稀土掺杂激光晶体中无辐射机制的研究及其对离子发光性质的影响
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摘要
稀土离子发光性质的研究,是稀土发光和激光材料和器件研究的基础。在稀土离子发光研究中,无辐射机制的研究是和辐射跃迁研究同等重要的。无辐射机制对离子发光的影响是双方面的:有些无辐射机制只是以热的形式消耗激发光能量,是不利的;但有些无辐射机制却对光子吸收、能量传递、以及特殊能级上的粒子数布居有着重要的辅助作用。因此,要实现理想波长的高效光辐射,不仅要研究稀土离子的辐射特性,还要分析其内部的无辐射机制。本论文从“离子与基质间无辐射相互作用”和“离子间无辐射相互作用”两个方面对稀土激光晶体中的无辐射机制及其对离子发光性质的影响进行了较为系统的理论和实验研究。具体研究内容分为以下两个部分:
一、以Er~(3+)-Yb~(3+)共掺Gd_2SiO_5(GSO)、Lu_2SiO_5(LSO)和(Lu_(0.5)Gd_(0.5))_2SiO_5(LGSO)晶体为研究对象,研究了三种样品的上转换发光、红外发光特性、以及各波段发射强度对温度的依赖关系。分析了多声子辅助弛豫(MPR)和多声子辅助能量传递(MPET)两种“离子与基质间无辐射相互作用”对离子发光的影响。主要研究结果和创新点有:
(1)研究了Er~(3+)-Yb~(3+)共掺GSO、LSO和LGSO晶体的上转换和红外发光性质。三种样品都具有较强的红绿光上转换发射,它们在975 nm半导体激光二极管(LD)激发下的上转换发射效率分别为:0.58×10~(-3)cm~2/W(GSO绿光),1.16×10~(-3)cm~2/W(GSO红光),0.89×10~(-3)cm~2/W(LSO绿光),1.04×10~(-3)cm~2/W(LSO红光),0.83×10~(-3)cm~2/W(LGSO绿光),0.93×10~(-3)cm~2/W(LGSO红光)。三种晶体的1.5μm附近红外发光性质也比较突出,它们在975 nm LD激发下1540 nm附近的发射截面分别达到:1.03×10~(-20)cm~2(GSO),0.793×10~(-20) cm~2(LSO)和0.994×10~(-20) cm~2(LGSO)。
(2)通过分析温度变化对各波段发射强度的影响,着重研究了“离子与基质间无辐射相互作用”对Er~(3+)-Yb~(3+)共掺体系上转换和红外发光的影响。实验结果显示三种晶体的可见和红外波段发射都呈现出有规律的温度依赖特性。另外,三个样品的1.5μm附近红外发光在高温下仍然保持较高的发射效率,在实际应用中是非常具有研究意义的。我们在综合考虑无辐射MPR和MPET机制的基瓷?建立了较完整的速率方程组,较合理地解释了实验结果。
二、以不同浓度Tm~(3+)单掺和Tm~(3+)(高浓度)-Yb~(3+)共掺NaY(WO_4)_2(NYW)晶体为研究对象,研究了离子浓度变化、不同掺杂体系(Tm~(3+)单掺和Tm~(3+)-Yb~(3+)共掺)、以及激发波长对样品蓝色上转换发光的影响。通过对不同情况下发光情况的比较,分析了“离子间无辐射相互作用”交叉弛豫(CR)过程对上转换发光的影响。主要研究结果和创新点有:
(1)测量了不同浓度Tm~(3+)单掺NYW晶体的吸收谱、荧光谱、800 nm LD激发下上转换光谱和红外荧光光谱,结合Judd-Ofelt(J-O)理论和Miyakawa-Dexter's(M-D)理论,分析了Tm~(3+):NYW晶体中的上转换机制和离子浓度对上转换发光的影响。推断出四种影响上转换发光效率的无辐射CR过程:~3H_5+~1G_4→~3H_6+~1D_2,~3H_5+~3H_5→~3H_6+~3F_3,~1G_4+~3H_6→~3F_4+~3F_3,~1G_4+~3H_6→~3F_3+~3F_4,并较好地解释了实验结果。
(2)研究了800 nm和975 nm LD激发下Tm~(3+)(高浓度)-Yb~(3+):NYW晶体的发光性质。通过与同浓度单掺样品的上转换和红外发光结果进行比较,并结合两种情况下CR几率的M-D理论计算结果,得出:共掺Yb~(3+)离子,除了能够提高激发光吸收效率外,还具有减弱激活离子间无辐射CR机制的效果,从而提高蓝光上转换发射效率;改变激发光的波长,虽然不影响CR过程的发生几率,但会改变上转换机制的整体步骤,从而减弱或消除某些不利的CR过程,或者将其变为对某些能级粒子数布居有利的机制,实现了控制离子间无辐射相互作用来提高发射效率的目的。
以上研究结果表明,无论是“离子与基质间无辐射相互作用”(MPR和MPET),还是“离子间无辐射相互作用”(CR),对稀土离子发光都有重要的影响。这些过程都具有一定的发生规律和影响因素,因此,适当地控制外界条件,能够使这些无辐射机制对某些频率的发射起到积极的作用。
Non-radiative mechanisms in rare-earth ions doped crystals were researched from two aspects:"non-radiative interaction between ions and host material" and "non-radiative interaction between doped ions".The main research includes two parts.
