Relaxation in systems with hierarchical organization: Analytical derivation of the relaxation and dispersion functions

We report a successful attempt to derive a closed-form expression for the relaxation function of a complex system by solving a set of coupled kinetic equations connecting the excitation/de-excitation rates to the number of particles (such as electrical charges, dipoles, etc.) in excited states. Our approach, originating from developments in dielectric and mechanical relaxation studies, allows the use of a unified treatment for a wide array of natural processes which often pose challenges to theoretical modeling. We use the notions that (i) a dipole represents any pair formed by a particle in an excited state (such as an energy level in optically excited molecules, or an electrode in dielectric spectroscopy) and its image in the ground state (or reference electrode), that (ii) coupling between such dipoles may be described as particle transfer from one excited state to another with lower energy, and that (iii) the relaxation function for such a system of dipoles is mathematically equivalent to the cumulative distribution function of particles, i.e., the total number of particles that are still in an excited state at a time t following excitation. Taken together, these ideas naturally lead to the identification of two types of relaxation – parallel and serial relaxation – and allow one to tackle systems with either geometrical or physical self-similarity within a unified mathematical scheme.     

Production and purification of bacterial membrane vesicles for biotechnology applications: Challenges and opportunities

Bacterial membrane vesicles (BMVs) are bi-layered nanostructures derived from Gram-negative and Gram-positive bacteria. Among other pathophysiological roles, BMVs are critical messengers in intercellular communication. As a result, BMVs are emerging as a promising technology for the development of numerous therapeutic applications. Despite the remarkable progress in unveiling BMV biology and functions in recent years, their successful isolation and purification have been limited. Several challenges related to vesicle purity, yield, and scalability severely hamper the further development of BMVs for biotechnology and clinical applications. This review focuses on the current technologies and methodologies used in BMV production and purification, such as ultracentrifugation, density-gradient centrifugation, size-exclusion chromatography, ultrafiltration, and precipitation. We also discuss the current challenges related to BMV isolation, large-scale production, storage, and stability that limit their application. More importantly, the present work explains the most recent strategies proposed for overcoming those challenges. Finally, we summarize the ongoing applications of BMVs in the biotechnological field.     

Understanding of nuclear quadrupole interactions of 35 Cl, 79 Br and 129 I and binding energies of solid halogens at first-principles level

This paper deals with the understanding at a first-principles level of the nuclear quadrupole interaction (NQI) parameters of solid chlorine, bromine and iodine as well as the intermolecular binding of these molecules in the solid. The electronic structure investigations that we have carried out to study these properties of the solid halogens are based on the Hartree–Fock Cluster approach using the Roothaan variational procedure with electron correlation effects included using many-body perturbation theory with the empty orbitals used in the perturbation theory investigations for the excited states. The results of our investigations provide good agreement with the measured NQI parameters primarily from the Hartree–Fock one electron wave-functions with many-body effects making minor contributions. The binding (dissociation) energies for the molecules with the solid state environment on the other hand arises from intermolecular many body effects identified as the Van der Waals attraction with one-electron Hartree–Fock contribution being repulsive in nature.     

First-principles cluster study of electronic structures, locations and hyperfine interactions of isolated atoms and ions in silicon

The electronic structures of the dilute transition metal (TM) impurities, V^2?+?, Cr^?+?, Mn^2?+?, and Mn⁰ in silicon have been studied using the Hartree–Fock (HF) procedure combined with many-body perturbation theory (MBPT). The systems studied involved the TM impurities at the hexagonal interstitial (H _i ), tetrahedral interstitial (T _i ) and substitutional (S) locations. Investigations of the binding energy and local potential energy surface of the TM impurity-Si systems indicate that the TM impurities are binding at the T _i location. Hyperfine interaction constants (A) of the TM impurities at the T _i and S sites are presented and compared with available experimental results (Woodbury and Ludwig, J Phys Rev 117:102, 1960a, Phys Rev Lett 5:98, b) from Electron Paramagnetic Resonance (EPR) measurements.     

First principles electronic structure investigation of order of singlet and triplet states of oxyhemoglobin and analysis of possible influence of muon trapping

Interest in the possibility of magnetic character for oxyhemoglobin (OxyHb) has been recently stimulated by the observations of muon spin-lattice relaxation effects studied (Nagamine et al., Proc Jpn Acad Ser B Phys Biol Sci 83:120–126, 2007) with the muon-spin rotation (μSR) technique. In view of this, we have carried out first-principles electronic structure investigations involving Hartree–Fock theory combined with many body perturbation effects for the singlet and triplet states of OxyHb. Our results indicate that using two recent x-ray structural data (Paoli et al., J Mol Biol 256:775, 1996; Park et al., J Mol Biol 360:690, 2006) for OxyHb, for only Hartree–Fock theory without many-body effects included, the singlet state lies above the triplet state by energies of about 0.08 and 0.13 a.u. for the two structures in Paoli et al. (J Mol Biol 256:775, 1996) and Park et al. (J Mol Biol 360:690, 2006). Incorporation of many-body effects by the perturbation method reverses the order, with the triplet state located 0.18 and 0.14 a.u. above the singlet state for the structures in Paoli et al. (J Mol Biol 256:775, 1996) and Park et al. (J Mol Biol 360:690, 2006). Physical reasons for these relative orderings of the singlet and triplet states will be discussed. It is clear that OxyHb by itself would be in a singlet state at room temperature or below, since from our calculation, the triplet state lies about KT above the singlet state with T having the value of 44,098 K and 56,449 K for the two structural data in Paoli et al. (J Mol Biol 256:775, 1996) and Park et al. (J Mol Biol 360:690, 2006). As regards the muon spin-lattice relaxation effects obtained by recent μSR measurements (by Nagamine et al., Proc Jpn Acad Ser B Phys Biol Sci 83:120–126, 2007) at room temperature, the sensitive dependence of the singlet-triplet separation on many-body effects in our investigation suggests that it is possible that the singlet-triplet separation could be reversed or reduced significantly when a muon is trapped near an oxygen atom of the oxygen molecule, allowing the triplet to be occupied at room temperature and lead to significant muon spin-lattice relaxation.     

First principles study of nuclear quadrupole interactions in the molecular solid BF3 and the nature of binding between the molecules

The LPCTrap facility is coupled to the low-energy beam line LIRAT of the SPIRAL source at GANIL (France). The facility comprises an RFQ trap for beam preparation and a transparent Paul trap for in-trap decay studies. The system has been tested for several ion species. The Paul trap has been fully characterized for ⁶Li⁺ and ²³Na⁺ ions. This characterization together with GEANT4 simulations of the in-trap decay setup (Paul trap and detection system) has permitted to predict the effect of the size of the ion cloud on the decay study of ⁶He⁺.