...
  • 主题
高级搜索  >
历史搜索 清空历史
首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Ohmic Brownian Oscillator Approach to Hole-Burning and Photo-Echo Spectroscopies
【24h】

Ohmic Brownian Oscillator Approach to Hole-Burning and Photo-Echo Spectroscopies

机译：Ohmic Brownian振荡器方法用于烧孔和光回波光谱

获取原文
获取原文并翻译 | 示例
           
页面导航
  • 摘要
  • 著录项
  • 相似文献
  • 相关主题

摘要

The multimode Brownian oscillator (MBO) model has been at the forefront in interpreting the subsystembath interaction manifestations in optical spectroscopy for probing homogeneous structure of chromophores in crystals and amorphous solids. The spectroscopic consequences of employing the underdamped MBO model with Ohmic dissipation in linear absorption, photon-echo, and hole-burning data of chromophores in solid hosts at low temperatures are investigated. The zero-phonon line (ZPL) in homogeneous linear absorption spectrum, the slow-decay component (due to ZPL) in photon-echo signal, and the zero-phonon hole (ZPH) in hole-burned spectra in host molecular solids at low temperatures are usually resolved from the multiphonontransitions structure. In the MBO model, the harmonic vibrations (Brownian oscillators) are linearly coupled to bath modes. This coupling, with Ohmic dissipation, results in a maximum contribution of the bath modes to the ZPL region. This contribution affects the width of the ZPL profile, which should only be determined by pure electronic dephasing as dictated by experiments. It is therefore important to study how the MBO model bath modes contribute to the ZPL, ZPH, and slow-decay component profiles. Analytical expressions for the linear absorption spectrum and width and Franck-Condon factor of the ZPL are derived. Homogeneous linear absorption spectra, two-pulse photon-echo, and hole-burning calculations are carried out with model systems of which the parameter values are typical for real systems. The MBO model ZPL, ZPH, and slowdecay component were not seen in linear absorption, hole-burning, and two-pulse photon-echo profiles, respectively. The hole-burned spectrum is produced by blending the line broadening function, g(t;T), of the MBO model and Small hole-burning formula. This full (inclusion of Matsubara series) form of g(t;T) has not been exploited before in any spectroscopic calculation. It is concluded that the MBO model ZPL and ZPH widths and the electronic exponential decay are better exhibited in the corresponding profiles when using non-Ohmic spectral density.
机译：多模式布朗振荡器（MBO）模型在解释光谱学中的子系统浴相互作用表现以探测晶体和无定形固体中发色团的均匀结构方面一直处于前沿。研究了在低温条件下在固态主体中发色团的线性吸收，光子回波和空穴燃烧数据中使用带有欧姆耗散的欠阻尼MBO模型的光谱学结果。均质线性吸收光谱中的零声子线（ZPL），光子回波信号中的慢衰减分量（归因于ZPL）和低分子主体固体中空穴燃烧谱中的零声子空穴（ZPH）温度通常由多声子跃迁结构决定。在MBO模型中，谐波振动（布朗振荡器）线性耦合到浴池模式。具有欧姆耗散的这种耦合导致浴模式对ZPL区域的贡献最大。这种影响会影响ZPL轮廓的宽度，ZPL轮廓的宽度只能由实验确定，通过纯电子移相来确定。因此，重要的是研究MBO模型浴模式如何影响ZPL，ZPH和慢衰减成分分布。推导了ZPL的线性吸收光谱和宽度以及Franck-Condon因子的解析表达式。均质线性吸收光谱，两脉冲光子回波和空穴燃烧计算是通过模型系统进行的，其中参数值对于实际系统而言是典型的。 MBO模型ZPL，ZPH和慢衰减分量分别在线性吸收，空穴燃烧和两脉冲光子-回波剖面中未看到。空穴燃烧光谱是通过将MBO模型的线展宽函数g（t; T）与小空穴燃烧公式混合而成的。 g（t; T）的完整形式（包括Matsubara系列）尚未在任何光谱计算中得到利用。结论是，当使用非欧姆频谱密度时，MBO模型的ZPL和ZPH宽度以及电子指数衰减在相应的轮廓中表现得更好。

著录项

相似文献

  • 外文文献
  • 中文文献
  • 专利
获取原文

客服邮箱：kefu@zhangqiaokeyan.com

京公网安备：11010802029741号 ICP备案号：京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有

  • 客服微信

  • 服务号