A novel
organic–inorganic hybrid guanidine fluoromolybdate,
[C(NH2)3]2MoO2F4·H2O, was successfully synthesized via our proposed
cation–anion synergetic interaction strategy. The title compound
features a unique Chinese-knot structure constructed by hydrogen-bonding
interactions, which induces an all-around improvement of the optical
band gap, second-harmonic-generation effect, and phase-matchable ability
compared with the reported fluoromolybdates, demonstrating that it
is a promising UV nonlinear-optical material.