Organic light-emitting diodes （OLEDs） have been extensively studied since the first efficient device based on small molecular luminescent materials was reported by Tang. Organic electroluminescent material, one of t...Organic light-emitting diodes （OLEDs） have been extensively studied since the first efficient device based on small molecular luminescent materials was reported by Tang. Organic electroluminescent material, one of the centerpieces of OLEDs, has been the focus of studies by many material scientists. To obtain high luminosity and to keep material costs low, a few remarkable design concepts have been developed. Aggregation-induced emission （AIE） materials were invented to overcome the common fluorescence-quenching problem, and cross-dipole stacking of fluorescent molecules was shown to be an effective method to get high solid-state luminescence. To exceed the limit of internal quantum efficiency of conventional fluorescent materials, phosphorescent materials were successfully applied in highly efficient electroluminescent devices. Most recently, delayed flu- orescent materials via reverse-intersystem crossing （RISC） from triplet to singlet and the ＂hot exciton＂ materials based on hy- bridized local and charge-transfer （HLCT） states were developed to he a new generation of low-cost luminescent materials as efficient as phosphorescent materials. In terms of the device-fabrication process, solution-processible small molecular lumi- nescent materials possess the advantages of high purity （vs. polymers） and low procession cost （vs. vacuum deposition）, which are garnering them increasing attention. Herein, we review the progress of the development of small-molecule luminescent materials with different design concepts and features, and also briefly examine future development tendencies of luminescent materials.展开更多
Organic afterglow materials are highly desirable for optoelectronic applications,but they usually suffer from complex preparation process,low quantum efficiency,and short lifetime due to the ultrafast deactivation of ...Organic afterglow materials are highly desirable for optoelectronic applications,but they usually suffer from complex preparation process,low quantum efficiency,and short lifetime due to the ultrafast deactivation of the highly active excited states involved.Here,we succeeded in achieving solventfree thermal syntheses of high-efficiency afterglow CDs@zeolite composite materials by simply grinding the solid raw materials of zeolite and precursor CDs at room temperature,followed by thermal crystallization.This method afforded maximum embedding of CDs into growing zeolite crystals,as well as strong host–guest interaction to surpass the nonradiative transition of CDs,thus producing composite materials with ultralong dual emission of thermally activated delayed fluorescence and room temperature phosphorescence with a record high lifetime of 1.7 and 2.1 s,respectively,and the quantum yield of 90.7%.Furthermore,in a preliminary experiment,we applied the composite materials in alternatingcurrent light-emitting diode supplementary lighting,which exhibited a promising potential in optoelectronic applications.展开更多
A purely organic D-π-A-π-D type emitter showing thermally activated delayed fluorescence(TADF)and room temperature phosphorescence(RTP)was designed and synthesized by utilizing the benzophenone as an acceptor and th...A purely organic D-π-A-π-D type emitter showing thermally activated delayed fluorescence(TADF)and room temperature phosphorescence(RTP)was designed and synthesized by utilizing the benzophenone as an acceptor and the N-phenyl-2-napthylamine as a donor moiety.It exhibits considerable TADF character in doped PMMA film and room temperature phosphorescence with a long lifetime of 74 ms at466 nm in solid state.The devices with the configuration of ITO/Mo_(2) O_(3)(4 nm)/mCP(30 nm)/mCP:x wt%NP2 BP/TmTyPB(60 nm)/LiF(1.5 nm)/AI(100 nm)were prepared by vacuum evaporation to explore their electroluminescent performance.Intere stingly,the non-doped device has obtained near-white emission with a fluorescence emission peak at 475 nm and a phosphore scence emission peak at 563 nm having the CIE coordinate of(0.23,0.32)and the maximum external quantum efficiency of 1.09%.展开更多
