We have measured the first-order Raman spectra of CuAlSe2 and the second-order Raman spectra of CuAlS2 and CuAlSe2, and reexamined two-phonon absorption spectra of CuAlS2. Lattice dynamical calculations have been performed using a rigid ion model. Force constants and charges as fitting parameters have been determined so as to reproduce zone-center phonon frequencies and the two-phonon spectra observed. Calculated two-phonon density of states shows reasonable agreements with those spectra.
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