X射线激发深层肌体温度传感材料La_2O_2S∶Yb~(3+),Er~(3+)的测温性质研究
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摘要
Yb~(3+)、Er~(3+)共掺杂上转换发光材料能被红外光激发,可用于肌体内部温度测量,但上转换材料效率较低,无法实现较深组织温度探测。考虑到Er~(3+)能级可被多种光源布居,较好肌体穿透性的X射线无疑是理想的激发源。本文首次报道了一种新型的深层肌体温度传感材料La_2O_2S∶Yb~(3+),Er~(3+)。数据表明,X射线激发下,在不同温度下的两个绿光发射强度比符合玻尔兹曼分布,最高测温灵敏度达到了0.011 5 K~(-1)。我们相信Yb~(3+)、Er~(3+)共掺的La_2O_2S是可以应用于临床的理想测温材料。
Yb~(3+),Er~(3+)co-doped up-conversion luminescent materials can be used to measure the internal temperature of tissue under infrared light excitation,but the lower efficiency of up-conversion materials makes it impossible to detect deep tissue temperature. Considering that Er~(3+)energy levels can be populated by various light sources,X-ray is undoubtedly an ideal excitation source with better penetration. In this article,we first reported a novel deep tissue temperature sensing material La_2O_2S∶ Yb~(3+),Er~(3+). The data show that the fluorescence intensity ratio of the two green levels at different temperatures conforms to Boltzmann distribution under X-ray excitation,and the maximum sensor sensitivity is 0. 011 5 K~(-1). We believe that Yb~(3+),Er~(3+)co-doped La_2O_2S can be used as an ideal temperature measuring material for clinical application.
Yb~(3+),Er~(3+)co-doped up-conversion luminescent materials can be used to measure the internal temperature of tissue under infrared light excitation,but the lower efficiency of up-conversion materials makes it impossible to detect deep tissue temperature. Considering that Er~(3+)energy levels can be populated by various light sources,X-ray is undoubtedly an ideal excitation source with better penetration. In this article,we first reported a novel deep tissue temperature sensing material La_2O_2S∶ Yb~(3+),Er~(3+). The data show that the fluorescence intensity ratio of the two green levels at different temperatures conforms to Boltzmann distribution under X-ray excitation,and the maximum sensor sensitivity is 0. 011 5 K~(-1). We believe that Yb~(3+),Er~(3+)co-doped La_2O_2S can be used as an ideal temperature measuring material for clinical application.
引文
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[26] LIU G G,FU L L,GAO Z Y,et al.. Investigation into the temperature sensing behavior of Yb3+sensitized Er3+doped Y2O3,YAG and La Al O3phosphors[J]. RSC Adv.,2015,5(64):51820-51827.
[27]YANG Y M,MI C,YU F,et al.. Optical thermometry based on the upconversion fluorescence from Yb3+/Er3+codoped La2O2S phosphor[J]. Ceram. Int.,2013,40(7):9875-9880.
[28]LI X D,SONG Y J,YANG Y M,et al.. Structure and optical thermometry characterization of Er3+/Yb3+co-doped Ba Gd2Cu O5[J]. J. Nanosci. Nanotechnol.,2016,16(4):3542-3546.
[29]刘延洲,杨艳民,郭彦明,等. Er3+∶Yb3+共掺杂Ba Gd2Zn O5纳米晶体上转换光学温度传感[J].光谱学与光谱分析,2015,35(2):329-333.LIU Y Z,YANG Y M,GUO Y M,et al.. Er3+∶Yb3+Co-doped nanocrystals Ba Gd2Zn O5of Up-conversion optical temperature sensing[J]. Spectrosc. Spectr. Anal.,2015,35(2):329-333.(in Chinese)
[30]MAURICE E,MONNOM G,DUSSARDIER B,et al.. Erbium-doped silica fibers for intrinsic fiber-optic temperature sensors[J]. Appl. Opt.,1995,34(34):8019-8025.
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[32]WADE S A,COLLINS S F,BAXTER G W. Fluorescence intensity ratio technique for optical fiber point temperature sensing[J]. J. Appl. Phys.,2003,94(8):4743-4756.
[33]MACIEL G S,MENEZES L D,GOMES A S L,et al.. Temperature sensor based on frequency upconversion in Er3+-doped fluoroindate glass[J]. IEEE Photon. Technol. Lett.,1995,7(12):1474-1476.
