We have observed reversible light-induced mechanical switching for individual organic molecules bound to a metal surface. Scanning tunneling microscopy (STM) was used to image the features of individual azobenzene molecules on Au(111) before and after reversibly cycling their mechanical structure between trans and cis states using light. Azobenzene molecules were engineered to increase their surface photomechanical activity by attaching varying numbers of tert-butyl (TB) ligands ("legs") to the azobenzene phenyl rings. STM images show that increasing the number of TB legs "lifts" the azobenzene molecules from the substrate, thereby increasing molecular photomechanical activity by decreasing molecule-surface coupling.
Topological superconductors represent a newly predicted phase of matter that is topologically distinct from conventional superconducting condensates of Cooper pairs. As a manifestation of their topological character, topological superconductors support solid-state realizations of Majorana fermions at their boundaries. The recently discovered superconductor Cu(x)Bi(2)Se(3) has been theoretically proposed as an odd-parity superconductor in the time-reversal-invariant topological superconductor class, and point-contact spectroscopy measurements have reported the observation of zero-bias conductance peaks corresponding to Majorana states in this material. Here we report scanning tunneling microscopy measurements of the superconducting energy gap in Cu(x)Bi(2)Se(3) as a function of spatial position and applied magnetic field. The tunneling spectrum shows that the density of states at the Fermi level is fully gapped without any in-gap states. The spectrum is well described by the Bardeen-Cooper-Schrieffer theory with a momentum independent order parameter, which suggests that Cu(x)Bi(2)Se(3) is a classical s-wave superconductor contrary to previous expectations and measurements.
We have used single-molecule-resolved scanning tunneling microscopy to measure the photomechanical switching rates of azobenzene-derived molecules at a gold surface during exposure to UV and visible light. This enables the direct determination of both the forward and reverse photoswitching cross sections for surface-mounted molecules at different wavelengths. In a dramatic departure from molecular behavior in solution-based environments, visible light does not efficiently reverse the reaction for azobenzene-derived molecules at a gold surface.
We measured the response of the surface state spectrum of epitaxial Sb(2)Te(3) thin films to applied gate electric fields by low temperature scanning tunneling microscopy. The gate dependent shift of the Fermi level and the screening effect from bulk carriers vary as a function of film thickness. We observed a gap opening at the Dirac point for films thinner than four quintuple layers, due to the coupling of the top and bottom surfaces. Moreover, the top surface state band gap of the three quintuple layer films was found to be tunable by a back gate, indicating the possibility of observing a topological phase transition in this system. Our results are well explained by an effective model of 3D topological insulator thin films with structure inversion asymmetry, indicating that three quintuple layer Sb(2)Te(3) films are topologically nontrivial and belong to the quantum spin Hall insulator class.
Single-molecule-resolved scanning tunneling microscopy of tetra-tert-butyl azobenzene (TTB-AB) molecules adsorbed onto Au(111) reveals chirality selection rules in their photoswitching behavior. This observation is enabled by the fact that trans-TTB-AB molecules self-assemble into homochiral domains. Cis-TTB-AB molecules produced via photoisomerization are found in two distinct conformations with final state chirality determined by the initial trans isomer chirality. Based on these observations and ab initio calculations, we propose a new inversion-based dynamical photoswitching mechanism for azobenzene molecules at a surface.
Electrical field control of the carrier density of topological insulators (TI) has greatly expanded the possible practical use of these materials. However, the combination of low temperature local probe studies and a gate tunable TI device remains challenging. We have overcome this limitation by scanning tunneling microscopy and spectroscopy measurements on in-situ molecular beam epitaxy growth of Bi 2 Se 3 films on SrTiO 3 substrates with pre-patterned electrodes. Using this gating method, we are able to shift the Fermi level of the top surface states by ≈250 meV on a 3 nm thick Bi 2 Se 3 device. We report field effect studies of the surface state dispersion, band gap, and electronic structure at the Fermi level.
Photomechanical switching (photoisomerization) of molecules at a surface is found to strongly depend on molecule-molecule interactions and molecule-surface orientation. Scanning tunneling microscopy was used to image photoswitching behavior in the single-molecule limit of tetra-tert-butyl-azobenzene molecules adsorbed onto Au(111) at 30 K. Photoswitching behavior varied strongly with surface molecular island structure, and self-patterned stripes of switching and nonswitching regions were observed having approximately 10 nm pitch. These findings can be summarized into photoswitching selection rules that highlight the important role played by a molecule's nanoscale environment in determining its switching properties.
Heterogeneous
interfaces exhibit remarkable material properties resulting from their
structural motifs, the judicious placement of functional chemical
groups, etc. It has been a long-standing challenge to manipulate and
design interface structures at the atomic level to achieve new functionalities.
Here, we demonstrate that by modifying the length of the backbone
in alkanolamines one can control the packing density of organic monolayers
adsorbed on rutile TiO2 and the interaction strength between
their amine functional group and the substrate. As a result, we observed
strikingly different activities in CO2 capture by the amine
functional group of different alkanolamines on TiO2(110).
Synchrotron photoelectron spectroscopy at near-ambient CO2 pressures showed that adsorbed 2-amino-1-ethanol (monoethanolamine,
MEA) is inactive, whereas the amine group in 3-amino-1-propanol (3AP)/TiO2(110) readily reacts with and captures CO2. Our
results suggest that the geometry of the interface plays a decisive
role in the reactivity of adsorbed functionalized organic molecules,
such as solid-supported alkanolamines for CO2 capture.
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