Persistent luminescence is a unique optical phenomenon that continues to emit light for minutes or even hours after the excitation stops,which can significantly enhance the sensitivity and signal-to-noise ratio of ima...Persistent luminescence is a unique optical phenomenon that continues to emit light for minutes or even hours after the excitation stops,which can significantly enhance the sensitivity and signal-to-noise ratio of imaging[1].Among numerous persistent luminescence materials,lanthanide-doped fluoride nanoparticles have shown tunable persistent luminescence across the UV-vis-NIR spectrum(200-1700 nm)under X-ray excitation and adjustable size,promising significant applications in deep-tissue imaging[2,3],security encryption,and data storage[4].In particular,those exhibiting NIR-II luminescence(1000-1700 nm)provide key advantages such as deeper tissue penetration,higher contrast,and minimal interference from biological autofluorescence.However,challenges such as low brightness and rapid signal decay,especially in the NIR-II region,limit their effectiveness in long-term monitoring,including tumor theranostics[5].Traditional approaches like size control and surface passivation yield only marginal improvements,underscoring the need for next-generation nanoparticles with superior NIR-II brightness.展开更多
The dysbiosis of oral microbiota contributes to diseases such as periodontitis and certain cancers by triggering the host inflammatory response.Developing methods for the immediate and sensitive identification of oral...The dysbiosis of oral microbiota contributes to diseases such as periodontitis and certain cancers by triggering the host inflammatory response.Developing methods for the immediate and sensitive identification of oral microorganism is crucial for the rapid diagnosis and early interventions of associated diseases.Traditional methods for microbial detection primarily include the plate culturing,polymerase chain reaction and enzyme-linked immunosorbent assay,which are either time-consuming or laborious.Herein,we reported a persistent luminescence-encoded multiple-channel optical sensing array and achieved the rapid and accurate identification of oral-derived microorganisms.Our results demonstrate that electrostatic attractions and hydrophobic-hydrophobic interactions dominate the binding of the persistent luminescent nanoprobes to oral microorganisms and the microbial identification process can be finished within 30 min.Specifically,a total of 7 oral-derived microorganisms demonstrate their own response patterns and were differentiated by linear discriminant analysis(LDA)with the accuracy up to 100%both in the solution and artificial saliva samples.Moreover,the persistent luminescence encoded array sensor could also discern the microorganism mixtures with the accuracy up to 100%.The proposed persistent luminescence encoding sensor arrays in this work might offer new ideas for rapid and accurate oralderived microorganism detection,and provide new ways for disease diagnosis associated with microbial metabolism.展开更多
The electronic structure of the strontium aluminate （SrAl2O4：Eu^2＋） materials was studied with a combined experimental and theo- retical approach. The UV-VUV synchrotron radiation was applied in the experimental s...The electronic structure of the strontium aluminate （SrAl2O4：Eu^2＋） materials was studied with a combined experimental and theo- retical approach. The UV-VUV synchrotron radiation was applied in the experimental study while the electronic structure of the non-optimized and optimized crystal structure were investigated theoretically by using the density functional theory. The structure of the valence and conduction bands as well as the band gap energy of the material together with the position of the Eu2＋ 4f7 85712 ground state were calculated. The calculated band gap energy （6.4 eV） agreed well with the experimental value of 6.6 eV. The valence band consisted mainly of oxygen states whereas the bottom of the conduction band of strontium states. In agreement with the experimental results, the calculated 4f7 8S7r2 ground state of Eu2＋ lies in the energy gap of the host. The position of the 4f7 ground state depended on the Coulomb repulsion strength. The position of the 4f7 ground state with respect to the valence and conduction bands was discussed using theoretical and experimental evidence available.展开更多
Persistent luminescence nanoparticles(PLNPs)are a kind of phosphors that can remain luminescent for seconds to several days after the stoppage of excitation.Lanthanides show the special capability to largely broaden t...Persistent luminescence nanoparticles(PLNPs)are a kind of phosphors that can remain luminescent for seconds to several days after the stoppage of excitation.Lanthanides show the special capability to largely broaden the emission range and enhance the luminescence intensity of PLNPs due to their dense energy structure and unique electronic configurations.In the past decades,various methods have been developed for the synthesis of lanthanide-based PLNPs with excellent pe rsistent luminescence propertie s,and the lanthanide-based PLNPs are widely studied in areas including biome dicine,energy,and information storage.In this review,we summarized the research progress in the synthe sis of lanthanidebased PLNPs and outline d several typical synthesis methods.We discussed the fundamental concepts of preparation methods as well as the advantages and drawbacks of the typical synthetic approache s.Moreove r,the current challenges and the potential solutions for the development of lanthanide-based PLNP s are also discussed in an attempt to provide strate gies to further improve the optical properties of lanthanide-based PLNPs.We hope this review can contribute to the design of lanthanide-based PLNPs with desired properties and further promote their applications in biomedicine,energy,and information science.展开更多
The electronic and defect energy level structure of polyerystalline Sr2MgSi2OT：Eu^2＋,R^3＋ persistent luminescence materials were studied with thermoluminescence and different synchrotron radiation spectroscopies （...The electronic and defect energy level structure of polyerystalline Sr2MgSi2OT：Eu^2＋,R^3＋ persistent luminescence materials were studied with thermoluminescence and different synchrotron radiation spectroscopies （UV-VUV emission and excitation, X-ray absorption near-edge spectroscopy （XANES） and extended X-ray absorption f＇me structure （EXAFS））. Special attention was paid on the effect of the R3＋ co-dopants on the persistent luminescence properties of the materials. Theoretical calculations using the density functional theory （DFT） were carried out simultaneously with the experimental work. The experimental band gap energy （Eg） value of ca. 7.1 eV agreed very well with the DFT value of 6.7 eV. The variation of the Eg value was attempted to relate with the trap structure as well as with the different properties of the R3＋ co-dopants. The trap level energy distribution depended strongly on the R3＋ co-dopant except for the shallowest trap energy above the room temperature remaining practically the same, however. The different processes in the mechanism of persistent luminescence from Sr2MgSi2OT：Eu^2＋,R^3＋ were assembled and their contributions discussed.展开更多