Nano Research volume 13,pages1614–1619(2020)Cite this article 236 Accesses Metrics details Abstract Optical silicon(Si)-based materials are highly attractive due to their widespread applications ranging from electron...Nano Research volume 13,pages1614–1619(2020)Cite this article 236 Accesses Metrics details Abstract Optical silicon(Si)-based materials are highly attractive due to their widespread applications ranging from electronics to biomedicine.It is worth noting that while extensive efforts have been devoted to developing fluorescent Si-based structures,there currently exist no examples of Si-based materials featuring phosphorescence emission,severely limiting Si-based wide-ranging optical applications.To address this critical issue,we herein introduce a kind of Si-based material,in which metal-organic frameworks(MOFs)are in-situ growing on the surface of Si nanoparticles(SiNPs)assisted by microwave irradiation.Of particular significance,the resultant materials,i.e.,MOFs-encapsulated SiNPs(MOFs@SiNPs)could exhibit pH-responsive fluorescence,whose maximum emission wavelength is red-shifted from 442 to 592 nm when the pH increases from 2 to 13.More importantly,distinct room-temperature phosphorescence(maximum emission wavelength:505 nm)could be observed in this system,with long lifetime of 215 ms.Taking advantages of above-mentioned unique optical properties,the MOFs@SiNPs are further employed as high-quality anti-counterfeiting inks for advanced encryption.In comparison to conventional fluorescence anti-counterfeiting techniques(static fluorescence outputs are generally used,thus being easily duplicated and leading to counterfeiting risk),pH-responsive fluorescence and room-temperature phosphorescence of the resultant MOFs@SiNPs-based ink could offer advanced multi-modal security,which is therefore capable of realizing higher-level information security against counterfeiting.展开更多
Aggregation-induced thermally activated delayed fluorescence(TADF)phenomena have attracted extensive attention recently.In this paper,several theoretical models including monomer,dimer,and complex are used for the exp...Aggregation-induced thermally activated delayed fluorescence(TADF)phenomena have attracted extensive attention recently.In this paper,several theoretical models including monomer,dimer,and complex are used for the explanation of the luminescent properties of(R)-5-(9H-carbazol-9-yl)-2-(1,2,3,4-tetrahydronaphthalen-1-yl)isoindoline-1,3-dione((R)-ImNCz),which was recently reported[Chemical Engineering Journal 418129167(2021)].The polarizable continuum model(PCM)and the combined quantum mechanics and molecular mechanics(QM/MM)method are adopted in simulation of the property of the molecule in the gas phase,solvated in acetonitrile and in aggregation states.It is found that large spin–orbit coupling(SOC)constants and a smaller energy gap between the first singlet excited state and the first triplet excited state(△E_(st))in prism-like single crystals(SC_(p)-form)are responsible for the TADF of(R)-lmNCz,while no TADF is found in block-like single crystals(SC_(b)-form)with a larger △E_(st).The multiple ultralong phosphorescence(UOP)peaks in the spectrum are of complex origins,and they are related not only to ImNCz but also to a minor amount of impurities(ImNBd)in the crystal prepared in the laboratory.The dimer has similar phosphorescence emission wavelengths to the(R)-lmNCz-SC_(p) monomers.The complex composed of(R)-lmNCz and(R)-lmNBd contributes to the phosphorescent emission peak at about 600 nm,and the phosphorescent emission peak at about 650 nm is generated by(R)-lmNBd.This indicates that the impurity could also contribute to emission in molecular crystals.The present calculations clarify the relationship between the molecular aggregation and the light-emitting properties of the TADF emitters and will therefore be helpful for the design of potentially more useful TADF emitters.展开更多
The control of excited states and related emissive properties of gold(Ⅲ)complexes mainly depends on the modulation of intramolecular electronic interactions among gold(Ⅲ)metal center,chelating ligands and/or periphe...The control of excited states and related emissive properties of gold(Ⅲ)complexes mainly depends on the modulation of intramolecular electronic interactions among gold(Ⅲ)metal center,chelating ligands and/or peripheral groups.However,luminescent gold(Ⅲ)systems based on intermolecular electronic interactions have never been explored.Here we report a series of proof-of-concept gold(Ⅲ)exciplexes using a simple gold(Ⅲ)complex,AuDPPy,as an electron acceptor.The emissive properties of gold(Ⅲ)exciplexes can be regulated by combining AuDPPy with different donors.Inspiringly,these gold(Ⅲ)exciplexes have donor-dependent emission mechanisms:dominant phosphorescence or dual radiative channels of thermally activated delayed fluorescence(TADF)and phosphorescence.Consequently,these gold(Ⅲ)exciplexes deliver green-to-red electroluminescence with external quantum efficiencies(EQEs)of up to 10.1%.More importantly,using these gold(Ⅲ)exciplexes to host multi-resonance TADF emitters results in narrowband yellow,orange,and deep-red electroluminescence with high EQEs of 23.5%,24.4%,and 27.4%,respectively,competitive to the highest values for gold(Ⅲ)OLEDs in similar color gamut.展开更多
