Dynamics of Quasi-ordered Structure in a Regio-regulated pi-Conjugated Polymer:Poly(4-methylthiazole-2,5-diyl)

Dynamics of regio-regulated Poly(4-methylthiazole-2,5-diyl) [HH-P4MeTz] was inves tigated by solid-state 1H, 2D, 13C NMR spectroscopies, and differential scanning calorimetry(DSC) measurements. DSC, 2D quadrupolar echo NMR, 13C cross-polarization and magic-angle spinning(CPMAS) NMR, and 2D spin-echo(2DSE) CPMAS NMR spectroscopy suggest existence of a quasi-ordered phase in which backbone twists take place with weakened pi-stackings. Two-dimensional exchange 2D NMR(2DEX) detected slow dynamics with a rate of an order of 10^2Hz for the CD_3 group in d_3-HH-P4MeTz at 288K. The frequency dependence of proton longitudinal relaxation rate at 288K shows a omega^-1/2 dependence, which is due to the one-dimensional diffusion-like motion of backbone conformational modulation waves. The diffusion rate was estimated as 3+/-2 GHz, which was approximately 10^7 times larger than that estimated by 2DEX NMR measurements. These results suggest that there exists anomalous dispersion of modulation waves in HH-P4MeTz. The one-dimensional group velocity of the wave packet is responsible for the behavior of proton longitudinal relaxation time. On the other hand, the 2DEX NMR is sensitive to phase velocity of the nutation of methyl groups that is associated with backbone twists. From proton T_1 and T_2 measurements, the activation energy was estimated as 2.9 and 3.4 kcal/mol, respectively. These were in agreement with 3.0 kcal/mol determined by Moller-Plesset(MP2) molecular orbital(MO) calculation. We also performed chemical shielding calculation of the methyl-carbon in order to understand chemical shift tensor behavior, leading to the fact that a quasi-ordered phase coexist with the crystalline phase.Comment: 14 pages, 11 figures, to appear in Phys.Rev.

Zero-dynamics principle for perfect quantum memory in linear networks

In this paper, we study a general linear networked system that contains a tunable memory subsystem; that is, it is decoupled from an optical field for state transportation during the storage process, while it couples to the field during the writing or reading process. The input is given by a single photon state or a coherent state in a pulsed light field. We then completely and explicitly characterize the condition required on the pulse shape achieving the perfect state transfer from the light field to the memory subsystem. The key idea to obtain this result is the use of zero-dynamics principle, which in our case means that, for perfect state transfer, the output field during the writing process must be a vacuum. A useful interpretation of the result in terms of the transfer function is also given. Moreover, a four-nodes network composed of atomic ensembles is studied as an example, demonstrating how the input field state is transferred to the memory subsystem and how the input pulse shape to be engineered for perfect memory looks like.Comment: 31 pages, 5 figure

Investigation of in-plane nuclear field formation in single self-assembled quantum dots

We studied the formation mechanism of the in-plane nuclear field in single self-assembled In$_{0.75}$Al$_{0.25}$As/Al$_{0.3}$Ga$_{0.7}$As quantum dots. The Hanle curves with an anomalously large width and hysteretic behavior at the critical transverse magnetic field were observed in many single quantum dots grown in the same QD sample. In order to explain the anomalies in the Hanle curve indicating the formation of a large nuclear field perpendicular to the photo-injected electron spin polarization, we propose a new model based on the current phenomenological model for dynamic nuclear spin polarization. The model includes the effects of the nuclear quadrupole interaction and the sign inversion between in-plane and out-of-plane g-factors, and the model calculations reproduce successfully the characteristics of the observed anomalies in the Hanle curves.Comment: 7 pages, 6 figure

Supercooled Liquids Under Shear: Theory and Simulation

We analyze the behavior of supercooled fluids under shear both theoretically and numerically. Theoretically, we generalize the mode-coupling theory of supercooled fluids to systems under stationary shear flow. Our starting point is the set of generalized fluctuating hydrodynamic equations with a convection term. A nonlinear integro-differential equation for the intermediate scattering function is constructed. This theory is applied to a two-dimensional colloidal suspension. The shear rate dependence of the intermediate scattering function and the shear viscosity is analyzed. We have also performed extensive numerical simulations of a two-dimensional binary liquid with soft-core interactions near, but above, the glass transition temperature. Both theoretical and numerical results show: (i) A drastic reduction of the structural relaxation time and the shear viscosity due to shear. Both the structural relaxation time and the viscosity decrease as $\dot{\gamma}^{-\nu}$ with an exponent $\nu \leq 1$, where $\dot{\gamma}$ is the shear rate. (ii) Almost isotropic dynamics regardless of the strength of the anisotropic shear flow.Comment: 14 pages, 14 figure

Supercooled liquids under shear: A mode-coupling theory approach

We generalize the mode-coupling theory of supercooled fluids to systems under stationary shear flow. Our starting point is the generalized fluctuating hydrodynamic equations with a convection term. The method is applied to a two dimensional colloidal suspension. The shear rate dependence of the intermediate scattering function and shear viscosity is analyzed. The results show a drastic reduction of the structural relaxation time due to shear and strong shear thinning behavior of the viscosity which are in qualitative agreement with recent simulations. The microscopic theory with minimal assumptions can explain the behavior far beyond the linear response regime.Comment: 4 pages, 2 figures, Proceedings to Slow Dynamics in Complex Systems November3-8, 2003 -- Sendai, Japa

Implementation of Lees-Edwards periodic boundary conditions for direct numerical simulations of particle dispersions under shear flow

A general methodology is presented to perform direct numerical simulations of particle dispersions in a shear flow with Lees-Edwards periodic boundary conditions. The Navier-Stokes equation is solved in oblique coordinates to resolve the incompatibility of the fluid motions with the sheared geometry, and the force coupling between colloidal particles and the host fluid is imposed by using a smoothed profile method. The validity of the method is carefully examined by comparing the present numerical results with experimental viscosity data for particle dispersions in a wide range of volume fractions and shear rates including nonlinear shear-thinning regimes

Supercooled Liquids under Shear: Computational Approach

We have performed molecular dynamics simulations for a model two-dimensional soft-core mixture in a supercooled state. The mixture exhibits a slow structural relaxation in a quiescent state, however, the relaxation is much enhanced in sheared states. There observed surprisingly small anisotropy both in the coherent and incoherent density correlation functions even under extremely strong shear which is $10^3$ times faster than the structural relaxation rate. The present simulation results agree well with predictions of the recently developed mode-coupling theory in shear.Comment: 2 pages, 2 figure