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A new diamond-like semiconductor (DLS), Li4HgGe2S7, is the first example exhibiting unusual 10-membered LiS4 rings in the reported quaternary sulfide DLSs. Remarkably, Li4HgGe2S7 exhibits excellent performances with concurrently large NLO coefficients and impressive LDT, which satisfy the essential requirements of IR NLO candidates.

Graphical abstract: The first quaternary diamond-like semiconductor with 10-membered LiS4 rings exhibiting excellent nonlinear optical performances

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