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Intrinsic localized modes in the charge-transfer solid PtCl

We report a theoretical analysis of intrinsic localized modes in a quasi-one-dimensional charge-transfer solid, [Pt(en)2][Pt(en)2Cl2](ClO4)4(PtCl). We discuss strongly non-linear features of resonant Raman overtone scattering measurements on PtCl, arising from quantum intrinsic localized (multiphonon) modes (ILMs) and ILM-plus-phonon states. We show that Raman scattering data display clear signs of a non-thermalization of the lattice degrees of freedom, manifested in a non-equilibrium density of intrinsic localized modes. Adiabatic lattice dynamics is used in a model two-band Peierls-Hubbard Hamiltonian, including a screened Coulomb interaction between neighbouring sites. The Hamiltonian is diagonalized on a finite chain. The calculated adiabatic potential for Peierls distortion of the Cl sublattice displays characteristic non-analytic points, related to a lattice-distortion-induced charge transfer. Possible non-adiabatic effects on ILMs are discussed.