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The control of the density and type of line defects on two-dimensional (2D) materials enable the development of new methods to tailor their physical and chemical properties. In particular, mirror twin boundaries (MTBs) on transition metal dichacogenides have attracted much interest due to their metallic state with charge density wave transition and spin-charge separation property. In this work, we demonstrate the self-assembly of 2,3-diaminophenazine (DAP) molecule porous structure with alternate L-type and T-type aggregated configurations on the MoSe2 hexagonal wagon-wheel pattern surface. This site-specific molecular self-assembly is attributed to the more chemically reactive metallic MTBs compared to the pristine semiconducting MoSe2 domains. First-principles calculations reveal that the active MTBs couple with amino groups in the DAP molecules facilitating the DAP assembly. Our results demonstrate the site-dependent electronic and chemical properties of MoSe2 monolayers, which can be exploited as a natural template to create ordered nanostructures. Mirror twin boundaries (MTBs) have been observed as metallic line defects in 2D transition metal dichalcogenides, but their chemical properties are not well understood. Here, the authors show that MTB defect networks on MoSe2 are more chemically reactive to organic molecules than pristine domains, and can template the self-assembly of hexagonal organic porous structures. [ABSTRACT FROM AUTHOR]

The control of the density and type of line defects on two-dimensional (2D) materials enable the development of new methods to tailor their physical and chemical properties. In particular, mirror twin boundaries (MTBs) on transition metal dichacogenides have attracted much interest due to their metallic state with charge density wave transition and spin-charge separation property. In this work, we demonstrate the self-assembly of 2,3-diaminophenazine (DAP) molecule porous structure with alternate L-type and T-type aggregated configurations on the MoSe 2 hexagonal wagon-wheel pattern surface. This site-specific molecular self-assembly is attributed to the more chemically reactive metallic MTBs compared to the pristine semiconducting MoSe 2 domains. First-principles calculations reveal that the active MTBs couple with amino groups in the DAP molecules facilitating the DAP assembly. Our results demonstrate the site-dependent electronic and chemical properties of MoSe 2 monolayers, which can be exploited as a natural template to create ordered nanostructures.

In emerging optoelectronic applications, such as water photolysis, exciton fission and novel photovoltaics involving low-dimensional nanomaterials, hot-carrier relaxation and extraction mechanisms play an indispensable and intriguing role in their photo-electron conversion processes. Two-dimensional transition metal dichalcogenides have attracted much attention in above fields recently; however, insight into the relaxation mechanism of hot electron-hole pairs in the band nesting region denoted as C-excitons, remains elusive. Using MoS 2 monolayers as a model two-dimensional transition metal dichalcogenide system, here we report a slower hot-carrier cooling for C-excitons, in comparison with band-edge excitons. We deduce that this effect arises from the favourable band alignment and transient excited-state Coulomb environment, rather than solely on quantum confinement in two-dimension systems. We identify the screening-sensitive bandgap renormalization for MoS 2 monolayer/graphene heterostructures, and confirm the initial hot-carrier extraction for the C-exciton state with an unprecedented efficiency of 80%, accompanied by a twofold reduction in the exciton binding energy.