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CuInP2S6 (CIPS) is an emerging layered ferroelectric material with a TC aboveroom temperature. When synthesized with Cu deficiencies (i.e.,Cu1-xIn1+x/3P2S6), the material segregates into CIPS and In4/3P2S6 (IPS)self-assembled heterostructures within the same single crystal. Thissegregation results in significant in-plane and out-of-plane strains betweenthe CIPS and IPS phases as the volume fraction of CIPS (IPS) domains shrink(grow) with decreasing Cu fraction. Here, we synthesized CIPS with varyingamounts of Cu (x = 0, 0.2, 0.3, 0.4, 0.5, 0.7, 0.8 and 1) and measured thestrains between the CIPS and IPS phases through the evolution of the respectiveRaman, infrared, and optical reflectance spectra. Density functional theorycalculations revealed vibrational modes unique to the CIPS and IPS phases,which can be used to distinguish between the two phases through two-dimensionalRaman mapping. A comparison of the composition-dependent frequencies andintensities of the CIPS and IPS Raman peaks showed interesting trends withdecreasing CIPS phase fraction (i.e., Cu/In ratio). Our data reveal red- andblue-shifted Raman and infrared peak frequencies that we correlate to latticestrains arising from the segregation of the material into CIPS and IPS chemicaldomains. The strain is highest for a Cu/In ratio of 0.33 (Cu0.4In1.2P2S6),which we attribute to equal and opposite strains exerted by the CIPS and IPSphases on each other. In addition, bandgaps extracted from the opticalreflectance spectra revealed a decrease in values, with the lowest value (~ 2.3eV) for Cu0.4In1.2P2S6.

Investigating strain between phase-segregated domains in Cu-deficient CuInP2S6