The near-infrared(NIR)persistent luminescence materials(PLMs)can remain long-lasting luminescence after removal of the excitation light,which permits bioimaging with high sensitivity owing to the absence of background...The near-infrared(NIR)persistent luminescence materials(PLMs)can remain long-lasting luminescence after removal of the excitation light,which permits bioimaging with high sensitivity owing to the absence of background fluorescence interference from in situ excitation.Recently,the NIR PLMs have aroused intensive research interest in bioimaging.However,the optimal excitation wavelength of current NIR PLMs is located in the ultraviolet region with shallow tissue penetration,making it difficult to activate effectively in vivo,and seriously hindering their further application in bioimaging.Herein,we report a novel kind of Cr^(3+)ions and Y^(3+)ions co-doped NIR PLM,Zn_(1.3)Ga_(1.4)Sn_(0.3)O_(4):Cr^(3+),Y^(3+)(ZGSCY),which emits NIR persistent luminescence at 696 nm.Compared with Zn_(1.3)Ga_(1.4)Sn_(0.3)O_(4):Cr^(3+)(ZGSC)excited by the light with a wavelength in the biological window(>650 nm),after being co-doped with Y^(3+)ions,the NIR persistent luminescence performance of ZGSCY is significantly improved because of the increase of trap concentration in the matrix.In addition,we synthesized ZGSCY nanoparticles(NPs)by the combustion method,which exhibit excellent optical properties after being excited by the light with a wavelength in the biological window.After surface modification with PEG,the ZGSCY NPs present low cytotoxicity.Notably,due to the co-doping of Y^(3+)ions,the signal-to-noise ratio(SNR)of ZGSCY NPs in vivo imaging is about 1.8 times higher than that of the ZGSC NPs.Furthermore,the rechargeable in vivo imaging and passive tumor-targeted imaging are successfully achieved by activating with a lightemitting diode(LED,659 nm)after intravenous injection of ZGSCY.Thus,this kind of NIR PLM with high excitation efficiency performance in the biological window is expected to promote its biomedical application in deep tissues.展开更多
X-ray-activated luminescence materials have broad application prospects in photodynamic therapy of deep tissue.Among them,X-ray-activated persistent luminescence materials(PLMs)exhibiting multiple emission peaks have ...X-ray-activated luminescence materials have broad application prospects in photodynamic therapy of deep tissue.Among them,X-ray-activated persistent luminescence materials(PLMs)exhibiting multiple emission peaks have drawn extensive attention for the ir capacity to achieve a combination of bioimaging and therapeutic functions.Here,we developed a novel PLM,LiYGeO_4:Bi^(3+),Pr^(3+),that simultaneously exhibits UV and NIR dual persistent luminescence(PersL)emissions after irradiation by X-ray.The material can be re peatedly excited by X-ray and emits similar lumine scence intensity every time,which shows good PersL stability.In addition,LiYGeO_4:Bi^(3+),Pr^(3+)exhibits photostimulated PersL properties by stimulation with a red light-emitting diode(LED)or NIR laser after long-term decay.This work provides a new choice of X-ray-excited PLMs with UV and NIR dual emission and the novel phosphor shows promise as a potential candidate for the integration of treatment and diagnosis of deep tumors.展开更多
In recent years,persistent luminescence materials(PLMs)excited by X-rays and emitting in biological windows have received extensive attention in the field of high-sensitivity bioimaging.Transition metal Mn^(2+)is an i...In recent years,persistent luminescence materials(PLMs)excited by X-rays and emitting in biological windows have received extensive attention in the field of high-sensitivity bioimaging.Transition metal Mn^(2+)is an ideal emission center,but few studies focus on Mn^(2+)-doped PLMs with X-ray excitation and biological window emission.Here,we report a Mn^(2+)-doped PLM,LiYGeO_(4):Mn^(2+)(LYGM),with excellent biological window persistent luminescence emission.After excitation by UV,LYGM produces a durable biological window of persistent luminescence emission at 660 nm for up to 20 h.More importantly.LYGM can be repeatedly excited by X-rays,resulting in long-term biological window persistent luminescence emission.In addition,we obtain LYGM around 200 nm in diameter by ball milling and centrifugation and improve its biocompatibility by surface modification to apply it to in vivo imaging in mice.After LYGM are injected into mice through the tail vein,in situ excitation of X-rays can be achieved.After the persistent luminescence decays,LYGM can be re-excited for repeated imaging.Therefore,LYGM shows potential prospects for in vivo deep tissue and long-term bioimaging.展开更多
Here, we report the direct hydrothermal synthesis of 1 D-based Zn2GeO4：Mn2＋ persistent luminescent nanobelts （ZGO：Mn PLNBs）. The ZGO：Mn PLNBs exhibit rapid growth rate, and nanobelts can be obtained after 30 rai...Here, we report the direct hydrothermal synthesis of 1 D-based Zn2GeO4：Mn2＋ persistent luminescent nanobelts （ZGO：Mn PLNBs）. The ZGO：Mn PLNBs exhibit rapid growth rate, and nanobelts can be obtained after 30 rain of hydrothermal treatment. The persistent luminescence performance can be fine-turned upon prolonging the hydrothermal time. Furthermore, the doping ratio of Mn2＋ exhibits influence on the persistent luminescence properties of ZGO：Mn PLNBs, and 2% doping of Mn2＋ shows superior persistent luminescence with decay time of longer than 20min. The developed 1D-based ZGO：Mn PLNBs can be simply prepared with the hydrothermal method and show tunable morphology and persistent luminescence. We believe that this solid-state-reaction-free chemical approach avoids the current key drawback in regard to PLNMs development, and thus will promote the broad use of these unique nanostructured PLNMs in developing optical device for imaging.展开更多
