本文主要研究内容
作者（2019）在《掺杂玻璃和微晶玻璃的光子学应用研究》一文中研究指出：近几十年来,掺杂稀土(RE)离子的氟氧微晶玻璃(GCs)中的上转换(UC)发光由于其在上转换激光、太阳能电池、彩色显示和光学等领域的潜在应用而受到广泛的研究。经过热处理后,稀土离子从氧化物区迁移到析出的氟化物纳米晶(NCs)中,大大降低非辐射跃迁的速率,从而提高发光效率。通过利用稀土离子之间的能量传递或利用过渡金属离子或金属纳米颗粒对稀土离子的敏化,可以提高这类材料中的上转换发光,然而上转换发光相对较低的量子效率(η<1%)仍然是氟氧微晶玻璃应用的面临的主要挑战。从这一角度出发,我们试图通过研究稀土离子周围的局部环境以及对上转换发光有很大影响的局部结构来理解稀土掺杂氟氧微晶玻璃中上转换发光增强机理,并通过更好地了解玻璃和微晶玻璃的详细结构,来进一步提高上转换发光。在第三章中,研究了Er3+-Yb3+共掺的含CaF2纳米晶的透明铝硅酸盐微晶玻璃,并观察到了增强的上转换发光。根据光谱和微结构表征,我们认为氟化物纳米晶的析出与熔融玻璃中富氟域的存在有关,透射电镜观察也支持这一结果。分子动力学模拟结果表明,氟化物纳米晶的析出始于由富氟和富氧区组成的相分离的熔融玻璃,而析晶后稀土离子的空间分布和连接稀土离子的键的振动能量几乎没有变化。在微晶玻璃形成过程中,氟化物区域和稀土离子周围的含氧多面体都会经历显著的有序化,这可能也会影响玻璃和微晶玻璃的上转换发光。因此,我们将微晶玻璃上转换发光的增强归因于析晶后局域有序度的变化以及稀土离子局域对称性的变化,而不是析晶时稀土离子从富氟相向氟化物纳米晶的偏析。在第四章中,发现含有CaF2:Yb3+,Er3+纳米晶的微晶玻璃的上转换发光增强远大于相同掺杂的含LaF3:Yb3+,Er3+纳米晶的微晶玻璃。我们实验和理论研究表明,含CaF2微晶玻璃中更大上转换发光增强可能与两者在显微结构、晶粒尺寸稀土离子周围的局域结构以及硅酸盐区域的结构刚性等方面的差异有关,而低声子能量与观测到的高效上转换发光之间没有联系。此外,还发现在高度有序的硅酸盐区域中均匀分布的纳米晶中,稀土离子周围的配位场的高对称性有利于促进能量传递过程并最大限度地降低非辐射松弛过程的速率。在第五章中,对于纯氧化物微晶玻璃,其中声子能量在结晶前后没有变化,我们研究发现上转换发光在LaBGeO5:Yb3+,Er3+微晶玻璃,表面结晶微晶玻璃和完全结晶的陶瓷和对应的玻璃相比都表现出显著的增强。通过结构表征,我们发现三方结构的LaBGeO5:Yb3+,Er3+纳米晶的成核和结晶首先发生在玻璃表面,然后再向晶体内部生长。利用Eu3+离子作为探针并通过Judd-Osfelt理论计算,我们对稀土离子局域环境的对称性进行了评估,发现对称性随着结晶过程而逐渐提高。因此,完全结晶的LaBGeO5:Yb3+,Er3+陶瓷的具有最大的上转换发光强度。我们将LaBGeO5:Yb3+,Er3+微晶玻璃、表面结晶的微晶玻璃和陶瓷中上转换发光的增强归因于结构有序性的,以及稀土离子局域环境对称性的改变,从而最大限度地降低了非辐射弛豫的速率。综上所述,我们的研究结果丰富了我们对氟化物和氧化物微晶玻璃中上转换发光增强的理解,并为类似体系的上转换发光的增强机制描绘了一个普适的物理图像,从而推动这些体系在光伏、上转换激光等领域的应用。将等离子体纳米结构集成到固态器件中,是实现纳米光子学、生物医学和能源等众多应用的关键一步。除了胶体组装和纳米制造过程,如电子束光刻,也可以直接在透明介质中析出这些等离子体纳米晶,但目前仍然限于少数贵金属纳米颗粒。在第六章中,我们研究表明,超小尺寸(～2 nm)的等离子体Cu2-xSe纳米颗粒可以通过Cu+和Se2-之间的自限域的固相反应从硼硅酸盐玻璃基体中析出,并且所得到的玻璃的局域表面等离子体共振(LSPR)峰的位置可以通过控制反应条件来调节。Cu2-xSe纳米颗粒的强近红外宽带等离子体共振效应使得这一等离子体玻璃具有很强的非线性光学(NLO)响应,表现出显著和激发功率相关的非线性吸收。由于这一Cu2-xSe等离子体纳米颗粒掺杂的玻璃具有优异的非线性光学特性,在光开关以及光限幅等领域有相当应用前景。基于金属-有机框架(MOF)材料的玻璃是一个新发现的可通过熔体淬冷法制备的玻璃体系。在第七章中,我们发现了MOF玻璃的发光行为,即掺杂钴的ZIF-62玻璃[Zn1-x Cox(Im)1.9(bIm)0.1,x=0,0.1和0.5],该玻璃通过将ZIF-62晶体熔化-淬冷后得到。我们所合成的ZIF晶体主要为纳米到微米级的小球,研究发现它具有超高的玻璃形成能力,形成玻璃过程中MOF的长程结构垮塌但是短程有序得到保留。我们观察到了晶体和玻璃相的超宽带中红外(中红外)发光(波长范围为1.5μm4.8 μm),这一中红外发光源于Co-N配体中Co2+离子的d-d跃迁。基于MOF发光玻璃的发现可能为大块MOF玻璃(如中红外激光)的光子学应用铺平道路。
Abstract