Upconversion(UC),infrared emission(near 1540 nm),and the temperature dependent luminescence properties of Er~(3+)-yb~(3+) co-doped Gd_2SiO_5(GSO),Lu_2SiO_5 (LSO) and(Lu_(0.5)Gd_(0.5))_2SiO_5(LGSO) laser crystals are researched.The UC emission bandwidth is very broad containing multiple peaks,and the normalized UC efficiencies can reach up to 0.58×10~(-3) cm~2/W(GSO,green emission),1.16×10~(-3) cm~2/W(GSO,red emission),0.89×10~(-3) cm~2/W(LSO,green emission),1.04×10~(-3) cm~2/W(LSO,red emission),0.83×10~(-3) cm~2/W(LGSO,green emission),and 0.93×10~(-3) cm~2/W(LGSO,red emission).Broad infrared emission(1540 nm) in Er~(3+)-yb~(3+) co-doped LSO and LGSO crystals are measured under excitation of 975 nm.The emission cross-section near 1540 nm can reach up to 0.793×10~(-20) cm~2(LSO) and 0.994×10~(-20) cm~2(LGSO),respectively.The temperature-dependent luminescence properties of these crystals are also investigated.Upconversion near The rate equations considering the multi-phonon assistant relaxations(MPR) and multi-phonon assistant energy transfer(MPET) as the temperature-dependent functions were adopted to analyze the results.Our study indicates that Er~(3+)-Yb~(3+) co-doped GSO,LSO and LGSO crystals are promising gain media for developing the solid-state 1.5μm optical amplifiers and tunable UC lasers.
Upconversion blue emissions of Tm~(3+) ions doped NaY(WO_4)_2(NYW) crystals are investigated with different doping concentration and three different near-infrared pump mechanisms(800 nm pump Tm~(3+):NYW,800 nm pump Tm~(3+)-Yb~(3+):NYW,980 nm pump Tm~(3+)-Yb~(3+):NYW).The dependence of upconversion efficiency on ion concentration and pump mechanisms is analyzed from the scope of concentration quenching effect.Four cross relaxation(CR) processes:~3H_5 +~1G_4→~3H_6 +~1D_2,~3H_5+ ~3H_5→~3H_6 +~3F_3,~1G_4 +~3H_6→~3F_4 +~3F_3,~1G_4 +~3H_6→~3F_3 +~3F_4,which influence the upconversion dominantly in Tm~(3+) heavy-doped system,are demonstrated theoretically and experimentally.The results indicate that Yb~(3+) ions can weaken the concentration quenching effect of Tm~(3+) ions significantly so that the blue emission efficiency can be enhanced by one order of magnitude.At the same time,the wavelength of pump source also has considerable influence on both the population of some crucial energy levels and the upconversion mechanism.Experiments show that the upconversion blue emission in Tm~(3+)/Yb~(3+) co-doped NaY(WO_4)_2 crystal under 980 nm LD excitation is the most intensive of these three different near-infrared pump mechanisms.The conclusions are confirmed by spectra measurements and calculations of Judd-Ofelt(J-O) theory and Miyakawa -Dexter's(M-D) theory.
