NOVEL TWO-DIMENSIONAL MATERIALS FROM HIGH-THROUGHPUT COMPUTATIONAL EXFOLIATION Nicola Marzari, EPFL
GREAT ENTHUSIASM FOR COMPUTATIONAL MATERIALS DISCOVERY
NATURE, OCT 2014 THE TOP 100 PAPERS: 12 papers on density- functional theory in the top-100 most cited papers in the entire scientific literature, ever.
MOST CITED PAPERS IN THE HISTORY OF APS Journal # cites Title Author(s) 1 PRL (1996) 78085 Generalized Gradient Approximation Made Simple Perdew, Burke, Ernzerhof 2 PRB (1988) 67303 Development of the Colle-Salvetti Correlation-Energy … Lee, Yang, Parr 3 PRB (1996) 41683 Efficient Iterative Schemes for Ab Initio Total-Energy … Kresse and Furthmuller 4 PR (1965) 36841 Self-Consistent Equations Including Exchange and Correlation … Kohn and Sham 5 PRA (1988) 36659 Density-Functional Exchange-Energy Approximation ... Becke 6 PRB (1976) 31865 Special Points for Brillouin-Zone Integrations Monkhorst and Pack 7 PRB (1999) 30940 From Ultrasoft Pseudopotentials to the Projector Augmented … Kresse and Joubert 8 PRB (1994) 30801 Projector Augmented-Wave Method Blochl 9 PR (1964) 30563 Inhomogeneous Electron Gas Hohenberg and Kohn 10 PRB (1993) 19903 Ab initio Molecular Dynamics for Liquid Metals Kresse and Hafner 11 PRB (1992) 17286 Accurate and Simple Analytic Representation of the Electron … Perdew and Wang 12 PRB (1990) 15618 Soft Self-Consistent Pseudopotentials in a Generalized … Vanderbilt 13 PRB (1992) 15142 Atoms, Molecules, Solids, and Surfaces - Applications of the … Perdew, Chevary, … 14 PRB (1981) 14673 Self-Interaction Correction to Density-Functional Approx. … Perdew and Zunger 15 PRB (1986) 13907 Density-Functional Approx. for the Correlation-Energy … Perdew 16 RMP (2009) 13513 The Electronic Properties of Graphene Castro Neto et al. 17 PR (1934) 12353 Note on an Approximation Treatment for Many-Electron Systems Moller and Plesset 18 PRB (1972) 11840 Optical Constants on Noble Metals Johnson and Christy Marzari 19 PRB (1991) 11580 Efficient Pseudopotentials for Plane-Wave Calculations Troullier and Martins (11 Apr 2019) 20 PRL (1980) 10784 Ground-State of the Electron-Gas by a Stochastic Method Ceperley and Alder
THE BUSINESS MODEL Computing power 1993-2018 Sum of the top 500 supercomputers Number 1 Number 500 If brick-and-mortar laboratories were to follow this pace, an experiment that took one year in 1989 would take one second in 2018 (30-million-fold increase)
1) PREDICTIVE ACCURACY 2) REALISTIC COMPLEXITY 3) MATERIALS’ INFORMATICS
HOW WELL CAN WE REPRODUCE THE REAL WORLD? G. Prandini, G.M. Rignanese, and N. Marzari (2019)
HOW WELL CAN WE REPRODUCE THE REAL WORLD? THEORY EXPTS (Kim 2010) C.-H. Park et al., Nano Letters (2014) T. Y. Kim, C.-H. Park, and N. Marzari, Nano Letters (2016)
COMPUTATIONAL EXFOLIATION OF COMPUTATIONAL EXFOLIATION OF ALL KNOWN INORGANIC MATERIALS ALL KNOWN INORGANIC MATERIALS
PHYSICS AND CHEMISTRY IN LOW DIMENSIONS Binnig, Rohrer 1986 Laughlin, Störmer, Fert, Grünberg von Klitzing 1985 Tsui 1989 2007 Geim and Novoselov 2010 Bednorz and Müller 1987 Ertl 2007
HOW DO WE PRODUCE 2D MATERIALS? Mechanical (e.g. Geim/Novoselov, fig. from Nature/NUS) or liquid exfoliation (e.g. Nicolosi/Coleman, fig. from Science). Also, bottom- up: CVD and wet chemical synthesis.
HIGH-THROUGHPUT COMPUTATIONAL EXFOLIATION Exfoliation Applications Characterization High e/h mobility External databases (ICSD, COD) Topological CDW, spintronics Geometrically Electronic layered VdW-DFT Plasmonics Magnetic electronic structure, binding energies Photocatalysis Mechanical Membranes Building on a previous study of 92 two-dimensional ……. compounds: S. Lebègue et al., PRX (2013); see also R. Hennig et al., PRL (2017) and E. Reed et al., Nano Letters (2017).
