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Tunable trimers:using temperature and pressure to control luminescent emission in gold(i) pyrazolate-based trimers


Reference:

Woodall, C. H., Fuertes Lorda, S., Beavers, C. M., Hatcher, L. E., Parlett, A., Shepherd, H. J., Christensen, J., Teat, S. J., Intissar, M., Rodrigue-Witchel, A., Suffren, Y., Reber, C., Hendon, C. H., Tiana, D., Walsh, A. and Raithby, P. R., 2014. Tunable trimers:using temperature and pressure to control luminescent emission in gold(i) pyrazolate-based trimers. Chemistry - A European Journal, 20 (51), pp. 16933-16942.

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    Official URL:

    http://dx.doi.org/10.1002/chem.201404058

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    Abstract

    A systematic investigation into the relationship between the solid-state luminescence and the intermolecular AuAu interactions in a series of pyrazolate-based gold(I) trimers; tris(μ2-pyrazolato-N,N')-tri-gold(I) (1), tris(μ2-3,4,5- trimethylpyrazolato-N,N')-tri-gold(I) (2), tris(μ2-3-methyl-5- phenylpyrazolato-N,N')-tri-gold(I) (3) and tris(μ2-3,5-diphenylpyrazolato- N,N')-tri-gold(I) (4) has been carried out using variable temperature and high pressure X-ray crystallography, solid-state emission spectroscopy, Raman spectroscopy and computational techniques. Single-crystal X-ray studies show that there is a significant reduction in the intertrimer AuAu distances both with decreasing temperature and increasing pressure. In the four complexes, the reduction in temperature from 293 to 100 K is accompanied by a reduction in the shortest intermolecular AuAu contacts of between 0.04 and 0.08 The solid-state luminescent emission spectra of 1 and 2 display a red shift with decreasing temperature or increasing pressure. Compound 3 does not emit under ambient conditions but displays increasingly red-shifted luminescence upon cooling or compression. Compound 4 remains emissionless, consistent with the absence of intermolecular AuAu interactions. The largest pressure induced shift in emission is observed in 2 with a red shift of approximately 630 cm-1 per GPa between ambient and 3.80 GPa. The shifts in all the complexes can be correlated with changes in AuAu distance observed by diffraction.

    Details

    Item Type Articles
    CreatorsWoodall, C. H., Fuertes Lorda, S., Beavers, C. M., Hatcher, L. E., Parlett, A., Shepherd, H. J., Christensen, J., Teat, S. J., Intissar, M., Rodrigue-Witchel, A., Suffren, Y., Reber, C., Hendon, C. H., Tiana, D., Walsh, A. and Raithby, P. R.
    DOI10.1002/chem.201404058
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    URLURL Type
    http://www.scopus.com/inward/record.url?scp=84915747957&partnerID=8YFLogxKUNSPECIFIED
    Uncontrolled Keywordsaurophilicity,crystallography,gold,high pressure,luminescence
    DepartmentsFaculty of Science > Chemistry
    Research CentresCentre for Sustainable Chemical Technologies
    RefereedYes
    StatusPublished
    ID Code42426

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