A warm-white emitting persistent luminescence phosphor Lu3Al2Ga3O12：Pr^3＋ was synthesized by solid state method at 1600 °C in air. The refined crystal structure of Lu3Al2Ga3O12 host was solved by X-ray diffract...A warm-white emitting persistent luminescence phosphor Lu3Al2Ga3O12：Pr^3＋ was synthesized by solid state method at 1600 °C in air. The refined crystal structure of Lu3Al2Ga3O12 host was solved by X-ray diffraction（XRD）. The photoluminescence spectra, decay curve and thermoluminescence were investigated. It was revealed that the persistent luminescence originated from the f-f transitions of Pr^3＋ emitters at Lu^3＋ sites in LuO8 polyhedrons, and it showed white color due to the ^3P0→^3H4, ^3P1→^3H5, ^3P0→^3H5, ^3P0→^3H6, ^3P0→^3F2, ^3P0→^3F3 and ^3P0→^3F4 transitions of Pr^3＋ emitters in a wide range. The persistent luminescence of Pr^3＋ in this host could be promoted by f-d transition（278 nm） but f-f transitions, due to the different thermal activation energy. The persistent luminescence of the optimal sample could be actually recorded for 3 h by the definition of 0.32 mcd/m^2 and was visible for more than 7 h by dark-adapted vision in darkness. The initial depth of the dominant shallow traps was calculated to be about 0.56 eV, which is suitable for persistent luminescence. The different roles of the shallow and deep traps on the persistent decay process were investigated. Accordingly, the persistent luminescence processes and mechanism of the as-synthesized Lu3Al2Ga3O12：Pr^3＋ phosphors were proposed.展开更多
By studying energy transfer and persistent energy transfer properties in Eu, Mn co-doped calcium aluminate CaAl_2O_4, it was found that traditional persistent luminescence mechanisms had difficulty in explaining persi...By studying energy transfer and persistent energy transfer properties in Eu, Mn co-doped calcium aluminate CaAl_2O_4, it was found that traditional persistent luminescence mechanisms had difficulty in explaining persistent energy transfer property between Eu^（2＋） and Mn^（2＋） ions. Based on this question, a mechanism was suggested in which vibrational energy levels were considered as a Morse potential, and trap centers were distinguished into barriers and wells. Then, this phenomenon was explained by allowing energy transfer and persistent energy transfer could have different preference to different vibrational energy levels. Properties of trap centers were also discussed by using the concept of Madelung energy.展开更多
A green long persistent luminescence（LPL） phosphor Ca3Ga4O9：Tb3＋/Zn2＋ was prepared. Ca3 Ga4 O9 matrix exhibits blue self-activated LPL due to the creation of intrinsic traps. When Tb3＋ is doped, the photolumines...A green long persistent luminescence（LPL） phosphor Ca3Ga4O9：Tb3＋/Zn2＋ was prepared. Ca3 Ga4 O9 matrix exhibits blue self-activated LPL due to the creation of intrinsic traps. When Tb3＋ is doped, the photoluminescence（PL） and LPL colors change from blue to green with their intensities significantly enhanced. The doping of Zn^（2＋） evidently improves the PL and LPL performances of the Ca3Ga4O9 matrix and Ca3Ga4O9：Tb^（3＋）. The thermoluminescence（TL） spectra show that a successive trap distribution is formed by multiple intrinsic traps with different depths in the Ca3 Ga4 O9 matrix, and the incorporation of Tb^（3＋） and Zn^（2＋） effectively increases the densities of these intrinsic traps. The existence of a successive trap distribution makes the Ca3 Ga4 O9：Tb^（3＋）/Zn^（2＋） phosphor exhibit thermally stable PL and LPL, It is indicated that this phosphor shows great promise for the application such as high-temperature LPL phosphor.展开更多
Pe rsistent luminescence(Pers L)materials are widely used in safety indication,traffic and transportation signs,architectural decoration and other fields.In this paper,(Y_(1-x)Ce_(x))(Al_(0.9995)Cr_(0.0005))_(2)Ga_(3)...Pe rsistent luminescence(Pers L)materials are widely used in safety indication,traffic and transportation signs,architectural decoration and other fields.In this paper,(Y_(1-x)Ce_(x))(Al_(0.9995)Cr_(0.0005))_(2)Ga_(3)O_(12)(x=0.001,0.002,0.003,0.005)transparent ceramics were successfully prepared by solid-state reaction method in air followed by HIP post-treatment.With the increase of Cedoping concentration,the optical quality of the as-prepared ceramics is improved and the morphology is denser.Luminescent quenching occurs when the Ceconcentration is more than 0.2%.The as-prepared transparent ceramics we re annealed in different atmosphere s.From the PersL decay curve s,the transparent ce ramics after air annealing show the best PersL performance:luminance with 4424.0 mcd/m^(2)and PersL duration over865 min after ceasing 365 nm excitation,respectively.The effects of Cedoping concentration and annealing atmospheres are also discussed in detail.展开更多
The roles of different point defects in persistent luminescence of SrAl2O4：Eu,Dy phosphors were investigated. The research results showed that Dyer plays an important role in the persistent luminescence of SrA1EO4：E...The roles of different point defects in persistent luminescence of SrAl2O4：Eu,Dy phosphors were investigated. The research results showed that Dyer plays an important role in the persistent luminescence of SrA1EO4：Eu, Dy phosphors. It can serve as the electron trap of suitable depth for persistent luminescence. V~ does not serve as the electron trap of suitable depth, but its existence can increase the depth of electron traps. There is interaction between the Dy^3＋（ DySr ） and the Eu^2＋（Eu^x Sr ）, and only if the distance between the Dy^3＋（DySr） and the Eu^2＋ （Eu^x Sr） is close enough, the Dyer can work as an effective electron trap. The point defect of V＂ Sr can be hole trap, but the change of its density in crystal matrix does not arouse the obvious change of persistent luminescence.展开更多
Near infrared to near infrared(NIR-NIR)photo-stimulated persistent luminescence(PSPL)has shown excellent potential in high-resolution bioimaging for deep tissues.However,the PSPL in NIR-Ⅱregion(900-1700 nm)is still l...Near infrared to near infrared(NIR-NIR)photo-stimulated persistent luminescence(PSPL)has shown excellent potential in high-resolution bioimaging for deep tissues.However,the PSPL in NIR-Ⅱregion(900-1700 nm)is still lacking.In this work,Ca_(2)Ga_(2)GeO_(7):Yb^(3+),Tb^(3+)(CGGYT)phosphor with unique lowdimensional crystal structure was synthesized by high-temperature solid-state reaction.Thanks to the carriers transferring from deep traps to shallow ones induced by low energy light,the 978 nm PSPL originating from ^(2)F_(5/2) to ^(2)F_(7/2) transition of Yb^(3+)induced by multimode stimulating(980 nm or WLED)is successfully realized after pre-excited by UV lamp.The NIR PSPL of the specimen can be repeatedly stimulated after placed in dark for 12 h.Moreover,the results indicate that codoping with Tb^(3+)can significantly enhance the NIR-ⅡPSPL owing to the quantum cutting persistent energy transfer(QC PET)from Tb^(3+)to Yb^(3+).Our study points to a new direction for the future development of multimode PSPL materials for bioimaging or multimode optical storage applications.展开更多
