A family of five hybrid ABX3 perovskites has been
synthesized using hypophosphite (H2POO)- as the X-site ion. These
compounds adopt the general formula [Am]Mn(H2POO)3,
where Am = guanidinium (HUA), formamidinium (FA), imidazolium
(IM), triazolium (TRZ), and dabconium (DAB). We explore the
diverse structural and phase transition behavior of these materials
through single-crystal diffraction measurements and demonstrate
contrasting magnetism in two of the phases, Am = GUA
and FA, that arises from structural distortions. The results show
that hypophosphite perovskites offer a promising platform for
generating new functional materials.Y.W., F.B., and A.K.C. gratefully thank the Ras Al Khaimah Center for Advanced Materials for financial support. S.S. gratefully thanks the Winston Churchill Foundation of the USA for financial support. R.M. thanks SERB, New Delhi for a JC Bose Fellowship. DFT calculations were performed at the Cambridge HPCS and the UK National Supercomputing Service, ARCHER. Access to the latter was obtained via the MCC consortium and funded by EPSRC under Grant No. EP/L000202/1. Magnetic measurements were carried out using the Advanced Materials Characterization Suite, funded by EPSRC Strategic Equipment Grant EP/M000524/1