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Differential optical absorption spectroscopy of trace gas species and aerosols in the Upper Ohio River Valley.

机译:差分光学吸收光谱法,用于分析俄亥俄州上游河谷中的痕量气体和气溶胶。

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摘要

In this research, it is hypothesized that recently developed theoretical considerations of atmospheric radiative transfer in horizontally in-homogeneous atmospheres can be applied to the remote measurement of anthropogenic plumes. To this end, a MAX-DOAS spectrometer, designed around a B&W-TEK BTU142 spectrometer was constructed and characterized. It was found that the MAX-DOAS spectrometer has a measured resolution of 0.282 nm, and a noise level of 178 counts at 75% pixel saturation, sufficient to resolve accurately the absorptions of important atmospheric species, including SO2, NO 2, HCHO, and O4. The theory of MAX-DOAS spectral analysis was examined in detail, in particular the processing of reference absorption cross-section spectra for use in regression analyses of scattered solar radiation. For the purposes of inversion, optimal estimation software was designed and investigated for suitability in retrieving vertical profiles of atmospheric species. This software is shown to perform well under conditions of both typical and non-typical noise levels using synthetic spectral data and known profiles of three atmospheric species. Furthermore, an extensive examination of the residuals of DOAS spectral analysis was performed, to validate the assumption of normally distributed errors in the inversion process. Investigated methodologies were applied to spectral data collected over nine days in 2008 in the Upper Ohio River Valley. Aerosol extinction coefficient profiles were successfully retrieved, with an average peak value of 0.549 km-1. For the same measurement period, in-plume measurements of SO2 and NO 2 concentration from a coal-fired power plant were conducted using recently developed methodologies to account for in-plume solar radiative transfer effects.
机译:在这项研究中,假设最近开发的关于水平不均匀大气中大气辐射传输的理论考虑可以用于人为羽流的远程测量。为此,构造并表征了围绕B&W-TEK BTU142光谱仪设计的MAX-DOAS光谱仪。发现MAX-DOAS光谱仪的测量分辨率为0.282 nm,在像素饱和度为75%时的噪声水平为178,足以准确解析重要大气物质的吸收,包括SO2,NO 2,HCHO和O4详细研究了MAX-DOAS光谱分析的理论,特别是参考吸收截面光谱的处理,用于散射太阳辐射的回归分析。为了进行反演,设计并研究了最佳估计软件,以适合于检索大气物种的垂直剖面。使用合成光谱数据和三种大气物质的已知曲线,该软件在典型噪声和非典型噪声水平下均表现良好。此外,对DOAS频谱分析的残差进行了广泛的检查,以验证反演过程中正态分布误差的假设。研究方法应用于2008年在上俄亥俄河谷采集的9天以上的光谱数据。成功获得了气溶胶消光系数图,平均峰值为0.549 km-1。在相同的测量时间段内,使用最近开发的方法对燃煤电厂的SO2和NO 2浓度进行了室内测量,以解决室内太阳辐射传递效应。

著录项

  • 作者

    Beekman, Christopher Paul.;

  • 作者单位

    The Ohio State University.;

  • 授予单位 The Ohio State University.;
  • 学科 Atmospheric Chemistry.
  • 学位 Ph.D.
  • 年度 2010
  • 页码 208 p.
  • 总页数 208
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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