Chiral nanomaterials hold significant promise for enhancing clinical therapeutic outcomes,thanks to their unique chiral selectivity in biological systems.Despite this potential,the innovative approach has garnered lim...Chiral nanomaterials hold significant promise for enhancing clinical therapeutic outcomes,thanks to their unique chiral selectivity in biological systems.Despite this potential,the innovative approach has garnered limited focus in the realm of cancer therapy.In this work,we synthesized multi-shelled mesoporous silica nanocarriers by a biphasic stratification reaction system.Owing to a lamellar micelle spiral self-assembly happens at the water/oil bio-interface,the fabricated silica nanosphere has a unique chirality which is different from conventional dendritic mesoporous silica nanoparticles.On one hand,after loading with the clinically approved dye molecule indocyanine green(ICG),the long-off peak fluorescence at second near-infrared window(NIR II,1000-1700 nm)exhibits excellent photostability,with a significant enhancement under continuous exposure to daylight or an 808 nm laser,which is highly beneficial for long-duration surgical navigation in clinical settings.On the other hand,due to its unique chiral architecture,chiral nanostructured mesoporous silica(cSi)nanocarriers demonstrate unparalleled cellular uptake capability compared to traditional mesoporous silica.Furthermore,thanks to cSi's targeted accumulation in tumor tissues and its ability to synergistically promote photothermal augmented chiral-specific tumor cell killing,the malignant tissue is effectively suppressed,heralding a new way in cancer-fighting.展开更多
The Ni^(2+)ion has garnered increasing attention due to its broadband emission in the near infrared(NIR)Ⅱ region(1000-1700 nm).However,it exhibits low light absorption efficiency and cannot be effectively excited by ...The Ni^(2+)ion has garnered increasing attention due to its broadband emission in the near infrared(NIR)Ⅱ region(1000-1700 nm).However,it exhibits low light absorption efficiency and cannot be effectively excited by blue light chips,thereby significantly impeding its commercial application.Herein,we introduced the Cr^(3+)sensitizer ion into MgGa_(2)O_(4):0.01Ni^(2+),which remarkably enhanced the absorption efficiency of blue light and improved the photoluminescence properties.It is noteworthy that the MgGa_(2)O_(4):0.24Cr^(3+),0.01Ni^(2+),2 wt%H_(3)BO_(3) sample exhibits a broadband emission spanning from 1000 to 1600 nm,with an emission peak at 1290 nm,achieving high internal and external photoluminescence quantum yields of 81.91%and 62.51%,respectively.The occupancy of Cr^(3+)ions at the lattice sites in MgGa_(2)O_(4) was comprehensively discussed and analyzed using various optical characterization techniques.Additionally,based on X-ray absorption near-edge structure spectra and low-temperature photoluminescence spectra,it has been determined that the energy level of Cr^(3+)in tetrahedral sites acts as an intermediate level for energy transfer from Cr^(3+)to Ni^(2+),leading to high energy transfer efficiency.The electro-optical conversion efficiency of the packaged NIR phosphor-converted light-emitting diode device reaches 11.38%under a driven current of 20 mA,and the NIR output power can reach up to 52.66 mW at 350 mA,showcasing the exceptional electro-optical properties of the as-fabricated NIR pc-LED within the NIR Ⅱ range.展开更多
The launch of the big data era puts forward challenges for information preservation technology,both in storage capacity and security.Herein,a brand new optical storage medium,transparent glass ceramic(TGC)embedded wit...The launch of the big data era puts forward challenges for information preservation technology,both in storage capacity and security.Herein,a brand new optical storage medium,transparent glass ceramic(TGC)embedded with photostimulated LiGa5O8:Mn2+nanocrystals,capable of achieving bit-by-bit optical data write-in and read-out in a photon trapping/detrapping mode,is developed.The highly ordered nanostructure enables light–matter interaction with high encoding/decoding resolution and low bit error rate.Importantly,going beyond traditional 2D optical storage,the high transparency of the studied bulk medium makes 3D volumetric optical data storage(ODS)possible,which brings about the merits of expanded storage capacity and improved information security.Demonstration application confirmed the erasable-rewritable 3D storage of binary data and display items in TGC with intensity/wavelength multiplexing.The present work highlights a great leap in photostimulated material for ODS application and hopefully stimulates the development of new multi-dimensional ODS media.展开更多