jin ji shi nian lai ,can za xi tu (RE)li zi de fu yang wei jing bo li (GCs)zhong de shang zhuai huan (UC)fa guang you yu ji zai shang zhuai huan ji guang 、tai yang neng dian chi 、cai se xian shi he guang xue deng ling yu de qian zai ying yong er shou dao an fan de yan jiu 。jing guo re chu li hou ,xi tu li zi cong yang hua wu ou qian yi dao xi chu de fu hua wu na mi jing (NCs)zhong ,da da jiang di fei fu she yue qian de su lv ,cong er di gao fa guang xiao lv 。tong guo li yong xi tu li zi zhi jian de neng liang chuan di huo li yong guo du jin shu li zi huo jin shu na mi ke li dui xi tu li zi de min hua ,ke yi di gao zhe lei cai liao zhong de shang zhuai huan fa guang ,ran er shang zhuai huan fa guang xiang dui jiao di de liang zi xiao lv (η<1%)reng ran shi fu yang wei jing bo li ying yong de mian lin de zhu yao tiao zhan 。cong zhe yi jiao du chu fa ,wo men shi tu tong guo yan jiu xi tu li zi zhou wei de ju bu huan jing yi ji dui shang zhuai huan fa guang you hen da ying xiang de ju bu jie gou lai li jie xi tu can za fu yang wei jing bo li zhong shang zhuai huan fa guang zeng jiang ji li ,bing tong guo geng hao de le jie bo li he wei jing bo li de xiang xi jie gou ,lai jin yi bu di gao shang zhuai huan fa guang 。zai di san zhang zhong ,yan jiu le Er3+-Yb3+gong can de han CaF2na mi jing de tou ming lv gui suan yan wei jing bo li ,bing guan cha dao le zeng jiang de shang zhuai huan fa guang 。gen ju guang pu he wei jie gou biao zheng ,wo men ren wei fu hua wu na mi jing de xi chu yu rong rong bo li zhong fu fu yu de cun zai you guan ,tou she dian jing guan cha ye zhi chi zhe yi jie guo 。fen zi dong li xue mo ni jie guo biao ming ,fu hua wu na mi jing de xi chu shi yu you fu fu he fu yang ou zu cheng de xiang fen li de rong rong bo li ,er xi jing hou xi tu li zi de kong jian fen bu he lian jie xi tu li zi de jian de zhen dong neng liang ji hu mei you bian hua 。zai wei jing bo li xing cheng guo cheng zhong ,fu hua wu ou yu he xi tu li zi zhou wei de han yang duo mian ti dou hui jing li xian zhe de you xu hua ,zhe ke neng ye hui ying xiang bo li he wei jing bo li de shang zhuai huan fa guang 。yin ci ,wo men jiang wei jing bo li shang zhuai huan fa guang de zeng jiang gui yin yu xi jing hou ju yu you xu du de bian hua yi ji xi tu li zi ju yu dui chen xing de bian hua ,er bu shi xi jing shi xi tu li zi cong fu fu xiang xiang fu hua wu na mi jing de pian xi 。zai di si zhang zhong ,fa xian han you CaF2:Yb3+,Er3+na mi jing de wei jing bo li de shang zhuai huan fa guang zeng jiang yuan da yu xiang tong can za de han LaF3:Yb3+,Er3+na mi jing de wei jing bo li 。