Proximity-Induced Exchange Interaction and Prolonged Valley Lifetime in MoSe2/CrSBr Van-Der-Waals Heterostructure with Orthogonal Spin Textures

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Abstract
Heterostructures, composed of semiconducting transition-metal dichalcogenides (TMDC) and magnetic van-der-Waals materials, offer exciting prospects for the manipulation of the TMDC valley properties via proximity interaction with the magnetic material. We show that the atomic proximity of monolayer MoSe2 and the antiferromagnetic van-der-Waals crystal CrSBr leads to an unexpected breaking of time-reversal symmetry, with originally perpendicular spin directions in both materials. The observed effect can be traced back to a proximity-induced exchange interaction via first-principles calculations. The resulting spin splitting in MoSe2 is determined experimentally and theoretically to be on the order of a few meV. Moreover, we find a more than 2 orders of magnitude longer valley lifetime of spin-polarized charge carriers in the heterostructure, as compared to monolayer MoSe2/SiO2, driven by a Mott transition in the type-III band-aligned heterostructure.
Funding Information
  • Generalitat Valenciana (PhD fellowship)
  • Deutscher Akademischer Austauschdienst (57705443)
  • Ministry of Education, Culture, Sports, Science and Technology
  • Deutsche Forschungsgemeinschaft (549364913, SFB 1277 314695032 B05, SFB 1277 314695032 B07, SFB 1277 314695032 B11, SPP 2244 443361515, SPP 2244 443416183)
  • European Commission (101027187, 101103355)
  • Minist??rio da Ci??ncia, Tecnologia e Inova????o (311678/2020-3)
  • European Commission (863098, 881603)
  • Ministry of Education, Culture, Sports, Science and Technology (21H05233, 23H02052)
  • Funda????o de Amparo ?? Pesquisa do Estado de S??o Paulo (14/19142-1, 2014/07375-2, 2015/13771-0, 2022/10340-2, 22/00419-0, 22/08329-0, 23/01313-4)
  • Coordena????o de Aperfei??oamento de Pessoal de N??vel Superior (57705443)

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