Thermally activated delayed fluorescence(TADF)materials with both high photoluminescence quantum yield(PLQY)and fast reverse intersystem crossing(RISC)are strongly desired to realize efficient and stable organic light...Thermally activated delayed fluorescence(TADF)materials with both high photoluminescence quantum yield(PLQY)and fast reverse intersystem crossing(RISC)are strongly desired to realize efficient and stable organic light-emitting diodes(OLEDs).Control of excited-state dynamics via molecular design plays a central role in optimizing the PLQY and RISC rate of TADF materials but remains challenging.Here,3 TADF emitters possessing similar molecular structures,similar high PLQYs(89.5%to 96.3%),and approximate energy levels of the lowest excited singlet states(S_(1)),but significantly different spin-flipping RISC rates(0.03×10^(6) s^(−1) vs.2.26×10^(6) s^(−1))and exciton lifetime(297.1 to 332.8μs vs.6.0μs)were systematically synthesized to deeply investigate the feasibility of spin-flip between charge-transfer excited states(^(3)CT–^(1)CT)transition.展开更多
Thermo-enhanced nanothermometry has attracted considerable attention owing to its high thermal sen-sitivity;however,most studies are focused on upconversion nanoparticles(NPs)in the form of powder.In the field of bioa...Thermo-enhanced nanothermometry has attracted considerable attention owing to its high thermal sen-sitivity;however,most studies are focused on upconversion nanoparticles(NPs)in the form of powder.In the field of bioapplication,it is imperative to investigate the performance of NPs dispersed in aqueous solutions to expedite their in vivo utilization.Particularly,the influence of-OH on the thermal properties of these NPs remains unclear.Herein,we investigated the thermal properties ofα-NaYbF_(4):2%Er,2%Ce@NaYF_(4)NPs with different shell thicknesses emitting in the second near-infrared(NIR-II)region.Both powder and aqueous solution-dispersed NPs exhibit thermal enhancements due to a reduction in the-OH content and a blue shift of-OH vibration at elevated temperatures,respectively.The observed blue shift of-OH vibration is attributed to the conversion of 4-coordinated hydrogen-bound water into 2-co-ordinated hydrogen-bound water.By separately introducing LiCl and D_(2)O to an aqueous solution,we demonstrated how the blue shift and-OH content affect the thermal enhancement factor in aqueous solutions.These findings underscore the crucial role of-OH groups in nanothermometry for bioapplica-tions while also providing insights for designing highly thermally sensitive nanothermometers.展开更多
基金supported by Joint Funds for the innovation of science and Technology,Fujian province Joint Funds for the Innovation of Science and Technology,Fujian province(No.2021Y9022 to F.Q.X.)Fujian Provincial Natural Science Foundation(No.2022J01415 to X.Y.W.).
文摘Chiral nanomaterials hold significant promise for enhancing clinical therapeutic outcomes,thanks to their unique chiral selectivity in biological systems.Despite this potential,the innovative approach has garnered limited focus in the realm of cancer therapy.In this work,we synthesized multi-shelled mesoporous silica nanocarriers by a biphasic stratification reaction system.Owing to a lamellar micelle spiral self-assembly happens at the water/oil bio-interface,the fabricated silica nanosphere has a unique chirality which is different from conventional dendritic mesoporous silica nanoparticles.On one hand,after loading with the clinically approved dye molecule indocyanine green(ICG),the long-off peak fluorescence at second near-infrared window(NIR II,1000-1700 nm)exhibits excellent photostability,with a significant enhancement under continuous exposure to daylight or an 808 nm laser,which is highly beneficial for long-duration surgical navigation in clinical settings.On the other hand,due to its unique chiral architecture,chiral nanostructured mesoporous silica(cSi)nanocarriers demonstrate unparalleled cellular uptake capability compared to traditional mesoporous silica.Furthermore,thanks to cSi's targeted accumulation in tumor tissues and its ability to synergistically promote photothermal augmented chiral-specific tumor cell killing,the malignant tissue is effectively suppressed,heralding a new way in cancer-fighting.
