Coherent storage of photoexcited triplet states using 29Si nuclear spins in silicon

Pulsed electron paramagnetic resonance spectroscopy of the photoexcited, metastable triplet state of the oxygen-vacancy center in silicon reveals that the lifetime of the m(s)=±1 sublevels differs significantly from that of the m(s)=0 state. We exploit this significant difference in decay rates to the ground singlet state to achieve nearly ~100% electron-spin polarization within the triplet. We further demonstrate the transfer of a coherent state of the triplet electron spin to, and from, a hyperfine-coupled, nearest-neighbor (29)Si nuclear spin. We measure the coherence time of the (29)Si nuclear spin employed in this operation and find it to be unaffected by the presence of the triplet electron spin and equal to the bulk value measured by nuclear magnetic resonance.     

A discrete interaction model/quantum mechanical method for simulating surface-enhanced Raman spectroscopy

We have derived and implemented analytical gradients for the discrete interaction model/quantum mechanics (DIM/QM) method. DIM/QM combines an atomistic electrodynamics model with time-dependent density functional theory and thus enables modeling of the optical properties for a molecule while taking into account the local environment of a nanoparticle's surface. The DIM/QM analytical gradients allow for geometry optimizations, vibrational frequencies, and Raman spectra to be simulated for molecules interacting with metal nanoparticles. We have simulated the surface-enhanced Raman scattering (SERS) spectra for pyridine adsorbed on different sites of icosahedral nanoparticles with diameters between 1 and 8 nm. To describe the adsorption of the pyridine molecule onto the metal surface, we have implemented a coordination-dependent force field to differentiate the various local surface environments. We find that the DIM/QM method predicts geometries and frequencies that are in good agreement with full QM simulations and experiments. For the simulated SERS spectra of pyridine, we find a significant dependence on the adsorption site and the size of the metal nanoparticle. This illustrates the importance of accounting for the local environment around the molecule. The Raman enhancement factors are shown to roughly mirror the magnitude of the nanoparticle's local field about the molecule. Because the simulated nanoparticles are small, the plasmon peaks are quite broad which results in weak local electric fields and thus modest Raman enhancement factors.     

A continuum mechanical theory for turbulence: a generalized Navier–Stokes-<Emphasis Type="Italic">α</Emphasis> equation with boundary conditions

We develop a continuum-mechanical formulation and generalization of the Navier–Stokes-α equation based on a recently developed framework for fluid-dynamical theories involving higher-order gradient dependencies. Our flow equation involves two length scales α and β. The first of these enters the theory through the specific free-energy α ²|D|², where D is the symmetric part of the gradient of the filtered velocity, and contributes a dispersive term to the flow equation. The remaining scale is associated with a dissipative hyperstress which depends linearly on the gradient of the filtered vorticity and which contributes a viscous term, with coefficient proportional to β ², to the flow equation. In contrast to Lagrangian averaging, our formulation delivers boundary conditions and a complete structure based on thermodynamics applied to an isothermal system. For a fixed surface without slip, the standard no-slip condition is augmented by a wall-eddy condition involving another length scale ℓ characteristic of eddies shed at the boundary and referred to as the wall-eddy length. As an application, we consider the classical problem of turbulent flow in a plane, rectangular channel of gap 2h with fixed, impermeable, slip-free walls and make comparisons with results obtained from direct numerical simulations. We find that α/β ~ Re ^0.470 and ℓ/h ~ Re ^−0.772, where Re is the Reynolds number. The first result, which arises as a consequence of identifying the specific free-energy with the specific turbulent kinetic energy, indicates that the choice β = α required to reduce our flow equation to the Navier–Stokes-α equation is likely to be problematic. The second result evinces the classical scaling relation η/L ~ Re ^−3/4 for the ratio of the Kolmogorov microscale η to the integral length scale L.      

A finite-deformation,gradient theory of single-crystal plasticity with free energy dependent on the accumulation of geometrically necessary dislocations

This paper develops a gradient theory of single-crystal plasticity based on a system of microscopic force balances, one balance for each slip system, derived from the principle of virtual power, and a mechanical version of the second law that includes, via the microscopic forces, work performed during plastic flow. When combined with thermodynamically consistent constitutive relations the microscopic force balances become nonlocal flow rules for the individual slip systems in the form of partial differential equations requiring boundary conditions. Central ingredients in the theory are geometrically necessary edge and screw dislocations together with a free energy that accounts for work hardening through a dependence on the accumulation of geometrically necessary dislocations.     

The coloured Jones function

The invariantsJ _K,k of a framed knotK coloured by the irreducibleSU(2) _q -module of dimensionk are studied as a function ofk by means of the universalR-matrix. It is shown that whenJ _K,k is written as a power series inh withq=e ^h , the coefficient ofh ^d is an odd polynomial ink of degree at most 2d+1. This coefficient is a Vassiliev invariant ofK. In the second part of the paper it is shown that ask varies, these invariants span ad-dimensional subspace of the space of all Vassiliev invariants of degreed for framed knots. The analogous questions for unframed knots are also studied.Partially supported by NSF Grant DMS-9123657     

The characterization of structure by computer

A comprehensive approach to a computer-based system of structure characterization must include capabilities in both spectrum interpretation and structure generation, and a link between the two that is transparent to the user. Program CASE is undergoing development with these requirements in mind. Structure generation is based on the new concept of structure reduction, which appears to offer advantages in efficiency of execution over procedures based on structure assembly. An experimental version of the program possesses some problem-solving ability.     

The stability of boundary conditions for an angled-derivative difference scheme

Tidal forcing of the shallow water equations is typical of a class of problems where an approximate equilibrium solution is sought by long time integration of a differential equation system. A combination of the angled-derivative scheme with a staggered leap-frog scheme is sometimes used to discretise this problem. It is shown here why great care then needs to be taken with the boundary conditions to ensure that spurious solution modes do not lead to numerical instabilities. Various techniques are employed to analyse two simple model problems and display instabilities met in practical computations; these are then used to deduce a set of stable boundary conditions.Dedicated to Professor J. Crank on the occasion of his 80th birthday