红外激光纳米增益材料制备及大功率激光输出特性研究
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摘要
激光增益介质一般包括固体（例如Nd~(3+):YAG、Yb~(3+):YAG）、半导体（例如GaAs、InP）、液体（例如有机染料溶液、掺Nd~(3+)无机液体）、气体（例如CO_2、He-Ne）等。传统上，这些增益介质都是体材料或块材料。近年来，半导体纳米晶体材料（量子点）作为激光增益介质得到了人们的极大关注。量子点由于其特殊的量子限域效应、量子尺寸效应等，使得其展现出与普通体材料完全不同的光学、电学特性，例如其发光谱由连续谱变为分立的离散谱、发光波长与其尺寸有关、明显的斯托克斯频移，等等，使得其在光电子增益型器件（光放大器、激光器）、太阳能电池、生物医学、示踪剂等方面开拓了极为广阔的应用前景。
本文主要围绕先进制造技术中的加工源――激光器开展工作。由于激光加工光源通常为红外激光器，因此，本文从红外激光增益介质材料制备入手，制备了PbSe量子点玻璃和量子点光纤。提出了新型的波长可调谐的光纤激光器――PbSe量子点光纤激光器（QDFL），分析了其动力学机理，进行了数值计算和模拟，得到了量子点光纤激光具有掺杂饱和浓度低、光纤饱和长度短、泵浦效率高等特点，然而，光纤温升较为明显。同时，针对目前普遍存在的大功率横流CO_2激光光束质量问题展开研究，理论分析了其横模的形成机理，建立了较为完整的激光能级粒子数速率方程，进行了数值计算和模拟，得到了电极结构和气体流速是影响激光横模和功率主要因素的结论。主要工作如下：
1.采用ZnSe代替Se作为PbSe量子点的硒源，通过高温熔融-热处理法，成功制备了较高浓度的PbSe量子点硅酸盐玻璃。通过X射线衍射（XRD）、透射电子显微镜（TEM）、荧光光谱（PL）等方法对PbSe量子点玻璃进行表征。结果表明，制备的PbSe量子点在玻璃中的含量高，且PL峰值强度和FWHM大。同时探索不同热处理条件对量子点尺寸和荧光发射的峰值波长、半高宽和辐射强度的影响。
2.采用高温熔融-热处理法尝试制备PbSe量子点碲酸盐玻璃。通过XRD等方法进行检测，结果表明，碲酸盐玻璃中没有PbSe量子点晶体析出。我们总结分析了实验结果，并对形成原因做了探讨。
3.采用熔融拉丝法，将PbSe量子点硅酸盐玻璃拉制成量子点光纤。用光学显微镜、XRD和TEM等方法对其进行了观测与分析。结果表明，制备的光纤直径均匀、表面光滑、直径与普通光纤接近（125μm）。通过热处理后，光纤中含有一定量的PbSe量子点，其机械性能与普通的SiO_2光纤差不多。
4.利用PbSe量子点作为光纤激光增益介质，基于PbSe量子点的吸收和发射谱，建立了二能级系统的粒子数速率方程、光传播方程和热传导方程，并数值求解之，探索了不同泵浦方式对QDFL输出功率的影响，分析了QDFL的温度分布特点，发现QDFL的温度远高于传统的掺镱光纤激光器，提出了改善QDFL热效应的方案。
5.针对大功率横流CO_2激光器管板式电极结构，由麦克斯韦方程给出电场空间分布，据此求解时空分布的激光能级粒子数速率方程，得到了激光强度的横向分布。实验测量了激光横模，实验结果与数值模拟得到的激光能量分布基本一致。结果表明电极结构决定了激光横模峰值大小，而气体流动速率影响激光增益峰值和峰值沿气流方向出现的位置。
本文的工作为探索和发现新的红外激光增益介质，探讨其激射产生的机理，从而为今后进一步实际研制新型量子点红外激光器提供依据。对大功率CO_2横模机理的分析和研究，有助于改善和控制激光横模，提高激光模式的稳定性，从而提高激光加工的质量。
Laser gain media generally include solids (such as Nd~(3+):YAG, Yd~(3+):YAG),semiconductors (such as GaAs, InP), liquids (such as organic dye solution, Nd~(3+)dopedinorganic solution), and gases (such as CO_2, He-Ne). Conventionally, these gain media arebulk materials. Recently, semiconductor nanocrystal materials, i.e., quantum dots (QDs),which are used as laser gain media, have been attracting considerable attention in the world.Due to quantum confinement effects and quantum size effects, QDs exhibit unique optical andelectrical properties, for instance, discrete emission spectra, tunable emission wavelengths,and obvious Stokes shifts. Then, QD shows widely prospective applications in optoelectronicgain devices (optical amplifiers and lasers), solar cells, biomedical fluorescence probes, andtracers.
