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Frozen‐phonon calculations on structurally related tetragonal Cu2ZnSnSe4 and monoclinic Cu2SnSe3 reveal similarities in the shape and overall composition of vibration spectra, but also marked deviations in the frequency and nature of certain modes. These deviations are often induced by different connectivity on the cation sublattice and can be traced to a specific structural motive. In the analysis...
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