三价镧系离子发光的超快相干控制
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摘要
稀土离子的发光谱可以从近红外到可见,甚至到紫外波段。稀土离子发光的增强和调谐对其在生物荧光标记,发光显示,光存储和固体激光器等领域的应用有着重要的意义。基于飞秒脉冲整形的相干量子控制技术广泛用于研究光与物质材料的非线性相互作用,特别是用于研究多光子吸收,高次谐波,拉曼散射,共振增强多光子电离光电子谱。本论文基于飞秒脉冲整形的相干控制技术,理论和实验研究了部分三价稀土离子的发光增强与调谐。具体研究内容如下：
(1)介绍了稀土离子的发光特性,稀土离子上转换发光机制,常见的调谐和增强稀土离子上转换发光的方法。综述了相干控制的思想,脉冲整形技术,和常用的多光子跃迁理论。
(2)π相位调制的超短激光脉冲激发Pr3+离子可以使双光子吸收几率增强到12.3倍。整形脉冲对应双光子吸收几率远远大于傅里叶变换受限脉冲对应的双光子吸收几率。但是,整形脉冲的光强是傅里叶变换受限脉冲光强的37%。π相位调制也可以使双光子吸收几率降低到傅里叶变换受限脉冲双光子吸收几率的58%。我们讨论了中间态能级漂移和末态能级展宽对双光吸收几率的影响。
(3)分别对中心频率位于10650cm-1和7650cm-1的超短激光脉冲进行相位调制,激发Er3+, Tm3+, Yb3+共掺的稀土离子实现双光子吸收和发光的相干控制。与傅里叶变换受限脉冲对应的双光子吸收相比,整形脉冲对应的蓝,绿,红的双光子吸收几率可以分别在0-13.3,0-14.5,0-1.0范围内调制。镧系离子能级结构和激光频谱对相干特性的影响也做了讨论。蓝光和绿光的双光子吸收几率会随着激光频谱带宽增加而增加,随着末态能级带宽增加而减小。如果中间能级在10100-10500cm-1范围内漂移,蓝光和绿光的双光子跃迁几率的变化范围分别为7-15和8-17。
(4)我们从实验和理论上研究了7π相位整形的800nm飞秒激光脉冲对Er3+掺杂的玻璃样品的绿光的量子相干控制。实验结果表明,随着激光脉冲的强度增强到几个10'2W/cm2,π相位整形脉冲对应的绿光发光强度可以超越傅里叶变换受限脉冲对应的绿光发光强度。根据四阶微扰理论研究了双光子和四光子过程的相干控制,很好的解释了实验结果。
(5)由于飞秒激光脉冲激光频谱较宽,飞秒激发共振增强多光子电离光电子谱有两个缺点：分辨率低,选择性差。我们提出用π相位和余弦相位组合的相位调制方法实现Na原子(2+1)共振增强多光子电离光电子谱的高分辨选择激发。我们的理论结果表明,π相位调制能够有效的提高(2+1)共振增强多光子电离光电子能谱的分辨率,再加一个余弦相位调制可以实现两个相邻激发态的选择激发。
The emission spectrum of rare earth ions spans near-infrared to visible, even to ultraviolet band. The tunable and tense upconversion emission of rare earth ions is very important for these applications in biological labeling, light emitting displays, optical data storage, and solid-state lasers. Quantum coherent control based on the femtosecond pulse shaping is widely used to study the nonlinear processes between the light and the materiel, for example, multiphoton absorption, Raman scattering, higher harmonics, resonance-enhanced multiphoton-ionization photoelectron spectroscopy. In this thesis, the enhancing and tuning of trivalent rare earth ions have been studied theoretically and experimentally by quantum coherent control based on the femtosecond pulse shaping. The main research contents are as follows:
(1) The luminescence properties of rare earth ions, the mechanism of upconversion luminescence, and the common method for tuning and enhancing upconversion emission were systematically introduced. The idea of coherent control, pulse shaping technique, and the multiphoton transition theory were simply reviewed.
