The structure of 1-phenyl-3-benzoylamino-4-benzoylpyrazol-2-in-5-one

Crystal and molecular structure of 1-phenyl-3-benzoylamino-4-benzoylpyrazol-2-in-5-one as a product of the benzoylation of 1-phenyl-3-benzoylaminopyrazol-2-in-5-one was characterised by X-ray single crystal diffraction. It is shown that 1-phenyl-3-benzoylamino-4-benzoylpyrazol-2-in-5-one exists in the solid phase in an NH-tautomeric form, which is stabilised by two intramolecular hydrogen bonds and one intermolecular bond with the solvate dioxane molecule, the latter being used as a solvent for recrystallisation.     

Theoretical studies on the hydrolysis of mono-phosphate and tri-phosphate in gas phase and aqueous solution

Phosphate hydrolysis by GTPases plays an important role as a molecular switch in signal transduction and as an initiator of many other biological processes. Despite the centrality of this ubiquitous reaction, the mechanism is still poorly understood. As a first step to understand the mechanisms of this process, the nonenzymatic hydrolysis of mono-phosphate and tri-phosphate esters were systematically studied in gas phase and aqueous solution using hybrid density functional methods. The dielectric effect of the environment on the energetics of these processes was also explored. Theoretical results show that for mono-phosphate ester, the dissociative pathway is much more favorable than the associative pathway. However, the reaction barriers for the dissociative and associative pathways of tri-phosphate hydrolysis are very close in aqueous solution, though the dissociative pathway is more favorable in the gas phase. High dielectric solvents, such as water, significantly lower the activation barrier of the associative pathway due to the greater solvation energy of the associative transition states than that of the reactant complex. By contrast, the barrier of the dissociative pathway, with respect to the gas phase, is less sensitive to the surrounding dielectric. In the associative hydrolysis pathway of the tri-phosphate ester, negative charge is transferred from the gamma-phosphate to beta-phosphate through the bridging ester oxygen and results in Pgamma-O bond dissociation. No analogous charge transfer was observed in the dissociative pathway, where Pgamma-O bond dissociation resulted from proton transfer from the gamma-phosphate to the bridge oxygen. Finally, the active participation of local water molecules can significantly lower the activation energy of the dissociative pathway for both mono-phosphate and tri-phosphate.     

Quantum algorithm for alchemical optimization in material design

The development of tailored materials for specific applications is an active field of research in chemistry, material science and drug discovery. The number of possible molecules obtainable from a set of atomic species grow exponentially with the size of the system, limiting the efficiency of classical sampling algorithms. On the other hand, quantum computers can provide an efficient solution to the sampling of the chemical compound space for the optimization of a given molecular property. In this work, we propose a quantum algorithm for addressing the material design problem with a favourable scaling. The core of this approach is the representation of the space of candidate structures as a linear superposition of all possible atomic compositions. The corresponding ‘alchemical’ Hamiltonian drives the optimization in both the atomic and electronic spaces leading to the selection of the best fitting molecule, which optimizes a given property of the system, e.g., the interaction with an external potential as in drug design. The quantum advantage resides in the efficient calculation of the electronic structure properties together with the sampling of the exponentially large chemical compound space. We demonstrate both in simulations and with IBM Quantum hardware the efficiency of our scheme and highlight the results in a few test cases. This preliminary study can serve as a basis for the development of further material design quantum algorithms for near-term quantum computers.

‘Alchemical’ quantum algorithm for the simultaneous optimisation of chemical composition and electronic structure for material design. By exploiting quantum mechanical principles this approach will boost drug discovery in the near future.     

Ab initio density functional theory: the best of both worlds?

Density functional theory (DFT), in its current local, gradient corrected, and hybrid implementations and their extensions, is approaching an impasse. To continue to progress toward the quality of results demanded by today's ab initio quantum chemistry encourages a new direction. We believe ab initio DFT is a promising route to pursue. Whereas conventional DFT cannot describe weak interactions, photoelectron spectra, or many potential energy surfaces, ab initio DFT, even in its initial, optimized effective potential, second-order many-body perturbation theory form [OEP (2)-semi canonical], is shown to do all well. In fact, we obtain accuracy that frequently exceeds MP2, being competitive with coupled-cluster theory in some cases. Furthermore, this is accomplished within a relatively fast computational procedure that scales like iterative second order. We illustrate our results with several molecular examples including Ne2,Be2,F2, and benzene.     