Benefiting from the large Stokes shift between fluorescence and phosphorescence,fluorescence/phosphorescence dual-emitting carbon dots(CDs)have gradually entered at the stage of single-phase white light-emitting diode...Benefiting from the large Stokes shift between fluorescence and phosphorescence,fluorescence/phosphorescence dual-emitting carbon dots(CDs)have gradually entered at the stage of single-phase white light-emitting diodes(WLEDs)as‘green material'.However,most of the developed dual-emitting CDs have weak phosphorescence,short emission wavelength and narrow emission band,resulting in relatively bluish white light emission and low color rendering index(CRI).Herein,an ultrabroad-band fluorescence/phosphorescence dual-emitting CD-based material(UB-CD@BA)is prepared by thermal treatment of boric acid(BA)and CDs with large conjugated structure.The stable covalent bonding between CDs and BA,as well as three-dimensional spatial restriction effect of selfpolymerization BA molecules around CDs during long-term heating efficiently rigidified the single/triplet excited states of CDs from non-radiative deactivation,thus producing strong dual emissive materials with the high phosphorescence quantum yield of 21%.Remarkable,the prepared UB-CD@BA powders exhibit bright pure white light emission with Commission Internationale de l'Eclairage(CIE)coordinates of(0.32,0.33)and the highest reported full width at half maximum of 250 nm.Based on the unique characteristics of UB-CD@BA,it was used as a color conversion layer to prepare a WLED with CIE coordinates of(0.35,0.33)and the CRI value of 87.展开更多
基金supported by the National Natural Science Foundation of China(21334002,51303057,51373054,91233113)the National Basic Research Program of China(2013CB834705,2014CB643504,2015CB655003)+1 种基金the Fundamental Research Funds for the Central Universities(2013ZZ0001)the Introduced Innovative R&D Team of Guangdong(201101C0105067115)
文摘Organic light-emitting diodes （OLEDs） have been extensively studied since the first efficient device based on small molecular luminescent materials was reported by Tang. Organic electroluminescent material, one of the centerpieces of OLEDs, has been the focus of studies by many material scientists. To obtain high luminosity and to keep material costs low, a few remarkable design concepts have been developed. Aggregation-induced emission （AIE） materials were invented to overcome the common fluorescence-quenching problem, and cross-dipole stacking of fluorescent molecules was shown to be an effective method to get high solid-state luminescence. To exceed the limit of internal quantum efficiency of conventional fluorescent materials, phosphorescent materials were successfully applied in highly efficient electroluminescent devices. Most recently, delayed flu- orescent materials via reverse-intersystem crossing （RISC） from triplet to singlet and the ＂hot exciton＂ materials based on hy- bridized local and charge-transfer （HLCT） states were developed to he a new generation of low-cost luminescent materials as efficient as phosphorescent materials. In terms of the device-fabrication process, solution-processible small molecular lumi- nescent materials possess the advantages of high purity （vs. polymers） and low procession cost （vs. vacuum deposition）, which are garnering them increasing attention. Herein, we review the progress of the development of small-molecule luminescent materials with different design concepts and features, and also briefly examine future development tendencies of luminescent materials.
基金Foundation of China(grant nos.21621001,21920102005,21835002,and 21671075)the 111 Project of China(B17020)the financial supports.
文摘Organic afterglow materials are highly desirable for optoelectronic applications,but they usually suffer from complex preparation process,low quantum efficiency,and short lifetime due to the ultrafast deactivation of the highly active excited states involved.Here,we succeeded in achieving solventfree thermal syntheses of high-efficiency afterglow CDs@zeolite composite materials by simply grinding the solid raw materials of zeolite and precursor CDs at room temperature,followed by thermal crystallization.This method afforded maximum embedding of CDs into growing zeolite crystals,as well as strong host–guest interaction to surpass the nonradiative transition of CDs,thus producing composite materials with ultralong dual emission of thermally activated delayed fluorescence and room temperature phosphorescence with a record high lifetime of 1.7 and 2.1 s,respectively,and the quantum yield of 90.7%.Furthermore,in a preliminary experiment,we applied the composite materials in alternatingcurrent light-emitting diode supplementary lighting,which exhibited a promising potential in optoelectronic applications.
