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For applications exploiting the valley pseudospin degree of freedom intransition metal dichalcogenide monolayers, efficient preparation of electronsor holes in a single valley is essential. Here, we show that a magnetic fieldof 7 Tesla leads to a near-complete valley polarization of electrons in MoSe2monolayer with a density 1.6x10^{12} cm^{-2}; in the absence of exchangeinteractions favoring single-valley occupancy, a similar degree of valleypolarization would have required a pseudospin g-factor exceeding 40. Toinvestigate the magnetic response, we use polarization resolvedphotoluminescence as well as resonant reflection measurements. In the latter,we observe gate voltage dependent transfer of oscillator strength from theexciton to the attractive-Fermi-polaron: stark differences in the spectrum ofthe two light helicities provide a confirmation of valley polarization. Ourfindings suggest an interaction induced giant paramagnetic response of MoSe2,which paves the way for valleytronics applications.

Giant paramagnetism induced valley polarization of electrons in charge-tunable monolayer MoSe2