B. J. Powell

Towards quantum chemistry on a quantum computer

Exact first-principles calculations of molecular properties are currently intractable because their computational cost grows exponentially with both the number of atoms and basis set size. A solution is to move to a radically different model of computing by building a quantum computer, which is a device that uses quantum systems themselves to store and process data. Here we report the application of the latest photonic quantum computer technology to calculate properties of the smallest molecular system: the hydrogen molecule in a minimal basis. We calculate the complete energy spectrum to 20 bits of precision and discuss how the technique can be expanded to solve large-scale chemical problems that lie beyond the reach of modern supercomputers. These results represent an early practical step toward a powerful tool with a broad range of quantum-chemical applications.

A first-principles density-functional calculation of the electronic and vibrational structure of the key melanin monomers.

We report first-principles density-functional calculations for hydroquinone (HQ), indolequinone (IQ), and semiquinone (SQ). These molecules are believed to be the basic building blocks of the eumelanins, a class of biomacromolecules with important biological functions (including photoprotection) and with the potential for certain bioengineering applications. We have used the difference of self-consistent fields method to study the energy gap between the highest occupied molecular orbital and the lowest unoccupied molecular orbital, Delta(HL). We show that Delta(HL) is similar in IQ and SQ, but approximately twice as large in HQ. This may have important implications for our understanding of the observed broadband optical absorption of the eumelanins. The possibility of using this difference in Delta(HL) to molecularly engineer the electronic properties of eumelanins is discussed. We calculate the infrared and Raman spectra of the three redox forms from first principles. Each of the molecules have significantly different infrared and Raman signatures, and so these spectra could be used in situ to nondestructively identify the monomeric content of macromolecules. It is hoped that this may be a helpful analytical tool in determining the structure of eumelanin macromolecules and hence in helping to determine the structure-property-function relationships that control the behavior of the eumelanins.

Quantum frustration in organic Mott insulators: from spin liquids to unconventional superconductors

We review the interplay of frustration and strong electronic correlations in quasi-two-dimensional organic charge transfer salts, such as (BEDT-TTF)2X and EtnMe4−nPn[Pd(dmit)2]2. These two forces drive a range of exotic phases including spin liquids, valence bond crystals, pseudogapped metals and unconventional superconductivity. Of particular interest is that in several materials pressure drives a first-order transition from a spin liquid Mott insulating state to a superconducting state. Experiments on these materials raise a number of profound questions about the quantum behaviour of frustrated systems, particularly the intimate connection between spin liquids and superconductivity. Insights into these questions have come from a wide range of theoretical techniques including first principles electronic structure, quantum many-body theory and quantum field theory. In this review we introduce some of the basic ideas of the field by discussing a simple frustrated Heisenberg model with four spins. We then describe the key experimental results, emphasizing that for two materials, κ-(BEDT-TTF)2Cu2(CN)3 and EtMe3Sb[Pd(dmit)2]2, there is strong evidence for a spin liquid ground state, and for another, EtMe3P[Pd(dmit)2]2, there is evidence of a valence bond crystal ground state. We review theoretical attempts to explain these phenomena, arguing that they can be captured by a Hubbard model on the anisotropic triangular lattice at half filling, and that resonating valence bond wavefunctions capture most of the essential physics. We review evidence that this Hubbard model can have a spin liquid ground state for a range of parameters that are realistic for the relevant materials. In particular, spatial anisotropy and ring exchange are key to destabilizing magnetic order. We conclude by summarizing the progress made thus far and identifying some of the key questions still to be answered.

A unified explanation of the Kadowaki–Woods ratio in strongly correlated metals

The Kadowaki–Woods ratio attempts to relate the temperature dependence of a metal to its heat capacity. However, as it takes different values for different classes of metals it is not universal. By including effects related to carrier density and spatial dimensionality, a much more universal ratio, which describes the properties of many different systems, has been achieved.

On the origin of electrical conductivity in the bio-electronic material melanin

The skin pigment melanin is one of a few bio-macromolecules that display electrical and photo-conductivity in the solid-state. A model for melanin charge transport based on amorphous semiconductivity has been widely accepted for 40 years. In this letter, we show that a central pillar in support of this hypothesis, namely experimental agreement with a hydrated dielectric model, is an artefact related to measurement geometry and non-equilibrium behaviour. Our results cast significant doubt on the validity of the amorphous semiconductor model and are a reminder of the difficulties of electrical measurements on low conductivity, disordered organic materials.

Theories of phosphorescence in organo-transition metal complexes – From relativistic effects to simple models and design principles for organic light-emitting diodes

We review theories of phosphorescence in cyclometalated complexes. We focus primarily on pseudooctahedrally coordinated

Effects of Fluorination on Iridium(III) Complex Phosphorescence: Magnetic Circular Dichroism and Relativistic Time-Dependent Density Functional Theory

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Spin–Orbit Coupling in Phosphorescent Iridium(III) Complexes

metals (e.g., [Os(II)(bpy)

Gaseous Adsorption in Melanins: Hydrophilic Biomacromolecules with High Electrical Conductivities

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Dependence of the superconducting transition temperature of organic molecular crystals on intrinsically nonmagnetic disorder: A signature of either unconventional superconductivity or the atypical formation of magnetic moments

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