Jakub S. Prauzner-Bechcicki

Two-mode squeezed vacuum state coupled to the common thermal reservoir

Entangled states play a crucial role in quantum information protocols, thus the dynamical behaviour of entanglement is of great importance. In this letter, we consider a two-mode squeezed vacuum state coupled to one thermal reservoir as a model of an entangled state embedded in an environment. As a criterion for entanglement we use a continuous-variable equivalent of the Peres–Horodecki criterion, namely the Simon criterion. To quantify entanglement we use the logarithmic negativity. We derive a condition, which assures that the state remains entangled in spite of the interaction with the reservoir. Moreover for the case of interaction with vacuum as an environment we show that a state of interest after infinitely long interaction is not only entangled, but also pure. For comparison we also consider a model in which each mode is coupled to its own reservoir.

Supramolecular ordering of PTCDA molecules: the key role of dispersion forces in an unusual transition from physisorbed into chemisorbed state.

Adsorption and self-assembly of large π-conjugated 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA) molecules on rutile TiO(2)(110) surface have been investigated using a combination of high-resolution scanning tunneling microscopy (STM), low-energy electron diffraction, and density functional theory calculations with inclusion of Grimme treatment of the dispersion forces (DFT-D). Evolution of the STM images as a function of PTCDA coverage is caused by transition of the adsorption mode from physisorbed single adspecies and meandering stripes into spontaneously ordered chemisorbed molecular assemblies. This change in the adsorption fashion is accompanied by significant bending of the intrinsically flat, yet elastic, PTCDA molecule, which allows for strong electronic coupling of the dye adspecies with the TiO(2) substrate. Extensive DFT-D modeling has revealed that adsorption is controlled by interfacial and intermolecular dispersion forces playing a dominant role in the adsorption of single PTCDA species, their self-organization into the meandering stripes, and at the monolayer coverage acting collectively to surmount the chemisorption energy barrier associated with the molecule bending. Analysis of the resulting density of states has revealed that alignment of the energy levels and strong electronic coupling at the PTCDA/TiO(2) interface are beneficial for dye sensitization purposes.

Adsorption of organic molecules on the TiO2(011) surface: STM study

High resolution scanning tunneling microscopy has been applied to investigate adsorption and self-assembly of large organic molecules on the TiO(2)(011) surface. The (011) face of the rutile titania has been rarely examined in this context. With respect to possible industrial applications of rutile, quite often in a powder form, knowledge on behavior of organic molecules on that face is required. In the presented study we fill in the gap and report on experiments focused on the self-assembly of organic nanostructures on the TiO(2)(011) surface. We use three different kinds of organic molecules of potential interest in various applications, namely, PTCDA and CuPc representing flat, planar stacking species, and Violet Landers specially designed for new applications in molecular electronics. In order to reach a complete picture of molecular behavior, extended studies with different surface coverage ranging from single molecule up to 2 monolayer (ML) thick films are performed. Our results show that the adsorption behavior is significantly different from previously observed for widely used metallic templates. Creation of highly ordered molecular lines, quasi-ordered wetting layers, controlled geometrical reorientation upon thermal treatment, existence of specific adsorption geometries, and prospects for tip-induced molecule ordering and manipulation provide better understanding and add new phenomena to the knowledge on the (011) face of rutile titania.

Time-Resolved Quantum Dynamics of Double Ionization in Strong Laser Fields

Quantum calculations of a (1+1)-dimensional model for double ionization in strong laser fields are used to trace the time evolution from the ground state through ionization and rescattering to the two-electron escape. The subspace of symmetric escape, a prime characteristic of nonsequential double ionization, remains accessible by a judicious choice of 1D coordinates for the electrons. The time-resolved ionization fluxes show the onset of single and double ionization, the sequence of events during the pulse, and the influences of pulse duration and reveal the relative importance of sequential and nonsequential double ionization, even when ionization takes place during the same field cycle.

