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部分大气分子的红外吸收光谱研究
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  • 英文题名:IR Absorption Spectroscopy Studies of Atmospheric Interested Molecules
  • 作者:王乐
  • 论文级别:博士
  • 学科专业名称:化学物理
  • 学位年度:2006
  • 导师:胡水明
  • 学科代码:070304
  • 学位授予单位:中国科学技术大学
  • 论文提交日期:2006-10-01
摘要
光谱学的发展历史很长,最早可以追溯到牛顿1665年用三棱镜把太阳光分为7种颜色开始。随着上个世纪激光和计算机技术的发展,极大的推进了光谱技术的进步,一系列在记录光谱手段上的革新和改进纷纷出现。
     在有关多原子分子的不同研究中,高分辨振转跃迁光谱对更好的了解分子能级结构和内部能量转移起到很大的作用。一条观测到的光谱谱线包含有三个方面的信息:频率(位置)、强度和线形,因此分子光谱的很多工作就是围绕着这几个方面来展开的。跃迁频率对应于分子上下态能级差,而谱线强度则正比于分子上下态能级的跃迁几率,它不仅包含分子的势能面和波函数的信息,并且还反映出分子的偶极矩面的信息。线形是有多方面的因素来决定的,它是分子的能级的自然线宽、气体分子间碰撞造成的压力展宽、分子平动引起的多普勒展宽和光谱仪器本身的仪器展宽的卷积的结果。
     本论文展示的工作主要集中在部分大气分子的吸收光谱的记录和分析,主要集中在谱线位置和强度的研究。第一章将综述本论文主要研究的几个气体分子已有工作,然后介绍在记录这些光谱中所用到的;第二章介绍几种气体分子谱线位置的解析工作;第三章将介绍几种分子谱线强度研究。
     第一章将首先介绍本文所研究的几种主要的气体分子在红外吸收光谱的研究近况和被HITRAN数据库收录的情况。我们也介绍了三种记录光谱的实验手段,分别为:傅立叶变换光谱技术(Fourier Transform Spectroscopy);激光腔内吸收光谱技术(Intracavity Laser Absorption Spectroscopy)和腔内衰荡光谱技术(cavity Ring Down Spectroscopy)。
     在第二章中,我们使用FTS和ICLAS技术对记录了N_2O、C_2H_2、CO_2等分子及其同位素的吸收光谱。并解析其谱线位置。首先我们讨论了线型分子的能级理论和跃迁选择定则。并示例线型分子红外谱带的三种类型。
     其中对于N_2O分子,我们使用FTS记录它5000至10000cm~(-1)波段范围的高分辨吸收光谱。在这段的解析中,新发现了~(14)N_2O分子的10个冷
The development of the Molecular Spectroscopy has a long history, since the Newton divided the sunlight into seven single color light by using a prism in 1665. The developments of the laser and computer technology in last century also lead a revolution of the molecular spectroscopy.
    Among different kinds of studies on the polyatomic molecules, the high resolution spectroscopy of rotational and vibrational transitions contributes to the better understanding of the energy-level structure and intramolecular energy transfer. An observed spectral line yields the following information: frequency, intensity and line shape. The frequency corresponds to the difference of upper and lower energy levels. The intensity is proportional to the possibility of transition, which involves information from the energy surface and the dipole moment surface as well. Line shape is determined by many factors, which is the convolution of energy life time broadening function, collision broadening function, Doppler broadening function and instrumental function.
    The present work is devoted to record and analysis the highly excited vibrational state of interested atmosphere molecules. Mainly the work focuses on the line positions and intensities. The first chapter reviews the recent studies on the molecules concerning in this thesis, and presents different sensitive spectroscopy techniques used in the experiments; the second chapter presents the rotational analysis of the spectra of several molecules; the third chapter presents the line intensity studies of these molecules.
    In the first chapter of the thesis, we cite the HITRAN Database to review the studies on the molecules concerning in this thesis. We also present different highly sensitive spectroscopy techniques used in the experiments, it includes the Fourier Transform Spectroscopy (FTS), Intracavity Laser Absorption Spectroscopy (ICLAS), Cavity Ring Down Spectroscopy (CRDS).
    In the second chapter, FTS, ICLAS-VeCSEL were used to present a systematical investigation on IR spectra of N_2O, C_2H_2, CO_2. First, we briefly introduce the theory of the energy level and the select rules of the linear molecule. Then we show three types of the transition of the linear molecule.
    The absorption spectrum of the natural sample of nitrous oxide has been recorded at Doppler limited resolution with a Fourier-transform spectrometer in the spectral range
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