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
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
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
Recently, the localized surface plasmon resonance (LSPR) concept was expanded from noble metals to doped semiconductor nanocrystals (NCs). However, the strengthening of the intrinsically very weak LSPR in NCs rema...Recently, the localized surface plasmon resonance (LSPR) concept was expanded from noble metals to doped semiconductor nanocrystals (NCs). However, the strengthening of the intrinsically very weak LSPR in NCs remains a great challenge for its applications in optics, electronics and optoelectronics fields. In this work, we report on the remarkable strengthening and controllability of LSPR in ZnO through a dual-doping strategy. First, high quality In-doped ZnO (IZO) NCs with intense LSPR were synthesized by a simple single-pot method. Importantly, the LSPR can be tuned by simply adjusting the concentration of In dopant, as well as by UV light irradiation (photo-induced doping). The pattern of electricity of an IZO NC film matches the shift of LSPR independent of dopant concentration. The UV light irradiation clearly enhanced the electrical properties of the films (350 fl/sq) due to increase carrier density explained by LSPR and confirmed by X-ray photoelectron spectroscopy, The IZO NCs can be easily dispersed in various organic solvents and serve as inks for assembling uniform films via solution processes. These IZO NC ink is promising for application in next-generation solution-based field effect transistors and other optoelec- tronic devices.展开更多
Rare earth doping has been widely applied in many functional nanomaterials with desirable properties and functions,which would have a significant effect on the growth process of the materials.However,the controlling s...Rare earth doping has been widely applied in many functional nanomaterials with desirable properties and functions,which would have a significant effect on the growth process of the materials.However,the controlling strategy is limited into high concentration of lanthanide doping,which produces concentration quenching of the lanthanide ion luminescence with an increase in the Ln^(3+)concentration,resulting in lowering the fluorescence quantum yield of lanthanide ion.Herein,for the first time,we demonstrate simultaneous control of the structures and luminescence properties of BaCO_3nanocrystals via a small amount of Tb^(3+)doping strategy.In fact,Tb^(3+)would partially occupy Ba^(2+)sites,resulting in the changes to the structures of the BaCO_3nanocrystals,which is primarily determined by charge modulation,including the contributions from the surfaces of crystal nuclei and building blocks.These structurally modified nanocrystals exhibit tunable luminescence properties,thus emerging as potential candidates for photonic devices such as light-emitting diodes and color displays.展开更多
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.
基金supported by the National Key Research and Development Program of China (2016YFB0401701)the National Basic Research Program of China (2014CB931702)+5 种基金the National Natural Science Foundation of China (61604074, 51572128)the National Natural Science Foundation of China and the Research Grants Council (NSFC-RGC5151101197)the Natural Science Foundation of Jiangsu Province (BK20160827)the China Postdoctoral Science Foundation (2016M590455)the Fundamental Research Funds for the Central Universities (30915012205, 30916015106)PAPD of Jiangsu Higher Education Institutions, the Opened Fund of the State Key Laboratory on Integrated Optoelectronics (2015IOSKLKF15)
文摘Recently, the localized surface plasmon resonance (LSPR) concept was expanded from noble metals to doped semiconductor nanocrystals (NCs). However, the strengthening of the intrinsically very weak LSPR in NCs remains a great challenge for its applications in optics, electronics and optoelectronics fields. In this work, we report on the remarkable strengthening and controllability of LSPR in ZnO through a dual-doping strategy. First, high quality In-doped ZnO (IZO) NCs with intense LSPR were synthesized by a simple single-pot method. Importantly, the LSPR can be tuned by simply adjusting the concentration of In dopant, as well as by UV light irradiation (photo-induced doping). The pattern of electricity of an IZO NC film matches the shift of LSPR independent of dopant concentration. The UV light irradiation clearly enhanced the electrical properties of the films (350 fl/sq) due to increase carrier density explained by LSPR and confirmed by X-ray photoelectron spectroscopy, The IZO NCs can be easily dispersed in various organic solvents and serve as inks for assembling uniform films via solution processes. These IZO NC ink is promising for application in next-generation solution-based field effect transistors and other optoelec- tronic devices.
基金supported by the National Natural Science Foundation of China (21403189, 21371149) Natural Science Foundation of Hebei Province (B2017203198)+1 种基金China Postdoctoral Science Foundation (2014M551047)Yanshan University Doctoral Foundation (B790)
文摘Rare earth doping has been widely applied in many functional nanomaterials with desirable properties and functions,which would have a significant effect on the growth process of the materials.However,the controlling strategy is limited into high concentration of lanthanide doping,which produces concentration quenching of the lanthanide ion luminescence with an increase in the Ln^(3+)concentration,resulting in lowering the fluorescence quantum yield of lanthanide ion.Herein,for the first time,we demonstrate simultaneous control of the structures and luminescence properties of BaCO_3nanocrystals via a small amount of Tb^(3+)doping strategy.In fact,Tb^(3+)would partially occupy Ba^(2+)sites,resulting in the changes to the structures of the BaCO_3nanocrystals,which is primarily determined by charge modulation,including the contributions from the surfaces of crystal nuclei and building blocks.These structurally modified nanocrystals exhibit tunable luminescence properties,thus emerging as potential candidates for photonic devices such as light-emitting diodes and color displays.