Glass ceramics Ba2LaFT:xDy3+ are obtained through the conventional melt-quenching technique, and their lu- minescent properties are investigated. Under 350 nm excitation, the emission spectra consists of a strong bl...Glass ceramics Ba2LaFT:xDy3+ are obtained through the conventional melt-quenching technique, and their lu- minescent properties are investigated. Under 350 nm excitation, the emission spectra consists of a strong blue- yellow band as well as a weak red emission centered at 660 nm, which are attributed to the 4F9/2 →6H15/2, 4F9/2→6H13/2 and 4F9/2 → 6Hll/2 transitions of the Dy3+ ion, respectively. The corresponding Commission Internationale de L'Eclairage (CIE) chromaticity coordinate for a sample of 2 mol.% Dy203 after being heat-treated at 690℃ is (0.313, 0.328). It is concluded that the formed materials may have the possibility of applications for white light-emitting diodes (LEDs).展开更多
High sensitizer and activator concentrations have been increasingly examined to improve the performance of multi-color emissive upconversion(UC)nanocrystals(UCNC)like NaYF_(4):Yb,Er and first strategies were reported ...High sensitizer and activator concentrations have been increasingly examined to improve the performance of multi-color emissive upconversion(UC)nanocrystals(UCNC)like NaYF_(4):Yb,Er and first strategies were reported to reduce concentration quenching in highly doped UCNC.UC luminescence(UCL)is,however,controlled not only by dopant concentration,yet by an interplay of different parameters including size,crystal and shell quality,and excitation power density(P).Thus,identifying optimum dopant concentrations requires systematic studies of UCNC designed to minimize additional quenching pathways and quantitative spectroscopy.Here,we quantify the dopant concentration dependence of the UCL quantum yield(ΦUC)of solid NaYF_(4):Yb,Er/NaYF_(4):Lu upconversion core/shell nanocrystals of varying Yb3+and Er3+concentrations(Yb3+series:20%‒98%Yb3+;2%Er3+;Er3+series:60%Yb3+;2%‒40%Er3+).To circumvent other luminescence quenching processes,an elaborate synthesis yielding OH-free UCNC with recordΦUC of~9%and~25 nm core particles with a thick surface shell were used.High Yb3+concentrations barely reduceΦUC from~9%(20%Yb3+)to~7%(98%Yb3+)for an Er3+concentration of 2%,thereby allowing to strongly increase the particle absorption cross section and UCNC brightness.Although an increased Er3+concentration reducesΦUC from~7%(2%Er3+)to 1%(40%)for 60%Yb3+.Nevertheless,at very high P(>1 MW/cm^(2))used for microscopic studies,highly Er3+-doped UCNC display a high brightness because of reduced saturation.These findings underline the importance of synthesis control and will pave the road to many fundamental studies of UC materials.展开更多
Transition-metal ions doped nanocrystals(NCs),specifically Mn-doped NCs,hold great potential in the field of photocatalysis,especially,to improve photocatalytic performance for singlet oxygen(1O2)generation.Here,we re...Transition-metal ions doped nanocrystals(NCs),specifically Mn-doped NCs,hold great potential in the field of photocatalysis,especially,to improve photocatalytic performance for singlet oxygen(1O2)generation.Here,we report the design of a novel Mn-doped NC-based nanocomposites,specifically,silica-coated Mn-doped CdS/ZnS NCs decorated with Pt NCs(denoted as Mn-NCs@SiO2-Pt),which enhance photocatalytic 1O2 generation.Owing to the long-lived Mn excited state(on the order of ms),the energy-transfer between Mn-NCs and molecular oxygen is facilitated with the assistance of the Pt NCs adhered to the Mn-NC@SiO2 surface.Therefore,the Mn-NCs@SiO2-Pt composites,integrate the advantages of Mn-doped NCs,a protective silica layer,and Pt NCs to exhibit excellent catalytic activity and selectivity for the selective oxidation of primary benzylic alcohols to aldehydes through an 1O2 engaged oxidation process under visible-light irradiation.This work paves the way for enhancing catalytic performance via facilitated energy transfer relaxation by utilizing the long-lived excited-state of Mn2+dopant ions in nanocomposites.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.61275180 and51472125)the K.C.Wong Magna Fund of Ningbo University
文摘Glass ceramics Ba2LaFT:xDy3+ are obtained through the conventional melt-quenching technique, and their lu- minescent properties are investigated. Under 350 nm excitation, the emission spectra consists of a strong blue- yellow band as well as a weak red emission centered at 660 nm, which are attributed to the 4F9/2 →6H15/2, 4F9/2→6H13/2 and 4F9/2 → 6Hll/2 transitions of the Dy3+ ion, respectively. The corresponding Commission Internationale de L'Eclairage (CIE) chromaticity coordinate for a sample of 2 mol.% Dy203 after being heat-treated at 690℃ is (0.313, 0.328). It is concluded that the formed materials may have the possibility of applications for white light-emitting diodes (LEDs).
