Compressed Sensing (CS) techniques are used to measure and reconstruct surface dynamical processes with a helium spin-echo spectrometer for the first time. Helium atom scattering is a well established method for examining the surface structure and dynamics of materials at atomic sized resolution and the spin-echo technique opens up the possibility of compressing the data acquisition process. CS methods demonstrating the compressibility of spin-echo spectra are presented for several measurements. Recent developments on structured multilevel sampling that are empirically and theoretically shown to substantially improve upon the state of the art CS techniques are implemented. In addition, wavelet based CS approximations, founded on a new continuous CS approach, are used to construct continuous spectra. In order to measure both surface diffusion and surface phonons, which appear usually on different energy scales, standard CS techniques are not sufficient. However, the new continuous CS wavelet approach allows simultaneous analysis of surface phonons and molecular diffusion while reducing acquisition times substantially. The developed methodology is not exclusive to Helium atom scattering and can also be applied to other scattering frameworks such as neutron spin-echo and Raman spectroscopy.
1 February 2021 in Physical Chemistry Chemical Physics
This paper presents material properties particularly suited to be measured with helium scattering techniques. Below a specific science case example illustrating the measurement of the electron–phonon coupling constant λ on a topological insulator surface.
We have studied the topological insulator (111) by means of helium atom scattering. The average electron-phonon coupling of (111) is determined by adapting a recently developed quantum-theoretical derivation of the helium scattering probabilities to the case of degenerate semiconductors. Based on the Debye-Waller attenuation of the elastic diffraction peaks of (111), measured at surface temperatures between 110 and , we find to be in the range of . This method allows us to extract a correctly averaged and to address the discrepancy between previous studies. The relatively modest value of is not surprising even though some individual phonons may provide a larger electron-phonon interaction. Furthermore, the surface Debye temperature of (111) is determined as . The electronic surface corrugation was analyzed based on close-coupling calculations. By using a corrugated Morse potential a peak-to-peak corrugation of 9% of the lattice constant is obtained.
4 November 2015 in The Journal of Physical Chemistry C
Using helium atom scattering, we have studied the structure and dynamics of a graphene layer prepared in situ on a Ni(111) surface. Graphene/Ni(111) exhibits a helium reflectivity of ∼20% for a thermal helium atom beam and a particularly small surface electron density corrugation ((0.06 ± 0.02) Å peak to peak height). The Debye–Waller attenuation of the elastic diffraction peaks of graphene/Ni(111) and Ni(111) was measured at surface temperatures between 150 and 740 K. A surface Debye temperature of θD = (784 ± 14) K is determined for the graphene/Ni(111) system and θD = (388 ± 7) K for Ni(111), suggesting that the interlayer interaction between graphene and the Ni substrate is intermediary between those for strongly interacting systems like graphene/Ru(0001) and weakly interacting systems like graphene/Pt(111). In addition we present measurements of low frequency surface phonon modes on graphene/Ni(111) where the phonon modes of the Ni(111) substrate can be clearly observed. The similarity of these findings with the graphene/Ru(0001) system indicates that the bonding of graphene to a metal substrate alters the dynamic properties of the graphene surface strongly and is responsible for the high helium reflectivity of these systems.
The surface phonon dispersion curves of Bi(111) have been measured by inelastic helium atom scattering (HAS) along the two symmetry directions. The complex set of observed dispersion curves, including several branches in the acoustic region, plus a localized and a resonant branch in the optical region, is interpreted by means of calculations based on density functional perturbation theory (DFPT). It is recognized that the upper phonon branches in the acoustic region starting at about meV and meV at zero wave vector correspond to shear-vertical and longitudinal modes localized on the third surface layer (second bilayer), respectively. The HAS ability of detecting subsurface phonons previously observed for Pb(111) multilayers is attributed to the comparatively strong electron-phonon interaction, and confirmed through a DFPT calculation of the phonon-induced surface charge-density oscillations. A comparison of the integrated HAS intensities with those of Pb(111) multilayers measured under similar kinematic conditions allows for an estimation of the electron-phonon mass-enhancement parameter for the Bi(111) surface. An anomaly at the point, quite sharp at 123 K but very broad at room temperature, is associated with recombination processes of bulk -point pocket electrons with bulk pocket holes at either or equivalent points.
7 February 2020 in The Journal of Physical Chemistry Letters
Atom scattering has been demonstrated to be a sensitive probe of the electron-phonon interaction parameter $\lambda$ at metal and metal-overlayer surfaces. Here it is shown that the theory linking $\lambda$ to the thermal attenuation of atom scattering spectra (the Debye-Waller factor), can be applied to topological semimetal surfaces, like the quasi-one dimensional charge-density-wave system Bi(114) and the layered pnictogen chalcogenides.