Josep M. Luis

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Oxo-transfer chemistry mediated by iron underpins many biological processes and today is emerging as synthetically very important for the catalytic oxidation of C-H and C=C moieties that are hard to activate conventionally. Despite the vast amount of research in this area, experimental characterization of the reactive species under catalytic conditions is(More)
The spectroscopic and chemical characterization of a new synthetic non-heme iron(IV)-oxo species [Fe(IV)(O)((Me,H) Pytacn)(S)](2+) (2, (Me,H)Pytacn=1-(2'-pyridylmethyl)-4,7-dimethyl-1,4,7-triazacyclononane, S=CH(3)CN or H(2)O) is described. Complex 2 was prepared by reaction of [Fe(II)(CF(3)SO(3))(2)((Me,H) Pytacn)] (1) with peracetic acid. Complex 2 bears(More)
A set of exchange-correlation functionals, including BLYP, PBE0, B3LYP, BHandHLYP, CAM-B3LYP, LC-BLYP, and HSE, has been used to determine static and dynamic nonresonant (nuclear relaxation) vibrational (hyper)polarizabilities for a series of all-trans polymethineimine (PMI) oligomers containing up to eight monomer units. These functionals are assessed(More)
A general reduced dimensionality finite field nuclear relaxation method for calculating vibrational nonlinear optical properties of molecules with large contributions due to anharmonic motions is introduced. In an initial application to the umbrella (inversion) motion of NH(3) it is found that difficulties associated with a conventional single well(More)
In this study we report on the electronic and vibrational (hyper)polarizabilities of donor-acceptor-substituted azobenzene. It is observed that both electronic and vibrational contributions to the electric dipole first hyperpolarizability of investigated photoactive molecule substantially depend on the conformation. The contributions to the nuclear(More)
Recently, we reported that the basis set has a profound influence on the computed values for spin-state splittings [J. Phys. Chem. A 2008, 112, 6384]. In particular, small Gaussian-type orbital (GTO) basis sets were shown to be unreliable for the prediction of them. Here, we report simple modifications of the small Pople-type Gaussian-type orbital basis(More)
Density functional theory (DFT) is employed to: 1) propose a viable catalytic cycle consistent with our experimental results for the mechanism of chemically driven (Ce(IV) ) O2 generation from water, mediated by nonheme iron complexes; and 2) to unravel the role of the ligand on the nonheme iron catalyst in the water oxidation reaction activity. To this(More)