Reversible switching of single tin phthalocyanine molecules on the InAs(111)A surface

Individual tin phthalocyanine (SnPc) molecules adsorbed on the InAs(111)A surface were studied by low-temperature scanning tunnelling microscopy (STM) at 5?K. Consistently with the nonplanar molecular structure, SnPc adopts two in-plane adsorption geometries with the centre Sn atom either above (SnPc(up)) or below (SnPc(down)) the molecular plane. Depending on the current and bias applied to the tunnel junction, the molecule can be reversibly switched between the two conformations, implying a controlled transfer of the Sn atom through the molecular plane. The SnPc(down) conformer is characterized by an enhanced surface bonding as compared to the SnPc(up) conformer. SnPc(up) molecules can be repositioned by the STM tip by means of lateral manipulation, whereas this is not feasible for SnPc(down) molecules. The reversible switching process thus enables one to either laterally move the molecule or anchor it to the semiconductor surface.     

Absorption of surface polaritons by molecules near the surface of a metallic slab

The cross section for absorption of surface polaritons (SP) by molecules above a metallic slab is calculated quantum mechanically. It shows a strong dependence on the thickness of the slab. This feature, even more pronounced, should also appear in more complex processes involving SP. It is also argued that SP guided by thin metallic films should be a useful tool in the spectroscopy of absorbates.     

Laser-induced resonance shifts of single molecules self-coupled by a metallic surface

The spectral properties of single molecules placed near a metallic surface are investigated at low temperatures. Because of the high quality factor of the optical resonance, a laser-induced shift of the molecular lines is evidenced for the first time. The shift dependence on the laser excitation intensity and on the dephasing rate of the transition dipole is studied. A simple theoretical model of a laser-driven molecule self-coupled by a mirror is developed to qualitatively interpret the observations.     

Switching and nonswitching phases of photomechanical molecules in dissipative environments

We study the effects of dissipation on photoisomerization (PI). The result suggests the existence of two types of environment depending on whether it entangles with the molecule. With entanglement there is a quantum phase transition between a state where PI persists, to a state where PI is quenched by the environment. Without entanglement, the environment only quantitatively modifies the PI behavior. We discuss the relevance of our results to a recent STM experiment, and predict the signature of the quantum phase transition in optical absorption spectra.     

Ionization of hydrogen Rydberg molecules at a metal surface

The interaction of a beam of Rydberg molecules with a metal surface is investigated for the first time. Hydrogen molecules in a supersonic expansion are excited to Rydberg states with principal quantum number n, in the range 17-22 and are directed at a small angle onto a flat surface of either aluminum or gold. Detection of ions produced when Rydberg electrons tunnel into the metal surface provides information on the interaction between the Rydberg molecules and the surface potential. The experimental results suggest that, when close to the metal surface, the Rydberg molecules undergo a process of surface-induced rotational autoionization. It is found that the surface-ionization cross section shows strong resonances as a function of the applied electric field, which are independent of the metal studied.     

Formation of a metallic layer from individual atoms

Adsorption of copper, gold and beryllium on (110), (100), and (211) single-crystal planes of tungsten leads to essentially different work-function changes. It is known from numerous investigations of alkali-metal adsorption on metal substrates that the work-function variation reflects the electronic processes occurring during the formation of the adlayer. It is obvious that copper, gold and beryllium adsorption is accompanied by a wide variety of physical processes different from those appearing in alkali-metal adsorption. The existing experimental data concerning work-function changes induced by copper, gold and beryllium adsorption are compiled. A model is developed, which may explain these changes.     

Reversible switching of ultrastrong light-molecule coupling

We demonstrate that photochromic molecules enable switching from the weak- to ultrastrong-coupling regime reversibly, by using all-optical control. This switch is achieved by photochemically inducing conformational changes in the molecule. Remarkably, a Rabi splitting of 700 meV is measured at room temperature, corresponding to 32% of the molecular transition energy. A similar coupling strength is demonstrated in a plasmonic structure. Such systems present a unique combination of coupling strength and functional capacities.     

Conduction switching of photochromic molecules

We report a theoretical study of single molecule conduction switching of photochromic dithienylethene molecules. The light-induced intramolecular transformation drives a swapping of the highest occupied molecular orbital and lowest unoccupied molecular orbital between two distinct conjugated paths. The shuffling of single and double bonds produces a significant conductance change when the molecule is sandwiched between metal electrodes. We model the switching event using quantum molecular dynamics and the conductance changes using Green's function electronic transport theory. We find large on-off conductance ratios (between 10 and over 100) depending on the side group outside the switching core.     

Angular emission profiles of dye molecules excited by surface plasmon waves at a metal surface

The angular distribution of fluorescence emission from dye molecules excited by surface plasmon waves in a silver film is reported. Coupling of the emitted fluorescence to a surface plasmon mode at the Stokes shifted wavelength results in a sharply peaked angular profile in the prism half space. Fresnel theory is used to model experimental results obtained for thick and thin sample dye films and for micron-size particles containing dye.     