Our work shows that both "non-radiative interaction between ions and host material"(MPR and MPET) and "non-radiative interaction between ions"(CR) are the improtant influencing factors to the luminescence properties.The rules of these non-radiative energy transfer mechanisms can be investigated and found,and they can be controlled to be benefitial to some specifical radiation.
一、以Er~(3+)-Yb~(3+)共掺Gd_2SiO_5(GSO)、Lu_2SiO_5(LSO)和(Lu_(0.5)Gd_(0.5))_2SiO_5(LGSO)晶体为研究对象,研究了三种样品的上转换发光、红外发光特性、以及各波段发射强度对温度的依赖关系。分析了多声子辅助弛豫(MPR)和多声子辅助能量传递(MPET)两种“离子与基质间无辐射相互作用”对离子发光的影响。主要研究结果和创新点有:
(1)研究了Er~(3+)-Yb~(3+)共掺GSO、LSO和LGSO晶体的上转换和红外发光性质。三种样品都具有较强的红绿光上转换发射,它们在975 nm半导体激光二极管(LD)激发下的上转换发射效率分别为:0.58×10~(-3)cm~2/W(GSO绿光),1.16×10~(-3)cm~2/W(GSO红光),0.89×10~(-3)cm~2/W(LSO绿光),1.04×10~(-3)cm~2/W(LSO红光),0.83×10~(-3)cm~2/W(LGSO绿光),0.93×10~(-3)cm~2/W(LGSO红光)。三种晶体的1.5μm附近红外发光性质也比较突出,它们在975 nm LD激发下1540 nm附近的发射截面分别达到:1.03×10~(-20)cm~2(GSO),0.793×10~(-20) cm~2(LSO)和0.994×10~(-20) cm~2(LGSO)。
(2)通过分析温度变化对各波段发射强度的影响,着重研究了“离子与基质间无辐射相互作用”对Er~(3+)-Yb~(3+)共掺体系上转换和红外发光的影响。实验结果显示三种晶体的可见和红外波段发射都呈现出有规律的温度依赖特性。另外,三个样品的1.5μm附近红外发光在高温下仍然保持较高的发射效率,在实际应用中是非常具有研究意义的。我们在综合考虑无辐射MPR和MPET机制的基瓷?建立了较完整的速率方程组,较合理地解释了实验结果。
二、以不同浓度Tm~(3+)单掺和Tm~(3+)(高浓度)-Yb~(3+)共掺NaY(WO_4)_2(NYW)晶体为研究对象,研究了离子浓度变化、不同掺杂体系(Tm~(3+)单掺和Tm~(3+)-Yb~(3+)共掺)、以及激发波长对样品蓝色上转换发光的影响。通过对不同情况下发光情况的比较,分析了“离子间无辐射相互作用”交叉弛豫(CR)过程对上转换发光的影响。主要研究结果和创新点有:
(1)测量了不同浓度Tm~(3+)单掺NYW晶体的吸收谱、荧光谱、800 nm LD激发下上转换光谱和红外荧光光谱,结合Judd-Ofelt(J-O)理论和Miyakawa-Dexter's(M-D)理论,分析了Tm~(3+):NYW晶体中的上转换机制和离子浓度对上转换发光的影响。推断出四种影响上转换发光效率的无辐射CR过程:~3H_5+~1G_4→~3H_6+~1D_2,~3H_5+~3H_5→~3H_6+~3F_3,~1G_4+~3H_6→~3F_4+~3F_3,~1G_4+~3H_6→~3F_3+~3F_4,并较好地解释了实验结果。
(2)研究了800 nm和975 nm LD激发下Tm~(3+)(高浓度)-Yb~(3+):NYW晶体的发光性质。通过与同浓度单掺样品的上转换和红外发光结果进行比较,并结合两种情况下CR几率的M-D理论计算结果,得出:共掺Yb~(3+)离子,除了能够提高激发光吸收效率外,还具有减弱激活离子间无辐射CR机制的效果,从而提高蓝光上转换发射效率;改变激发光的波长,虽然不影响CR过程的发生几率,但会改变上转换机制的整体步骤,从而减弱或消除某些不利的CR过程,或者将其变为对某些能级粒子数布居有利的机制,实现了控制离子间无辐射相互作用来提高发射效率的目的。
以上研究结果表明,无论是“离子与基质间无辐射相互作用”(MPR和MPET),还是“离子间无辐射相互作用”(CR),对稀土离子发光都有重要的影响。这些过程都具有一定的发生规律和影响因素,因此,适当地控制外界条件,能够使这些无辐射机制对某些频率的发射起到积极的作用。
Non-radiative mechanisms in rare-earth ions doped crystals were researched from two aspects:"non-radiative interaction between ions and host material" and "non-radiative interaction between doped ions".The main research includes two parts.