The crystal and electronic structure of the Eu^2＋ doped and defect containing Sr2MgSi2O7 persistent luminescence material were studied using the density functional theory （DFT）. The defects may act as energy storag...The crystal and electronic structure of the Eu^2＋ doped and defect containing Sr2MgSi2O7 persistent luminescence material were studied using the density functional theory （DFT）. The defects may act as energy storage or even luminescence quenching centres in these materials, however their role is very difficult to confirm experimentally. The probability of vacancy formation was studied using the total energy of the defect containing host. Significant structural modifications in the environment of the isolated defects, especially the strontium vacancy, as well as defect aggregates were found. The experimental band gap energy of Sr2MgSi2O7 was well reproduced by the calculations. The defect induced electron traps close to the host＇s conduction band were found to act as energy storage sites contributing to its efficient persistent luminescence. The interactions between the defects were found to modify both the Eu^2＋ 4f^7 ground state energy as well as the trap structure. The effect of charge compensation induced by the rare earth co-doping on the defect structure and energy storage properties of the persistent luminescence materials was discussed.展开更多
In very recent years,ultraviolet(UV)persistent luminescent materials(PLMs)have attracted widespread attention due to their potential biological applications.However,owing to the lack of suitable emitters and hosts,the...In very recent years,ultraviolet(UV)persistent luminescent materials(PLMs)have attracted widespread attention due to their potential biological applications.However,owing to the lack of suitable emitters and hosts,the design and development of excellent UV PLMs remain challenging.Here,we report a new Gd-based PLM NaGdGeO_(4):Bi^(3+)with super-long UVA persistent luminescence(PersL).By further codoping Li^(+)ions to increase the concentration of traps,the UVA PersL intensity of NaGdGeO_(4):Bi^(3+)is increased by 5.5 times.The optimal NaGdGeO_(4):Bi^(3+),Li^(+)exhibits excellent UVA PersL and can persist for more than 200 h.Moreover,the phosphor NaGdGeO_(4):Bi^(3+),Li^(+)also exhibits photostimulated property with a red LED or NIR laser excitation after the long-term decay,and can be activated by X-ray.This promising Gd-based UVA PLM is expected to have potential applications in biomedicine through triggering photocatalysts or photosensitizers by its UVA PersL to achieve photodynamic therapy and its potential ability of magnetic resonance(MR)imaging due to Gd^(3+)ions as MR imaging probe contained in the host NaGdGeO_(4).展开更多
Persistent luminescence (PersL) materials,as environmentally friendly and energy-saving materials,have broad application prospects in many fields such as lighting,chemistry and even biomedicine.However,studies on the ...Persistent luminescence (PersL) materials,as environmentally friendly and energy-saving materials,have broad application prospects in many fields such as lighting,chemistry and even biomedicine.However,studies on the types,performances and mechanism of PersL materials are still insufficient,which significantly restricts their development and application.Under this consideration,we successfully synthesized a yellow PersL material CaSrGa_(4)O_(8)(CSG).The crystal structure was studied in detail through Rotation Electron Diffraction (RED) and Powder X-ray Diffraction (PXRD).What’s more,by co-doping Mn^(2+) and Yb^(3+),the afterglow brightness of CSG could be increased by nearly 20 times,and the afterglow duration could reach more than 6 h.It is worth mentioning that the samples also have excellent performances in mechanical luminescence (ML),photostimulated luminescence (PSL) and cathodoluminescence (CL),which was also investigated systematically.Finally,an anti-counterfeiting label was designed by the samples to reveal the potential of their application in anti-counterfeiting.The results showed that our research not only provided a new candidate PersL material for multifunctional applications,but also gave good help for studying the physical and chemical properties of CSG.展开更多
Recently,the ultraviolet(UV)persistent luminescence material(PLM)has attracted extensive attention.However,the design and development of new UV PLM and exploring their promising advanced application remain challenges....Recently,the ultraviolet(UV)persistent luminescence material(PLM)has attracted extensive attention.However,the design and development of new UV PLM and exploring their promising advanced application remain challenges.Here,we developed a new dopant-free self-activated UVA PLM,Zn_(2)Al_(2)SiO_(7),which could be applied in anti-counterfeiting field.Zn_(2)Al_(2)SiO_(7)shows UVA persistent luminescence(PersL)peaking at 380 nm after 254 nm UV lamp excitation.Addition of Yb^(3+),the UVA PersL intensity and time are raised obviously,and the UVA PersL time lasts more than 24 h.In addition,Yb^(3+)-doped Zn_(2)Al_(2)SiO_(7)exhibits photostimulated properties with different light source.Finally,we design anticounterfeiting pattern based on intensity and time resolution from PersL of Zn_(2)Al_(2)SiO_(7),showing its advantages in the anti-counterfeiting field.展开更多
The research of long persistent luminescence(LPL)materials has yield brilliant results in many fields.However,the efforts are still needed for the regulation of the LPL performance.In this work,a series of LPL metal o...The research of long persistent luminescence(LPL)materials has yield brilliant results in many fields.However,the efforts are still needed for the regulation of the LPL performance.In this work,a series of LPL metal organic halides with rich halogen-bond interactions,Py-CdX_(2)(X=Cl,Br,I)were synthesized through self-assembly by Cd X_(2)and pyridine solvent.The steady-state emission redshifted and phosphorescence lifetime declined as the halogen atoms are aggravated.Three halides exhibit adjustable emission from blue to green and multiple phosphorescence from green to yellow at room temperature by changing the excitation wavelengths.Surprisingly,Py-CdX_(2)can emit the visible color-tunable LPL from green to yellow after removing different excitation sources at ambient conditions.Combing the results of theoretical calculation and experimental analysis,it is found that heavy atom effect and the rich intermolecular halogen bond help realize LPL and multiple triplet states originated from the pyridine ring and the halogens.展开更多
基金supported by the Major Research Plan of the National Natural Science Foundation of China(No.92361202)National Natural Science Foundation of China(No.12204481).
