We present a new model compound with the S = 1/2 frustrated square lattice composed of the charge-transfer salt (o-MePy-V)PF6. Ab initio calculations indicate the formation of an S = 1/2 square lattice, in which six types of nearest-neighbor ferromagnetic- and antiferromagnetic interactions cause frustration. By applying a magnetic field, we observe an unusually gradual increase of magnetization and a subsequent 1/2-plateau-like behavior. A numerical analysis using the tensor network method qualitatively demonstrates such behaviors and suggests a collinear ordered state and a field-enhanced quantum fluctuation. Furthermore, the local magnetization and T1^-1 probed by nuclear magnetic resonance measurements support these findings.
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