Dynamic scanning probe microscopy of adsorbed molecules on graphite

We have used a combined dynamic scanning tunneling and atomic force microscope to study the organisation of weakly bound adsorbed molecules on a graphite substrate. Specifically we have acquired images of islands of the perylene derivative molecules. These weakly bound molecules may be imaged in dynamic STM, in which the probe is oscillated above the surface. We show that molecular resolution may be readily attained and that a similar mode of imaging may be realised using conventional STM arrangement. We also show, using tunnelling spectroscopy, the presence of an energy gap for the adsorbed molecules confirming a weak molecule-substrate interaction.Comment: 11 pages, 2 figure

Molecular random tilings as glasses

We have recently shown [Blunt et al., Science 322, 1077 (2008)] that p-terphenyl-3,5,3',5'-tetracarboxylic acid adsorbed on graphite self-assembles into a two-dimensional rhombus random tiling. This tiling is close to ideal, displaying long range correlations punctuated by sparse localised tiling defects. In this paper we explore the analogy between dynamic arrest in this type of random tilings and that of structural glasses. We show that the structural relaxation of these systems is via the propagation--reaction of tiling defects, giving rise to dynamic heterogeneity. We study the scaling properties of the dynamics, and discuss connections with kinetically constrained models of glasses.Comment: 5 pages, 5 figure

Harmonic Content of Strain-induced Potential Modulation in Unidirectional Lateral Superlattices

Detailed analysis of the commensurability oscillation (CO) has been performed on unidirectional lateral superlattices with periods ranging from a=92 to 184 nm. Fourier analysis reveals the second (and the third) harmonics along with the fundamental oscillation for a>=138 nm (184 nm) at low-enough temperature, evincing the presence of corresponding harmonics in the profile of the potential modulation. The harmonics manifest themselves in CO with demagnified amplitude due to the low-pass filtering action of the thermal damping factor; with a suitable consideration of the damping effect, the harmonics of the modulation potential are found to have the amplitudes V_2 and V_3 up to roughly 30% of that of the fundamental component V_1, despite the small ratio of the period a to the depth d = 99 nm of the two-dimensional electron gas (2DEG) from the surface. The dependence of V_n on a indicates that the fundamental component originates at the surface, while the higher harmonics arise from the effect of the strain that penetrates down into subsurface. The manipulation of high harmonics thus provides a useful technique to introduce small length-scale modulation into high-mobility 2DEGs located deep inside the wafer.Comment: 9 pages, 5 figure

Random and ordered phases of off-lattice rhombus tiles

We study the covering of the plane by non-overlapping rhombus tiles, a problem well-studied only in the limiting case of dimer coverings of regular lattices. We go beyond this limit by allowing tiles to take any position and orientation on the plane, to be of irregular shape, and to possess different types of attractive interactions. Using extensive numerical simulations we show that at large tile densities there is a phase transition from a fluid of rhombus tiles to a solid packing with broken rotational symmetry. We observe self-assembly of broken-symmetry phases, even at low densities, in the presence of attractive tile-tile interactions. Depending on tile shape and interactions the solid phase can be random, possessing critical orientational fluctuations, or crystalline. Our results suggest strategies for controlling tiling order in experiments involving `molecular rhombi'.Comment: Supp. Info. and version with high-res figures at http://nanotheory.lbl.gov/people/rhombus_paper/rhombus.htm

Nonequilibrium dynamics of fully frustrated Ising models at T=0

We consider two fully frustrated Ising models: the antiferromagnetic triangular model in a field of strength, $h=H T k_B$, as well as the Villain model on the square lattice. After a quench from a disordered initial state to T=0 we study the nonequilibrium dynamics of both models by Monte Carlo simulations. In a finite system of linear size, $L$, we define and measure sample dependent "first passage time", $t_r$, which is the number of Monte Carlo steps until the energy is relaxed to the ground-state value. The distribution of $t_r$, in particular its mean value, $$, is shown to obey the scaling relation, $\sim L^2 \ln(L/L_0)$, for both models. Scaling of the autocorrelation function of the antiferromagnetic triangular model is shown to involve logarithmic corrections, both at H=0 and at the field-induced Kosterlitz-Thouless transition, however the autocorrelation exponent is found to be $H$ dependent.Comment: 7 pages, 8 figure