文摘Persistent luminescence is a unique optical phenomenon that continues to emit light for minutes or even hours after the excitation stops,which can significantly enhance the sensitivity and signal-to-noise ratio of imaging[1].Among numerous persistent luminescence materials,lanthanide-doped fluoride nanoparticles have shown tunable persistent luminescence across the UV-vis-NIR spectrum(200-1700 nm)under X-ray excitation and adjustable size,promising significant applications in deep-tissue imaging[2,3],security encryption,and data storage[4].In particular,those exhibiting NIR-II luminescence(1000-1700 nm)provide key advantages such as deeper tissue penetration,higher contrast,and minimal interference from biological autofluorescence.However,challenges such as low brightness and rapid signal decay,especially in the NIR-II region,limit their effectiveness in long-term monitoring,including tumor theranostics[5].Traditional approaches like size control and surface passivation yield only marginal improvements,underscoring the need for next-generation nanoparticles with superior NIR-II brightness.
基金financially supported by Quanzhou high-level Talents Project Fund(No.2022C033R)the National Natural Science Foundation of China(Nos.21925401,52221001)+2 种基金the Fundamental Research Funds for the Central Universities(No.2042022rc0004)the Postdoctoral Innovative Research of Hubei Province of China(No.211000025)the interdisciplinary innovative talents foundation from Renmin Hospital of Wuhan University。
文摘The dysbiosis of oral microbiota contributes to diseases such as periodontitis and certain cancers by triggering the host inflammatory response.Developing methods for the immediate and sensitive identification of oral microorganism is crucial for the rapid diagnosis and early interventions of associated diseases.Traditional methods for microbial detection primarily include the plate culturing,polymerase chain reaction and enzyme-linked immunosorbent assay,which are either time-consuming or laborious.Herein,we reported a persistent luminescence-encoded multiple-channel optical sensing array and achieved the rapid and accurate identification of oral-derived microorganisms.Our results demonstrate that electrostatic attractions and hydrophobic-hydrophobic interactions dominate the binding of the persistent luminescent nanoprobes to oral microorganisms and the microbial identification process can be finished within 30 min.Specifically,a total of 7 oral-derived microorganisms demonstrate their own response patterns and were differentiated by linear discriminant analysis(LDA)with the accuracy up to 100%both in the solution and artificial saliva samples.Moreover,the persistent luminescence encoded array sensor could also discern the microorganism mixtures with the accuracy up to 100%.The proposed persistent luminescence encoding sensor arrays in this work might offer new ideas for rapid and accurate oralderived microorganism detection,and provide new ways for disease diagnosis associated with microbial metabolism.
基金supported by the Jenny and Antti Wihuri Foundation and the Academy of Finland Project (117057/2006)supported by the European Community-Research Infrastructure Action under the FP6 Structuring the European Research Area Programme (RII3-CT-2004-506008 (IA-SFS))supported by research mobility agreements (112816/2006/JH and 116142/2006/JH, 123976/2007/TL) between the Academy of Finland and the Academy of Sciences of the Czech Republic
文摘The electronic structure of the strontium aluminate （SrAl2O4：Eu^2＋） materials was studied with a combined experimental and theo- retical approach. The UV-VUV synchrotron radiation was applied in the experimental study while the electronic structure of the non-optimized and optimized crystal structure were investigated theoretically by using the density functional theory. The structure of the valence and conduction bands as well as the band gap energy of the material together with the position of the Eu2＋ 4f7 85712 ground state were calculated. The calculated band gap energy （6.4 eV） agreed well with the experimental value of 6.6 eV. The valence band consisted mainly of oxygen states whereas the bottom of the conduction band of strontium states. In agreement with the experimental results, the calculated 4f7 8S7r2 ground state of Eu2＋ lies in the energy gap of the host. The position of the 4f7 ground state depended on the Coulomb repulsion strength. The position of the 4f7 ground state with respect to the valence and conduction bands was discussed using theoretical and experimental evidence available.
基金Project supported by the National Key R&D Program of China(2021YFA1202400,2017YFA0208000)the National Natural Science Foundation of China(21925401,21904033,51902177)the Fundamental Research Funds for the Central Universities(2042021 kf0036)。
文摘Persistent luminescence nanoparticles(PLNPs)are a kind of phosphors that can remain luminescent for seconds to several days after the stoppage of excitation.Lanthanides show the special capability to largely broaden the emission range and enhance the luminescence intensity of PLNPs due to their dense energy structure and unique electronic configurations.In the past decades,various methods have been developed for the synthesis of lanthanide-based PLNPs with excellent pe rsistent luminescence propertie s,and the lanthanide-based PLNPs are widely studied in areas including biome dicine,energy,and information storage.In this review,we summarized the research progress in the synthe sis of lanthanidebased PLNPs and outline d several typical synthesis methods.We discussed the fundamental concepts of preparation methods as well as the advantages and drawbacks of the typical synthetic approache s.Moreove r,the current challenges and the potential solutions for the development of lanthanide-based PLNP s are also discussed in an attempt to provide strate gies to further improve the optical properties of lanthanide-based PLNPs.We hope this review can contribute to the design of lanthanide-based PLNPs with desired properties and further promote their applications in biomedicine,energy,and information science.
基金Project supported by the Turku University Foundation, Jenny and Antti Wihuri Foundation (Finland) and the Academy of Finland (117057/2006)supported by the European Community-Research Infrastructure Action under the FP6 Structuring the European Re-search Area Programme, RII3-CT-2004-506008 (IA-SFS)+1 种基金supported by the Integrated Infrastructure Initiative "Integrating Activity on Synchrotron and Free Electron Laser Science"supported by Research Mobility Agreements (112816/2006/JH and 116142/2006/JH, 123976/2007/TL) between the Academy of Finland and the Academy of Sciences of the Czech Republic
文摘The electronic and defect energy level structure of polyerystalline Sr2MgSi2OT：Eu^2＋,R^3＋ persistent luminescence materials were studied with thermoluminescence and different synchrotron radiation spectroscopies （UV-VUV emission and excitation, X-ray absorption near-edge spectroscopy （XANES） and extended X-ray absorption f＇me structure （EXAFS））. Special attention was paid on the effect of the R3＋ co-dopants on the persistent luminescence properties of the materials. Theoretical calculations using the density functional theory （DFT） were carried out simultaneously with the experimental work. The experimental band gap energy （Eg） value of ca. 7.1 eV agreed very well with the DFT value of 6.7 eV. The variation of the Eg value was attempted to relate with the trap structure as well as with the different properties of the R3＋ co-dopants. The trap level energy distribution depended strongly on the R3＋ co-dopant except for the shallowest trap energy above the room temperature remaining practically the same, however. The different processes in the mechanism of persistent luminescence from Sr2MgSi2OT：Eu^2＋,R^3＋ were assembled and their contributions discussed.
