Single-ion magnets(SIMs)are prominent candidates for promoting new technologies in quantum information processing(QIP).Herein,we present two new isostructural oxamato derivatives,namely,{n-Bu_(4)N[Ln(H_(2)edpba)_(2)]}...Single-ion magnets(SIMs)are prominent candidates for promoting new technologies in quantum information processing(QIP).Herein,we present two new isostructural oxamato derivatives,namely,{n-Bu_(4)N[Ln(H_(2)edpba)_(2)]}_(n),Ln=Tb^(3+)(1)and Gd^(3+)(2)[H_(2)edpba^(2-)=N,N’-2,2’-ethylenediphenylenebis(oxamate)],that are thermostable up to∼290℃.Single-crystal X-ray diffraction reveals that 1 and 2 are one-dimensional coordination polymers with a ribbon-like structure,and their metal centers are eight-coordinated with a D_(4d) symmetry.Cryomagnetic studies disclose the presence of slow magnetic relaxation(SMR)behavior for 1 and 2.For 1,the Raman effect dominates the SMR at a zero magnetic field,while Raman,Orbach,and reciprocating thermal behavior(RTB)mechanisms arise at higher fields.Conversely,RTB and the bottleneck effect were observed at 2.Solid-state photoluminescent data display a remarkable green luminescence emission,with intense and sharp bands ranging from 480 to 700 nm in the spectra,which are attributed to the ^(5)D_(4)→^(7)F_(J)(J=6-0)transitions of terbium(Ⅲ)ions.By monitoring the temperaturedependent lifetime of the ^(5)D_(4) state after the intensity decay of the emission band attributed to the ^(5)D_(4)→^(7)F_(5)(546 nm)transition,the complex shows a reasonable thermometric performance with a relative sensitivity of 2.77%K^(-1) at 448 K.1 behaves as a zero-field SIM and as a photoluminescent thermometer.展开更多
基金supported by the Conselho Nacional de Desenvolvimento Científico e Tecnológico(CNPq)Fundacao de Amparoà Pesquisa do Estado de Minas Gerais(FAPEMIG)+3 种基金Fundacao Carlos Chagas Filho de Amparoà Pesquisa do Estado do Rio de Janeiro(FAPERJ)Fundacao de Aperfeiçoamento de Pessoal de Nível Superior(CAPES,Finance Code 001)the Fundacao de AmparoàPesquisa do Estado de Sao Paulo(FAPESP)for the postdoctoral fellowship(2024/00198-0)for RVP,project 2021/08111-2for funding the EMU Project 2023/17024-1.
文摘Single-ion magnets(SIMs)are prominent candidates for promoting new technologies in quantum information processing(QIP).Herein,we present two new isostructural oxamato derivatives,namely,{n-Bu_(4)N[Ln(H_(2)edpba)_(2)]}_(n),Ln=Tb^(3+)(1)and Gd^(3+)(2)[H_(2)edpba^(2-)=N,N’-2,2’-ethylenediphenylenebis(oxamate)],that are thermostable up to∼290℃.Single-crystal X-ray diffraction reveals that 1 and 2 are one-dimensional coordination polymers with a ribbon-like structure,and their metal centers are eight-coordinated with a D_(4d) symmetry.Cryomagnetic studies disclose the presence of slow magnetic relaxation(SMR)behavior for 1 and 2.For 1,the Raman effect dominates the SMR at a zero magnetic field,while Raman,Orbach,and reciprocating thermal behavior(RTB)mechanisms arise at higher fields.Conversely,RTB and the bottleneck effect were observed at 2.Solid-state photoluminescent data display a remarkable green luminescence emission,with intense and sharp bands ranging from 480 to 700 nm in the spectra,which are attributed to the ^(5)D_(4)→^(7)F_(J)(J=6-0)transitions of terbium(Ⅲ)ions.By monitoring the temperaturedependent lifetime of the ^(5)D_(4) state after the intensity decay of the emission band attributed to the ^(5)D_(4)→^(7)F_(5)(546 nm)transition,the complex shows a reasonable thermometric performance with a relative sensitivity of 2.77%K^(-1) at 448 K.1 behaves as a zero-field SIM and as a photoluminescent thermometer.