[34]CHEN Y,CHEN G H,LIU X Y,et al.. Enhanced up-conversion luminescence and optical thermometry characteristics of Er3+/Yb3+co-doped transparent phosphate glass-ceramics[J]. J. Lumin.,2018,195:314-320.
[35]LI X M,CAO J K,WEI Y L,et al.. Optical thermometry based on up-conversion luminescence behavior of Er3+-doped transparent Sr2Yb F7glass-ceramics[J]. J. Am. Ceram. Soc.,2015,98(12):3824-3830.
[36]YU H,LI S,QI Y S,et al.. Optical thermometry based on up-conversion emission behavior of Ba2La F7nano-crystals embedded in glass matrix[J]. J. Lumin.,2018,194:433-439.
[37]CAI J J,WEI X T,HU F F,et al.. Up-conversion luminescence and optical thermometry properties of transparent glass ceramics containing Ca F2∶Yb3+/Er3+nanocrystals[J]. Ceram. Int.,2016,42(12):13990-13995.
[38]CAO J K,CHEN W P,XU D K,et al.. Wide-range thermometry based on green up-conversion of Yb3+/Er3+co-doped KLu2F7transparent bulk oxyfluoride glass ceramics[J]. J. Lumin.,2018,194:219-224.
[39]CAO J K,HU F F,CHEN L P,et al.. Optical thermometry based on up-conversion luminescence behavior of Er3+-doped KYb2F7nano-crystals in bulk glass ceramics[J]. J. Alloys Compd.,2017,693:326-331.
[40]LI X M,CAO J K,HU F F,et al.. Transparent Na5Gd9F32∶Er3+glass-ceramics:enhanced up-conversion luminescence and applications in optical temperature sensors[J]. RSC Adv.,2017,7(56):35147-35153.
[41]HU F F,CAO J K,WEI X T,et al.. Self-crystallized novel transparent Na5Yb9F32∶Er3+glass-ceramics for optical thermometry and spectral conversion[J]. J. Alloys Compd.,2017,722:669-675.
[42]ZOU Z S,WU T,LU H,et al.. Structure,luminescence and temperature sensing in rare earth doped glass ceramics containing Na Y(WO4)2nanocrystals[J]. RSC Adv.,2018,8(14):7679-7686.
[43]HU F F,CAO J K,WEI X T,et al.. Luminescence properties of Er3+-doped transparent Na Yb2F7glass-ceramics for optical thermometry and spectral conversion[J]. J. Mater. Chem. C,2016,4(42):9976-9985.
[44]CHEN D Q,LIU S,LI X Y,et al.. Gd-based oxyfluoride glass ceramics:phase transformation,optical spectroscopy and upconverting temperature sensing[J]. J. Eur. Ceram. Soc.,2017,37(13):4083-4094.
[45]CHEN D Q,WAN Z Y,ZHOU Y,et al.. Bulk glass ceramics containing Yb3+/Er3+∶β-Na Gd F4nanocrystals:phase-separation-controlled crystallization,optical spectroscopy and upconverted temperature sensing behavior[J]. J. Alloys Compd.,2015,638:21-28.
[46]LI C R,DONG B,LI S F,et al.. Er3+-Yb3+co-doped silicate glass for optical temperature sensor[J]. Chem. Phys.Lett.,2007,443(4-6):426-429.
[47]RAKOV N,MACIEL G S. Three-photon upconversion and optical thermometry characterization of Er3+∶Yb3+co-doped yttrium silicate powders[J]. Sens. Actuators B:Chem.,2012,164(1):96-100.
[48]杨艳民,焦福运,苏红新,等. Yb3+/Er3+共掺Ba Gd2Zn O5上转换发光动力学过程的研究[J].光谱学与光谱分析,2012,2(10):2637-2641.YANG Y M,JIAO F Y,SU H X,et al.. Preparation and up-conversion luminescence dynamic process of Yb3+/Er3+codoped Ba Gd2Zn O5[J]. Spectrosc. Spectr. Anal.,2012,32(10):2637-2641.(in Chinese)
[49]JUDD B R. Optical absorption intensities of rare-earth ions[J]. Phys. Rev.,1962,127(3):750-761.