基金Project supported by the National Natural Science Foundation of China(61705228,21507129)the Natural Science Foundation of Fujian ProvinceChina(2019J05159)。
文摘The near-infrared(NIR)persistent luminescence materials(PLMs)can remain long-lasting luminescence after removal of the excitation light,which permits bioimaging with high sensitivity owing to the absence of background fluorescence interference from in situ excitation.Recently,the NIR PLMs have aroused intensive research interest in bioimaging.However,the optimal excitation wavelength of current NIR PLMs is located in the ultraviolet region with shallow tissue penetration,making it difficult to activate effectively in vivo,and seriously hindering their further application in bioimaging.Herein,we report a novel kind of Cr^(3+)ions and Y^(3+)ions co-doped NIR PLM,Zn_(1.3)Ga_(1.4)Sn_(0.3)O_(4):Cr^(3+),Y^(3+)(ZGSCY),which emits NIR persistent luminescence at 696 nm.Compared with Zn_(1.3)Ga_(1.4)Sn_(0.3)O_(4):Cr^(3+)(ZGSC)excited by the light with a wavelength in the biological window(>650 nm),after being co-doped with Y^(3+)ions,the NIR persistent luminescence performance of ZGSCY is significantly improved because of the increase of trap concentration in the matrix.In addition,we synthesized ZGSCY nanoparticles(NPs)by the combustion method,which exhibit excellent optical properties after being excited by the light with a wavelength in the biological window.After surface modification with PEG,the ZGSCY NPs present low cytotoxicity.Notably,due to the co-doping of Y^(3+)ions,the signal-to-noise ratio(SNR)of ZGSCY NPs in vivo imaging is about 1.8 times higher than that of the ZGSC NPs.Furthermore,the rechargeable in vivo imaging and passive tumor-targeted imaging are successfully achieved by activating with a lightemitting diode(LED,659 nm)after intravenous injection of ZGSCY.Thus,this kind of NIR PLM with high excitation efficiency performance in the biological window is expected to promote its biomedical application in deep tissues.
基金Project supported by the National Natural Science Foundation of China(61705228,62105333)the Natural Science Foundation of Fujian Province,China(2019J05159)。
文摘X-ray-activated luminescence materials have broad application prospects in photodynamic therapy of deep tissue.Among them,X-ray-activated persistent luminescence materials(PLMs)exhibiting multiple emission peaks have drawn extensive attention for the ir capacity to achieve a combination of bioimaging and therapeutic functions.Here,we developed a novel PLM,LiYGeO_4:Bi^(3+),Pr^(3+),that simultaneously exhibits UV and NIR dual persistent luminescence(PersL)emissions after irradiation by X-ray.The material can be re peatedly excited by X-ray and emits similar lumine scence intensity every time,which shows good PersL stability.In addition,LiYGeO_4:Bi^(3+),Pr^(3+)exhibits photostimulated PersL properties by stimulation with a red light-emitting diode(LED)or NIR laser after long-term decay.This work provides a new choice of X-ray-excited PLMs with UV and NIR dual emission and the novel phosphor shows promise as a potential candidate for the integration of treatment and diagnosis of deep tumors.
基金Project supported by the National Natural Science Foundation of China(62105333)the Key Research Program of the Chinese Academy of Sciences(ZDRW-CN-2021-3)+1 种基金Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2020ZZ114)the Xiamen Medical and Health Guidance Project,China(3502Z20209124)。
文摘In recent years,persistent luminescence materials(PLMs)excited by X-rays and emitting in biological windows have received extensive attention in the field of high-sensitivity bioimaging.Transition metal Mn^(2+)is an ideal emission center,but few studies focus on Mn^(2+)-doped PLMs with X-ray excitation and biological window emission.Here,we report a Mn^(2+)-doped PLM,LiYGeO_(4):Mn^(2+)(LYGM),with excellent biological window persistent luminescence emission.After excitation by UV,LYGM produces a durable biological window of persistent luminescence emission at 660 nm for up to 20 h.More importantly.LYGM can be repeatedly excited by X-rays,resulting in long-term biological window persistent luminescence emission.In addition,we obtain LYGM around 200 nm in diameter by ball milling and centrifugation and improve its biocompatibility by surface modification to apply it to in vivo imaging in mice.After LYGM are injected into mice through the tail vein,in situ excitation of X-rays can be achieved.After the persistent luminescence decays,LYGM can be re-excited for repeated imaging.Therefore,LYGM shows potential prospects for in vivo deep tissue and long-term bioimaging.
基金supported by the National Key R&D Program of China (No. 2017YFA0208000)National Natural Science Foundation of China (No. 21675120)+2 种基金Ten Thousand Talents Program for Young Talents, Start-up Research Fund for Prof. Q. Yuan (No. 531107050973)State Key Laboratory of Chemo/Bio-Sensing and Chemometrics at Hunan University(No. 734106172)Open Funding Project of the State Key Laboratory of Biochemical Engineering (No. 4102010299)
文摘Here, we report the direct hydrothermal synthesis of 1 D-based Zn2GeO4：Mn2＋ persistent luminescent nanobelts （ZGO：Mn PLNBs）. The ZGO：Mn PLNBs exhibit rapid growth rate, and nanobelts can be obtained after 30 rain of hydrothermal treatment. The persistent luminescence performance can be fine-turned upon prolonging the hydrothermal time. Furthermore, the doping ratio of Mn2＋ exhibits influence on the persistent luminescence properties of ZGO：Mn PLNBs, and 2% doping of Mn2＋ shows superior persistent luminescence with decay time of longer than 20min. The developed 1D-based ZGO：Mn PLNBs can be simply prepared with the hydrothermal method and show tunable morphology and persistent luminescence. We believe that this solid-state-reaction-free chemical approach avoids the current key drawback in regard to PLNMs development, and thus will promote the broad use of these unique nanostructured PLNMs in developing optical device for imaging.
