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Compact ultrabroadband light-emitting diodes based on lanthanide-doped lead-free double perovskites

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Light(Science & Applications) 2022年第3期11卷 94-106页

作者： Shilin Jin Renfu Li Hai Huang Naizhong Jiang Jidong Lin Shaoxiong Wang Yuanhui Zheng xueyuan chen Daqin chen College of Physics and Energy Fujian Normal UniversityFujian Provincial Key Laboratory of Quantum Manipulation and New Energy MaterialsFuzhou 350117China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information Fuzhou 350116China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials and State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002China Fujian Provincial Collaborative Innovation Center for Advanced High-Field Superconducting Materials and Engineering Fuzhou 350117China Fujian Provincial Engineering Technology Research Center of Solar Energy Conversion and Energy Storage Fuzhou 350117China College of Chemistry Fuzhou UniversityFuzhou 350116China

Impurity doping is an effective approach to tuning the optoelectronic performance of host materials by imparting extrinsic electronic channels.Herein,a family of lanthanide(Ln^(3+))ions was successfully incorporated into a Bi:Cs_(2)AgInCl_(6) lead-free double-perovskite(DP)semiconductor,expanding the spectral range from visible(Vis)to near-infrared(NIR)and improving the photoluminescence quantum yield(PLQY).After multidoping with Nd,Yb,Er and Tm,Bi/Ln:Cs_(2)AgInCl_(6) yielded an ultrabroadband continuous emission spectrum with a full width at half-maximum of~365 nm originating from intrinsic self-trapped exciton recombination and abundant 4f-4f transitions of the Ln^(3+)dopants.Steady-state and transient-state spectra were used to ascertain the energy transfer and emissive processes.To avoid adverse energy interactions between the various Ln^(3+)ions in a single DP host,a heterogeneous architecture was designed to spatially confine different Ln^(3+)dopants via a“DP-in-glass composite”(DiG)structure.This bottom-up strategy endowed the prepared Ln^(3+)-doped DIG with a high PLQY of 40%(nearly three times as high as that of the multidoped DP)and superior long-term stability.Finally,a compact Vis-NIR ultrabroadband(400~2000 nm)light source was easily fabricated by coupling the DiG with a commercial UV LED chip,and this light source has promising applications in nondestructive spectroscopic analyses and multifunctional lighting.

关键词： dopant tuning double

Time-resolved luminescent nanoprobes based on lanthanide nucleotide self-assemblies for alkaline phosphatase detection

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Nano Research 2023年第8期16卷 11250-11258页

作者： Yunqin Zhang Yang Cao Yan Liu Yingjie Yang Mingmao chen Hang Gao Lushan Lin xueyuan chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China College of Biological Science and Engineering Fuzhou UniversityFuzhou 350108China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350117China Fujian College University of Chinese Academy of SciencesFuzhou 350002China

Currently,enzyme-responsive nanomaterials have shown great promise in prognosis or diagnosis of disease biomarker.However,the great obstacle for conventional enzyme-responsive nanomaterials frequently lies in autofluorescence interference,poor monodispersity,uncontrollable size and morphology,low optical stability,and biotoxicity,which fundamentally impede their practical application in biological systems.To overcome these deficiencies,we proposed a novel strategy for reliable and precise detection of an enzyme disease biomarker,alkaline phosphatase(ALP),through lanthanide(Ln^(3+))nucleotide nanoparticles(LNNPs)with extremely improved monodispersity and uniformity,which were achieved by the coordination self-assembly between ATP and Ln^(3+)inside micellar nanoreactor.Specifically,for ATP-Ce/Tb LNNPs,highly improved photoluminescence(PL)emission of Tb^(3+)can be achieved via efficient Ce^(3+)sensitization.We demonstrated that ALP could specifically cleave the phosphorus–oxygen(P–O)bonds of ATP and result in the collapse of ATP-Ce/Tb scaffold,finally leading to the PL quenching of Tb^(3+).By taking advantage of time-resolved(TR)PL technique,the fabricated ATP-Ce/Tb LNNPs presented superior selectivity and sensitivity for the ALP bioassay in complicated serum samples,thus revealing the great potential of ATP-Ce/Tb LNNPs in the areas of ALP-related disease prognosis and diagnosis.

