The transient EPR spectra and spin dynamics of coupled three-spin systems in photosynthetic reaction centres

The concept of introducing an additional, stable paramagnetic species into photosynthetic reaction centres to increase the information content of their spin polarized transient EPR spectra is investigated theoretically. The light-induced electron transfer in such systems generates a series of coupled three-spin states consisting of sequential photoinduced radical pairs coupled to the stable spin which acts as an “observer”. The spin polarized transient EPR spectra are investigated using the coupled three-spin system P⁺I⁻Q⁻ _A in pre-reduced bacterial reaction centres as a specific example which has been studied experimentally. The evolution of the spin system and the spin polarized EPR spectra of P⁺I⁻Q⁻ _A and Q⁻ _A following recombination of the radical pair (P = primary donor, I = primary acceptor, Q_A = quinone acceptor) are calculated numerically by solving the equations of motion for the density matrix. The net polarization of the observer spin is also calculated analytically by perturbation theory for the case of a single, short-lived, charge-separated state. The result bears a close resemblance to the chemically induced nuclear polarization (CIDNP) generated in photolysis reactions in which a nuclear spin plays the role of the observer interacting with the radical pair intermediates. However, because the Zeeman frequencies of the three electron spins involved are usually quite similar, the polarization of the electron observer spin in strong magnetic fields can reflect features of the CIDNP effect in both, high and low magnetic fields. The dependence of the quinone spin polarization on the exchange couplings in the three-spin system is investigated by numerical simulations, and it is shown that the observed emissive polarization pattern is compatible with either sign, positive or negative, for a range of exchange couplings, J_PI, in the primary pair. The microwave frequency and orientation dependence of the spectra are discussed as two of several possible criteria for determining the sign of J_PI.     

Homoclinic Solutions for Swift-Hohenberg and Suspension Bridge Type Equations

We establish the existence of homoclinic solutions for a class of fourth-order equations which includes the Swift-Hohenberg model and the suspension bridge equation. In the first case, the nonlinearity has three zeros, corresponding to a double-well potential, while in the second case the nonlinearity is asymptotically constant on one side. The Swift-Hohenberg model is a higher-order extension of the classical Fisher-Kolmogorov model. Its more complicated dynamics give rise to further possibilities of pattern formation. The suspension bridge equation was studied by Chen and McKenna (J. Differential Equations136 (1997), 325-355); we give a positive answer to an open question raised by the authors.     

Topological equivalence of discontinuous norms

We show that for everyp>0 there is an autohomeomorphismh of the countable infinite product of linesR ^Nsuch that for everyr>0,h maps the Hilbert cube [−r, r] ^N precisely onto the “elliptic cube” . This means that the supremum norm and, for instance, the Hilbert norm (p=2) are topologically indistinguishable as functions onR ^N.The result is obtained by means of the Bing Shrinking Criterion. Research supported in part by a grant from NSF-EPSCoR Alabama.     

Polar decompositions and related classes of operators in spaces ∏κ

Polar decompositions with respect to an indefinite inner product are studied for bounded linear operators acting on a space. Criteria are given for existence of various forms of the polar decompositions, under the conditions that the range of a given operatorX is closed and that zero is not an irregular critical point of the selfadjoint operatorX ^[*]X. Both real and complex spaces are considered. Relevant classes of operators having a selfadjoint (in the sense of the indefinite inner product) square root, or a selfadjoint logarithm, are characterized.The work of this author was partially supported by INdAM-GNCS and MURSTThe work of this author was partially supported by NSF grant DMS-9988579.     

The Flooding Time in Random Graphs

Based on our analysis of the hopcount of the shortest path between two arbitrary nodes in the class G _p (N) of random graphs, the corresponding flooding time is investigated. The flooding time T _N (p) is the minimum time needed to reach all other nodes from one node. We show that, after scaling, the flooding time T _N (p) converges in distribution to the two-fold convolution ^(2*) of the Gumbel distribution function (z)=exp (–e ^–z ), when the link density p _N satisfies Np _N /(log N)³ if N .     

Sound power flux measurements in strongly exited ducts with flow

This contribution describes new robust procedures for the measurement of sound power flux at appropriate axial positions along a duct with flow, using pairs of flush wall mounted microphones, or pressure transducers. The technology includes the application of selective averaging, order tracking, and optimized sampling rate methods to identify the small fraction of the total fluctuating wave energy that is being propagated along the flow path in a reverberent, or highly reactive duct system. Such measurements can also be used to quantify the local acoustic characteristics that govern the generation, transfer, and propagation of wave energy in the system. Illustrative examples include the determination of the acoustic characteristics of individual silencing elements installed in IC engine intakes and exhausts both on the flow bench and during controlled acceleration or run down on a test bed, where the wave component spectral levels approached 170 dB.     

Effective Field Theories for Disordered Systems from a Generalized Phase Formulation

We consider a spinless particle moving in a d-dimensional box, subject to periodic boundary conditions, and in the presence of a random potential. Introducing the logarithm of the wave function transforms the time-independent Schrödinger equation into a stochastic differential equation with the random potential acting as the source. Using this as our starting point we write functional integral representations for the disorder averaged density of states, the two point correlator of the absolute value of the wave function, and inverse participation ratios. We also show how a deterministic or random magnetic field can be included in the formalism.     

Construction of the Incipient Infinite Cluster for Spread-out Oriented Percolation Above 4 + 1 Dimensions

 We construct the incipient infinite cluster measure (IIC) for sufficiently spread-out oriented percolation on ℤ ^d × ℤ₊, for d +1 > 4+1. We consider two different constructions. For the first construction, we define ℙ ⁿ (E) by taking the probability of the intersection of an event E with the event that the origin is connected to (x,n)  ℤ ^d × ℤ₊, summing this probability over x  ℤ ^d , and normalising the sum to get a probability measure. We let n → ∞ and prove existence of a limiting measure ℙ_∞, the IIC. For the second construction, we condition the connected cluster of the origin in critical oriented percolation to survive to time n, and let n → ∞. Under the assumption that the critical survival probability is asymptotic to a multiple of n ⁻¹, we prove existence of a limiting measure ℚ_∞, with ℚ_∞ = ℙ_∞. In addition, we study the asymptotic behaviour of the size of the level set of the cluster of the origin, and the dimension of the cluster of the origin, under ℙ_∞. Our methods involve minor extensions of the lace expansion methods used in a previous paper to relate critical oriented percolation to super-Brownian motion, for d+1 > 4+1. Received: 13 December 2001 / Accepted: 11 July 2002 Published online: 29 October 2002 RID="*" ID="*" Present address: Department of Mathematics and Computer Science, Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, The Netherlands. E-mail: rhofstad@win.tue.nl     

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