基金Project supported by the National Natural Science Foundation of China(10904057)the Fundamental Research Funds for Central Universities(Lzjbky-2015-112,Lzjbky-2015-113)the National Science Foundation for Fostering Talents in Basic Research of the National Natural Science Foundation of China(041105,041106)
文摘A warm-white emitting persistent luminescence phosphor Lu3Al2Ga3O12：Pr^3＋ was synthesized by solid state method at 1600 °C in air. The refined crystal structure of Lu3Al2Ga3O12 host was solved by X-ray diffraction（XRD）. The photoluminescence spectra, decay curve and thermoluminescence were investigated. It was revealed that the persistent luminescence originated from the f-f transitions of Pr^3＋ emitters at Lu^3＋ sites in LuO8 polyhedrons, and it showed white color due to the ^3P0→^3H4, ^3P1→^3H5, ^3P0→^3H5, ^3P0→^3H6, ^3P0→^3F2, ^3P0→^3F3 and ^3P0→^3F4 transitions of Pr^3＋ emitters in a wide range. The persistent luminescence of Pr^3＋ in this host could be promoted by f-d transition（278 nm） but f-f transitions, due to the different thermal activation energy. The persistent luminescence of the optimal sample could be actually recorded for 3 h by the definition of 0.32 mcd/m^2 and was visible for more than 7 h by dark-adapted vision in darkness. The initial depth of the dominant shallow traps was calculated to be about 0.56 eV, which is suitable for persistent luminescence. The different roles of the shallow and deep traps on the persistent decay process were investigated. Accordingly, the persistent luminescence processes and mechanism of the as-synthesized Lu3Al2Ga3O12：Pr^3＋ phosphors were proposed.
基金supported by the National Natural Science Foundation of China(51372105)
文摘By studying energy transfer and persistent energy transfer properties in Eu, Mn co-doped calcium aluminate CaAl_2O_4, it was found that traditional persistent luminescence mechanisms had difficulty in explaining persistent energy transfer property between Eu^（2＋） and Mn^（2＋） ions. Based on this question, a mechanism was suggested in which vibrational energy levels were considered as a Morse potential, and trap centers were distinguished into barriers and wells. Then, this phenomenon was explained by allowing energy transfer and persistent energy transfer could have different preference to different vibrational energy levels. Properties of trap centers were also discussed by using the concept of Madelung energy.
基金supported by the National Natural Science Foundation of China(11774138)the Society Development Foundation of Yunnan Province(2016FA021)the Kunming University of Science and Technology(KKSY201632046)
文摘A green long persistent luminescence（LPL） phosphor Ca3Ga4O9：Tb3＋/Zn2＋ was prepared. Ca3 Ga4 O9 matrix exhibits blue self-activated LPL due to the creation of intrinsic traps. When Tb3＋ is doped, the photoluminescence（PL） and LPL colors change from blue to green with their intensities significantly enhanced. The doping of Zn^（2＋） evidently improves the PL and LPL performances of the Ca3Ga4O9 matrix and Ca3Ga4O9：Tb^（3＋）. The thermoluminescence（TL） spectra show that a successive trap distribution is formed by multiple intrinsic traps with different depths in the Ca3 Ga4 O9 matrix, and the incorporation of Tb^（3＋） and Zn^（2＋） effectively increases the densities of these intrinsic traps. The existence of a successive trap distribution makes the Ca3 Ga4 O9：Tb^（3＋）/Zn^（2＋） phosphor exhibit thermally stable PL and LPL, It is indicated that this phosphor shows great promise for the application such as high-temperature LPL phosphor.
基金Project supported by the National Key R&D Program of China(2021YFE0104800)Joint Funds of the National Natural Science Foundation of China(U1932160)National Center for Research and Development(WPC2/1/SCAPOL/2021)。
文摘Pe rsistent luminescence(Pers L)materials are widely used in safety indication,traffic and transportation signs,architectural decoration and other fields.In this paper,(Y_(1-x)Ce_(x))(Al_(0.9995)Cr_(0.0005))_(2)Ga_(3)O_(12)(x=0.001,0.002,0.003,0.005)transparent ceramics were successfully prepared by solid-state reaction method in air followed by HIP post-treatment.With the increase of Cedoping concentration,the optical quality of the as-prepared ceramics is improved and the morphology is denser.Luminescent quenching occurs when the Ceconcentration is more than 0.2%.The as-prepared transparent ceramics we re annealed in different atmosphere s.From the PersL decay curve s,the transparent ce ramics after air annealing show the best PersL performance:luminance with 4424.0 mcd/m^(2)and PersL duration over865 min after ceasing 365 nm excitation,respectively.The effects of Cedoping concentration and annealing atmospheres are also discussed in detail.
基金This study is financially supported by the Jiangxi University of Finance and Economy (Project No. 0421205) Jiangxi Provincial Department of Education (Project No. (2007) 260)
文摘The roles of different point defects in persistent luminescence of SrAl2O4：Eu,Dy phosphors were investigated. The research results showed that Dyer plays an important role in the persistent luminescence of SrA1EO4：Eu, Dy phosphors. It can serve as the electron trap of suitable depth for persistent luminescence. V~ does not serve as the electron trap of suitable depth, but its existence can increase the depth of electron traps. There is interaction between the Dy^3＋（ DySr ） and the Eu^2＋（Eu^x Sr ）, and only if the distance between the Dy^3＋（DySr） and the Eu^2＋ （Eu^x Sr） is close enough, the Dyer can work as an effective electron trap. The point defect of V＂ Sr can be hole trap, but the change of its density in crystal matrix does not arouse the obvious change of persistent luminescence.
基金Project supported by the National Natural Science Foundation of China-Yunnan Joint Fund(U1902222)the National Natural Science Foundation of China(11774138,11664022,51862020 and 11804255)the Natural Science Foundation of Yunnan Province(2019HC016)。
文摘Near infrared to near infrared(NIR-NIR)photo-stimulated persistent luminescence(PSPL)has shown excellent potential in high-resolution bioimaging for deep tissues.However,the PSPL in NIR-Ⅱregion(900-1700 nm)is still lacking.In this work,Ca_(2)Ga_(2)GeO_(7):Yb^(3+),Tb^(3+)(CGGYT)phosphor with unique lowdimensional crystal structure was synthesized by high-temperature solid-state reaction.Thanks to the carriers transferring from deep traps to shallow ones induced by low energy light,the 978 nm PSPL originating from ^(2)F_(5/2) to ^(2)F_(7/2) transition of Yb^(3+)induced by multimode stimulating(980 nm or WLED)is successfully realized after pre-excited by UV lamp.The NIR PSPL of the specimen can be repeatedly stimulated after placed in dark for 12 h.Moreover,the results indicate that codoping with Tb^(3+)can significantly enhance the NIR-ⅡPSPL owing to the quantum cutting persistent energy transfer(QC PET)from Tb^(3+)to Yb^(3+).Our study points to a new direction for the future development of multimode PSPL materials for bioimaging or multimode optical storage applications.