[50]OFELT G S. Intensities of crystal spectra of rare-earth ions[J]. J. Chem. Phys.,1962,37(3):511-520.
[51]JRGENSEN C K,JUDD B R. Hypersensitive pseudoquadrupole transitions in lanthanides[J]. Mol. Phys.,1964,8(3):281-290.
[2]林杨杨,陈铠炀,唐霞艳,等. Er3+/Yb3+共掺杂氧氟硼硅酸盐微晶玻璃绿色上转换发光的温度特性[J].发光学报,2015,36(9):1001-1005.LIN Y Y,CHEN K Y,TANG X Z,et al.. Temperature characteristic of green upconversion luminescence in Er3+/Yb3+codoped oxyfluoride borosilicate glass ceramics[J]. Chin. J. Lumin.,2015,36(9):1001-1005.(in Chinese)
[3]LI D Y,TIAN L L,HUANG Z,et al.. Optical temperature sensor based on infrared excited green upconversion emission in hexagonal phase Na Lu F4∶Yb3+/Er3+nanorods[J]. J. Nanosci. Nanotechnol.,2016,16(4):3641-3645.
[4]ZHENG H,CHEN B J,YU H Q,et al.. Microwave-assisted hydrothermal synthesis and temperature sensing application of Er3+/Yb3+doped Na Y(WO4)2microstructures[J]. J. Colloid Interface Sci.,2014,420:27-34.
[5]SAVCHUK O A,CARVAJAL J J,CASCALES C,et al.. Benefits of silica core-shell structures on the temperature sensing properties of Er,Yb∶Gd VO4up-conversion nanoparticles[J]. ACS Appl. Mater. Interfaces,2016,8(11):7266-7273.
[6]ARAI K,HONDA N,MORI T,et al.. Sensitivity-enhancing scheme of a polarimetric heterodyne sensor using a birefringent fiber loop[J]. Opt. Lett.,1990,15(19):1103-1105.
[7]ZHANG W W,WANG G Y,BAXTER G W,et al.. Methods for broadband spectral analysis:intrinsic fluorescence temperature sensing as an example[J]. Appl. Spectrosc.,2017,71(6):1256-1262.
[8]GAO Y,HUANG F,LIN H,et al.. A novel optical thermometry strategy based on diverse thermal response from two intervalence charge transfer states[J]. Adv. Funct. Mater.,2016,26(18):3139-3145.
[9]DONG B,HUA R N,CAO B S,et al.. Size dependence of the upconverted luminescence of Na YF4∶Er,Yb microspheres for use in ratiometric thermometry[J]. Phys. Chem. Chem. Phys.,2014,16(37):20009-20012.
[10]FANG H W,WEI X T,ZHOU S S,et al.. Terbium and holmium codoped yttrium phosphate as non-contact optical temperature sensors[J]. RSC Adv.,2017,7(17):10200-10205.
[11]VETRONE F,NACCACHE R,ZAMARRN A,et al.. Temperature sensing using fluorescent nanothermometers[J]. ACS Nano,2010,4(6):3254-3258.
[12]SINGH S K,KUMAR K,RAI S B. Er3+/Yb3+codoped Gd2O3nano-phosphor for optical thermometry[J]. Sens. Actuators A:Phys.,2009,149(1):16-20.
[13]JIANG S,ZENG P,LIAO L Q,et al.. Optical thermometry based on upconverted luminescence in transparent glass ceramics containing Na YF4∶Yb3+/Er3+nanocrystals[J]. J. Alloys Compd.,2014,617:538-541.
[14]DUBEY A,SONI A K,KUMARI A,et al.. Enhanced green upconversion emission in Na YF4∶Er3+/Yb3+/Li+phosphors for optical thermometry[J]. J. Alloys Compd.,2017,693:194-200.
[15]MUKHOPADHYAY L,RAI V K,BOKOLIA R,et al.. 980 nm excited Er3+/Yb3+/Li+/Ba2+∶Na Zn PO4upconverting phosphors in optical thermometry[J]. J. Lumin.,2017,187:368-377.
[16]YANG X X,FU Z L,YANG Y M,et al.. Optical temperature sensing behavior of high-efficiency upconversion:Er3+-Yb3+Co-doped Na Y(MoO4)2phosphor[J]. J. Am. Ceram. Soc.,2015,98(8):2595-2600.