wo men shi yan he li lun yan jiu biao ming ,han CaF2wei jing bo li zhong geng da shang zhuai huan fa guang zeng jiang ke neng yu liang zhe zai xian wei jie gou 、jing li che cun xi tu li zi zhou wei de ju yu jie gou yi ji gui suan yan ou yu de jie gou gang xing deng fang mian de cha yi you guan ,er di sheng zi neng liang yu guan ce dao de gao xiao shang zhuai huan fa guang zhi jian mei you lian ji 。ci wai ,hai fa xian zai gao du you xu de gui suan yan ou yu zhong jun yun fen bu de na mi jing zhong ,xi tu li zi zhou wei de pei wei chang de gao dui chen xing you li yu cu jin neng liang chuan di guo cheng bing zui da xian du de jiang di fei fu she song chi guo cheng de su lv 。zai di wu zhang zhong ,dui yu chun yang hua wu wei jing bo li ,ji zhong sheng zi neng liang zai jie jing qian hou mei you bian hua ,wo men yan jiu fa xian shang zhuai huan fa guang zai LaBGeO5:Yb3+,Er3+wei jing bo li ,biao mian jie jing wei jing bo li he wan quan jie jing de tao ci he dui ying de bo li xiang bi dou biao xian chu xian zhe de zeng jiang 。tong guo jie gou biao zheng ,wo men fa xian san fang jie gou de LaBGeO5:Yb3+,Er3+na mi jing de cheng he he jie jing shou xian fa sheng zai bo li biao mian ,ran hou zai xiang jing ti nei bu sheng chang 。li yong Eu3+li zi zuo wei tan zhen bing tong guo Judd-Osfeltli lun ji suan ,wo men dui xi tu li zi ju yu huan jing de dui chen xing jin hang le ping gu ,fa xian dui chen xing sui zhao jie jing guo cheng er zhu jian di gao 。yin ci ,wan quan jie jing de LaBGeO5:Yb3+,Er3+tao ci de ju you zui da de shang zhuai huan fa guang jiang du 。wo men jiang LaBGeO5:Yb3+,Er3+wei jing bo li 、biao mian jie jing de wei jing bo li he tao ci zhong shang zhuai huan fa guang de zeng jiang gui yin yu jie gou you xu xing de ,yi ji xi tu li zi ju yu huan jing dui chen xing de gai bian ,cong er zui da xian du de jiang di le fei fu she chi yu de su lv 。zeng shang suo shu ,wo men de yan jiu jie guo feng fu le wo men dui fu hua wu he yang hua wu wei jing bo li zhong shang zhuai huan fa guang zeng jiang de li jie ,bing wei lei shi ti ji de shang zhuai huan fa guang de zeng jiang ji zhi miao hui le yi ge pu kuo de wu li tu xiang ,cong er tui dong zhe xie ti ji zai guang fu 、shang zhuai huan ji guang deng ling yu de ying yong 。jiang deng li zi ti na mi jie gou ji cheng dao gu tai qi jian zhong ,shi shi xian na mi guang zi xue 、sheng wu yi xue he neng yuan deng zhong duo ying yong de guan jian yi bu 。