AUTOMATIC WORKFLOWS: FROM STRUCTURE TO PROPERTY Input: Structure 20 DFT calculations Relaxation of of deformed structures input structure Fits Output: Elastic tensor
Automation Data Environment Sharing http://www.aiida.net (MIT BSD, with Robert Bosch) G. Pizzi et al., Comp. Mat. Sci. 111, 218 (2016)
AN OPERATING SYSTEM FOR COMPUTATIONAL SCIENCE G. Pizzi et al., Comp. Mat. Sci. 111, 218 (2016)
AN OPERATING SYSTEM FOR COMPUTATIONAL SCIENCE
ALL DATA FROM COMPLEX WORKFLOWS AS DIRECTED ACYCLIC GRAPHS Nodes: Calculations Codes Data
LET’S START FROM A MATERIAL (VOBr 2 )
FROM ICSD TO A WORKING STRUCTURE Primitive cell & structure symmetry refinement
3D RELAXATION Quantum ESPRESSO Workflow Lowdimfinder on Individual DFT relaxed structure calculations
MAGNETIC SCREENING OF THE 2D MONOLAYER Electronic & magnetic workflow
REMOVING MECHANICAL INSTABILITIES Phonon calculation Stabilization procedure Displace atoms along unstable eigenvectors Final atomic/cellr elaxation
STABILITY ANALYSIS Band structures Phonon dispersions T. Sohier et al., Nano Letters (2017)
FINALLY…
INFRASTRUCTURE AND DISSEMINATION http://materialscloud.org
GEOMETRIC IDENTIFICATION OF LAYERED MATERIALS S. Alvarez, Dalton Transactions (2013) 𝒘𝒆𝒙 + 𝒔 𝒌 𝒘𝒆𝒙 − ∆ 𝒆 𝒋,𝒌 < 𝒔 𝒋
HOW RELIABLE ARE THE FUNCTIONALS? RPA from T. Björkman et al., PRL 108, 235502 (2012)`
HOW MANY CANDIDATES? GEOMETRIC SCREENING Unique to Unique to Common Total COD ICSD to both 479986 * Entries analyzed 307616 172370 186282 * CIF inputs 99212 87070 Unique 3D structures 60354 34548 13521 108423 Layered 3D structures 1180 3257 1182 5619 * At this level unicity is not tested
HOW MANY CANDIDATES? QUANTUM SCREENING Not exfoliable Potentially 789 monolayers exfoliable Easily 1036 monolayers exfoliable Difference in interlayer distance when computed with/without vdW functionals (%) E b < 30 meV/Å 2 (DF2-C09) or E b < 35 meV/Å 2 (rVV10) → 2D, easily exfoliable • • In-between → 2D, potentially exfoliable • E b > 130 meV/Å 2 → not 2D (discarded)
2D PROTOTYPES
ELECTRICAL TRANSPORT: AN AiiDA MOBILITY WORKFLOW - FET-doping explicitly included - Open-boundary conditions - Automation: Identification of relevant pockets, adaptive sampling - Systematic integration of el-ph couplings - Efficient/robust numerical solution to Boltzmann equation T. Sohier et al., Phys. Rev. Materials (2018)
UNDERSTANDING Material P 4 (h) P 4 (e) MoS 2 (e) WS 2 (e) As(e) WSe 2 (e) Mobility 612 307 139 61 45 24 (300 K, cm 2 /Vs) Mobility increases <-> number of valleys decreases T. Sohier et al., Phys. Rev. Materials (2018)
ENGINEERING Arsenene T. Sohier et al., arXiv (2019)
SOME FERMIOLOGY… Magnetic metals and insulators Half-semiconductors Plasmonics and TC In collaboration with K. Thygesen (DTU)
Z 2 TOPOLOGICAL INSULATORS A. Marrazzo et al ., in preparation (2019)
THE DISCOVERY OF JACUTINGAITE
THE DISCOVERY OF JACUTINGAITE Classified as potentially exfoliable (binding energy of 60 meV Å -2 )
THE DISCOVERY OF JACUTINGAITE Classified as potentially exfoliable (binding energy of 60 meV Å -2 )
THE KANE-MELE PHYSICS OF JACUTINGAITE
THE KANE-MELE PHYSICS OF JACUTINGAITE
THE KANE-MELE PHYSICS OF JACUTINGAITE
THE KANE-MELE PHYSICS OF JACUTINGAITE
THE KANE-MELE PHYSICS OF JACUTINGAITE
arXiv
SINGLE CRYSTAL ARPES, EXFOLIATION A. Tamai and F. Baumberger (U. of Geneva) A. Vymazalová (Czech A. Murello, F. Stellacci (EPFL) Geological Survey) K Pt 2 HgSe 3 single crystals, Transport, A. Morpurgo E. Giannini (U. of Geneva) (U. of Geneva) M K G K M K
THERE IS PLENTY OF ROOM AT THE TOP • High electron/hole mobility devices • Topological insulators, quantum computing • Ferromagnetic/spintronics in 2D • Charge-density waves and superconductors • Plasmonics, transparent conductors 3D layered parents: • Solid-state ionic conductors • Hydrogen or oxygen evolution catalysts • Membranes for filtration/separation • Piezo, ferro, and thermoelectrics N. Mounet, M. Gibertini, P. Schwaller, D. Campi, A. Merkys, A. Marrazzo, T. Sohier, I. E. Castelli, A. Cepellotti, G. Pizzi and N. Marzari, Nature Nanotechnology 13, 246 (2018)
2D ACKNOWLEDGMENTS Nicolas Mounet Marco Gibertini Philippe Schwaller Davide Campi Andrius Merkys CERN U. of Geneva IBM/Cambridge Vilnius Antimo Marrazzo Andrea Cepellotti Giovanni Pizzi Thibault Sohier Ivano E. Castelli DTU Harvard U.
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