Knoesel Ernst, Bonn Mischa, Shan Jie, Wang Feng, Heinz Tony F
Department of Physics and Astronomy, Rowan University, Glassboro, New Jersey 08028, USA.
J Chem Phys. 2004 Jul 1;121(1):394-404. doi: 10.1063/1.1757442.
We present investigations of the transient photoconductivity and recombination dynamics of quasifree electrons in liquid n-hexane and cyclohexane performed using terahertz time-domain spectroscopy (THz-TDS). Quasifree electrons are generated by two-photon photoionization of the liquid using a femtosecond ultraviolet pulse, and the resulting changes in the complex conductivity are probed by a THz electromagnetic pulse at a variable delay. The detection of time-domain wave forms of the THz electric field permits the direct determination of both the real and the imaginary part of the conductivity of the electrons over a wide frequency range. The change in conductivity can be described by the Drude model, thus yielding the quasifree electron density and scattering time. The electron density is found to decay on a time scale of a few hundred picoseconds, which becomes shorter with increasing excitation density. The dynamics can be described by a model that assumes nongeminate recombination between electrons and positive ions. In addition, a strong dependence of the quasifree electron density on temperature is observed, in agreement with a two-state model in which the electron may exist in either a quasifree or a bound state.
我们展示了利用太赫兹时域光谱(THz-TDS)对正己烷和环己烷液体中准自由电子的瞬态光电导率和复合动力学进行的研究。准自由电子通过使用飞秒紫外脉冲对液体进行双光子光电离产生,并且通过可变延迟的太赫兹电磁脉冲探测复电导率的变化。对太赫兹电场时域波形的检测允许在很宽的频率范围内直接确定电子电导率的实部和虚部。电导率的变化可以用德鲁德模型来描述,从而得到准自由电子密度和散射时间。发现电子密度在几百皮秒的时间尺度上衰减,随着激发密度的增加,衰减时间变短。这种动力学可以用一个假设电子与正离子之间非成对复合的模型来描述。此外,观察到准自由电子密度对温度有强烈的依赖性,这与电子可能处于准自由态或束缚态的双态模型一致。