local mode of the surface plasmon, can provide a high-sensitive and high-spatial-resolution optical analytical approach. The basic principle of TERS, common experimental setups, various SPM technologies, and excitation/collection configurations are introduced as well as recent research progress with respect to TERS.

Molecular resonant dissociation of surface-adsorbed molecules by plasmonic nanoscissors.

The ability to break individual bonds or specific modes in chemical reactions is an ardently sought goal by chemists and physicists. While photochemistry based methodologies are very successful in controlling e.g.

Direct visual evidence for chemical mechanism of SERRS of the S-complex of pyrimidine molecule adsorbed on silver nanoparticle via charge transfer.

In this paper, the S-complex of pyrimidine molecule absorbed on silver clusters was employed as a model molecule to study the enhancement mechanism in surface-enhanced resonance Raman scattering (SERRS). We described the chemical enhancement of SERRS through charge transfer (CT) from Ag20 to pyrimidine on resonance excitation, and electromagnetic enhancement through intracluster charge redistribution (CR) on the electronic intracluster collective oscillation excitation. It is shown that SERRS process of the pyrimidine molecule absorbed on silver clusters with different incident wavelength are dominated by different enhancement mechanisms.

Insight into vibration mode-resolved plasmon enhanced Raman optical activity.

Vibration mode-resolved plasmon enhanced Raman optical activities (PE-ROA) are investigated experimentally and theoretically. It is found that the profile of PE-ROA is significantly different from that of ROA. Our experimental results revealed that PE-ROA is not a universal method for the enhancement of ROA.