基金Project supported by Turku University FoundationJenny and Antti Wihuri Foundation (Finland)+2 种基金the Academy of Finland (contract #117057/2006,#134459/2010)research mobility agreements (112816/2006/JH,116142/2006/JH,123976/2007/TL) between the Academy of Finland and the Academy of Sciences of the Czech Republicthe Czech research project (AVOZ10100521 (PN))
文摘The crystal and electronic structure of the Eu^2＋ doped and defect containing Sr2MgSi2O7 persistent luminescence material were studied using the density functional theory （DFT）. The defects may act as energy storage or even luminescence quenching centres in these materials, however their role is very difficult to confirm experimentally. The probability of vacancy formation was studied using the total energy of the defect containing host. Significant structural modifications in the environment of the isolated defects, especially the strontium vacancy, as well as defect aggregates were found. The experimental band gap energy of Sr2MgSi2O7 was well reproduced by the calculations. The defect induced electron traps close to the host＇s conduction band were found to act as energy storage sites contributing to its efficient persistent luminescence. The interactions between the defects were found to modify both the Eu^2＋ 4f^7 ground state energy as well as the trap structure. The effect of charge compensation induced by the rare earth co-doping on the defect structure and energy storage properties of the persistent luminescence materials was discussed.
基金Project supported by National Natural Science Foundation of China(61705228,21507129)Natural Science Foundation of Fujian Province,China(2019J05159)。
文摘In very recent years,ultraviolet(UV)persistent luminescent materials(PLMs)have attracted widespread attention due to their potential biological applications.However,owing to the lack of suitable emitters and hosts,the design and development of excellent UV PLMs remain challenging.Here,we report a new Gd-based PLM NaGdGeO_(4):Bi^(3+)with super-long UVA persistent luminescence(PersL).By further codoping Li^(+)ions to increase the concentration of traps,the UVA PersL intensity of NaGdGeO_(4):Bi^(3+)is increased by 5.5 times.The optimal NaGdGeO_(4):Bi^(3+),Li^(+)exhibits excellent UVA PersL and can persist for more than 200 h.Moreover,the phosphor NaGdGeO_(4):Bi^(3+),Li^(+)also exhibits photostimulated property with a red LED or NIR laser excitation after the long-term decay,and can be activated by X-ray.This promising Gd-based UVA PLM is expected to have potential applications in biomedicine through triggering photocatalysts or photosensitizers by its UVA PersL to achieve photodynamic therapy and its potential ability of magnetic resonance(MR)imaging due to Gd^(3+)ions as MR imaging probe contained in the host NaGdGeO_(4).
基金supported by the Department of Industry and Information Technology of Gansu Province and Baotou Rare Earth Research Institute。
文摘Persistent luminescence (PersL) materials,as environmentally friendly and energy-saving materials,have broad application prospects in many fields such as lighting,chemistry and even biomedicine.However,studies on the types,performances and mechanism of PersL materials are still insufficient,which significantly restricts their development and application.Under this consideration,we successfully synthesized a yellow PersL material CaSrGa_(4)O_(8)(CSG).The crystal structure was studied in detail through Rotation Electron Diffraction (RED) and Powder X-ray Diffraction (PXRD).What’s more,by co-doping Mn^(2+) and Yb^(3+),the afterglow brightness of CSG could be increased by nearly 20 times,and the afterglow duration could reach more than 6 h.It is worth mentioning that the samples also have excellent performances in mechanical luminescence (ML),photostimulated luminescence (PSL) and cathodoluminescence (CL),which was also investigated systematically.Finally,an anti-counterfeiting label was designed by the samples to reveal the potential of their application in anti-counterfeiting.The results showed that our research not only provided a new candidate PersL material for multifunctional applications,but also gave good help for studying the physical and chemical properties of CSG.
基金Project supported by the National Natural Science Foundation of China(61705228,62105333,11864015)the Natural Science Foundation of Fujian Province,China(2019J05159)。
文摘Recently,the ultraviolet(UV)persistent luminescence material(PLM)has attracted extensive attention.However,the design and development of new UV PLM and exploring their promising advanced application remain challenges.Here,we developed a new dopant-free self-activated UVA PLM,Zn_(2)Al_(2)SiO_(7),which could be applied in anti-counterfeiting field.Zn_(2)Al_(2)SiO_(7)shows UVA persistent luminescence(PersL)peaking at 380 nm after 254 nm UV lamp excitation.Addition of Yb^(3+),the UVA PersL intensity and time are raised obviously,and the UVA PersL time lasts more than 24 h.In addition,Yb^(3+)-doped Zn_(2)Al_(2)SiO_(7)exhibits photostimulated properties with different light source.Finally,we design anticounterfeiting pattern based on intensity and time resolution from PersL of Zn_(2)Al_(2)SiO_(7),showing its advantages in the anti-counterfeiting field.
基金financially supported by National Natural Science Foundation of China(No.22101162)Start-up Foundation of Shaanxi University of Science&Technology(No.126022036)。
文摘The research of long persistent luminescence(LPL)materials has yield brilliant results in many fields.However,the efforts are still needed for the regulation of the LPL performance.In this work,a series of LPL metal organic halides with rich halogen-bond interactions,Py-CdX_(2)(X=Cl,Br,I)were synthesized through self-assembly by Cd X_(2)and pyridine solvent.The steady-state emission redshifted and phosphorescence lifetime declined as the halogen atoms are aggravated.Three halides exhibit adjustable emission from blue to green and multiple phosphorescence from green to yellow at room temperature by changing the excitation wavelengths.Surprisingly,Py-CdX_(2)can emit the visible color-tunable LPL from green to yellow after removing different excitation sources at ambient conditions.Combing the results of theoretical calculation and experimental analysis,it is found that heavy atom effect and the rich intermolecular halogen bond help realize LPL and multiple triplet states originated from the pyridine ring and the halogens.