关键词： alkaline phosphatase(ALP)-responsive micellar nanoreactor coordination self-assembly lanthanide sensitization time-resolved photoluminescence(TRPL)

Convergence Analysis of Village Collective Economy Based on a Long-Term (1978-2018) Observation of 40 Villages in the Suburbs of Beijing

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中国财政与经济研究(英文) 2023年第1期12卷 110-128,F0003页

作者： xueyuan chen Yuqing Zhou Ning Weng Beijing Rural Economy Research Center Agricultural Development Bank of China Fujian Academy of Agricultural Sciences

This paper uses the follow-up survey data of six time points between 1978 and 2018 from 40 fixed observation points in Beijing suburbs by stratified sampling,and makes a long-term observation and analysis of the convergence of village collective economy(VCE).The main findings are as follows.(1)Since the start of reform and opening-up,the gap between villages in terms of total village economic income(TVEI)and total assets of village collectives has obviously widened,and the gap between villages in terms of the number of members of VCE organizations has also widened to a certain extent.(2)There is a big gap in VCE between villages in urban-rural fringe,plain and mountainous areas,and the convergence of"space club"appears.(3)In the early stage of reform and opening up,the VCE development had the opportunity to reshuffle,but from 1998 to 2018,village development showed a trend of"goodmedium-poor"'hierarchical solidification.Therefore,it is necessary to explore a new path of cross-village joint development,especially to develop and strengthen the township-level collective economy,so as to promote farmers'common prosperity in ruralareas.

关键词： collective economy convergence regional disparity ""space club"convergence

A new class of luminescent nanoprobes based on main-group Sb^(3+) emitters

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Nano Research 2022年第1期15卷 179-185页

作者： Chunguang Zhang Meiran Zhang Wei Zheng Jiaojiao Wei Shiteng Wang Ping Huang Xingwen cheng Tao Dai Zhuo chen xueyuan chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China Fujian Science Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Inorganic luminescent nanocrystals(NCs)doped with main-group ns^(2)-metal ions have evoked tremendous interest in many technological fields owing to their superior optical properties.Herein,we report a new class of luminescent nanoprobes based on 5s2-metal Sb3+-doped CaS NCs that are excitable by using a near ultraviolet light-emitting diode.The optical properties and excited-state dynamics of Sb3+in CaS NCs are comprehensively surveyed through temperature-dependent steady-state and transient photoluminescence(PL)spectroscopies.Owing to the strong electron-phonon coupling of Sb^(3+)in CaS NCs,Sb3+ions experience a dynamic Jahn-Taller distortion on the excited state,which results in bright green PL of Sb3+with a broad emission band,a large Stokes shift,and a high PL quantum yield up to 17.3%.By taking advantage of the intense PL of Sb^(3+),we show in proof-of-concept experiments the application of biotinylated CaS:Sb^(3+)NCs as sensitive luminescent nanoprobes for biotin receptor-targeted cancer cell imaging and zebrafish imaging with a high imaging contrast.These findings provide fundamental insights into the excited-state dynamics of Sb^(3+)in CaS NCs,thus laying a foundation for future design of novel and versatile luminescent nanoprobes via main-group ns2-metal doping.

关键词： CaS Sb^(3+) photoluminescence excited-state dynamics nanoprobe bioimaging

Superiority of indocyanine green-enhanced near-infrared fluorescence-guided imaging for laparoscopic lymph node dissection in patients with early-stage endometrial cancer: A retrospective cohort study

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Laparoscopic, Endoscopic and Robotic Surgery 2023年第3期6卷 103-108页

作者： Wenzhi Xu Jianqiong Li Saihua chen Jiaren Zhang xueyuan chen Jianhua Yang Department of Obstetrics and Gynecology Sir Run Run Shaw HospitalZhejiang University School of MedicineHangzhou 310016China Key Laboratory of Reproductive Dysfunction Management of Zhejiang Province Zhejiang University School of MedicineHangzhou 310016China Department of Obstetrics and Gynecology Tiantai People's HospitalTaizhou 317200China Department of Obstetrics and Gynecology Traditional Chinese Medical Hospital of YongkangYongkang 321300China