[17]MADSEN S J,SUN C H,TROMBERG B J,et al.. Repetitive 5-aminolevulinic acid-mediated photodynamic therapy on human glioma spheroids[J]. J. Neurooncol.,2003,62(3):243-250.
[18]ORION E,MATZ H,WOLFR. Interferons:unapproved uses,dosages,or indications[J]. Clin. Dermatol.,2002,20(5):493-504.
[19]YANG Y M,MI C,JIAO F Y,et al.. A novel multifunctional upconversion phosphor:Yb3+/Er3+codoped La2S3[J]. J.Am. Ceram. Soc.,2014,97(6):1769-1775.
[20]LIU Y F,CHEN W,WANG S P,et al.. Investigation of water-soluble X-ray luminescence nanoparticles for photodynamic activation[J]. Appl. Phys. Lett.,2008,92(4):043901-1-3.
[21]RAHMAN W N,BISHARA N,ACKERLY T,et al.. Enhancement of radiation effects by gold nanoparticles for superficial radiation therapy[J]. Nanomed.:Nanotechnol. Biol. Med.,2009,5(2):136-142.
[22]CARTER J D,CHENG N N,QU Y Q,et al.. Nanoscale energy deposition by X-ray absorbing nanostructures[J]. J.Phys. Chem. B,2007,111(40):11622-11625.
[23]BRIXNER L H. New X-ray phosphors[J]. Mater. Chem. Phys.,1987,16(3-4):253-281.
[24]CHEN H Y,PATRICK A L,YANG Z Q,et al.. High-resolution chemical imaging through tissue with an X-ray scintillator sensor[J]. Anal. Chem.,2011,83(13):5045-5049.
[25]YANG Y M,MI C. Highly sensitive optical thermometry based on the upconversion fluorescence from Yb3+/Er3+codoped La2(WO4)3∶Yb3+,Er3+phosphor[C]. International Conference on Optical Instruments and Technology:Optical Sensors and Applications,Beijing,2013.
[26] LIU G G,FU L L,GAO Z Y,et al.. Investigation into the temperature sensing behavior of Yb3+sensitized Er3+doped Y2O3,YAG and La Al O3phosphors[J]. RSC Adv.,2015,5(64):51820-51827.
[27]YANG Y M,MI C,YU F,et al.. Optical thermometry based on the upconversion fluorescence from Yb3+/Er3+codoped La2O2S phosphor[J]. Ceram. Int.,2013,40(7):9875-9880.
[28]LI X D,SONG Y J,YANG Y M,et al.. Structure and optical thermometry characterization of Er3+/Yb3+co-doped Ba Gd2Cu O5[J]. J. Nanosci. Nanotechnol.,2016,16(4):3542-3546.
[29]刘延洲,杨艳民,郭彦明,等. Er3+∶Yb3+共掺杂Ba Gd2Zn O5纳米晶体上转换光学温度传感[J].光谱学与光谱分析,2015,35(2):329-333.LIU Y Z,YANG Y M,GUO Y M,et al.. Er3+∶Yb3+Co-doped nanocrystals Ba Gd2Zn O5of Up-conversion optical temperature sensing[J]. Spectrosc. Spectr. Anal.,2015,35(2):329-333.(in Chinese)
[30]MAURICE E,MONNOM G,DUSSARDIER B,et al.. Erbium-doped silica fibers for intrinsic fiber-optic temperature sensors[J]. Appl. Opt.,1995,34(34):8019-8025.
[31]SHINN M D,SIBLEY W A,DREXHAGE M G,et al.. Optical transitions of Er3+ions in fluorozirconate glass[J]. Phys.Rev. B,1983,27(11):6635-6648.
[32]WADE S A,COLLINS S F,BAXTER G W. Fluorescence intensity ratio technique for optical fiber point temperature sensing[J]. J. Appl. Phys.,2003,94(8):4743-4756.
[33]MACIEL G S,MENEZES L D,GOMES A S L,et al.. Temperature sensor based on frequency upconversion in Er3+-doped fluoroindate glass[J]. IEEE Photon. Technol. Lett.,1995,7(12):1474-1476.
[34]CHEN Y,CHEN G H,LIU X Y,et al.. Enhanced up-conversion luminescence and optical thermometry characteristics of Er3+/Yb3+co-doped transparent phosphate glass-ceramics[J]. J. Lumin.,2018,195:314-320.
