Beta relaxation in the shear mechanics of viscous liquids: Phenomenology and network modeling of the alpha-beta merging region

The phenomenology of the beta relaxation process in the shear-mechanical response of glass-forming liquids is summarized and compared to that of the dielectric beta process. Furthermore, we discuss how to model the observations by means of standard viscoelastic modeling elements. Necessary physical requirements to such a model are outlined, and it is argued that physically relevant models must be additive in the shear compliance of the alpha and beta parts. A model based on these considerations is proposed and fitted to data for Polyisobutylene 680.     

A combined measurement of thermal and mechanical relaxation

In order to describe relaxation the thermodynamic coefficient can be generalized into a complex frequency-dependent cross response function. We explore theoretically the possibility of measuring for a supercooled liquid near the glass transition. This is done by placing a thermistor in the middle of the liquid which itself is contained in a spherical piezoelectric shell. The piezoelectric voltage response to a thermal power generated in the thermistor is found to be proportional to but factors pertaining to heat diffusion and adiabatic compressibility κ_S(ω) do also intervene. We estimate a measurable piezoelectric voltage of 1 mV to be generated at 1 Hz for a heating power of 0.3 mW. Together with κ_S(ω) and the longitudinal specific heat c_l(ω) which may also be found in the same setup a complete triple of thermoviscoelastic response functions may be determined when supplemented with shear modulus data.     

Multipolar interactions in the D pocket of thrombin: large differences between tricyclic imide and lactam inhibitors

Two series of tricyclic inhibitors of the serine protease thrombin, imides (+/-)-1-(+/-)-8 and lactams (+/-)-9-(+/-)-13, were analysed to evaluate contributions of orthogonal multipolar interactions with the backbone C=O moiety of Asn98 to the free enthalpy of protein-ligand complexation. The lactam derivatives are much more potent and more selective inhibitors (K(i) values between 0.065 and 0.005 microM, selectivity for thrombin over trypsin between 361- and 1609-fold) than the imide compounds (Ki values between 0.057 and 23.7 microM, selectivity for thrombin over trypsin between 3- and 67-fold). The increase in potency and selectivity is explained by the favorable occupancy of the P-pocket of thrombin by the additional isopropyl substituent in the lactam derivatives. The nature of the substituent on the benzyl ring filling the D pocket strongly influences binding potency in the imide series, with Ki values increasing in the sequence: F < OCH2O < Cl < H < OMe < OH < N(pyr)< Br. This sequence can be explained by both steric fit and the occurrence of orthogonal multipolar interactions with the backbone C[double bond, length as m-dash]O moiety of Asn98. In contrast, the substituent on the benzyl ring hardly affects the ligand potency in the lactam series. This discrepancy was clarified by the comparison of X-ray structures solved for co-crystals of thrombin with imide and lactam ligands. Whereas the benzyl substituents in the imide inhibitors are sufficiently close (< or =3.5 Angstroms) to the C=O group of Asn98 to allow for attractive orthogonal multipolar interactions, the distances in the lactam series are too large (> or =4 Angstroms) for attractive dipolar contacts to be effective.     

Predicting catalysis: understanding ammonia synthesis from first-principles calculations

Here, we give a full account of a large collaborative effort toward an atomic-scale understanding of modern industrial ammonia production over ruthenium catalysts. We show that overall rates of ammonia production can be determined by applying various levels of theory (including transition state theory with or without tunneling corrections, and quantum dynamics) to a range of relevant elementary reaction steps, such as N(2) dissociation, H(2) dissociation, and hydrogenation of the intermediate reactants. A complete kinetic model based on the most relevant elementary steps can be established for any given point along an industrial reactor, and the kinetic results can be integrated over the catalyst bed to determine the industrial reactor yield. We find that, given the present uncertainties, the rate of ammonia production is well-determined directly from our atomic-scale calculations. Furthermore, our studies provide new insight into several related fields, for instance, gas-phase and electrochemical ammonia synthesis. The success of predicting the outcome of a catalytic reaction from first-principles calculations supports our point of view that, in the future, theory will be a fully integrated tool in the search for the next generation of catalysts.     

Diagnostics and rubrics for assessing learning across the computational science curriculum

We describe our experiences with learning assessment in a new computational science program. We report on the development and pilot testing of assessment tools in both core and cognate courses. Specifically, we detail a diagnostic assessment that predicted success in our introductory computational science course with reasonable reliability; we give an account of our use of an existing assessment tool to investigate how introducing computational thinking in a cognate course influences learning of the traditional course material; and we discuss rubric development for project evaluation.     

Dimensions of random self-affine multifractal Sierpinski sponges in {{\mathbb{R}}^d}

In this paper we study the Hausdorff and packing dimensions and the Rényi dimensions of random self-affine multifractal Sierpinski sponges in ${{\mathbb{R}}^{d}}$ .     

A Quantitative Balian-Low Theorem

We study functions generating Gabor Riesz bases on the integer lattice. The classical Balian-Low theorem (BLT) restricts the simultaneous time and frequency localization of such functions. We obtain a quantitative estimate on their Zak transform that extends both this result and the more general (p,q) Balian-Low theorem. Moreover, we establish a family of quantitative amalgam-type Balian-Low theorems that contain both the amalgam BLT and the classical BLT as special cases.     

QCD exotics

I review first some theoretical motivations for violation of Lorentz and/or CPT Invariance. Although the latter symmetries may be violated in a quantum gravity setting, nevertheless there are situations in which these violations are due to a given classical background geometry that may characterised early epochs of our Universe, and in fact be responsible for the observed dominance of matter over antimatter in the Universe. In this way I estimate some of the coefficients of the Standard Model Extension (SME), which is a framework for a field theoretic study of such a breakdown of fundamental symmetries. Then I describe briefly some tests of these symmetries, giving emphasis in low-energy antiproton physics and electric dipole moment measurements, of interest to this conference. I also mention the rôle of entangled states of neutral mesons in providing independent measurements of T(ime reversal) and CP Violation, thus providing independent tests of CPT symmetry, as well as novel (“smoking-gun” type) tests of decoherence-induced CPT violation, which may characterise some models of quantum gravity.