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Modulation of third-order nonlinear optical properties by backbone modification of polymeric pillared-layer heterometallic clusters

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Three polymeric heterothiometallic clusters with 3D pillar-layer-alternating honeycomblike frameworks are synthesized by a one-pot self-assembly reaction. Z-scan experiments demonstrate that the nonlinear optical (NLO) behavior of these clusters can be modulated by modifying the conjugated chain of the connecting backbone ligands (see figure). Time-dependent density functional theory calculations support and rationalize the observed NLO modulation.

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