Objective:Laparoscopic pelvic lymph node dissection(LPND),which is an effective therapy for endometrial cancer,is challenging because of the complexity of the procedure and the occurrence of postoperative complications.This study aimed to explore whether indocyanine green(ICG)-enhanced nearinfrared(NIR)fluorescence-guided LPND is superior to LPND in the context of early-stage endometrial carcinoma.Methods:In this retrospective study,we included the medical records of 190 patients with early-stage endometrioid adenocarcinoma who underwent LPND at the Department of Obstetrics and Gynecology,Sir Run Run Shaw Hospital,Zhejiang University School of Medicine between January 2019 and January 2021.Depending on whether ICG-enhanced NIR fluorescence guidance was used,the patients were assigned to the ICG group or non-ICG group.Patients were followed-up for one year after surgery.Data on demographic characteristics,pathological results,operative outcomes,and complications were collected and analyzed.Results:The baseline characteristics were comparable between the ICG group and non-ICG group,including age,BMI,pregnancy history,and preoperative hemoglobin.For surgical outcomes,the patients in ICG group had significantly lower intraoperative blood loss(50 mL vs.120 mL,p<0.001),less postoperative pelvic drainage time(4.14±1.44 d vs.5.70±1.89 d,p¼0.001),shorter duration of hospital stay(5.26±1.41 d vs.7.37±1.85 d,p¼0.003),higher number of positive pelvic lymph nodes(PLNs)(1 vs.0,p¼0.003),and more PLN-positive cases(16.0%vs.3.6%,p¼0.003)than the patients in non-ICG group.However,no significant differences were noted in blood transfusion requirement,operative time,hemoglobin level decreases,number of PLNs harvested,or the presence of lymphocysts between the two groups.Conclusion:Our study showed that ICG-enhanced NIR fluorescence-guided operation may improve the accuracy and safety of LPND.

关键词： Endometrial cancer Laparoscopic surgery Lymphadenectomy Indocyanine green Near-infrared fluorescence

Lanthanide-Doped Inorganic Nanoprobes for Luminescent Assays of Biomarkers

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Accounts of Materials Research 2023年第2期4卷 193-204页

作者： Luping Wang Siyuan Han chenliang Li Datao Tu xueyuan chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials and State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 China University of Chinese Academy of Sciences Beijing 100049 China

Tremendous progress in nanomaterial and nanotechnology has been made in recent years,which greatly contributes to the development of inorganic nanoparticles(NPs)as luminescent probes in diverse biomedical applications.In particular,these luminescent nanoprobes are widely employed for sensitive assays of biomarkers like disease markers.Generally,the luminescent bioassay technologies mainly rely on conventional molecular probes such as lanthanide(Ln3+)chelates or organic dyes,which suffer from inferior photochemical stability,low photobleaching,potential long-term toxicity,or high background noise.In contrast,Ln3+-doped NPs possess distinct physicochemical properties including better photostability,lower toxicity,and superior optical properties like long photoluminescent(PL)lifetime,narrow emission band,and tunable spectral range from the ultraviolet to the second near-infrared(NIR-II),which make them extremely ideal as luminescent nanoprobes.As such,enormous research enthusiasm has been invested in this fascinating field of Ln3+-doped luminescent nanoprobes in recent years.Accordingly,background-free luminescent bioassays with high signal-to-noise have been achieved by employing Ln3+-doped NPs on the basis of their downshifting luminescence(DSL)with a long PL lifetime,NIR-II luminescence with long-wavelength emissions,or upconverting luminescence(UCL)upon NIR excitation.However,there are still key challenges for Ln3+-doped nanoprobes owing to their low brightness and quantum yield,which restrict their biomedical applications.During the past decade,we have explored efficient approaches for the synthesis and design of highly efficient Ln3+-doped nanoprobes toward ultrasensitive luminescent bioassay of disease markers.In this Account,we summarize our most recent endeavors toward the development of inorganic Ln3+-doped NPs as sensitive nanoprobes for luminescent bioassays.First,we overview the approaches of controlled synthesis and optical manipulation to obtain highly efficient Ln3+-doped NPs with desirable optical p

关键词： properties luminescence lifetime

Unraveling the triplet excited-state dynamics of Bi^(3+)in vacancyordered double perovskite Cs_(2)SnCl_(6) nanocrystals

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Nano Research 2022年第7期15卷 6422-6429页

作者： Mengyao Jin Wei Zheng Zhongliang Gong Ping Huang Renfu Li Jin Xu Xingwen cheng Wei Zhang xueyuan chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry Fuzhou UniversityFuzhou 350116China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Luminescent metal halides doped with ns^(2-)metal ions such as 6s^(2-)metal Bi^(3+)have aroused reviving interest owing to their outstanding optical properties;however,the origin of the photoluminescence(PL)remains controversial and unclear.Herein,we report a strategy for the controlled synthesis of Bi^(3+)-doped vacancy-ordered double perovskite Cs_(2)SnCl_(6)nanocrystals(NCs)and unravel the triplet excited-state dynamics of Bi^(3+)through temperature-dependent PL and ultrafast femtosecond transient absorption spectroscopies.Owing to the aliovalent Bi^(3+)doping in the spatially confined zero-dimensional(0D)structure of Cs2SnCl6,Bi^(3+)ions experience an enhancive Jahn-Teller distortion in the excited state,which results in intense broadband blue PL originating from the inter-configurational 3P0,1→1S0 transitions of Bi^(3+)at 450 nm,with a large Stokes shift and a quantum yield of 35.2%.Specifically,an unusual thermal-enhanced Jahn-Teller splitting of the excitation band and a remarkable transition of the PL lifetime from ms at 10 K toμs at 300 K were observed,as solid evidence for the isolated Bi^(3+)emission.These findings clarify the controversy about the PL origin in ns^(2-)metal ion-doped lead-free luminescent metal halides,thereby paving the way for exploring their optoelectronic applications.