(2) The two-photon absorption (TPA) probability in a Pr3+ion system is enhanced to12.3by the shaped ultrashort laser pulses. The TPA is significantly higher than that achieved by a transform-limit pulse. However, the laser intensity of shaped pulses is reduced to37%of the initial transform-limited pulse. In this method, the TPA probability can also be reduced to58%. Furthermore, the effect of the shift of the intermediate energy level and the bandwidth of final states on TPA probability was discussed.
(3) We presented a new scheme for quantum coherent control of two-photon absorption (TPA) and color emission in codoped lanthanide ions of Er3+/Tm3+/Yb3+ by properly phase shaping two infrared ultrashort laser beams at central frequencies of10650cm-1and7650cm-1, respectively. Compared with the results irradiated by transform-limited pulses, the TPA probabilities of the blue, green and red emissions are independently controlled in the ranges0-13.3,0-14.5and0-1.0, respectively. The effects of the energy states of lanthanide ions and the laser spectral bandwidths on the coherent features were also discussed. The TPA probabilities for the blue and green emissions increase with the laser spectral bandwidths and decrease with the energy bandwidths of the final level states. As the intermediate energy level shifts in the range10100-10500cm-1, the TPA probabilities for the blue and green emissions change in the ranges7-15and8-17, respectively.
(4) We experimentally and theoretically studied the coherent quantum control of green emission in Er3+-doped glass by π-phase-shaped800nm femtosecond laser pulses. The experimental results show that the green emission intensity is enhanced over the transform-limited pulse by7r-phase-shaped pulses as the laser field increases to several1012W/cm2. Coherent control of multiphoton absorption is studied based on the fourth-order perturbation theory, and the theoretical results accord well with the experimental observations.
(5) Femtosecond laser-induced resonance-enhanced multiphoton-ionization photoelectron spectroscopy (REMPI-PS) is faced with two drawbacks of low spectral resolution and poor selective excitation due to the broad spectral bandwidth. We proposed a scheme to obtain a high-resolution selective excitation of (2+1) REMPI-PS by combining π and cosinusoidal phase modulation. Our theoretical results indicate that the (2+1) REMPI-PS signals related to neighboring excited states can be differentiated from their indistinguishable photoelectron spectra by the π phase modulation, and then their selective excitation can be realized by supplementally adding the cosinusoidal phase modulation.
(1)介绍了稀土离子的发光特性,稀土离子上转换发光机制,常见的调谐和增强稀土离子上转换发光的方法。综述了相干控制的思想,脉冲整形技术,和常用的多光子跃迁理论。
(2)π相位调制的超短激光脉冲激发Pr3+离子可以使双光子吸收几率增强到12.3倍。整形脉冲对应双光子吸收几率远远大于傅里叶变换受限脉冲对应的双光子吸收几率。但是,整形脉冲的光强是傅里叶变换受限脉冲光强的37%。π相位调制也可以使双光子吸收几率降低到傅里叶变换受限脉冲双光子吸收几率的58%。我们讨论了中间态能级漂移和末态能级展宽对双光吸收几率的影响。
(3)分别对中心频率位于10650cm-1和7650cm-1的超短激光脉冲进行相位调制,激发Er3+, Tm3+, Yb3+共掺的稀土离子实现双光子吸收和发光的相干控制。与傅里叶变换受限脉冲对应的双光子吸收相比,整形脉冲对应的蓝,绿,红的双光子吸收几率可以分别在0-13.3,0-14.5,0-1.0范围内调制。镧系离子能级结构和激光频谱对相干特性的影响也做了讨论。蓝光和绿光的双光子吸收几率会随着激光频谱带宽增加而增加,随着末态能级带宽增加而减小。如果中间能级在10100-10500cm-1范围内漂移,蓝光和绿光的双光子跃迁几率的变化范围分别为7-15和8-17。
(4)我们从实验和理论上研究了7π相位整形的800nm飞秒激光脉冲对Er3+掺杂的玻璃样品的绿光的量子相干控制。实验结果表明,随着激光脉冲的强度增强到几个10'2W/cm2,π相位整形脉冲对应的绿光发光强度可以超越傅里叶变换受限脉冲对应的绿光发光强度。根据四阶微扰理论研究了双光子和四光子过程的相干控制,很好的解释了实验结果。
(5)由于飞秒激光脉冲激光频谱较宽,飞秒激发共振增强多光子电离光电子谱有两个缺点：分辨率低,选择性差。我们提出用π相位和余弦相位组合的相位调制方法实现Na原子(2+1)共振增强多光子电离光电子谱的高分辨选择激发。我们的理论结果表明,π相位调制能够有效的提高(2+1)共振增强多光子电离光电子能谱的分辨率,再加一个余弦相位调制可以实现两个相邻激发态的选择激发。
