Genesis of magnetism in graphene/MoS 2 van der Waals heterostructures via interface engineering using Cr-adsorption Renu Singla a , Sarvesh Kumar b , Timothy A. Hackett c , Ali H. Reshak d, e, f , Manish K. Kashyap a, * a Department of Physics, Kurukshetra University, Kurukshetra, 136119, Haryana, India b Inter-University Accelerator Centre (IUAC), Aruna Asaf Ali Marg, New Delhi,110067, India c Department of Biochemistry, University of Nebraska-Lincoln, Lincoln, NE, 68588-0664, USA d Physics Department, College of Science, University of Basrah, Basrah, Iraq e Department of Instrumentation and Control Engineering, Faculty of Mechanical Engineering, CTU in Prague, Technicka 4, Prague 6,166 07, Czech Republic f Center of Excellence Geopolymer and GreenTechnology, School of Material Engineering, University Malaysia Perlis, 01007, Kangar, Perlis, Malaysia article info Article history: Received 2 September 2020 Received in revised form 27 October 2020 Accepted 29 October 2020 Available online xxx Keywords: DFT Nanomagnetism 2D heterostructure Graphene MoS 2 abstract Graphene/MoS 2 heterostructure (G/MS-H) has distinctive and superlative electronic properties as it contains features of both graphene and MoS 2 . Our first-principles calculations reveal this heterostructure has a little bandgap (40 meV) and zero magnetic moment in the pristine form. In the present work, we have attempted to induce magnetism in the resultant heterostructure by adsorbing Cr atom at (i) Top (G- Top) (ii) Hollow (G-Hollow) configurations in the graphene layer and (iii) Top (S-Top) and (iv) Hollow (S- Hollow) in the MoS 2 layer. However, only G-Top and S-Hollow are energetically favorable amid these configurations. Our results demonstrate that Cr-adsorption persuades the significant magnetic moment. Both the stable configurations (G-Top and S-Hollow) transpire metallicity with a Dirac point shift in the valence band. The magnetism originates from the interactions between Cr-3d states with C-2p and S-3p states. These results summarize that the resultant adsorbed heterostructure may serve as a phenomenal breakthrough for nanomagnetism. © 2020 Elsevier B.V. All rights reserved. 1. Introduction The latest progression and development in the research of novel 2D materials have opened up new avenues for the fabrication of very thin structures (in the range of nm) with restrained properties. The first member of this family is graphene, a 2D analog of carbon allotrope, graphite, and was synthesized in 2004 at the University of Manchester [1]. Graphene has several peculiar properties which proved its worth in almost all areas especially in photonics, elec- tronics, electrochemistry, optoelectronics, and photovoltaics [2e10]. Aside from tremendous applications, graphene has some shortcomings as well. It reserves zero bandgap and zero magnetic moment in a pristine form which limit its application to optoelec- tronics and spintronics [11e 14]. Previous theoretical and experi- mental studies showed the electronic and magnetic properties of graphene can be tackled easily by utilizing diverse substrates [15e21], chemical functionalization [22e27], forming nanoribbions [28,29], and with defects (tacking adatom, dopants and creating vacancies) [30e35]. The next popular members of 2D family that grabbed immense attention in their court is transition metal dichalcogenides (TMDs). TMDs form hexagonal lattice-like graphene and are represented as MX 2 where M represents a transition metal element from group IV to VI and X is a chalcogen element (S, Se, and Te). Unlike graphene, MoS 2 is a direct bandgap semiconductor with a handful of inter- esting and superlative optical, electronic, and mechanical properties [36e40]. Also, over time, as fabrication techniques improved, the era of van der Waals heterostructures speedily came into existence. These heterostructures are made up of the layering of different 2D materials like stacking Lego bricks in a precisely chosen sequence. In this way, many recent experimental and theoretical research in this area have shown that making heterostructure is an efficient way to * Corresponding author. E-mail addresses: manishdft@gmail.com, mkumar@kuk.ac.in (M.K. Kashyap). Contents lists available at ScienceDirect Journal of Alloys and Compounds journal homepage: http://www.elsevier.com/locate/jalcom https://doi.org/10.1016/j.jallcom.2020.157776 0925-8388/© 2020 Elsevier B.V. All rights reserved. Journal of Alloys and Compounds xxx (xxxx) xxx Please cite this article as: R. Singla, S. Kumar, T.A. Hackett et al., Genesis of magnetism in graphene/MoS 2 van der Waals heterostructures via interface engineering using Cr-adsorption, Journal of Alloys and Compounds, https://doi.org/10.1016/j.jallcom.2020.157776