[35]LI X M,CAO J K,WEI Y L,et al.. Optical thermometry based on up-conversion luminescence behavior of Er3+-doped transparent Sr2Yb F7glass-ceramics[J]. J. Am. Ceram. Soc.,2015,98(12):3824-3830.
[36]YU H,LI S,QI Y S,et al.. Optical thermometry based on up-conversion emission behavior of Ba2La F7nano-crystals embedded in glass matrix[J]. J. Lumin.,2018,194:433-439.
[37]CAI J J,WEI X T,HU F F,et al.. Up-conversion luminescence and optical thermometry properties of transparent glass ceramics containing Ca F2∶Yb3+/Er3+nanocrystals[J]. Ceram. Int.,2016,42(12):13990-13995.
[38]CAO J K,CHEN W P,XU D K,et al.. Wide-range thermometry based on green up-conversion of Yb3+/Er3+co-doped KLu2F7transparent bulk oxyfluoride glass ceramics[J]. J. Lumin.,2018,194:219-224.
[39]CAO J K,HU F F,CHEN L P,et al.. Optical thermometry based on up-conversion luminescence behavior of Er3+-doped KYb2F7nano-crystals in bulk glass ceramics[J]. J. Alloys Compd.,2017,693:326-331.
[40]LI X M,CAO J K,HU F F,et al.. Transparent Na5Gd9F32∶Er3+glass-ceramics:enhanced up-conversion luminescence and applications in optical temperature sensors[J]. RSC Adv.,2017,7(56):35147-35153.
[41]HU F F,CAO J K,WEI X T,et al.. Self-crystallized novel transparent Na5Yb9F32∶Er3+glass-ceramics for optical thermometry and spectral conversion[J]. J. Alloys Compd.,2017,722:669-675.
[42]ZOU Z S,WU T,LU H,et al.. Structure,luminescence and temperature sensing in rare earth doped glass ceramics containing Na Y(WO4)2nanocrystals[J]. RSC Adv.,2018,8(14):7679-7686.
[43]HU F F,CAO J K,WEI X T,et al.. Luminescence properties of Er3+-doped transparent Na Yb2F7glass-ceramics for optical thermometry and spectral conversion[J]. J. Mater. Chem. C,2016,4(42):9976-9985.
[44]CHEN D Q,LIU S,LI X Y,et al.. Gd-based oxyfluoride glass ceramics:phase transformation,optical spectroscopy and upconverting temperature sensing[J]. J. Eur. Ceram. Soc.,2017,37(13):4083-4094.
[45]CHEN D Q,WAN Z Y,ZHOU Y,et al.. Bulk glass ceramics containing Yb3+/Er3+∶β-Na Gd F4nanocrystals:phase-separation-controlled crystallization,optical spectroscopy and upconverted temperature sensing behavior[J]. J. Alloys Compd.,2015,638:21-28.
[46]LI C R,DONG B,LI S F,et al.. Er3+-Yb3+co-doped silicate glass for optical temperature sensor[J]. Chem. Phys.Lett.,2007,443(4-6):426-429.
[47]RAKOV N,MACIEL G S. Three-photon upconversion and optical thermometry characterization of Er3+∶Yb3+co-doped yttrium silicate powders[J]. Sens. Actuators B:Chem.,2012,164(1):96-100.
[48]杨艳民,焦福运,苏红新,等. Yb3+/Er3+共掺Ba Gd2Zn O5上转换发光动力学过程的研究[J].光谱学与光谱分析,2012,2(10):2637-2641.YANG Y M,JIAO F Y,SU H X,et al.. Preparation and up-conversion luminescence dynamic process of Yb3+/Er3+codoped Ba Gd2Zn O5[J]. Spectrosc. Spectr. Anal.,2012,32(10):2637-2641.(in Chinese)
[49]JUDD B R. Optical absorption intensities of rare-earth ions[J]. Phys. Rev.,1962,127(3):750-761.
[50]OFELT G S. Intensities of crystal spectra of rare-earth ions[J]. J. Chem. Phys.,1962,37(3):511-520.
[51]JRGENSEN C K,JUDD B R. Hypersensitive pseudoquadrupole transitions in lanthanides[J]. Mol. Phys.,1964,8(3):281-290.