稀土掺杂红外下转换材料研究
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摘要
近几年来,随着人们对能源问题和环境问题的日益关注,开发清洁、可再生的新能源成了各国发展战略的重点。太阳能由于具有清洁环保、利用价值高,并且取之不尽用之不竭等优点,而被人们寄予厚望。如何提高太阳能电池的能量转换效率成了人们研究的热点。红外下转换材料可以将硅太阳能电池响应较差的高能光子转换成为响应较好的近红外光子,并且量子效率有望超过100%,因此受到研究人员的广泛关注。我们就红外下转换材料中存在的问题,进行了深入研究。本论文将介绍相关研究内容。
论文包含四章,绪论部分介绍了相关的基本知识和研究背景,第二至第四章分别介绍了三种不同基质的红外下转换材料的研究结果。
第二章介绍的是在蓝色荧光粉BAM:Eu2+中掺入yb3+来实现宽带激发红外下转换的尝试。BAM:Eu2+为已经商品化的蓝色荧光粉,研究与应用已经比较成熟。BAM:Eu2+,Yb3+尚未有人研究,如果能实现高效的红外下转换,将有很好的应用前景。我们用燃烧法制备了成相良好的BAM:Eu2+,Yb3+样品,并成功观察到了宽带激发的红外下转换发光。但由Ef+的发光强度和衰减随yb3+的掺杂浓度的变化关系,发现BAM中Eu2+→Yb3+能量传递效率较低。经过对BAM结构以及能量传递机理的分析,我们认为主要原因是稀土离子在BAM中取代的是Ba2+,而Ba2+的格位之间距离太长。该工作为红外下转换材料中基质的选择提供了一些思路。
第三章介绍了以YAG为基质,Ce3+-Yb3+、Tb3+-Yb3+、Pr3+-Yb3+三个系列红外下转换材料的发光性质和机理。我们用相同的方法和条件合成了YAG:Ce3+,Yb3+、YAG:Tb3+,Yb3+和YAG:Pr3+,Yb3+三个系列样品,都观察到了红外下转换发光。由这三个系列发光性质的对比,证明Ce3+-Yb3+、Tb3+-Yb3+、 Pr3+-Yb3+这三种离子对的能量传递机理各不相同,分别为电荷迁移态能量传递、共合作能量传递和分步能量传递。并且由这三种离子对激发和发射光谱的对比,说明Ce3+-YB3+比其它两种离子对更适合用于提高太阳能电池的效率,为红外下转换材料的进一步研究中关于离子对的选择提供了有价值的参考。
第四章介绍了一种用基质吸收紫外光子的红外下转换材料。此前的红外下转换材料研究都是选择在400多纳米具有发光的材料,以匹配yb3+的4f能级差的2倍,实现共合作能量传递。我们首次在不发光的Y2MoO6基质中掺杂yb3+实现了红外下转换。Y2MoO6:Yb3+在波长大于350nm的区域也有很强吸收,与之前的基质吸收红外下转换材料相比,距离用于提高太阳能电池效率的目标更近了一步。该工作对于基质到Yb3+能量传递的机理以及红外下转换材料基质的选择具有启发意义。目前稀土掺杂的Y2MoO6发光材料研究还比较少,我们用Eu3+作为“探针”,通过选择激发的低温高分辨光谱对稀土离子在该基质中占据格位的数目以及对称性等进行了研究。实验结果表明材料中存在3个发光中心,分别对应Y2MoO6中Y3+的3种格位；掺杂浓度不同,稀土离子在3种格位的占据比例也有所不同；温度较高时三种格位的稀土离子存在能量传递。该工作对于Y2MoO6在发光以及其它领域的进一步研究具有一定参考价值。
In recent years, as people increasingly concerned about energy and environmental problems, the new energy resources has become a hot topic. The research on solar power attracts great attentions. Enhancing the energy conversion efficiency of solar cells is an important issue of concern. Infrared downconversion materials, which can convert one high-energy photon into two or more low-energy infrared photons which can be better absorbed by silicon crystal, is a promising approach to enhance the energy conversion efficiency of Si solar cells. We conducted intensive studies on the infrared downconversion materials in expectation of their potential application in solar cell. This paper presents our research results.
