Strain-driven spin-flop transition and collapse of the giant magnon gap in the bilayer iridate Sr$_3$Ir$_2$O$_7$

Abstract

The bilayer iridate Sr$_3$Ir$_2$O$_7$ is a $c$-axis collinear antiferromagnet, held there by a giant interlayer pseudodipolar anisotropy, whereas single-layer Sr$_2$IrO$_4$ cants in the $ab$ plane. We show from first principles that biaxial compression of a few percent ($\varepsilon_c\approx-2.4\%$) flops the easy axis of Sr$_3$Ir$_2$O$_7$ into the plane. A magnetic model Hamiltonian built from Wannier functions with no fitted parameter---reproducing the giant magnon gap of the bulk, so far known only from fits to experiment---identifies the mechanism. Compression collapses the interlayer exchange channel, whose straight Ir--O--Ir path weakens as the bent in-plane path strengthens. Hund's exchange sets the scale of the anisotropy and, beyond $J/U\approx0.15$, removes the collinear state altogether. The flop is not a rigid rotation---the ordered moments of the two states cross at $\varepsilon_c$---and it carries a stark fingerprint, in that the giant easy-axis magnon gap collapses to a gapless, Goldstone-like spectrum. Compressively strained films thus sit on a metamagnetic phase boundary ending in a zero-temperature bicritical point, a charge-neutral handle on spin--orbit-entangled order.