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We report on a systematic study of the magnetic properties on single crystalsof the solid solution Cs$_2$CuCl$_{4-x}$Br$_x$ (0 $\leq$ x $\leq$ 4), whichinclude the two known end-member compounds Cs$_2$CuCl$_4$ and Cs$_2$CuBr$_4$,classified as quasi-two-dimensional quantum antiferromagnets with differentdegrees of magnetic frustration. By comparative measurements of the magneticsusceptibility $\chi$($T$) on as many as eighteen different Br concentrations,we found that the inplane and out-of-plane magnetic correlations, probed by theposition and height of a maximum in the magnetic susceptibility, respectively,do not show a smooth variation with x. Instead three distinct concentrationregimes can be identified, which are separated by critical concentrationsx$_{c1}$ = 1 and x$_{c2}$ = 2. This unusual magnetic behavior can be explainedby considering the structural peculiarities of the materials, especially thedistorted Cu-halide tetrahedra, which support a site-selective replacement ofCl- by Br- ions. Consequently, the critical concentrations x$_{c1}$ (x$_{c2}$)mark particularly interesting systems, where one (two) halidesublatticepositions are fully occupied.

Distinct magnetic regimes through site-selective atom substitution in the frustrated quantum antiferromagnet Cs$_2$CuCl$_{4-x}$Br$_x$