Adsorption of Large Organic Molecules on Clean and Hydroxylated Rutile TiO2(110) Surfaces

Behavior of large organic molecules equipped with spacer groups (Violet Landers, VL) on the TiO(2)(110)-(1x1) surfaces is investigated by means of high-resolution scanning tunneling microscopy (STM). Two distinct adsorption geometries are observed. We demonstrate that the molecule adsorption morphology can be alternated by well-controlled STM tip-induced manipulation. It is used to probe the mobility of molecules and reveals locking in one of the analyzed adsorption sites, thus allow to enhance or reduce the mobility along the [001] direction. Field induced hydrogen desorption is used to perform lateral STM manipulation on a hydroxyl-free surface, which provides insight into the influence of surface hydroxyl groups on the molecule behavior. The ability to image with submolecular resolution both the central board and the spacer groups of the VL molecule is demonstrated.

[11]Anthrahelicene on InSb(001) c(8×2): A Low‐Temperature Scanning Probe Microscopy Study

The adsorption of individual [11]anthrahelicene molecules and their self-assembly into monolayer islands on an InSb(001) c(8×2) reconstructed surface is studied with low-temperature scanning probe microscopy. A racemic mixture is deposited on atomically flat terraces of InSb at room temperature. At lower coverage, the molecules tend to decorate atomic step edges of the substrate. At higher coverage, [11]anthrahelicene molecules form 2D islands. A quasi-hexagonal ordering of molecules within the layer is identified. Furthermore, it is shown that molecules adsorb with the helical axis almost perpendicular to the substrate. Interference between tunneling through the molecular layer and directly through space is reported. Finally, experimental results are compared to those of theoretical calculations.

STM tip-assisted engineering of molecular nanostructures: PTCDA islands on Ge(001):H surfaces.

Summary Islands composed of perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) molecules are grown on a hydrogen passivated Ge(001):H surface. The islands are studied with room temperature scanning tunneling microscopy and spectroscopy. The spontaneous and tip-induced formation of the top-most layer of the island is presented. Assistance of the scanning probe seems to be one of the factors that facilitate and speed the process of formation of the top-most layer.

Nonsequential double ionization of molecules

Double ionization of diatomic molecules by short linearly polarized laser pulses is analyzed. We consider the final stage of the ionization process, that is the decay of a highly excited two electron molecule, which is formed after rescattering. The saddles of the effective adiabatic potential energy close to which simultaneous escape of electrons takes place are identified. Numerical simulations of the ionization of molecules show that the process can be dominated by either sequential or nonsequential events. In order to increase the ratio of nonsequential to sequential ionizations very short laser pulses should be applied.

Transformations of PTCDA structures on rutile TiO2 induced by thermal annealing and intermolecular forces.

Summary Transformations of molecular structures formed by perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) molecules on a rutile TiO2(110) surface are studied with low-temperature scanning tunnelling microscopy. We demonstrate that metastable molecular assemblies transform into differently ordered structures either due to additional energy provided by thermal annealing or when the influence of intermolecular forces is increased by the enlarged amount of deposited molecules. Proper adjustment of molecular coverage and substrate temperature during deposition allows for fabrication of desired assemblies. Differences between PTCDA/TiO2(110) and PTCDA/TiO2(011) systems obtained through identical experimental procedures are discussed.

Scanning probe microscopy studies on the adsorption of selected molecular dyes on titania.

Titanium dioxide, or titania, sensitized with organic dyes is a very attractive platform for photovoltaic applications. In this context, the knowledge of properties of the titania–sensitizer junction is essential for designing efficient devices. Consequently, studies on the adsorption of organic dyes on titania surfaces and on the influence of the adsorption geometry on the energy level alignment between the substrate and an organic adsorbate are necessary. The method of choice for investigating the local environment of a single dye molecule is high-resolution scanning probe microscopy. Microscopic results combined with the outcome of common spectroscopic methods provide a better understanding of the mechanism taking place at the titania–sensitizer interface. In the following paper, we review the recent scanning probe microscopic research of a certain group of molecular assemblies on rutile titania surfaces as it pertains to dye-sensitized solar cell applications. We focus on experiments on adsorption of three types of prototypical dye molecules, i.e., perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA), phtalocyanines and porphyrins. Two interesting heteromolecular systems comprising molecules that are aligned with the given review are discussed as well.