Emergent Rhombus Tilings from Molecular Interactions with M-fold Rotational Symmetry

© 2015 American Physical Society. We show that model molecules with particular rotational symmetries can self-assemble into network structures equivalent to rhombus tilings. This assembly happens in an emergent way, in the sense that molecules spontaneously select irregular fourfold local coordination from a larger set of possible local binding geometries. The existence of such networks can be rationalized by simple geometrical arguments, but the same arguments do not guarantee a network's spontaneous self-assembly. This class of structures must in certain regimes of parameter space be able to reconfigure into networks equivalent to triangular tilings

Common physical framework explains phase behavior and dynamics of atomic, molecular, and polymeric network formers

We show that the self-assembly of a diverse collection of building blocks can be understood within a common physical framework. These building blocks, which form periodic honeycomb networks and nonperiodic variants thereof, range in size from atoms to micron-scale polymers and interact through mechanisms as different as hydrogen bonds and covalent forces. A combination of statistical mechanics and quantum mechanics shows that one can capture the physics that governs the assembly of these networks by resolving only the geometry and strength of building-block interactions. The resulting framework reproduces a broad range of phenomena seen experimentally, including periodic and nonperiodic networks in thermal equilibrium, and nonperiodic supercooled and glassy networks away from equilibrium. Our results show how simple “design criteria” control the assembly of a wide variety of networks and suggest that kinetic trapping can be a useful way of making functional assemblies

Magnetoresistance of a two-dimensional electron gas with spatially periodic lateral modulations: Exact consequences of Boltzmann's equation

On the basis of Boltzmann's equation, and including anisotropic scattering in the collision operator, we investigate the effect of one-dimensional superlattices on two-dimensional electron systems. In addition to superlattices defined by static electric and magnetic fields, we consider mobility superlattices describing a spatially modulated density of scattering centers. We prove that magnetic and electric superlattices in $x$-direction affect only the resistivity component $\rho_{xx}$ if the mobility is homogeneous, whereas a mobility lattice in $x$-direction in the absence of electric and magnetic modulations affects only $\rho_{yy}$. Solving Boltzmann's equation numerically, we calculate the positive magnetoresistance in weak magnetic fields and the Weiss oscillations in stronger fields within a unified approach.Comment: submitted to PR

Ordering, Flexibility and Frustration in Arrays of Porphyrin Nanorings

The regular packing of atoms, molecules and nanoparticles provides the basis for the understanding of structural order within condensed phases of matter. Typically the constituent particles are considered to be rigid with a fixed shape. Here we show, through a combined experimental and numerical study of the adsorption of cyclic porphyrin polymers, nanorings, on a graphite surface, that flexible molecules can exhibit a rich and complex packing behaviour. Depending on the number of porphyrin sub-units within the nanoring we observe either a highly ordered hexagonal phase or frustrated packing driven by directional interactions which for some arrangements is combined with the internal deformation of the cyclic polymer. Frustration and deformation occur in arrays of polymers with ten sub-units since close packing and co-alignment of neighbouring groups cannot be simultaneously realised for nanorings with this internal symmetry. *[email protected]

Magnetotunneling as a Probe of Luttinger-Liquid Behavior

A novel method for detecting Luttinger-liquid behavior is proposed. The idea is to measure the tunneling conductance between a quantum wire and a parallel two-dimensional electron system as a function of both the potential difference between them, $V$, and an in-plane magnetic field, $B$. We show that the two-parameter dependence on $B$ and $V$ allows for a determination of the characteristic dependence on wave vector $q$ and frequency $\omega$ of the {\it spectral function}, $A_{\rm LL}(q,\omega)$, of the quantum wire. In particular, the separation of spin and charge in the Luttinger liquid should manifest itself as singularities in the $I$-$V$-characteristic. The experimental feasibility of the proposal is discussed.Comment: Accepted for publication in Phys. Rev. Let