Electronegative ligands enhance charge transfer to Mn12 single-molecule magnets deposited on graphene

Combining single-molecule magnets (SMMs) and emergent two-dimensional substrates such as graphene may lead to device configurations that are promising for spintronics and quantum computing. However, to fully exploit the unique features of SMMs anchored to two-dimensional substrates, the choice of ligand attachments, which could affect the magnetic and electronic properties, is critical. In this work, we focus on hybrid junctions comprising CVD-grown graphene and [Mn 12O 12(O 2CR) 16(H 2O) 4]( R = CH 3 , CHCl 2) SMMs with different ligands. We find that [Mn 12O 12(O 2CCH 3) 16(H 2O) 4] SMMs barely change the graphene’s conductivity, while [Mn 12O 12(O 2CCHCl 2) 16(H 2O) 4] SMMs with more electronegative ligands, by means of charge transfer, remarkably modify the electronic transport in graphene as revealed by gate-voltage dependent magnetotransport measurements.Combining single-molecule magnets (SMMs) and emergent two-dimensional substrates such as graphene may lead to device configurations that are promising for spintronics and quantum computing. However, to fully exploit the unique features of SMMs anchored to two-dimensional substrates, the choice of ligand attachments, which could affect the magnetic and electronic properties, is critical. In this work, we focus on hybrid junctions comprising CVD-grown graphene and [Mn 12O 12(O 2CR) 16(H 2O) 4]( R = CH 3 , CHCl 2) SMMs with different ligands. We find that [Mn 12O 12(O 2CCH 3) 16(H 2O) 4] SMMs barely change the graphene’s conductivity, while [Mn 12O 12(O 2CCHCl 2) 16(H 2O) 4] SMMs with more electronegative ligands, by means of charge transfer, remarkably modify the electronic transport in graphene as revealed by gate-voltage dependent magnetotransport measurements.