High-optical-throughput individual nanoscale aperture in a multilayered metallic film

The optical transmission of an individual subwavelength aperture in a multilayered metal film is shown to be enhanced compared with that of a homogeneous metal film. The enhancement effect is due to the light coupling to surface plasmon excitation facilitated by a film periodicity. The sensitivity of the transmission to the dielectric filling of the aperture is also shown. The latter effect can be used to switch and control the transmittance. Devices based on enhanced transmission through nanosized apertures can find applications in high-density optical and magneto-optical data storage, high-resolution microscopy, and photolithography, where nanoscale light sources with high-optical-power throughput are required, as well as in sensor applications.     

The exchange-correlation energy of a metallic surface

The exchange-correlation energy of a metal surface is analyzed in terms of the wavelength of the fluctuations which contribute to it. A scheme is proposed to interpolate between the short-wavelength region properly described by the local density functional approximation and the long-wavelength region for which an exact limiting form is established. This interpolation scheme is tested and verified for the soluble infinite barrier model and then applied to realistic density profiles.     

Fermi surface and metallic properties of graphite at high pressures

A potential of superconductivity of pure graphite has been theoretically examined. At normal pressure, the carrier concentration is too low to exhibit superconductivity. On applying pressure, the band dispersion along the c-axis is significantly enhanced, resulting in an increase in the carrier concentration; 10²⁰ cm^-3 at p=30 GPa. This is favorable to observe superconductivity. Accurate Fermi surfaces are illustrated: a new Fermi surface appears around K point at p=25 GPa.     

Scattering of surface state electrons at large organic molecules

The scattering of surface state electrons at Lander-type molecules on Cu(111) is investigated by means of scanning tunneling microscope (STM) experiments at low temperature and model calculations. Specific information concerning the electronic interaction of the different internal groups of the molecule with the surface is obtained. Remarkably, the central molecular wire of the molecule, although decoupled from the surface by spacer groups and therefore not visible in STM images, is the main one responsible for scattering of surface state electrons.     

Kohn-Sham exchange potential for a metallic surface

The behavior of the surface barrier that forms at the metal-vacuum interface is important for several fields of surface science. Within the density functional theory framework, this surface barrier has two nontrivial components: exchange and correlation. Exact results are provided for the exchange component, for a jellium metal-vacuum interface, in a slab geometry. The Kohn-Sham exact-exchange potential V(x)(z) has been generated by using the optimized effective potential method, through an accurate numerical solution, imposing the correct boundary condition. It has been proved analytically, and confirmed numerically, that V(x)(z--> infinity) --> -e(2)/z; this conclusion is not affected by the inclusion of correlation effects. Also, the exact-exchange potential develops a shoulderlike structure close to the interface, on the vacuum side. The issue of the classical image potential is discussed.     

Spatial switching of quadratic solitons in engineered quasi-phase-matched structures

We show that a variety of quasi-phase-matched structures with engineered patterns can potentially be used for soliton control in quadratic nonlinear media. We study geometries with dislocations, tilts, and wells and predict spatial switching between different output soliton states. Experimental implementation conditions are discussed.     

On the interfacial capacitance of an electrolyte at a metallic electrode around zero surface charge

The behaviour of the capacitance of a planar double layer containing a restricted primitive model electrolyte (equi-sized rigid ions moving in a continuum dielectric) at and around zero surface charge is examined for a polarizable electrode with particular emphasis on a metallic surface. Capacitance results are reported for symmetric valency (1:1) salts encompassing a range of concentrations and temperatures covering both electrolyte solution and ionic liquid regimes. Although the modified Poisson–Boltzmann theory is principally employed, at higher concentrations the theoretical calculations have been supplemented by Monte Carlo simulations. Capacitance anomaly, that is, increase of capacitance with temperature at low temperatures, is seen to occur when the electrode is an insulator with a low dielectric constant or when it is unpolarized. No capacitance anomaly is, however, seen for a metallic electrode with an infinite dielectric constant and in this situation the capacitance increases (a) dramatically at low temperatures (strong coupling) at a given concentration, and (b) as concentration increases at a given temperature. These capacitance trends are consistent with earlier works in the presence or absence of surface polarization and, in particular, the results for a conducting electrode at ionic liquid concentrations are consistent with that recently reported by Loth et al. [Phys. Rev. E, 82, 056102 (2010)]. Overall the theoretical predictions are qualitative to semi-quantitative with the simulations.     

Reversible magnetization of surface superconductivity

Direct measurements of the surface superconducting magnetization of the PbTl system shows that this state is a thermodynamic reversible one.     

Electrostatic surface trap for cold polar molecules on a chipElectrostatic surface trap for cold polar molecules on a chipElectrostatic surface trap for cold polar molecules on a chip

We propose a simple scheme for trapping cold polar molecules in low-field seeking states on the surface of a chip by using a grounded metal plate and two finite-length charged wires that half embanked in an insulating suhstrate, calculate the electric field distributions generated by our charged-wire layout in free space and the corresponding Stark potentials for ND3 molecules, and analyze the dependence of the trapping center position on the geometric parameters. Moreover, the loading and trapping processes of cold ND3 molecules are studied by using the Monte Carlo method. Our study shows that the loading efficiency of the trap scheme can reach 11.5%, and the corresponding temperature of the trapped cold molecules is about 26.4 inK.