Ring structures fabricated from HgTe/HgCdTe quantum wells have been used to study AharonovBohm type conductance oscillations as a function of Rashba spin-orbit splitting strength. We observe non-monotonic phase changes indicating that an additional phase factor modifies the electron wave function. We associate these observations with the Aharonov-Casher effect. This is confirmed by comparison with numerical calculations of the magneto-conductance for a multichannel ring structure within the Landauer-Büttiker formalism. In the early 1980s it was shown that a quantum mechanical system acquires a geometric phase for a cyclic motion in parameter space. This geometric phase under adiabatic motion is called Berry phase [1], while its later generalization to include non-adiabatic motion is known as Aharonov-Anandan phase [2]. A manifestation of the Berry phase is the well known AharonovBohm (AB) phase [3] of an electrical charge which cycles around a magnetic flux. Aside from the AB effect, the first experimental observation of the Berry phase was reported in 1986 for photons in a wound optical fiber [4]. Another important Berry phase effect is the AharonovCasher (AC) effect [5], which has been proposed to occur when an electron propagates in a ring structure in an external magnetic field perpendicular to the ring plane in the presence of SO interaction [6].This AC effect can be seen when two partial waves move around the ring in different directions. They will acquire a phase difference which depends on the spin orientation with respect to the total magnetic field B tot = B ext + B ef f and the path of each partial wave. B ef f is the effective field induced by the SO interaction. The phase difference is approximately [6] where s =↑ and ↓ denote parallel and anti-parallel orientation to B tot , b = +1 for s =↑ and b = −1 for s =↓, and the superscript −(+) denotes a clockwise (counterclockwise) evolution, respectively. In the above equations, α is the SO parameter, r the ring radius, m * the effective electron mass and θ the angle between the external ( B ext ) and the total magnetic field B tot . For both equations, the first term on the right hand side can be identified with the AB phase and the second term of Eq. (1) with the geometric Berry or Aharonov-Anandan phase. The second term in Eq. (2) represents the dynamic part of the AC phase, i.e. the phase of a particle with a magnetic moment that moves around an electric field. From the expressions above, it can be seen that an increase of the AC phase will lead to a phase change that increases continuously with α, whereas the contribution due to the geometric phase results in a phase shift limited to ∆ϕ geom ≤ π.Both the AC phase [7] and the geometric phase [8, 9] depend on the SO interaction. As a result, one expects a complicated non-monotonic interference pattern as a function of magnetic field and SO interaction strength. So far, to our knowledge, apart from the AB effect no direct observation of phase related effects in solid state systems has been reported. Rec...
The adsorption of 4-mercaptopyridine (4MPy) molecules on reconstructed Au(111) is investigated by Scanning Tunneling Microscopy (STM) and Spectroscopy (STS) at low temperature and under ultra-high vacuum (UHV) conditions. As made visible by STM, at low coverage (<10%) 4MPy adsorbs preferentially at elbow sites of the Herringbone reconstruction and at step edges of the Au(111). Increasing coverage (but still <30%) results in formation of molecular chains followed, at even higher coverage, by a 3-dimensional growth. Detailed analysis of z-V spectroscopy (ramping the tunneling bias V while keeping the tunneling current constant) provides information on the bias dependent apparent height of a single 4MPy/Au(111) as well as on the local density of states (LDOS) of single and chain 4MPy molecules in comparison to the bare Au(111) surface revealing a significant shift of the lowest unoccupied molecular orbital (LUMO) towards lower energy for molecules within chains. Additionally, the data provide no evidence that for these samples prepared in UHV the adsorption of 4MPy on Au(111) requires mediating Au adatoms. Also, clear indications are given that the adsorption does not induce a strong reduction of the Au DOS close to its Fermi energy. Finally, in context of the apparent STM height of 4MPy molecules, the behavior of the differential barrier height Φ(diff)(V) = (∂(z)∂(V)I/∂(V)I)(2) on bare Au(111) and 4MPy/Au(111) is analyzed and the corresponding experimental values are applied to recover the LDOS of the molecule for unoccupied states according to a previously published numerical recipe [B. Koslowski, H. Pfeifer and P. Ziemann, Phys. Rev. B, 2009, 80, 165419 and M. Ziegler, N. Néel, A. Sperl, J. Kröger, and R. Berndt, Phys. Rev. B, 2009, 80, 125402]. In this way, one obtains a spectrum comprising a constant DOS of the Shockley-like surface state of Au(111) and a Lorentzian line attributed to the LUMO of 4MPy.
Vibrational spectroscopy is a powerful tool to identify molecules and to characterise their chemical state. Inelastic electron tunnelling spectroscopy (IETS) combined with scanning tunnelling microscopy (STM) allows the application of vibrational analysis to a single molecule. Up to now, IETS was restricted to small species due to the complexity of vibration spectra for larger molecules. We extend the horizon of IETS for both experiment and theory by measuring the STM-IETS spectra of mercaptopyridine adsorbed on the (111) surface of gold and comparing it to theoretical spectra. Such complex spectra with more than 20 lines can be reliably determined and computed leading to completely new insights. Experimentally, the vibrational spectra exhibit a dependence on the specific adsorption site of the molecules. Theoretically, this dependence is only accessible if anharmonic contributions to the interaction potentials are included. These joint experimental and theoretical advances open new perspectives for structure determination of organic adlayers.
SummaryTerthiophene (3T) molecules adsorbed on herringbone (HB) reconstructed Au(111) surfaces in the low coverage regime were investigated by means of low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS) under ultra-high vacuum conditions. The 3T molecules adsorb preferentially in fcc regions of the HB reconstruction with their longer axis oriented perpendicular to the soliton walls of the HB and at maximum mutual separation. The latter observation points to a repulsive interaction between molecules probably due to parallel electrical dipoles formed during adsorption. Constant-separation (I-V) and constant-current (z-V) STS clearly reveal the highest occupied (HOMO) and lowest unoccupied (LUMO) molecular orbitals, which are found at −1.2 eV and +2.3 eV, respectively. The HOMO–LUMO gap corresponds to that of a free molecule, indicating a rather weak interaction between 3T and Au(111). According to conductivity maps, the HOMO and LUMO are inhomogeneously distributed over the adsorbed 3T, with the HOMO being located at the ends of the linear molecule, and the LUMO symmetrically with respect to the longer axis of the molecule at the center of its flanks. Analysis of spectroscopic data reveals details of the contrast mechanism of 3T/Au(111) in STM. For that, the Shockley-like surface state of Au(111) plays an essential role and appears shifted outwards from the surface in the presence of the molecule. As a consequence, the molecule can be imaged even at a tunneling bias within its HOMO–LUMO gap. A more quantitative analysis of this detail resolves a previous discrepancy between the fairly small apparent STM height of 3T molecules (1.4–2.0 nm, depending on tunneling bias) and a corresponding larger value of 3.5 nm based on X-ray standing wave analysis. An additionally observed linear decrease of the differential tunneling barrier at positive bias when determined on top of a 3T molecule is compared to the bias independent barrier obtained on bare Au(111) surfaces. This striking difference of the barrier behavior with and without adsorbed molecules is interpreted as indicating an adsorption-induced dimensionality transition of the involved tunneling processes.
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