Monolayer transition metal dichalcogenides (TMDC) grown by chemical vapor deposition (CVD) are plagued by a significantly lower optical quality compared to exfoliated TMDC. In this work we show that the optical quality of CVD-grown MoSe 2 is completely recovered if the material is sandwiched in MoS 2 /MoSe 2 /MoS 2 trilayer van der Waals heterostructures. We show by means of density-functional theory that this 1 arXiv:1703.00806v2 [cond-mat.mes-hall] 14 Jun 2017 remarkable and unexpected result is due to defect healing: S atoms of the more reactive MoS 2 layers are donated to heal Se vacancy defects in the middle MoSe 2 layer. In addition, the trilayer structure exhibits a considerable charge-transfer mediated valley polarization of MoSe 2 without the need for resonant excitation. Our fabrication approach, relying solely on simple flake transfer technique, paves the way for the scalable production of large-area TMDC materials with excellent optical quality.
KeywordsChemical Vapor Deposition, transition metal dichalcogenides, van der Waals heterostructures, defect healing, charge transfer mediated valley polarization Monolayer transition metal dichalcogenides (TMDC) have a direct bandgap situated in the visible range, which makes them ideal building blocks for novel electronic and optoelectronic devices. [1][2][3][4][5][6][7][8][9][10] The bandgap of monolayer TMDCs occurs at the inequivalent (but degenerate) K and K' points of the hexagonal Brillouin zone. The broken inversion symmetry of a TMDC monolayer combined with the time reversal symmetry imposes opposite magnetic moments at the K and K' valleys. This in turn determines the characteristic circular dichroism exhibited by these materials, wherein each valley can be addressed separately with circularly polarized light of a given helicity. 11-13 Additionally, optical spectra are influenced by the strong spin-orbit coupling, which lifts the degeneracy of band states at the valence band edges, resulting in well-resolved A and B resonances, as observed in reflectivity or absorption spectra. 2,14-16 The interplay of spin-orbit coupling with broken inversion symmetry and time reversal symmetry locks the valley and spin degrees of freedom, making TMDC attractive candidates for valleytronics. 17 The spin-valley index locking along with the large 2 distance in the momentum space between K and K' valleys preserves the valley polarization observed in the degree of circular polarization (DCP) in helicity resolved photoluminescence emission. [18][19][20][21][22] Applications require a scalable fabrication platform providing high-quality large-area monolayer TMDC. Unfortunately, the most promising approach today, namely chemical vapor deposition (CVD) growth 23-27 struggles to compete with exfoliated TMDC in terms of sample quality. Low temperature PL spectroscopy of CVD-grown MoS 2 and MoSe 2 reveals broad emission from defect bound excitons, which is significantly more intense than the free exciton peak [28][29][30] and is related to chalcogen vacancies induced...