Desirable phosphors for lighting,scintillation and composite films must have good light absorption properties,high concentration quenching,high quantum efficiency,a narrow color emission,and so forth.In this work,we f...Desirable phosphors for lighting,scintillation and composite films must have good light absorption properties,high concentration quenching,high quantum efficiency,a narrow color emission,and so forth.In this work,we first show that undoped yttrium hafnate Y_(2)Hf_(2)O_(7)(YHO)nanoparticles(NPs)display dual blue and red bands after excitation using 330 nm light.Based on density functional theory(DFT)calculations,these two emission bands are correlated with the defect states arising in the band-gap region of YHO owing to the presence of neutral and charged oxygen defects.Once doped with Eu^(3+)ions(YHOE),the YHO NPs show a bright red emission,a long excited state lifetime and stable color coordinates upon near-UV and X-ray excitation.Concentration quenching is active when Eu^(3+)doping reaches 10 mol%with a critical distance of~4.43Å.This phenomenon indicates a high Eu^(3+)solubility within the YHO host and the absence of Eu^(3+)clusters.More importantly,the optical performance of the YHOE NPs has been further improved by lithium co-doping.The origin of the emission,structural stability,and role of Li^(+)-codoping are explored both experimentally and theoretically.DFT calculation results demonstrate that Li^(+)-co-doping increases the covalent character of the Eu^(3+)-O^(2-)bonding in the EuO8 polyhedra.Furthermore,the YHOE NPs have been dispersed into polyvinyl alcohol(PVA)to make transparent nanocomposite films,which show strong red emission under excitation at 270 and 393 nm.Overall,we demonstrate that the YHO NPs with Eu^(3+)and(Eu^(3+)/Li^(+))doping have a high emission intensity and quantum efficiency under UV and X-ray excitation,which makes them suitable for use as phosphors,scintillators and transparent films for lighting,imaging and detection applications.展开更多
基金support from the National Science Foundation under CHE(award#1710160)the IIT startup funds.SKG thanks the United States-India Education Foundation(USIEF)and the Institute of International Education(IIE)for his Fulbright Nehru Postdoctoral Fellowship(award#2268/FNPDR/2017).
文摘Desirable phosphors for lighting,scintillation and composite films must have good light absorption properties,high concentration quenching,high quantum efficiency,a narrow color emission,and so forth.In this work,we first show that undoped yttrium hafnate Y_(2)Hf_(2)O_(7)(YHO)nanoparticles(NPs)display dual blue and red bands after excitation using 330 nm light.Based on density functional theory(DFT)calculations,these two emission bands are correlated with the defect states arising in the band-gap region of YHO owing to the presence of neutral and charged oxygen defects.Once doped with Eu^(3+)ions(YHOE),the YHO NPs show a bright red emission,a long excited state lifetime and stable color coordinates upon near-UV and X-ray excitation.Concentration quenching is active when Eu^(3+)doping reaches 10 mol%with a critical distance of~4.43Å.This phenomenon indicates a high Eu^(3+)solubility within the YHO host and the absence of Eu^(3+)clusters.More importantly,the optical performance of the YHOE NPs has been further improved by lithium co-doping.The origin of the emission,structural stability,and role of Li^(+)-codoping are explored both experimentally and theoretically.DFT calculation results demonstrate that Li^(+)-co-doping increases the covalent character of the Eu^(3+)-O^(2-)bonding in the EuO8 polyhedra.Furthermore,the YHOE NPs have been dispersed into polyvinyl alcohol(PVA)to make transparent nanocomposite films,which show strong red emission under excitation at 270 and 393 nm.Overall,we demonstrate that the YHO NPs with Eu^(3+)and(Eu^(3+)/Li^(+))doping have a high emission intensity and quantum efficiency under UV and X-ray excitation,which makes them suitable for use as phosphors,scintillators and transparent films for lighting,imaging and detection applications.