Temperature influence on the dynamic binding capacity of a monolithic ion-exchange column

This work investigates the influence of temperature on the binding capacity of bovine serum albumin (BSA), soybean trypsin inhibitor and L-glutamic acid to a CIM (DEAE) weak anion-exchange disk monolithic column. The binding capacity was determined experimentally under dynamic conditions using frontal analysis. The effect on the dynamic binding capacity of dimers present in the BSA solution has been evaluated and a closed-loop frontal analysis was used to determine the equilibrium binding capacities. The binding capacity for both BSA and soybean trypsin inhibitor increased with increasing temperature. In the case of L-glutamic acid, an increase in the binding capacity was observed with temperature up to 20 degrees C. A further increase in temperature caused a decrease of the dynamic binding capacity.     

Observation of difluorinated higher fullerene anions by Knudsen cell mass spectrometry and determination of electron affinities of C60F2 and C70F2

Difluorinated higher fullerenes have been studied by Knudsen cell mass spectrometry. Thermal negative ions C_nF₂⁻ (n=60, 70, 72, 74, 76 and 78) were produced inside the effusion cell as well as the neutral molecules C₆₀F₂ and C₇₀F₂. From the equilibrium constants for the electron exchange reactions between difluorinated fullerenes and their parents electron affinity values were derived for C₆₀F₂ (2.74 eV) and C₇₀F₂ (2.80 eV).     

Chromatic number of Hasse diagrams,eyebrows and dimension

We construct posets of dimension 2 with highly chromatic Hasse diagrams. This solves a previous problem by Nesetril and Trotter.     

Ion beam modification and analysis of GdBaCuO thin film on Si substrates

The effects of ion implantation into thin films of the GbBaCuO on Si substrates without any buffer layer at 300 and 77 K have been studied. Using H⁺ ions, the superconducting transition temperature, the change of electrical properties from conducting to insulating, and the crystalline to amorphous structural transition in the films were studied as a function of ion dose. The implantation energy was 150 keV.     

Detection of Escherichia coli O157:H7 bacteria by a combination of immunofluorescent staining and capillary electrophoresis

As the number of incidents of bacterial infections continues to rise around the globe, simpler, faster, and more sensitive diagnostic techniques are required to improve the safety of the food supply and to screen for potential bacterial infections in humans. We present here direct and indirect approaches for the detection of bacteria, which are based upon a combination of immunofluorescent staining and capillary electrophoresis. In the direct approach, Escherichia coli O157:H7 bacteria stained with fluorescein-tagged specific antibodies are detected by CE, while in the indirect approach fluorescein-tagged specific antibodies to E. coli are first captured by E. coli O157:H7 bacteria and then released and detected by CE. We have identified suitable bacteria staining and CE protocols, which involved a 10 mM Tris-borate-EDTA (TBE) buffer, 0.25 micro g antibody/1 million bacteria, and capillaries dynamically coated with poly-N-hydroxyethylacrylamide (polyDuramide). We have also successfully detected the presence of E. coli O157:H7 in contaminated meat. The total time required for analysis was 6-8 h, which is less than that realized in most commercial assays presently available.     

Can luminescent quantum dots be efficient energy acceptors with organic dye donors?

We assessed the ability of luminescent quantum dots (QDs) to function as energy acceptors in fluorescence resonance energy transfer (FRET) assays, with organic dyes serving as donors. Either AlexaFluor 488 or Cy3 dye was attached to maltose binding protein (MBP) and used with various QD acceptors. Steady-state and time-resolved fluorescence measurements showed no apparent FRET from dye to QD. We attribute these observations to the dominance of a fast radiative decay rate of the donor excitation relative to a slow FRET decay rate. This is due to the long exciton lifetime of the acceptor compared to that of the dye, combined with substantial QD direct excitation.