关键词： bismuth luminescent nanocrystals metal halide excited-state dynamics electron-phonon coupling

Modulator-directed assembly of hybrid composites based on metalorganic frameworks and upconversion nanoparticles

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Nano Research 2023年第1期16卷 1482-1490页

作者： Yanhui Feng Xingjun Li Shan Lu Renfu Li Zhongliang Gong Xiaoying Shang Yifan Pei Wei Zheng Datao Tu xueyuan chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of chemistry Fuzhou universityFuzhou 350108China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350117China

Hybrid composites made of metal-organic frameworks(MOFs)and lanthanide-doped upconversion nanoparticles(UCNPs)have attracted considerable interest for their synergistically enhanced functions in various applications such as chemical sensing,photocatalysis,anticounterfeiting and nanomedicine.However,precise assembly of MOF/UCNP hybrid composites with tunable morphologies remains a challenge due to the lack of effective synthetic methods and fundamental understanding of the growth mechanisms.Herein,we propose a modulator-directed assembly strategy to synthesize a series of ZIF-8@UCNP composites(ZIF-8=zeolitic imidazolate framework-8).The UCNPs densely paved on the surface of ZIF-8 microcrystals and endowed the composites with intense upconversion blue emission,which were verified by steady-state/transient photoluminescence(PL)spectroscopy and single-particle imaging.Ethylenediamine(EDA)was firstly used as a modulator to fine-tune the predominant MOF facets and realized distinct morphologies of the composites.By adjusting the concentration of EDA from 0 to 25 mmol/L,the morphology of the ZIF-8@UCNP composites was tuned from rhombic dodecahedron(RD)to truncated rhombic dodecahedron(TRD),cube with truncated edges(CTE),cube,and finally a unique form of interpenetration twins(IT).The nucleation and growth process of the ZIF-8@UCNP composites was monitored by time-dependent scanning electron microscopy(SEM)images and the formation mechanism was thoroughly revealed.Furthermore,we demonstrated that the strategy for assembly of morphology-controllable ZIF-8@UCNP composites was generally applicable to various UCNPs with different sizes and shapes.The proposed strategy is expected to open up new avenues for the controllable synthesis of MOF/UCNP composites toward diverse applications.

关键词： metal-organic frameworks upconversion nanoparticles hybrid composites ethylenediamine modulator

A sandwiched luminescent heterostructure based on lanthanide-doped Gd_(2)O_(2)S@NaYF_(4)core/shell nanocrystals

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Aggregate 2023年第6期4卷 163-171页

作者： Dengfeng Yang Wei Zheng Ping Huang Meiran Zhang Wei Zhang Zhiqing Shao Wen Zhang Xiaodong Yi xueyuan chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouChina Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China FuzhouChina Fujian College University of Chinese Academy of SciencesFuzhouChina College of Chemistry Fuzhou UniversityFuzhouChina

Lanthanide(Ln^(3+))oxysulfide nanocrystals(NCs)have great prospect in many advanced technologies;however,they suffer from a low photoluminescence efficiency due to the volatility of sulfur and deleterious surface quenching effect.Herein,we report a novel sandwiched luminescent heterostructure based on Ln^(3+)-doped Gd_(2)O_(2)S@NaYF_(4)core/shell NCs with tunable sulfur content in the sandwich layer.By means of Eu^(3+)as the sensitive structural probes,we unravel the ligand-mediated structure control of the NCs from Gd_(2)O_(3):Ln^(3+)@NaYF_(4)to Gd_(2)O_(2)S:Ln^(3+)@NaYF_(4)with tailored S2–deficiency.Such a sandwich-type core/shell heterostructure enables us to achieve efficient and multicolor downshifting and upconversion luminescence(UCL),with up to 208.8 folds of enhancement in UCL intensity as compared to that of their core-only counterparts.These findings provide a general approach for the controlled synthesis of lanthanide oxysulfide@fluoride heterostructure,which offers a new way for the materials design towards diverse emerging applications.

关键词： Gd_(2)O_(2)S heterostructure lanthanide NaYF_(4) upconversion luminescence