基金the German Science Foundation DFG(grants RE 1203/18-1 and HA 1649/7-1)the EU(COST 1403)for financial support.
文摘High sensitizer and activator concentrations have been increasingly examined to improve the performance of multi-color emissive upconversion(UC)nanocrystals(UCNC)like NaYF_(4):Yb,Er and first strategies were reported to reduce concentration quenching in highly doped UCNC.UC luminescence(UCL)is,however,controlled not only by dopant concentration,yet by an interplay of different parameters including size,crystal and shell quality,and excitation power density(P).Thus,identifying optimum dopant concentrations requires systematic studies of UCNC designed to minimize additional quenching pathways and quantitative spectroscopy.Here,we quantify the dopant concentration dependence of the UCL quantum yield(ΦUC)of solid NaYF_(4):Yb,Er/NaYF_(4):Lu upconversion core/shell nanocrystals of varying Yb3+and Er3+concentrations(Yb3+series:20%‒98%Yb3+;2%Er3+;Er3+series:60%Yb3+;2%‒40%Er3+).To circumvent other luminescence quenching processes,an elaborate synthesis yielding OH-free UCNC with recordΦUC of~9%and~25 nm core particles with a thick surface shell were used.High Yb3+concentrations barely reduceΦUC from~9%(20%Yb3+)to~7%(98%Yb3+)for an Er3+concentration of 2%,thereby allowing to strongly increase the particle absorption cross section and UCNC brightness.Although an increased Er3+concentration reducesΦUC from~7%(2%Er3+)to 1%(40%)for 60%Yb3+.Nevertheless,at very high P(>1 MW/cm^(2))used for microscopic studies,highly Er3+-doped UCNC display a high brightness because of reduced saturation.These findings underline the importance of synthesis control and will pave the road to many fundamental studies of UC materials.
基金W.Z.acknowledges the support from the start-up grant of Syracuse University,ACS-PRF(No.59861-DNI5)NSF CHE MSN(No.05539CON04700).
文摘Transition-metal ions doped nanocrystals(NCs),specifically Mn-doped NCs,hold great potential in the field of photocatalysis,especially,to improve photocatalytic performance for singlet oxygen(1O2)generation.Here,we report the design of a novel Mn-doped NC-based nanocomposites,specifically,silica-coated Mn-doped CdS/ZnS NCs decorated with Pt NCs(denoted as Mn-NCs@SiO2-Pt),which enhance photocatalytic 1O2 generation.Owing to the long-lived Mn excited state(on the order of ms),the energy-transfer between Mn-NCs and molecular oxygen is facilitated with the assistance of the Pt NCs adhered to the Mn-NC@SiO2 surface.Therefore,the Mn-NCs@SiO2-Pt composites,integrate the advantages of Mn-doped NCs,a protective silica layer,and Pt NCs to exhibit excellent catalytic activity and selectivity for the selective oxidation of primary benzylic alcohols to aldehydes through an 1O2 engaged oxidation process under visible-light irradiation.This work paves the way for enhancing catalytic performance via facilitated energy transfer relaxation by utilizing the long-lived excited-state of Mn2+dopant ions in nanocomposites.