This dissertation is concentrated on the laser as a processing tool in the advancedmanufacturing technology. We begin with a preparation of the infrared (IR) lasing gain media,i.e., PbSe QD doped glasses and the QD fibers by using the high-temperature melting methoddue to usual energy source in laser processing is IR lasers. Following a QD doped fiber laser(QDFL) is proposed by analyzing its stimulated radiation mechanism, the lasing outputcharacteristics and temperature dependence in the fiber are simulated numerically. The resultsshow that QDFL has low saturated doping concentration, short saturated fiber length, andhigh pumping efficiency, however, temperature-rise effect can not be neglected. On the otherhand, in order to improve the beam quality of high power transverse-flow CO_2laser, we makea detailed analysis of forming laser transverse mode by establishing and numerically solvingthe lasing level-population rate equations. Obtained results show that the main factorsinfluencing the laser transverse mode and power are the electrode configuration and the gasflowing rate in the CO_2laser resonator.The study mainly includes the following aspects:
1. Using ZnSe as the source of Se for PbSe QDs to replace Se, a silicate glass doped withhigh concentration PbSe QDs is successfully prepared by using the high-temperature meltingmethod. The X-ray diffraction (XRD), transmission electron microscopy (TEM), andfluorescence spectra (PL) show that QD concentration in the glass is higher than that ofelement Se for PbSe QDs in the same thermal treatment condition. Moreover, both the PLpeak intensity and the FWHM are also larger than that of element Se as the source of Se forPbSe QDs. Effect of thermal treatment conditions on the size of QDs, PL peak wavelength, peak intensity, and FWHM are also studied in chapter2.
2. Some types of tellurite glasses doped with PbSe QDs are prepared in laboratory byusing the high-temperature melting method. However, the measured XRD shows that there isno crystal structure of PbSe QDs formed in such prepared glasses. The invalid causes of thismethod are analyzed in chapter3.
3. The PbSe QD doped fiber is fabricated by using the melt-drawing method. Themeasurements of an optical microscope, XRD, and TEM show that the fiber has a fixeddiameter (about125μm, close to the ordinary fiber), smooth surface, and circular cross section.The fiber contains a certain amount of PbSe QDs after thermal treatment. Its mechanicalstrength comes near usual SiO_2fibers.
4. A two-level model is established based on the observed single-peakphotoluminescence of PbSe QD used as the gain medium in the fiber. The optimal parameters(doping concentration, fiber length, and pumping power) of QDFL are determined bynumerically solving the rate equations, power-propagation equation, and heat conductionequation. The laser power and the temperature distribution under different pumpingconfigurations are analyzed. Comparing with the conventional Yd3+doped fiber laser, QDFLshows obvious the temperature rise effect of the fiber due to big absorption cross-section ofPbSe QD. Then, we propose an improvement in experiment to reduce the temperature riseeffect.
5. The lasing transverse energy distribution of a high power tube-plate transverse-flowCO_2laser is simulated numerically by solving the spacetime-resolving rate equations derivedfrom the discharging field determined by the Maxwell equation. It shows that the simulatedlasing distribution agrees with the experimental observation. Moreover, there is evidence toshow that the electrode configuration in the CO_2laser resonator determines the peak value oflasing transverses modes, while the gas flowing rate determines the lasing gain peak and thepeak position along the gas flowing direction.
