Multi-step atomic reaction enhanced by an atomic force microscope probe on Si(111) and Ge(111) surfaces

We present first-principles total-energy electronic-structure calculations that provide the microscopic mechanism of the adatom interchange reaction on the Sn- and Pb-covered Ge(111)-(2x8) and the Sb-covered Si(111)-(7x7) surfaces with and without the tip of the atomic force microscope (AFM). We find that, without the presence of the AFM tip on the Ge surface, the adatom interchange occurs through the migration of the adatom, the spontaneous formation of the dimer structures of the two adatoms, the dimer-dimer structural transitions that induce the exchange of the positions of the two adatoms, and then the backward migration of the adatom. We also find that the dimer structure is unfeasible at room temperature on the Si surface and the adatom interchange are hereby unlikely. With the presence of the tip, we find that the reaction pathways are essentially the same for the Ge surface but that the energy barriers of the migration and the exchange processes are substantially reduced by the AFM tip. We further find that the AFM tip induces the spontaneous formation of the dimer structure even on the Si surface, hereby opening a channel of the interchange of the adatoms. Our calculations show that the bond formation between the AFM tip atom and the surface adatom is essential for the atom manipulation using the AFM tip.Comment: 9 pages, 7 figure

Formation of a "Cluster Molecule" (C20)2 and its thermal stability

The possible formation of a "cluster molecule" (C20)2 from two single C20 fullerenes is studied by the tight-binding method. Several (C20)2 isomers in which C20 fullerenes are bound by strong covalent forces and retain their identity are found; actually, these C20 fullerenes play the role of "atoms" in the "cluster molecule". The so-called open-[2+2] isomer has a minimum energy. Its formation path and thermal stability at T = 2000 - 4000 K are analyzed in detail. This isomer loses its molecular structure due to either the decay of one of C20 fullerenes or the coalescence of two C20 fullerenes into a C40 cluster. The energy barriers for the metastable open-[2+2] configuration are calculated to be U = 2 - 5 eV.Comment: 21 pages, 8 figure

Breakdown of metastable step-flow growth on vicinal surfaces induced by nucleation

We consider the growth of a vicinal crystal surface in the presence of a step-edge barrier. For any value of the barrier strength, measured by the length l_es, nucleation of islands on terraces is always able to destroy asymptotically step-flow growth. The breakdown of the metastable step-flow occurs through the formation of a mound of critical width proportional to L_c=1/sqrt(l_es), the length associated to the linear instability of a high-symmetry surface. The time required for the destabilization grows exponentially with L_c. Thermal detachment from steps or islands, or a steeper slope increase the instability time but do not modify the above picture, nor change L_c significantly. Standard continuum theories cannot be used to evaluate the activation energy of the critical mound and the instability time. The dynamics of a mound can be described as a one dimensional random walk for its height k: attaining the critical height (i.e. the critical size) means that the probability to grow (k->k+1) becomes larger than the probability for the mound to shrink (k->k-1). Thermal detachment induces correlations in the random walk, otherwise absent.Comment: 10 pages. Minor changes. Accepted for publication in Phys. Rev.

Configurational Entropy and its Crisis in Metastable States: Ideal Glass Transition in a Dimer Model as a Paragidm of a Molecular Glass

We discuss the need for discretization to evaluate the configurational entropy in a general model. We also discuss the prescription using restricted partition function formalism to study the stationary limit of metastable states. We introduce a lattice model of dimers as a paradigm of molecular fluid and study metastability in it to investigate the root cause of glassy behavior. We demonstrate the existence of the entropy crisis in metastable states, from which it follows that the entropy crisis is the root cause underlying the ideal glass transition in systems with particles of all sizes. The orientational interactions in the model control the nature of the liquid-liquid transition observed in recent years in molecular glasses.Comment: 36 pages, 9 figure

Spectroscopy of Rb2_{2} dimers in solid 4^{4}He

We present experimental and theoretical studies of the absorption, emission and photodissociation spectra of Rb$_{2}$ molecules in solid helium. We have identified 11 absorption bands of Rb$_{2}$. All laser-excited molecular states are quenched by the interaction with the He matrix. The quenching results in efficient population of a metastable (1)$^{3}\Pi_{u}$ state, which emits fluorescence at 1042 nm. In order to explain the fluorescence at the forbidden transition and its time dependence we propose a new molecular exciplex Rb$_{2}(^{3}\Pi_{u})$He$_{2}$. We have also found evidence for the formation of diatomic bubble states following photodissociation of Rb$_{2}$

Quantum phase transition in Bose-Fermi mixtures

We study a quantum Bose-Fermi mixture near a broad Feshbach resonance at zero temperature. Within a quantum field theoretical model a two-step Gaussian approximation allows to capture the main features of the quantum phase diagram. We show that a repulsive boson-boson interaction is necessary for thermodynamic stability. The quantum phase diagram is mapped in chemical potential and density space, and both first and second order quantum phase transitions are found. We discuss typical characteristics of the first order transition, such as hysteresis or a droplet formation of the condensate which may be searched for experimentally.Comment: 16 pages, 17 figures; typos corrected, one figure adde

The Structure of the [Zn_In - V_P] Defect Complex in Zn Doped InP

We study the structure, the formation and binding energies and the transfer levels of the zinc-phosphorus vacancy complex [Zn_In - V_P] in Zn doped p-type InP, as a function of the charge, using plane wave ab initio DFT-LDA calculations in a 64 atom supercell. We find a binding energy of 0.39 eV for the complex, which is neutral in p-type material, the 0/-1 transfer level lying 0.50 eV above the valence band edge, all in agreement with recent positron annihilation experiments. This indicates that, whilst the formation of phosphorus vacancies (V_P) may be involved in carrier compensation in heavily Zn doped material, the formation of Zn-vacancy complexes is not. Regarding the structure: for charge states Q=+6 to -4 the Zn atom is in an sp^2 bonded DX position and electrons added/removed go to/come from the remaining dangling bonds on the triangle of In atoms. This reduces the effective vacancy volume monatonically as electrons are added to the complex, also in agreement with experiment. The reduction occurs through a combination of increased In-In bonding and increased Zn-In electrostatic attraction. In addition, for certain charge states we find complex Jahn-Teller behaviour in which up to three different structures, (with the In triangle dimerised, antidimerised or symmetric) are stable and are close to degenerate. We are able to predict and successfully explain the structural behaviour of this complex using a simple tight binding model.Comment: 10 pages text (postscript) plus 8 figures (jpeg). Submitted to Phys. Rev.