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Phonon anharmonicity in Cu-based layered thiophosphates

Rahul RaoMichael A. Susner
摘要
In this work, we performed temperature-dependent Raman spectroscopy studieson three layered metal thiophosphates: CuInP2S6, CuCrP2S6, andCuInP2S6-In4/3P2S6 heterostructures. These materials are emergingmultiferroics, with CuInP2S6 and CuInP2S6-In4/3P2S6 exhibiting room temperatureferrielectric polarization while CuCrP2S6 is both anti-ferroelectric andantiferromagnetic at low temperatures (<145 and <30 K, respectively). Westudied two prominent peaks in the Raman spectra of these compounds, namelytheir P-P and P-S stretching modes. First order linear fits to the modesoftening yielded coefficients similar to other layered materials. Furthermore,analysis of the phonon decay revealed the dominant role of anharmonic effectsrather than thermal expansion. In particular, the decay of the optical phononswas found to be governed by three-phonon processes in CuInP2S6 and CuCrP2S6 andby the four-phonon process in the CuInP2S6-In4/3P2S6 heterostructures. Thesephonon lifetimes were found to be less than 1 ps, indicating high scatteringrates and showing the potential for these materials to be used inthermoelectric applications.
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