title: Direct Chemical Fine-Tuning of Electronic Properties in Sc2Ir6-xPdxB.
abstract: Crystal orbital Hamilton population (COHP) bonding analysis has predicted that ScPd3B0.5is the least stable compound of the entire series Sc2Ir6-xPdxB. Here, we report a systematic study of Sc2Ir6-xPdxB (x=3, 5 and 6) by means of11B nuclear magnetic resonance (NMR), Knight shift (K) and nuclear spin-lattice relaxation rate (1/T1). NMR results combined with theoretical band structure calculations provide a measure of s- and non-s-character Fermi-level density of states. We present direct evidence that the enhanced s-state character of the Fermi level density of states (DOS) in ScPd3B0.5reduces the strength of the B 2p and Pd 4d hybridized states across the entire Sc2Ir6-xPdxB series. This hybridization strength relates to the opening of a deep pseudogap in the density of states of Sc2IrPd5B and the chemical bonding instability of ScPd3B0.5. This study is an experimental realization of a chemical fine-tuning of the electronic properties in intermetallic perovskites.
authors.affiliation: Department of Chemistry and Biochemistry, University of California at Los Angeles, 607 Charles E. Young Drive East, Los Angeles, California, 90095-1569, USA.
authors.forename: Dimitrios
authors.initials: D
authors.lastname: Koumoulis
authors.affiliation: Institut für Anorganische Chemie, Rheinisch-Westfälische Technische Hochschule Aachen, 52056, Aachen, Germany.
authors.forename: Jan P
authors.initials: JP
authors.lastname: Scheifers
authors.affiliation: Institut für Anorganische Chemie, Rheinisch-Westfälische Technische Hochschule Aachen, 52056, Aachen, Germany.
authors.forename: Rachid
authors.initials: R
authors.lastname: St Touzani
authors.affiliation: Institut für Anorganische Chemie, Rheinisch-Westfälische Technische Hochschule Aachen, 52056, Aachen, Germany. bfokwa@ucr.edu.|Department of Chemistry, University of California Riverside, Chemical Sciences Building, 501 Big Springs Road, Riverside, CA, 92521, USA. bfokwa@ucr.edu.
authors.forename: Boniface P T
authors.initials: BP
authors.lastname: Fokwa
authors.affiliation: Department of Chemistry and Biochemistry, University of California at Los Angeles, 607 Charles E. Young Drive East, Los Angeles, California, 90095-1569, USA. bouchard@chem.ucla.edu.|California NanoSystems Institute, University of California at Los Angeles, 570 Westwood Plaza, Building 114, Los Angeles, California, 90095-1569, USA. bouchard@chem.ucla.edu.
authors.forename: Louis-S
authors.initials: LS
authors.lastname: Bouchard
keywords: 11B NMR; Fermi level; chemical bonding; intermetallic perovskite; superstructure