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Mononuclear lanthanide(iii)-oxamate complexes as new photoluminescent field-induced single-molecule magnets: solid-state photophysical and magnetic properties

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Abstract

Implementing additional optical (luminescent) properties into the well-known class of single-molecule magnets (SMMs) is considered as a promising route toward obtaining the next generation of optomagnetic materials for quantum information storage and computing. Herein, we report a joint optical and magneto-structural study for the two novel series of lanthanide(III) complexes of general formula Bu4N[LnIII(HL)4(dmso)]·nH2O where H2L = N-(4-Xphenyl)oxamic acid with X = Cl and n = 2 [Ln = Eu (1_Cl), Gd (2_Cl), Dy (3_Cl), and Tb (4_Cl)] and X = F and n = 3 [Ln = Eu (1_F), Gd (2_F), Dy (3_F), and Tb (4_F)]. All these compounds are mononuclear species with each lanthanide(III) cation in a low-symmetry nine-coordinate environment (LnO9) which is constituted by four didentate monoprotonated oxamate groups and one dmso molecule. Magnetic measurements show the occurrence of field-induced SMM behavior for the Gd3+ (2_Cl and 2_F), Dy3+ (3_Cl and 3_F), and Tb3+ complexes (4_Cl and 4_F). Solid-state photophysical measurements for the Eu3+ (1_Cl and 1_F) and Tb3+ complexes (4_Cl and 4_F) reveal that both monoprotonated chloro- and fluoro-substituted phenyl(oxamate) ligands are able to sensitize the lanthanide(III)-based luminescence in the visible region, through an energy transfer process (“antenna effect”), as supported by theoretical calculations for Eu3+ compounds. In particular, 1_Cl and 1_F present a quantum efficiency of approximately 50%, being potentially suitable as efficient light conversion molecular devices (LCMDs).

Graphical abstract: Mononuclear lanthanide(iii)-oxamate complexes as new photoluminescent field-induced single-molecule magnets: solid-state photophysical and magnetic properties

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Supplementary files

Article information


Submitted
15 Jul 2020
Accepted
27 Jul 2020
First published
27 Jul 2020

Dalton Trans., 2020, Advance Article
Article type
Paper

Mononuclear lanthanide(III)-oxamate complexes as new photoluminescent field-induced single-molecule magnets: solid-state photophysical and magnetic properties

R. C. A. Vaz, I. O. Esteves, W. X. C. Oliveira, J. Honorato, F. T. Martins, L. F. Marques, G. L. dos Santos, R. O. Freire, L. T. Jesus, E. F. Pedroso, W. C. Nunes, M. Julve and C. L. M. Pereira, Dalton Trans., 2020, Advance Article , DOI: 10.1039/D0DT02497J

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