The research interests of my group are principally computational and are concerned with both d- and f-block transition metal chemistry. We study bonding and reaction mechanisms. Theoretical methods use density functional theory to calculate electronic ground states, optimize geometries, investigate fluxional processes and reaction pathways and model photoelectron (PE) spectra.
Calculations are carried out both on local work stations and using the Oxford Supercomputer centre.
PE spectroscopy is the principal experimental technique used for probing the electronic structure of transition metal compounds: this is coupled, where appropriate, to related information from n.m.r., e.s.r., magnetics, optical and structural studies. Interpretation of results, assisted by the calculations, stresses the development of simple models that enable useful qualitative predictions of structure and reactivity.
Specific areas of current interest include:
1. Organometallic structures, reactions and catalysis
Calculations model structures, identify transition states and explore of a reaction mechanism.
Figure 1 Calculated and experimental distances for Sn(P2C2R2)
2. PE studies using synchrotron radiation
PE band intensities vary with the photon energy used to generate the spectrum. The energies and intensity changes enable the orbital structure to be characterized.
Figure 2 PE spectrum of U(BH4)4 showing intensity changes with photon energy.
Mixed quantum mechanical and molecular mechanics calculations enable very large systems to be studied.
Figure 3 The metalloenzyme P450 cam
Properties of nanotubes containing 1-d crystals provide an interesting computational challenge.
Figure 4 Nano tube containing a KBr crystal