Ultrafast charge transfer and vibronic coupling in a laser-excited hybrid inorganic/organic interface

Hybrid interfaces formed by inorganic semiconductors and organic molecules are intriguing materials for opto-electronics. Interfacial charge transfer is primarily responsible for their peculiar electronic structure and optical response. Hence, it is essential to gain insight into this fundamental process also beyond the static picture. Ab initio methods based on real-time time-dependent density-functional theory coupled to the Ehrenfest molecular dynamics scheme are ideally suited for this problem. We investigate a laser-excited hybrid inorganic/organic interface formed by the electron acceptor molecule 2,3,5,6-tetrafluoro-7,7,8,8-tetracyano-quinodimethane (F4TCNQ) physisorbed on a hydrogenated silicon cluster, and we discuss the fundamental mechanisms of charge transfer in the ultrashort time window following the impulsive excitation. The considered interface is p-doped and exhibits charge transfer in the ground state. When it is excited by a resonant laser pulse, the charge transfer across the interface is additionally increased, but contrary to previous observations in all-organic donor/acceptor complexes, it is not further promoted by vibronic coupling. In the considered time window of 100 fs, the molecular vibrations are coupled to the electron dynamics and enhance intramolecular charge transfer. Our results highlight the complexity of the physics involved and demonstrate the ability of the adopted formalism to achieve a comprehensive understanding of ultrafast charge transfer in hybrid materials

Floppy modes and the free energy: Rigidity and connectivity percolation on Bethe Lattices

We show that negative of the number of floppy modes behaves as a free energy for both connectivity and rigidity percolation, and we illustrate this result using Bethe lattices. The rigidity transition on Bethe lattices is found to be first order at a bond concentration close to that predicted by Maxwell constraint counting. We calculate the probability of a bond being on the infinite cluster and also on the overconstrained part of the infinite cluster, and show how a specific heat can be defined as the second derivative of the free energy. We demonstrate that the Bethe lattice solution is equivalent to that of the random bond model, where points are joined randomly (with equal probability at all length scales) to have a given coordination, and then subsequently bonds are randomly removed.Comment: RevTeX 11 pages + epsfig embedded figures. Submitted to Phys. Rev.

Rapid state purification protocols for a Cooper pair box

We propose techniques for implementing two different rapid state purification schemes, within the constraints present in a superconducting charge qubit system. Both schemes use a continuous measurement of charge (z) measurements, and seek to minimize the time required to purify the conditional state. Our methods are designed to make the purification process relatively insensitive to rotations about the x-axis, due to the Josephson tunnelling Hamiltonian. The first proposed method, based on the scheme of Jacobs [Phys. Rev. A 67, 030301(R) (2003)] uses the measurement results to control bias (z) pulses so as to rotate the Bloch vector onto the x-axis of the Bloch sphere. The second proposed method, based on the scheme of Wiseman and Ralph [New J. Phys. 8, 90 (2006)] uses a simple feedback protocol which tightly rotates the Bloch vector about an axis almost parallel with the measurement axis. We compare the performance of these and other techniques by a number of different measures.Comment: 14 pages, 14 figures. v2: Revised version after referee comments. Accepted for publication by Physical Review

Statics and dynamics of domain patterns in hexagonal-orthorhombic ferroelastics

We study the statics and the dynamics of domain patterns in proper hexagonal-orthorhombic ferroelastics; these patterns are of particular interest because they provide a rare physical realization of disclinations in crystals. Both our static and dynamical theories are based entirely on classical, nonlinear elasticity theory; we use the minimal theory consistent with stability, symmetry and ability to explain qualitatively the observed patterns. After scaling, the only parameters of the static theory are a temperature variable and a stiffness variable. For moderate to large stiffness, our static results show nested stars, unnested stars, fans and other nodes, triangular and trapezoidal regions of trapped hexagonal phase, etc observed in electron microscopy of Ta4N and Mg-Cd alloys, and also in lead orthovanadate (which is trigonal-monoclinic); we even find imperfections in some nodes, like those observed. For small stiffness, we find patterns like those observed in the mineral Mg-cordierite. Our dynamical studies of growth and relaxation show the formation of these static patterns, and also transitory structures such as 12-armed bursts, streamers and striations which are also seen experimentally. The major aspects of the growth-relaxation process are quite unlike those in systems with conventional order parameters, for it is inherently nonlocal; for example, the changes from one snapshot to the next are not predictable by inspection.Comment: 9 pages, 3 figures (1 b&w, 2 colour); animations may be viewed at http://huron.physics.utoronto.ca/~curnoe/sim.htm

Cluster counting: The Hoshen-Kopelman algorithm vs. spanning tree approaches

Two basic approaches to the cluster counting task in the percolation and related models are discussed. The Hoshen-Kopelman multiple labeling technique for cluster statistics is redescribed. Modifications for random and aperiodic lattices are sketched as well as some parallelised versions of the algorithm are mentioned. The graph-theoretical basis for the spanning tree approaches is given by describing the "breadth-first search" and "depth-first search" procedures. Examples are given for extracting the elastic and geometric "backbone" of a percolation cluster. An implementation of the "pebble game" algorithm using a depth-first search method is also described.Comment: LaTeX, uses ijmpc1.sty(included), 18 pages, 3 figures, submitted to Intern. J. of Modern Physics

Heralded Two-Photon Entanglement from Probabilistic Quantum Logic Operations on Multiple Parametric Down-Conversion Sources

An ideal controlled-NOT gate followed by projective measurements can be used to identify specific Bell states of its two input qubits. When the input qubits are each members of independent Bell states, these projective measurements can be used to swap the post-selected entanglement onto the remaining two qubits. Here we apply this strategy to produce heralded two-photon polarization entanglement using Bell states that originate from independent parametric down-conversion sources, and a particular probabilistic controlled-NOT gate that is constructed from linear optical elements. The resulting implementation is closely related to an earlier proposal by Sliwa and Banaszek [quant-ph/0207117], and can be intuitively understood in terms of familiar quantum information protocols. The possibility of producing a ``pseudo-demand'' source of two-photon entanglement by storing and releasing these heralded pairs from independent cyclical quantum memory devices is also discussed.Comment: 5 pages, 4 figures; submitted to IEEE Journal of Selected Topics in Quantum Electronics, special issue on "Quantum Internet Technologies

Superlinear Scaling for Innovation in Cities

Superlinear scaling in cities, which appears in sociological quantities such as economic productivity and creative output relative to urban population size, has been observed but not been given a satisfactory theoretical explanation. Here we provide a network model for the superlinear relationship between population size and innovation found in cities, with a reasonable range for the exponent.Comment: 5 pages, 5 figures, 1 table, submitted to Phys. Rev. E; references corrected; figures corrected, references and brief discussion adde

On the Optical Activity of Steroidal 5,7-Dienes

Circular dichroism (CD) data are reported of a series of 9,10- stereoisomeric steroidal 5,7-dienes. In general the effects in the longest wavelength transition (270-280 nm) are large (Mm" 10---30) and consignate with respect to the diene helicity rule. The magnitude of the CD appears to vary markedly with the substituent at C-3 and at C-17, and with solvent. In the case of the 9a,10p-H dienes, variation of solvent and temperature can affect even the sign of the Cotton effect. This is explained from a change of geometry of the diene ring: solvation, substitution and temperature can affect the average geometry of the ring including the values of the angle of twist of the diene (ef> (6-7». The relevance of the observed chiroptical data for the theoretical description of the optical activity in the So-+ Sl transition of homoannular cisoid dienes is discussed