基金absolutely supported by Program for National Natural Scientific Foundation of China(Nos.91833304,61904120,61775155,61705158)Natural Science Foundation of Shanxi Province(Nos.201901D211090,201903D121100,201801D221124)+1 种基金the Fundamental Research Funds for the Central Universities,Shanxi Provincial Key Innovative Research Team in Science and Technology(No.201601D021043)the Joint Research Funds of Department of Science&Technology of Shaanxi Province and Northwestern Polytechnical University(No.2020GXLH-Z-006)。
文摘A purely organic D-π-A-π-D type emitter showing thermally activated delayed fluorescence(TADF)and room temperature phosphorescence(RTP)was designed and synthesized by utilizing the benzophenone as an acceptor and the N-phenyl-2-napthylamine as a donor moiety.It exhibits considerable TADF character in doped PMMA film and room temperature phosphorescence with a long lifetime of 74 ms at466 nm in solid state.The devices with the configuration of ITO/Mo_(2) O_(3)(4 nm)/mCP(30 nm)/mCP:x wt%NP2 BP/TmTyPB(60 nm)/LiF(1.5 nm)/AI(100 nm)were prepared by vacuum evaporation to explore their electroluminescent performance.Intere stingly,the non-doped device has obtained near-white emission with a fluorescence emission peak at 475 nm and a phosphore scence emission peak at 563 nm having the CIE coordinate of(0.23,0.32)and the maximum external quantum efficiency of 1.09%.
基金We appreciate financial support from the National Natural Science Foundation of China(Nos.21825402,31400860,21575096,and 21605109)the Natural Science Foundation of Jiangsu Province of China(Nos.BK20191417 and BK20170061)the Program for Jiangsu Specially-Appointed Professors to Prof.Yao He,a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD),111 Project as well as Collaborative Innovation Center of Suzhou Nano Science and Technology(NANO-CIC).
文摘Nano Research volume 13,pages1614–1619(2020)Cite this article 236 Accesses Metrics details Abstract Optical silicon(Si)-based materials are highly attractive due to their widespread applications ranging from electronics to biomedicine.It is worth noting that while extensive efforts have been devoted to developing fluorescent Si-based structures,there currently exist no examples of Si-based materials featuring phosphorescence emission,severely limiting Si-based wide-ranging optical applications.To address this critical issue,we herein introduce a kind of Si-based material,in which metal-organic frameworks(MOFs)are in-situ growing on the surface of Si nanoparticles(SiNPs)assisted by microwave irradiation.Of particular significance,the resultant materials,i.e.,MOFs-encapsulated SiNPs(MOFs@SiNPs)could exhibit pH-responsive fluorescence,whose maximum emission wavelength is red-shifted from 442 to 592 nm when the pH increases from 2 to 13.More importantly,distinct room-temperature phosphorescence(maximum emission wavelength:505 nm)could be observed in this system,with long lifetime of 215 ms.Taking advantages of above-mentioned unique optical properties,the MOFs@SiNPs are further employed as high-quality anti-counterfeiting inks for advanced encryption.In comparison to conventional fluorescence anti-counterfeiting techniques(static fluorescence outputs are generally used,thus being easily duplicated and leading to counterfeiting risk),pH-responsive fluorescence and room-temperature phosphorescence of the resultant MOFs@SiNPs-based ink could offer advanced multi-modal security,which is therefore capable of realizing higher-level information security against counterfeiting.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11974216,11874242,21933002 and 11904210)Shandong Provincial Natural Science Foundation,China(Grant No.ZR2019MA056)+1 种基金the support of the Taishan Scholar Project of Shandong Provincethe project funded by China Postdoctoral Science Foundation(Grant No.2018M642689)。
