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Titolo:
Donor-acceptor complexes incorporating ferrocenes: spectroelectrochemical characterisation, quadratic hyperpolarisabilities and the effects of oxidising and reducing agents
Autore:
Malaun, M; Kowallick, R; McDonagh, AM; Marcaccio, M; Paul, RL; Asselberghs, I; Clays, K; Persoons, A; Bildstein, B; Fiorini, C; Nunzi, JM; Ward, MD; McCleverty, JA;
Indirizzi:
Univ Bristol, Sch Chem, Bristol BS8 1TS, Avon, England Univ Bristol Bristol Avon England BS8 1TS Bristol BS8 1TS, Avon, England Univ Louvain, Ctr Res Mol Elect & Photon, Lab Chem & Biol Dynam, B-300 Louvain, Belgium Univ Louvain Louvain Belgium B-300 & Biol Dynam, B-300 Louvain, Belgium Innsbruck Univ, Inst Gen Inorgan & Theoret Chem, A-6020 Innsbruck, AustriaInnsbruck Univ Innsbruck Austria A-6020 Chem, A-6020 Innsbruck, Austria CEA Saclay, DEIN SPE Grp Composants Organ, LETI, CEA Technol Avances, F-91191 Gif Sur Yvette, France CEA Saclay Gif Sur Yvette France F-91191 F-91191 Gif Sur Yvette, France
Titolo Testata:
JOURNAL OF THE CHEMICAL SOCIETY-DALTON TRANSACTIONS
fascicolo: 20, , anno: 2001,
pagine: 3025 - 3038
SICI:
1472-7773(2001):20<3025:DCIFSC>2.0.ZU;2-4
Fonte:
ISI
Lingua:
ENG
Soggetto:
NONLINEAR-OPTICAL PROPERTIES; MONONITROSYL REDOX CENTERS; HYPER-RAYLEIGH SCATTERING; 2ND HARMONIC-GENERATION; 2ND-HARMONIC GENERATION; STILBENE DERIVATIVES; FIRST HYPERPOLARIZABILITIES; SESQUIFULVALENE COMPLEXES; ORGANOMETALLIC COMPOUNDS; ELECTRONIC-STRUCTURE;
Tipo documento:
Article
Natura:
Periodico
Settore Disciplinare:
Physical, Chemical & Earth Sciences
Citazioni:
78
Recensione:
Indirizzi per estratti:
Indirizzo: Ward, MD Univ Bristol, Sch Chem, Cantocks Close, Bristol BS8 1TS, Avon, England Univ Bristol Cantocks Close Bristol Avon England BS8 1TS England
Citazione:
M. Malaun et al., "Donor-acceptor complexes incorporating ferrocenes: spectroelectrochemical characterisation, quadratic hyperpolarisabilities and the effects of oxidising and reducing agents", J CHEM S DA, (20), 2001, pp. 3025-3038

Abstract

The donor-acceptor complexes [Fe(C5H5){C(5)H(4)QNHM(NO)(Tp(Me,Me))X}] {Tp(Me,Me) = tris(3,5-dimethylpyrazolyl) borate; Q = nothing, M = Mo, X = Cl, Br, I; M = W, X = Cl; Q = C6H4, M = Mo, X = Cl, Br, I; M = W, X = Cl; Q = CH=CHC6H4 or N=NC6H4, M = Mo, X = Cl), which contain 16-valence electron metal nitrosyl centres, [Fe(C5H5){C(5)H(4)QpyMo(NO)(Tp(Me,Me))Cl}] (py = 4-pyridyl; Q = CH=CH, CH=CHCO, N=CH and C6H4CH=CH), [Fe(C5Me4H){C5H4CH=CHpyMo(NO)(Tp(Me,Me))Cl}] and [Fe(C5Me4H)(C(5)Me(4)QpyZ)] {Q = CH=CH or CH=N, Z = Mo(NO)(Tp(Me,Me))Cl or W(CO)(5); Q=2,4-CH=CH(C4H2S) CH=CH, Z = W(CO)(5) or Me+I-}, some of which contain 17-valence electron molybdenum nitrosyl centres,and [Fe(C5Me4H){C5Me4CH=CH(C4H2S) CH=CHpy}], have been characterised electrochemically, by their electronic spectra, and spectroelectrochemically. Hyper-Rayleigh scattering was used to determine the rst hyperpolarisability,,the data showing that (a) is dependent on the metal in the acceptor fragment, (b) beta increased when Cl or Br was replaced by I and (c) beta increased when the number of methyl groups on the cyclopentadienyl rings increased. The beta -values for comparable complexes containing {Mo(NO)(Tp(Me,Me))Cl} and {W(CO)(5)} moieties were similar. Chemical oxidation of the ferrocenyl or chemical reduction of the molybdenum nitrosyl acceptor fragments in selected complexes caused a reduction of between 25% and 100% in the NLO response. X-Ray structural studies of [Fe(C5H5){C5H4NHMo(NO)(Tp(Me,Me))Cl}] (P (1) over bar) and [Fe(C5Me4H){C5Me4CH=CHpyMo(NO)(Tp(Me,Me))Cl}] (P (1) overbar) are reported.

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Documento generato il 01/12/20 alle ore 22:16:00