In chapter one, fundamental knowledge and research backgro und is introduced. The second to fourth chapters discuss three kinds of infrared downconversion materials doped with rare earth ions.
In chapter two, we attempted to achieve broadband excitation infrared downconversion in BAM:Eu2+,Yb3+. BAM:Eu2+, has been well studied as a blue phosphor in commercial use. BAM:Eu2+,Yb3+has not been investigated before, if it can achieve efficient infrared downconversion, it will have a good prospect of application We synthesized pure-phase Eu2+and Yb3+co-doped BAM by combustion method. When excited by UV light, blue and infrared emissions were both observed. The excitation spectra monitoring Yb3+emission matches well with the Eu2+4f7→4f65d1absorption, verifying the energy transfers from Eu2+to Yb3+. Luminescence intensity and the decay curves of the Eu2+emission hardly change with increasing Yb3+concentration. The results indicate the efficiency of energy transfer is low, which need to be improved in the future work for enhancing the solar cells efficiency.
Chapter three presents three infrared downconversion series doped with Ce3+-Yb3+, Tb3+-Yb3+, Pr3+-Yb3+respectively in YAG host. YAG:Ce3+,Yb3+, YAG:Tb3+,Yb3+and YAG:Pr3+,Yb3+samples were synthesised by co-precipitation method. Infrared downconversion luminescence were observed in all codoped samples. Experimental evidences of energy transfer from Ce3+, Tb3+and Pr3+to Yb3+were presented by the excitation spectra and decay curves. By contrast the energy transfer efficiency, we concluded that energy transfer mechanisms of Ce3+to Yb3+, Tb3+to Yb3+and Pr3+to Yb3+are different. The results also show that YAG:Ce3+,Yb3+ is suitable for spectral modification aiming at improving the efficiency of solar cells.
In chapter four we investigated single doped infrared downconversion materials. Upon ultraviolet light excitation, intense infrared emissions of Yb3+around974nm was observed in Y2MoO6:Yb3+samples. Owing to host absorption of Y2MoO6, a broad excitation band ranging from260to420nm was detected when the infrared emission was monitored, suggesting efficient energy transfer from host to Yb3+. Using Eu3+as a probe, low temperature high resolution emission and excitation spectra have been employed to study the local site symmetrys of the Y3+sites occupied by rare earth ions in Y2MoO6. Site selective excitation has shown three different luminescent centers, which correspond with three Y3+sites in Y2MoO6.
论文包含四章,绪论部分介绍了相关的基本知识和研究背景,第二至第四章分别介绍了三种不同基质的红外下转换材料的研究结果。
第二章介绍的是在蓝色荧光粉BAM:Eu2+中掺入yb3+来实现宽带激发红外下转换的尝试。BAM:Eu2+为已经商品化的蓝色荧光粉,研究与应用已经比较成熟。BAM:Eu2+,Yb3+尚未有人研究,如果能实现高效的红外下转换,将有很好的应用前景。我们用燃烧法制备了成相良好的BAM:Eu2+,Yb3+样品,并成功观察到了宽带激发的红外下转换发光。但由Ef+的发光强度和衰减随yb3+的掺杂浓度的变化关系,发现BAM中Eu2+→Yb3+能量传递效率较低。经过对BAM结构以及能量传递机理的分析,我们认为主要原因是稀土离子在BAM中取代的是Ba2+,而Ba2+的格位之间距离太长。该工作为红外下转换材料中基质的选择提供了一些思路。
第三章介绍了以YAG为基质,Ce3+-Yb3+、Tb3+-Yb3+、Pr3+-Yb3+三个系列红外下转换材料的发光性质和机理。我们用相同的方法和条件合成了YAG:Ce3+,Yb3+、YAG:Tb3+,Yb3+和YAG:Pr3+,Yb3+三个系列样品,都观察到了红外下转换发光。由这三个系列发光性质的对比,证明Ce3+-Yb3+、Tb3+-Yb3+、 Pr3+-Yb3+这三种离子对的能量传递机理各不相同,分别为电荷迁移态能量传递、共合作能量传递和分步能量传递。并且由这三种离子对激发和发射光谱的对比,说明Ce3+-YB3+比其它两种离子对更适合用于提高太阳能电池的效率,为红外下转换材料的进一步研究中关于离子对的选择提供了有价值的参考。
第四章介绍了一种用基质吸收紫外光子的红外下转换材料。此前的红外下转换材料研究都是选择在400多纳米具有发光的材料,以匹配yb3+的4f能级差的2倍,实现共合作能量传递。我们首次在不发光的Y2MoO6基质中掺杂yb3+实现了红外下转换。Y2MoO6:Yb3+在波长大于350nm的区域也有很强吸收,与之前的基质吸收红外下转换材料相比,距离用于提高太阳能电池效率的目标更近了一步。该工作对于基质到Yb3+能量传递的机理以及红外下转换材料基质的选择具有启发意义。目前稀土掺杂的Y2MoO6发光材料研究还比较少,我们用Eu3+作为“探针”,通过选择激发的低温高分辨光谱对稀土离子在该基质中占据格位的数目以及对称性等进行了研究。实验结果表明材料中存在3个发光中心,分别对应Y2MoO6中Y3+的3种格位；掺杂浓度不同,稀土离子在3种格位的占据比例也有所不同；温度较高时三种格位的稀土离子存在能量传递。该工作对于Y2MoO6在发光以及其它领域的进一步研究具有一定参考价值。