文摘Aggregation-induced thermally activated delayed fluorescence(TADF)phenomena have attracted extensive attention recently.In this paper,several theoretical models including monomer,dimer,and complex are used for the explanation of the luminescent properties of(R)-5-(9H-carbazol-9-yl)-2-(1,2,3,4-tetrahydronaphthalen-1-yl)isoindoline-1,3-dione((R)-ImNCz),which was recently reported[Chemical Engineering Journal 418129167(2021)].The polarizable continuum model(PCM)and the combined quantum mechanics and molecular mechanics(QM/MM)method are adopted in simulation of the property of the molecule in the gas phase,solvated in acetonitrile and in aggregation states.It is found that large spin–orbit coupling(SOC)constants and a smaller energy gap between the first singlet excited state and the first triplet excited state(△E_(st))in prism-like single crystals(SC_(p)-form)are responsible for the TADF of(R)-lmNCz,while no TADF is found in block-like single crystals(SC_(b)-form)with a larger △E_(st).The multiple ultralong phosphorescence(UOP)peaks in the spectrum are of complex origins,and they are related not only to ImNCz but also to a minor amount of impurities(ImNBd)in the crystal prepared in the laboratory.The dimer has similar phosphorescence emission wavelengths to the(R)-lmNCz-SC_(p) monomers.The complex composed of(R)-lmNCz and(R)-lmNBd contributes to the phosphorescent emission peak at about 600 nm,and the phosphorescent emission peak at about 650 nm is generated by(R)-lmNBd.This indicates that the impurity could also contribute to emission in molecular crystals.The present calculations clarify the relationship between the molecular aggregation and the light-emitting properties of the TADF emitters and will therefore be helpful for the design of potentially more useful TADF emitters.
基金supported by the National Natural Science Foundation of China(52022071,52130308)Shenzhen Fundamental Research Program(JCYJ20190808151209557,ZDSYS20210623091813040)。
文摘The control of excited states and related emissive properties of gold(Ⅲ)complexes mainly depends on the modulation of intramolecular electronic interactions among gold(Ⅲ)metal center,chelating ligands and/or peripheral groups.However,luminescent gold(Ⅲ)systems based on intermolecular electronic interactions have never been explored.Here we report a series of proof-of-concept gold(Ⅲ)exciplexes using a simple gold(Ⅲ)complex,AuDPPy,as an electron acceptor.The emissive properties of gold(Ⅲ)exciplexes can be regulated by combining AuDPPy with different donors.Inspiringly,these gold(Ⅲ)exciplexes have donor-dependent emission mechanisms:dominant phosphorescence or dual radiative channels of thermally activated delayed fluorescence(TADF)and phosphorescence.Consequently,these gold(Ⅲ)exciplexes deliver green-to-red electroluminescence with external quantum efficiencies(EQEs)of up to 10.1%.More importantly,using these gold(Ⅲ)exciplexes to host multi-resonance TADF emitters results in narrowband yellow,orange,and deep-red electroluminescence with high EQEs of 23.5%,24.4%,and 27.4%,respectively,competitive to the highest values for gold(Ⅲ)OLEDs in similar color gamut.
基金the support from the National Natural Science Foundation of China(Nos.52002152 and 62005106)the Natural Science Foundation of Jiangsu Province(Nos.BK20190864 and BK20190865)the Primary Research&Development Plan of Zhenjiang-Modern Agriculture(No.NY2021007)。
文摘Benefiting from the large Stokes shift between fluorescence and phosphorescence,fluorescence/phosphorescence dual-emitting carbon dots(CDs)have gradually entered at the stage of single-phase white light-emitting diodes(WLEDs)as‘green material'.However,most of the developed dual-emitting CDs have weak phosphorescence,short emission wavelength and narrow emission band,resulting in relatively bluish white light emission and low color rendering index(CRI).Herein,an ultrabroad-band fluorescence/phosphorescence dual-emitting CD-based material(UB-CD@BA)is prepared by thermal treatment of boric acid(BA)and CDs with large conjugated structure.The stable covalent bonding between CDs and BA,as well as three-dimensional spatial restriction effect of selfpolymerization BA molecules around CDs during long-term heating efficiently rigidified the single/triplet excited states of CDs from non-radiative deactivation,thus producing strong dual emissive materials with the high phosphorescence quantum yield of 21%.Remarkable,the prepared UB-CD@BA powders exhibit bright pure white light emission with Commission Internationale de l'Eclairage(CIE)coordinates of(0.32,0.33)and the highest reported full width at half maximum of 250 nm.Based on the unique characteristics of UB-CD@BA,it was used as a color conversion layer to prepare a WLED with CIE coordinates of(0.35,0.33)and the CRI value of 87.