基金supported by the National Key R&D Program of China(2021YFB3500401)the Natural Science Foundation of Fujian Province(2023J01214)。
文摘The Ni^(2+)ion has garnered increasing attention due to its broadband emission in the near infrared(NIR)Ⅱ region(1000-1700 nm).However,it exhibits low light absorption efficiency and cannot be effectively excited by blue light chips,thereby significantly impeding its commercial application.Herein,we introduced the Cr^(3+)sensitizer ion into MgGa_(2)O_(4):0.01Ni^(2+),which remarkably enhanced the absorption efficiency of blue light and improved the photoluminescence properties.It is noteworthy that the MgGa_(2)O_(4):0.24Cr^(3+),0.01Ni^(2+),2 wt%H_(3)BO_(3) sample exhibits a broadband emission spanning from 1000 to 1600 nm,with an emission peak at 1290 nm,achieving high internal and external photoluminescence quantum yields of 81.91%and 62.51%,respectively.The occupancy of Cr^(3+)ions at the lattice sites in MgGa_(2)O_(4) was comprehensively discussed and analyzed using various optical characterization techniques.Additionally,based on X-ray absorption near-edge structure spectra and low-temperature photoluminescence spectra,it has been determined that the energy level of Cr^(3+)in tetrahedral sites acts as an intermediate level for energy transfer from Cr^(3+)to Ni^(2+),leading to high energy transfer efficiency.The electro-optical conversion efficiency of the packaged NIR phosphor-converted light-emitting diode device reaches 11.38%under a driven current of 20 mA,and the NIR output power can reach up to 52.66 mW at 350 mA,showcasing the exceptional electro-optical properties of the as-fabricated NIR pc-LED within the NIR Ⅱ range.
基金supported by the National Natural Science Foundation of China(51872288,11774346,51972303 and 11974350)the Natural Science Foundation of Fujian Province(2019J01122).
文摘The launch of the big data era puts forward challenges for information preservation technology,both in storage capacity and security.Herein,a brand new optical storage medium,transparent glass ceramic(TGC)embedded with photostimulated LiGa5O8:Mn2+nanocrystals,capable of achieving bit-by-bit optical data write-in and read-out in a photon trapping/detrapping mode,is developed.The highly ordered nanostructure enables light–matter interaction with high encoding/decoding resolution and low bit error rate.Importantly,going beyond traditional 2D optical storage,the high transparency of the studied bulk medium makes 3D volumetric optical data storage(ODS)possible,which brings about the merits of expanded storage capacity and improved information security.Demonstration application confirmed the erasable-rewritable 3D storage of binary data and display items in TGC with intensity/wavelength multiplexing.The present work highlights a great leap in photostimulated material for ODS application and hopefully stimulates the development of new multi-dimensional ODS media.
基金the National Natural Science Foundation of China(Grant Nos.52073286 and 21805281)the Natural Science Foundation of Fujian Province(Grant No.2006L2005)+1 种基金the Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China(Grant Nos.2021ZR132 and 2021ZZ115)the Youth Innovation Foundation of Xiamen City(Grant Nos.3502Z20206082 and 3502Z20206083).
文摘Thermally activated delayed fluorescence(TADF)materials with both high photoluminescence quantum yield(PLQY)and fast reverse intersystem crossing(RISC)are strongly desired to realize efficient and stable organic light-emitting diodes(OLEDs).Control of excited-state dynamics via molecular design plays a central role in optimizing the PLQY and RISC rate of TADF materials but remains challenging.Here,3 TADF emitters possessing similar molecular structures,similar high PLQYs(89.5%to 96.3%),and approximate energy levels of the lowest excited singlet states(S_(1)),but significantly different spin-flipping RISC rates(0.03×10^(6) s^(−1) vs.2.26×10^(6) s^(−1))and exciton lifetime(297.1 to 332.8μs vs.6.0μs)were systematically synthesized to deeply investigate the feasibility of spin-flip between charge-transfer excited states(^(3)CT–^(1)CT)transition.
基金supported by the National Natural Science Foundation of China(no.12204480)the Natural Science Foundation of Fujian Province,China(no.2021J01518)the Xiamen Municipal Bureau of Science and Technology(3502Z20231040).
文摘Thermo-enhanced nanothermometry has attracted considerable attention owing to its high thermal sen-sitivity;however,most studies are focused on upconversion nanoparticles(NPs)in the form of powder.In the field of bioapplication,it is imperative to investigate the performance of NPs dispersed in aqueous solutions to expedite their in vivo utilization.Particularly,the influence of-OH on the thermal properties of these NPs remains unclear.Herein,we investigated the thermal properties ofα-NaYbF_(4):2%Er,2%Ce@NaYF_(4)NPs with different shell thicknesses emitting in the second near-infrared(NIR-II)region.Both powder and aqueous solution-dispersed NPs exhibit thermal enhancements due to a reduction in the-OH content and a blue shift of-OH vibration at elevated temperatures,respectively.The observed blue shift of-OH vibration is attributed to the conversion of 4-coordinated hydrogen-bound water into 2-co-ordinated hydrogen-bound water.By separately introducing LiCl and D_(2)O to an aqueous solution,we demonstrated how the blue shift and-OH content affect the thermal enhancement factor in aqueous solutions.These findings underscore the crucial role of-OH groups in nanothermometry for bioapplica-tions while also providing insights for designing highly thermally sensitive nanothermometers.