In recent years, as people increasingly concerned about energy and environmental problems, the new energy resources has become a hot topic. The research on solar power attracts great attentions. Enhancing the energy conversion efficiency of solar cells is an important issue of concern. Infrared downconversion materials, which can convert one high-energy photon into two or more low-energy infrared photons which can be better absorbed by silicon crystal, is a promising approach to enhance the energy conversion efficiency of Si solar cells. We conducted intensive studies on the infrared downconversion materials in expectation of their potential application in solar cell. This paper presents our research results.
In chapter one, fundamental knowledge and research backgro und is introduced. The second to fourth chapters discuss three kinds of infrared downconversion materials doped with rare earth ions.
In chapter two, we attempted to achieve broadband excitation infrared downconversion in BAM:Eu2+,Yb3+. BAM:Eu2+, has been well studied as a blue phosphor in commercial use. BAM:Eu2+,Yb3+has not been investigated before, if it can achieve efficient infrared downconversion, it will have a good prospect of application We synthesized pure-phase Eu2+and Yb3+co-doped BAM by combustion method. When excited by UV light, blue and infrared emissions were both observed. The excitation spectra monitoring Yb3+emission matches well with the Eu2+4f7→4f65d1absorption, verifying the energy transfers from Eu2+to Yb3+. Luminescence intensity and the decay curves of the Eu2+emission hardly change with increasing Yb3+concentration. The results indicate the efficiency of energy transfer is low, which need to be improved in the future work for enhancing the solar cells efficiency.
Chapter three presents three infrared downconversion series doped with Ce3+-Yb3+, Tb3+-Yb3+, Pr3+-Yb3+respectively in YAG host. YAG:Ce3+,Yb3+, YAG:Tb3+,Yb3+and YAG:Pr3+,Yb3+samples were synthesised by co-precipitation method. Infrared downconversion luminescence were observed in all codoped samples. Experimental evidences of energy transfer from Ce3+, Tb3+and Pr3+to Yb3+were presented by the excitation spectra and decay curves. By contrast the energy transfer efficiency, we concluded that energy transfer mechanisms of Ce3+to Yb3+, Tb3+to Yb3+and Pr3+to Yb3+are different. The results also show that YAG:Ce3+,Yb3+ is suitable for spectral modification aiming at improving the efficiency of solar cells.
In chapter four we investigated single doped infrared downconversion materials. Upon ultraviolet light excitation, intense infrared emissions of Yb3+around974nm was observed in Y2MoO6:Yb3+samples. Owing to host absorption of Y2MoO6, a broad excitation band ranging from260to420nm was detected when the infrared emission was monitored, suggesting efficient energy transfer from host to Yb3+. Using Eu3+as a probe, low temperature high resolution emission and excitation spectra have been employed to study the local site symmetrys of the Y3+sites occupied by rare earth ions in Y2MoO6. Site selective excitation has shown three different luminescent centers, which correspond with three Y3+sites in Y2MoO6.
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