“…Since then a few parallel efforts have been made in neutron scattering, high-field susceptibility / magnetization, NMR, and Raman scattering measurements. While NMR and Raman studies have been / will be reported in separate independent papers 17,18 µSR and the remaining studies and characterization of the specimens will be reported in three consecutive papers (I, II 20 and III 19 ). In this paper (I), we focus on µSR and low-field magnetic susceptibility measurements on Cu(Cl,Br)La(Nb,Ta) 2 O 7 , which demonstrate: (a) absence of static magnetism in (CuCl)LaNb 2 O 7 down to 15 mK confirming the spin-gapped ground state; (b) phase separation between partial volumes with a spin-gap and static magnetism in (CuCl)La(Nb,Ta) 2 O 7 ; (c) historydependent magnetization in the (Nb,Ta) and (Cl,Br) substitution systems; and (d) a uniform long-range collinear antiferromagnetic state in (CuBr)LaNb 2 O 7 .…”