Bootstrapped Dimensional Crossover of a Spin Density Wave

Abstract

Quantum materials display rich and myriad types of magnetic, electronic, and structural ordering, often with these ordering modes either competing with one another or “intertwining,” that is, reinforcing one another. Low-dimensional quantum materials influenced strongly by competing interactions and/or geometric frustration are particularly susceptible to such ordering phenomena and thus offer fertile ground for understanding the consequent emergent collective quantum phenomena. Such is the case of the quasi-2D materials R_{4}Ni_{3}O_{10} (R=La, Pr), in which intertwined charge- and spin-density waves (CDW and SDW) on the Ni sublattice have been identified and characterized. Not unexpectedly, these density waves are largely quasi-2D as a result of weak coupling between planes, compounded with magnetic frustration. In the case of R=Pr, however, we show here that exchange coupling between the transition-metal and rare-earth sublattices upon cooling overcomes both obstacles, leading to a dimensional crossover into a fully 3D-ordered and coupled SDW state on both sublattices, as an induced moment on notionally nonmagnetic Pr^{3+} opens exchange pathways in the third dimension. In the process, the structure of the SDW on the Ni sublattice is irreversibly altered, an effect that survives reheating of the material until the underlying CDW melts. This “bootstrapping” mechanism linking incommensurate SDWs on the two sublattices illustrates a new member of the multitude of quantum states that low-dimensional magnets can express, driven by coupled orders and modulated by frustrated exchange pathways.