chu le jiao ti zu zhuang he na mi zhi zao guo cheng ,ru dian zi shu guang ke ,ye ke yi zhi jie zai tou ming jie zhi zhong xi chu zhe xie deng li zi ti na mi jing ,dan mu qian reng ran xian yu shao shu gui jin shu na mi ke li 。zai di liu zhang zhong ,wo men yan jiu biao ming ,chao xiao che cun (～2 nm)de deng li zi ti Cu2-xSena mi ke li ke yi tong guo Cu+he Se2-zhi jian de zi xian yu de gu xiang fan ying cong peng gui suan yan bo li ji ti zhong xi chu ,bing ju suo de dao de bo li de ju yu biao mian deng li zi ti gong zhen (LSPR)feng de wei zhi ke yi tong guo kong zhi fan ying tiao jian lai diao jie 。Cu2-xSena mi ke li de jiang jin gong wai kuan dai deng li zi ti gong zhen xiao ying shi de zhe yi deng li zi ti bo li ju you hen jiang de fei xian xing guang xue (NLO)xiang ying ,biao xian chu xian zhe he ji fa gong lv xiang guan de fei xian xing xi shou 。you yu zhe yi Cu2-xSedeng li zi ti na mi ke li can za de bo li ju you you yi de fei xian xing guang xue te xing ,zai guang kai guan yi ji guang xian fu deng ling yu you xiang dang ying yong qian jing 。ji yu jin shu -you ji kuang jia (MOF)cai liao de bo li shi yi ge xin fa xian de ke tong guo rong ti cui leng fa zhi bei de bo li ti ji 。zai di qi zhang zhong ,wo men fa xian le MOFbo li de fa guang hang wei ,ji can za gu de ZIF-62bo li [Zn1-x Cox(Im)1.9(bIm)0.1,x=0,0.1he 0.5],gai bo li tong guo jiang ZIF-62jing ti rong hua -cui leng hou de dao 。wo men suo ge cheng de ZIFjing ti zhu yao wei na mi dao wei mi ji de xiao qiu ,yan jiu fa xian ta ju you chao gao de bo li xing cheng neng li ,xing cheng bo li guo cheng zhong MOFde chang cheng jie gou kua ta dan shi duan cheng you xu de dao bao liu 。wo men guan cha dao le jing ti he bo li xiang de chao kuan dai zhong gong wai (zhong gong wai )fa guang (bo chang fan wei wei 1.5μm4.8 μm),zhe yi zhong gong wai fa guang yuan yu Co-Npei ti zhong Co2+li zi de d-dyue qian 。ji yu MOFfa guang bo li de fa xian ke neng wei da kuai MOFbo li (ru zhong gong wai ji guang )de guang zi xue ying yong pu ping dao lu 。
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论文作者分别是来自浙江大学的，发表于刊物浙江大学2019-07-04论文，是一篇关于上转换论文,微晶玻璃论文,对称性论文,分子动力学模拟论文,等离子体晶体论文,可饱和吸收论文,金属有机框架论文,浙江大学2019-07-04论文的文章。本文可供学术参考使用，各位学者可以免费参考阅读下载，文章观点不代表本站观点，资料来自浙江大学2019-07-04论文网站，若本站收录的文献无意侵犯了您的著作版权，请联系我们删除。
标签：上转换论文; 微晶玻璃论文; 对称性论文; 分子动力学模拟论文; 等离子体晶体论文; 可饱和吸收论文; 金属有机框架论文; 浙江大学2019-07-04论文;