The work in this dissertation can be helpful for the development of novel IR lasers bypreparing PbSe QD doped glasses, investigating the stimulated emission generated in the QDdoped glass, and the laser propagation in the QD doped fiber. Obtained results for thetransverse mode of high power CO_2laser can be advisable for controlling lasing transversemodes, improving lasing stability, and enhancing the processing quality when the laser is usedas a light source.
本文主要围绕先进制造技术中的加工源――激光器开展工作。由于激光加工光源通常为红外激光器，因此，本文从红外激光增益介质材料制备入手，制备了PbSe量子点玻璃和量子点光纤。提出了新型的波长可调谐的光纤激光器――PbSe量子点光纤激光器（QDFL），分析了其动力学机理，进行了数值计算和模拟，得到了量子点光纤激光具有掺杂饱和浓度低、光纤饱和长度短、泵浦效率高等特点，然而，光纤温升较为明显。同时，针对目前普遍存在的大功率横流CO_2激光光束质量问题展开研究，理论分析了其横模的形成机理，建立了较为完整的激光能级粒子数速率方程，进行了数值计算和模拟，得到了电极结构和气体流速是影响激光横模和功率主要因素的结论。主要工作如下：
1.采用ZnSe代替Se作为PbSe量子点的硒源，通过高温熔融-热处理法，成功制备了较高浓度的PbSe量子点硅酸盐玻璃。通过X射线衍射（XRD）、透射电子显微镜（TEM）、荧光光谱（PL）等方法对PbSe量子点玻璃进行表征。结果表明，制备的PbSe量子点在玻璃中的含量高，且PL峰值强度和FWHM大。同时探索不同热处理条件对量子点尺寸和荧光发射的峰值波长、半高宽和辐射强度的影响。
2.采用高温熔融-热处理法尝试制备PbSe量子点碲酸盐玻璃。通过XRD等方法进行检测，结果表明，碲酸盐玻璃中没有PbSe量子点晶体析出。我们总结分析了实验结果，并对形成原因做了探讨。
3.采用熔融拉丝法，将PbSe量子点硅酸盐玻璃拉制成量子点光纤。用光学显微镜、XRD和TEM等方法对其进行了观测与分析。结果表明，制备的光纤直径均匀、表面光滑、直径与普通光纤接近（125μm）。通过热处理后，光纤中含有一定量的PbSe量子点，其机械性能与普通的SiO_2光纤差不多。
4.利用PbSe量子点作为光纤激光增益介质，基于PbSe量子点的吸收和发射谱，建立了二能级系统的粒子数速率方程、光传播方程和热传导方程，并数值求解之，探索了不同泵浦方式对QDFL输出功率的影响，分析了QDFL的温度分布特点，发现QDFL的温度远高于传统的掺镱光纤激光器，提出了改善QDFL热效应的方案。
5.针对大功率横流CO_2激光器管板式电极结构，由麦克斯韦方程给出电场空间分布，据此求解时空分布的激光能级粒子数速率方程，得到了激光强度的横向分布。实验测量了激光横模，实验结果与数值模拟得到的激光能量分布基本一致。结果表明电极结构决定了激光横模峰值大小，而气体流动速率影响激光增益峰值和峰值沿气流方向出现的位置。
本文的工作为探索和发现新的红外激光增益介质，探讨其激射产生的机理，从而为今后进一步实际研制新型量子点红外激光器提供依据。对大功率CO_2横模机理的分析和研究，有助于改善和控制激光横模，提高激光模式的稳定性，从而提高激光加工的质量。
Laser gain media generally include solids (such as Nd~(3+):YAG, Yd~(3+):YAG),semiconductors (such as GaAs, InP), liquids (such as organic dye solution, Nd~(3+)dopedinorganic solution), and gases (such as CO_2, He-Ne). Conventionally, these gain media arebulk materials. Recently, semiconductor nanocrystal materials, i.e., quantum dots (QDs),which are used as laser gain media, have been attracting considerable attention in the world.Due to quantum confinement effects and quantum size effects, QDs exhibit unique optical andelectrical properties, for instance, discrete emission spectra, tunable emission wavelengths,and obvious Stokes shifts. Then, QD shows widely prospective applications in optoelectronicgain devices (optical amplifiers and lasers), solar cells, biomedical fluorescence probes, andtracers.
