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      Quantum interference mediated vertical molecular tunneling transistors

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          Abstract

          We report graphene/self-assembly monolayer vertical molecular transistors operating in the quantum tunneling regime.

          Abstract

          Molecular transistors operating in the quantum tunneling regime represent potential electronic building blocks for future integrated circuits. However, due to their complex fabrication processes and poor stability, traditional molecular transistors can only operate stably at cryogenic temperatures. Here, through a combined experimental and theoretical investigation, we demonstrate a new design of vertical molecular tunneling transistors, with stable switching operations up to room temperature, formed from cross-plane graphene/self-assembled monolayer (SAM)/gold heterostructures. We show that vertical molecular junctions formed from pseudo- p-bis((4-(acetylthio)phenyl)ethynyl)- p-[2,2]cyclophane (PCP) SAMs exhibit destructive quantum interference (QI) effects, which are absent in 1,4-bis(((4-acetylthio)phenyl)ethynyl)benzene (OPE3) SAMs. Consequently, the zero-bias differential conductance of the former is only about 2% of the latter, resulting in an enhanced on-off current ratio for (PCP) SAMs. Field-effect control is achieved using an ionic liquid gate, whose strong vertical electric field penetrates through the graphene layer and tunes the energy levels of the SAMs. The resulting on-off current ratio achieved in PCP SAMs can reach up to ~330, about one order of magnitude higher than that of OPE3 SAMs. The demonstration of molecular junctions with combined QI effect and gate tunability represents a critical step toward functional devices in future molecular-scale electronics.

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          Efficient index handling of multidimensional periodic boundary conditions

          An efficient method is described to handle mesh indexes in multidimensional problems like numerical integration of partial differential equations, lattice model simulations, and determination of atomic neighbor lists. By creating an extended mesh, beyond the periodic unit cell, the stride in memory between equivalent pairs of mesh points is independent of their position within the cell. This allows to contract the mesh indexes of all dimensions into a single index, avoiding modulo and other implicit index operations.
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            The SIESTA method for ab initio order-N materials simulation

            We have developed and implemented a self-consistent density functional method using standard norm-conserving pseudopotentials and a flexible, numerical LCAO basis set, which includes multiple-zeta and polarization orbitals. Exchange and correlation are treated with the local spin density or generalized gradient approximations. The basis functions and the electron density are projected on a real-space grid, in order to calculate the Hartree and exchange-correlation potentials and matrix elements, with a number of operations that scales linearly with the size of the system. We use a modified energy functional, whose minimization produces orthogonal wavefunctions and the same energy and density as the Kohn-Sham energy functional, without the need of an explicit orthogonalization. Additionally, using localized Wannier-like electron wavefunctions allows the computation time and memory, required to minimize the energy, to also scale linearly with the size of the system. Forces and stresses are also calculated efficiently and accurately, thus allowing structural relaxation and molecular dynamics simulations.
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              2D materials and van der Waals heterostructures

              The physics of two-dimensional (2D) materials and heterostructures based on such crystals has been developing extremely fast. With new 2D materials, truly 2D physics has started to appear (e.g. absence of long-range order, 2D excitons, commensurate-incommensurate transition, etc). Novel heterostructure devices are also starting to appear - tunneling transistors, resonant tunneling diodes, light emitting diodes, etc. Composed from individual 2D crystals, such devices utilize the properties of those crystals to create functionalities that are not accessible to us in other heterostructures. We review the properties of novel 2D crystals and how their properties are used in new heterostructure devices.
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                Author and article information

                Journal
                Sci Adv
                Sci Adv
                SciAdv
                advances
                Science Advances
                American Association for the Advancement of Science
                2375-2548
                October 2018
                12 October 2018
                : 4
                : 10
                : eaat8237
                Affiliations
                [1 ]Department of Chemistry and Biochemistry, University of California, Los Angeles, Los Angeles, CA 90095, USA.
                [2 ]Physics Department, Lancaster University, Lancaster LA1 4YB, UK.
                [3 ]Stratingh Institute for Chemistry and Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 4, Groningen 9747 AG, Netherlands.
                [4 ]Department of Materials Science and Engineering, University of California, Los Angeles, Los Angeles, CA 90095, USA.
                [5 ]Key Laboratory for Micro-Nano Optoelectronic Devices of Ministry of Education, School of Physics and Electronics, Hunan University, Changsha 410082, China.
                [6 ]California NanoSystems Institute, University of California, Los Angeles, Los Angeles, CA 90095, USA.
                Author notes
                [*]

                These authors contributed equally to this work.

                []Corresponding author. Email: xduan@ 123456chem.ucla.edu (X.D.); c.lambert@ 123456lancaster.ac.uk (C.J.L.)
                Author information
                http://orcid.org/0000-0002-1513-8497
                http://orcid.org/0000-0001-8086-7613
                http://orcid.org/0000-0003-1135-6742
                http://orcid.org/0000-0001-6581-3385
                http://orcid.org/0000-0001-9424-8418
                http://orcid.org/0000-0003-4192-8430
                http://orcid.org/0000-0003-2368-4647
                http://orcid.org/0000-0003-1793-0741
                http://orcid.org/0000-0002-0895-2095
                http://orcid.org/0000-0002-4321-6288
                Article
                aat8237
                10.1126/sciadv.aat8237
                6184693
                30333991
                b49d7f86-c6b7-489e-aa60-9f5d9afb73f1
                Copyright © 2018 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

                This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.

                History
                : 09 April 2018
                : 04 September 2018
                Funding
                Funded by: doi http://dx.doi.org/10.13039/100000006, Office of Naval Research;
                Award ID: N00014-15-1-2368
                Categories
                Research Article
                Research Articles
                SciAdv r-articles
                Applied Physics
                Materials Science
                Applied Physics
                Custom metadata
                Eunice Diego

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