Research Article

Eliminating nonradiative decay in Cu(I) emitters: >99% quantum efficiency and microsecond lifetime

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Science  08 Feb 2019:
Vol. 363, Issue 6427, pp. 601-606
DOI: 10.1126/science.aav2865

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  • RE: Eliminating nonradiative decay in Cu(I) emitters: >99% quantum efficiency and microsecond lifetime
    • Timothy J H Hele, Research Fellow, Cavendish Laboratory, Cambridge University
    • Other Contributors:
      • Dan Credgington, Royal Society University Research Fellow, Cavendish Laboratory, Cambridge University

    We are delighted that the theoretical results of Hamze et al [1] match so closely those proposed for these systems over a year ago [2].

    Ref [2] proposed a three atom model consisting of the carbazole nitrogen, metal atom and carbene carbon, and determined the importance of the carbene 2p orbital, metal d orbitals and nitrogen 2p - in fact, the orbitals shown in figure 1D of the article by Hamze et al [1] are qualitatively identical to those in figure 4A of Ref [2]. Ref [2] notes the role of the metal atom as a chromophore, corroborated by the findings of Ref [1].

    The experimental findings of Hamze et al [1] have also verified the theoretical prediction from group theory in Ref [2] that HOMO to LUMO transitions are dipole-forbidden in the twisted geometry, such that in any twisted compound the optical absorption and emission should be substantially weaker than in a planar analogue - verified by comparison of compounds 1b and 2b in Ref [1].

    Furthermore, the theoretical model in Ref [2] can clarify and explain some of the experimental observations in Ref [1]. Ref [1] correctly suggests that copper d orbitals contribute to absorption and emission, but d to d transitions in themselves are forbidden by the Laporte selection rule [3]. However, if one includes the role of copper 4p orbitals in the LUMO (figure 4A of Ref [2]), 3d to 4p transitions are allowed, permitting the metal atom to contribute substantially to optical absorption and emission.

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    Competing Interests: None declared.