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The development of van der Waals (vdW) crystals and their heterostructureshas created a fascinating platform for exploring optoelectronic properties inthe two-dimensional (2D) limit. With the recent discovery of 2D magnets, thecontrol of the spin degree of freedom can be integrated to realize 2Dspin-optoelectronics with spontaneous time-reversal symmetry breaking. Here, wereport spin photovoltaic effects in vdW heterostructures of atomically thinmagnet chromium triiodide (CrI3) sandwiched by graphene contacts. In theabsence of a magnetic field, the photocurrent displays a distinct dependence onlight helicity, which can be tuned by varying the magnetic states and photonenergy. Circular polarization-resolved absorption measurements reveal thatthese observations originate from magnetic-order-coupled and thushelicity-dependent charge-transfer exciton states. The photocurrent displaysmultiple plateaus as the magnetic field is swept, which are associated withdifferent spin configurations enabled by the layered antiferromagnetism andspin-flip transitions in CrI3. Remarkably, giant photo-magnetocurrent isobserved, which tends to infinity for a small applied bias. Our results pavethe way to explore emergent photo-spintronics by engineering magnetic vdWheterostructures.

Spin Photovoltaic Effect in Magnetic van der Waals Heterostructures