This dissertation is concentrated on the laser as a processing tool in the advancedmanufacturing technology. We begin with a preparation of the infrared (IR) lasing gain media,i.e., PbSe QD doped glasses and the QD fibers by using the high-temperature melting methoddue to usual energy source in laser processing is IR lasers. Following a QD doped fiber laser(QDFL) is proposed by analyzing its stimulated radiation mechanism, the lasing outputcharacteristics and temperature dependence in the fiber are simulated numerically. The resultsshow that QDFL has low saturated doping concentration, short saturated fiber length, andhigh pumping efficiency, however, temperature-rise effect can not be neglected. On the otherhand, in order to improve the beam quality of high power transverse-flow CO_2laser, we makea detailed analysis of forming laser transverse mode by establishing and numerically solvingthe lasing level-population rate equations. Obtained results show that the main factorsinfluencing the laser transverse mode and power are the electrode configuration and the gasflowing rate in the CO_2laser resonator.The study mainly includes the following aspects:
1. Using ZnSe as the source of Se for PbSe QDs to replace Se, a silicate glass doped withhigh concentration PbSe QDs is successfully prepared by using the high-temperature meltingmethod. The X-ray diffraction (XRD), transmission electron microscopy (TEM), andfluorescence spectra (PL) show that QD concentration in the glass is higher than that ofelement Se for PbSe QDs in the same thermal treatment condition. Moreover, both the PLpeak intensity and the FWHM are also larger than that of element Se as the source of Se forPbSe QDs. Effect of thermal treatment conditions on the size of QDs, PL peak wavelength, peak intensity, and FWHM are also studied in chapter2.
2. Some types of tellurite glasses doped with PbSe QDs are prepared in laboratory byusing the high-temperature melting method. However, the measured XRD shows that there isno crystal structure of PbSe QDs formed in such prepared glasses. The invalid causes of thismethod are analyzed in chapter3.
3. The PbSe QD doped fiber is fabricated by using the melt-drawing method. Themeasurements of an optical microscope, XRD, and TEM show that the fiber has a fixeddiameter (about125μm, close to the ordinary fiber), smooth surface, and circular cross section.The fiber contains a certain amount of PbSe QDs after thermal treatment. Its mechanicalstrength comes near usual SiO_2fibers.
4. A two-level model is established based on the observed single-peakphotoluminescence of PbSe QD used as the gain medium in the fiber. The optimal parameters(doping concentration, fiber length, and pumping power) of QDFL are determined bynumerically solving the rate equations, power-propagation equation, and heat conductionequation. The laser power and the temperature distribution under different pumpingconfigurations are analyzed. Comparing with the conventional Yd3+doped fiber laser, QDFLshows obvious the temperature rise effect of the fiber due to big absorption cross-section ofPbSe QD. Then, we propose an improvement in experiment to reduce the temperature riseeffect.
5. The lasing transverse energy distribution of a high power tube-plate transverse-flowCO_2laser is simulated numerically by solving the spacetime-resolving rate equations derivedfrom the discharging field determined by the Maxwell equation. It shows that the simulatedlasing distribution agrees with the experimental observation. Moreover, there is evidence toshow that the electrode configuration in the CO_2laser resonator determines the peak value oflasing transverses modes, while the gas flowing rate determines the lasing gain peak and thepeak position along the gas flowing direction.
The work in this dissertation can be helpful for the development of novel IR lasers bypreparing PbSe QD doped glasses, investigating the stimulated emission generated in the QDdoped glass, and the laser propagation in the QD doped fiber. Obtained results for thetransverse mode of high power CO_2laser can be advisable for controlling lasing transversemodes, improving lasing stability, and enhancing the processing quality when the laser is usedas a light source.
引文
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