The emission spectrum of rare earth ions spans near-infrared to visible, even to ultraviolet band. The tunable and tense upconversion emission of rare earth ions is very important for these applications in biological labeling, light emitting displays, optical data storage, and solid-state lasers. Quantum coherent control based on the femtosecond pulse shaping is widely used to study the nonlinear processes between the light and the materiel, for example, multiphoton absorption, Raman scattering, higher harmonics, resonance-enhanced multiphoton-ionization photoelectron spectroscopy. In this thesis, the enhancing and tuning of trivalent rare earth ions have been studied theoretically and experimentally by quantum coherent control based on the femtosecond pulse shaping. The main research contents are as follows:
(1) The luminescence properties of rare earth ions, the mechanism of upconversion luminescence, and the common method for tuning and enhancing upconversion emission were systematically introduced. The idea of coherent control, pulse shaping technique, and the multiphoton transition theory were simply reviewed.
(2) The two-photon absorption (TPA) probability in a Pr3+ion system is enhanced to12.3by the shaped ultrashort laser pulses. The TPA is significantly higher than that achieved by a transform-limit pulse. However, the laser intensity of shaped pulses is reduced to37%of the initial transform-limited pulse. In this method, the TPA probability can also be reduced to58%. Furthermore, the effect of the shift of the intermediate energy level and the bandwidth of final states on TPA probability was discussed.
(3) We presented a new scheme for quantum coherent control of two-photon absorption (TPA) and color emission in codoped lanthanide ions of Er3+/Tm3+/Yb3+ by properly phase shaping two infrared ultrashort laser beams at central frequencies of10650cm-1and7650cm-1, respectively. Compared with the results irradiated by transform-limited pulses, the TPA probabilities of the blue, green and red emissions are independently controlled in the ranges0-13.3,0-14.5and0-1.0, respectively. The effects of the energy states of lanthanide ions and the laser spectral bandwidths on the coherent features were also discussed. The TPA probabilities for the blue and green emissions increase with the laser spectral bandwidths and decrease with the energy bandwidths of the final level states. As the intermediate energy level shifts in the range10100-10500cm-1, the TPA probabilities for the blue and green emissions change in the ranges7-15and8-17, respectively.
(4) We experimentally and theoretically studied the coherent quantum control of green emission in Er3+-doped glass by π-phase-shaped800nm femtosecond laser pulses. The experimental results show that the green emission intensity is enhanced over the transform-limited pulse by7r-phase-shaped pulses as the laser field increases to several1012W/cm2. Coherent control of multiphoton absorption is studied based on the fourth-order perturbation theory, and the theoretical results accord well with the experimental observations.
(5) Femtosecond laser-induced resonance-enhanced multiphoton-ionization photoelectron spectroscopy (REMPI-PS) is faced with two drawbacks of low spectral resolution and poor selective excitation due to the broad spectral bandwidth. We proposed a scheme to obtain a high-resolution selective excitation of (2+1) REMPI-PS by combining π and cosinusoidal phase modulation. Our theoretical results indicate that the (2+1) REMPI-PS signals related to neighboring excited states can be differentiated from their indistinguishable photoelectron spectra by the π phase modulation, and then their selective excitation can be realized by supplementally adding the cosinusoidal phase modulation.
引文
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