Harnessing Native Chromium Oxidation for Giant Orbital Torque and Field-Free Magnetization Switching in NiFe/Cr Bilayers

Abstract

Orbital currents offer charge-to-spin conversion beyond the efficiency limit of conventional heavy-metal Spin Hall sources. However, harnessing them has so far required either thick orbital-Hall materials or additional heavy-metal conversion layers. Here, we show that the native oxide of chromium, typically regarded as parasitic, transforms a simple NiFe\Cr bilayer into a self-contained dual-channel orbital-current source without the need for any conversion layer. First-principles calculations predict a nearly threefold enhancement of the orbital Hall conductivity upon surface oxygenation, driven by Cr(3d)-O(2p) hybridization. Experimentally, naturally oxidized NiFe\Cr heterostructures exhibit a giant damping-like torque efficiency of $3.9 \times 10^{6}$ $Ω^{-1}$ m$^{-1}$, exceeding Pt (Ta) by one (two) orders of magnitude. The torque depicts a non-monotonic Cr-thickness dependence which cannot be explained by a conventional model. We have developed a drift-diffusion model with an oxidation-gated interfacial source which quantitatively reproduces the data, revealing that the Cr-CrO$_x$ interface generates orbital currents over an order of magnitude stronger than the bulk orbital Hall channel with an orbital transport length of $\approx 4$ nm. The enhanced torque enables field-free magnetization switching at $1.58 \times 10^{11}$ A m$^{-2}$, outperforming heavy-metal and CuO$_x$ benchmarks. These results establish native oxidation as a scalable strategy for realizing efficient orbital-torque devices.