Photocarrier-Mediated Excitation of Coherent Phonons

The DECP model successfully explained the observed initial phase of the fully symmetric phonons in a number of opaque crystals [24]. The absence of the Eg mode was attributed to an exclusive coupling between the electrons photoexcited near the r point and the fully symmetric phonons. A recent density functional theory (DFT) calculation [23] demonstrated this exclusive coupling as the potential energy surface (Fig. 2.4). The minimum of the potential surface of the excited state shifted significantly along the trigonal (z) axis, 

As the lattice interacts with light only through electrons, both DECP and ISRS should rely on the electron-phonon coupling in the material. Distinction between the two models lies solely in the nature of the electronic transition. In this context, Merlin and coworkers proposed DECP to be a resonant case of ISRS with the excited state having an infinitely long lifetime [26,28]. This original resonant ISRS model failed to explain different initial phases for different coherent phonon modes in the same crystal [21,25]. Recently, the model was modified to include finite electronic lifetime [29] to have more flexibility to reproduce the experimental observations. 

In polar semiconductors, carrier-mediated generation occurs in the form of transient depletion field screening (TDFS) depicted in Fig. 2.5 [30]. The driving force in (2.1) can be expressed by the sum of the Raman term and the nonlinear longitudinal polarization [10]  

The nonlinear polarization can be divided into several different contributions  

The third term describes the polarization set up by ultrafast drift-diffusion currents, which can excite coherent phonons via TDFS (or via the buildup of electric Dember fields [9,10]). The first two terms represent the second- and the third-order nonlinear susceptibilities, respectively [31]. The fourth term describes the polarization associated with coherent electronic wavefunctions, which becomes important in semiconductor heterostructures. 

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