Upconversion(UC),infrared emission(near 1540 nm),and the temperature dependent luminescence properties of Er~(3+)-yb~(3+) co-doped Gd_2SiO_5(GSO),Lu_2SiO_5 (LSO) and(Lu_(0.5)Gd_(0.5))_2SiO_5(LGSO) laser crystals are researched.The UC emission bandwidth is very broad containing multiple peaks,and the normalized UC efficiencies can reach up to 0.58×10~(-3) cm~2/W(GSO,green emission),1.16×10~(-3) cm~2/W(GSO,red emission),0.89×10~(-3) cm~2/W(LSO,green emission),1.04×10~(-3) cm~2/W(LSO,red emission),0.83×10~(-3) cm~2/W(LGSO,green emission),and 0.93×10~(-3) cm~2/W(LGSO,red emission).Broad infrared emission(1540 nm) in Er~(3+)-yb~(3+) co-doped LSO and LGSO crystals are measured under excitation of 975 nm.The emission cross-section near 1540 nm can reach up to 0.793×10~(-20) cm~2(LSO) and 0.994×10~(-20) cm~2(LGSO),respectively.The temperature-dependent luminescence properties of these crystals are also investigated.Upconversion near The rate equations considering the multi-phonon assistant relaxations(MPR) and multi-phonon assistant energy transfer(MPET) as the temperature-dependent functions were adopted to analyze the results.Our study indicates that Er~(3+)-Yb~(3+) co-doped GSO,LSO and LGSO crystals are promising gain media for developing the solid-state 1.5μm optical amplifiers and tunable UC lasers.
Upconversion blue emissions of Tm~(3+) ions doped NaY(WO_4)_2(NYW) crystals are investigated with different doping concentration and three different near-infrared pump mechanisms(800 nm pump Tm~(3+):NYW,800 nm pump Tm~(3+)-Yb~(3+):NYW,980 nm pump Tm~(3+)-Yb~(3+):NYW).The dependence of upconversion efficiency on ion concentration and pump mechanisms is analyzed from the scope of concentration quenching effect.Four cross relaxation(CR) processes:~3H_5 +~1G_4→~3H_6 +~1D_2,~3H_5+ ~3H_5→~3H_6 +~3F_3,~1G_4 +~3H_6→~3F_4 +~3F_3,~1G_4 +~3H_6→~3F_3 +~3F_4,which influence the upconversion dominantly in Tm~(3+) heavy-doped system,are demonstrated theoretically and experimentally.The results indicate that Yb~(3+) ions can weaken the concentration quenching effect of Tm~(3+) ions significantly so that the blue emission efficiency can be enhanced by one order of magnitude.At the same time,the wavelength of pump source also has considerable influence on both the population of some crucial energy levels and the upconversion mechanism.Experiments show that the upconversion blue emission in Tm~(3+)/Yb~(3+) co-doped NaY(WO_4)_2 crystal under 980 nm LD excitation is the most intensive of these three different near-infrared pump mechanisms.The conclusions are confirmed by spectra measurements and calculations of Judd-Ofelt(J-O) theory and Miyakawa -Dexter's(M-D) theory.
Our work shows that both "non-radiative interaction between ions and host material"(MPR and MPET) and "non-radiative interaction between ions"(CR) are the improtant influencing factors to the luminescence properties.The rules of these non-radiative energy transfer mechanisms can be investigated and found,and they can be controlled to be benefitial to some specifical radiation.
引文
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