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Materials that rectify light into current in their bulk are desired for optoelectronic applications. In Weyl semimetals that break inversion symmetry, bulk photocurrents may arise due to nonlinear optical processes that are enhanced near the Weyl nodes. However, the photoresponse of these materials is commonly studied by scanning photocurrent microscopy, which convolves the effects of photocurrent generation and collection. Here we directly image the photocurrent flow inside the type-II Weyl semimetals WTe2 and TaIrTe4 using high-sensitivity quantum magnetometry with nitrogen-vacancy centre spins. We elucidate a mechanism for bulk photocurrent generation, which we call the anisotropic photothermoelectric effect, where unequal thermopowers along different crystal axes drive intricate circulations of photocurrent around the photoexcitation. Using overlapping scanning photocurrent microscopy and magnetic imaging at the interior and edges of the sample, we visualize how the anisotropic photothermoelectric effect stimulates the long-range photocurrent collected in our WTe2 and TaIrTe4 devices through the Shockley–Ramo mechanism. Our results highlight a widely relevant source of current flow and will inspire photodetectors that utilize bulk materials with thermoelectric anisotropy. 

Van der Waals (VdW) materials have opened new directions in the study of low dimensional magnetism. A largely unexplored arena is the intrinsic tuning of VdW magnets toward new ground states. Chromium trihalides provided the first such example with a change of interlayer magnetic coupling emerging upon exfoliation. Here, we take a different approach to engineer previously unknown ground states, not by exfoliation, but by tuning the spin-orbit coupling (SOC) of the nonmagnetic ligand atoms (Cl, Br, I). We synthesize a three-halide series, CrCl 3 − x − y Br x I y , and map their magnetic properties as a function of Cl, Br, and I content. The resulting triangular phase diagrams unveil a frustrated regime near CrCl 3 . First-principles calculations confirm that the frustration is driven by a competition between the chromium and halide SOCs. Furthermore, we reveal a field-induced change of interlayer coupling in the bulk of CrCl 3 − x − y Br x I y crystals at the same field as in the exfoliation experiments.