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NOVEL TWO-DIMENSIONAL MATERIALS FROM HIGH-THROUGHPUT COMPUTATIONAL - - PowerPoint PPT Presentation

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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

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NOVEL TWO-DIMENSIONAL MATERIALS FROM HIGH-THROUGHPUT COMPUTATIONAL EXFOLIATION Nicola Marzari, EPFL

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GREAT ENTHUSIASM FOR COMPUTATIONAL MATERIALS DISCOVERY

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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.

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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 19 PRB (1991) 11580 Efficient Pseudopotentials for Plane-Wave Calculations Troullier and Martins 20 PRL (1980) 10784 Ground-State of the Electron-Gas by a Stochastic Method Ceperley and Alder

MOST CITED PAPERS IN THE HISTORY OF APS

Marzari (11 Apr 2019)

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THE BUSINESS MODEL

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)

Computing power 1993-2018

Sum of the top 500 supercomputers Number 1 Number 500

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1) PREDICTIVE ACCURACY 2) REALISTIC COMPLEXITY 3) MATERIALS’ INFORMATICS

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HOW WELL CAN WE REPRODUCE THE REAL WORLD?

  • G. Prandini, G.M. Rignanese, and N. Marzari (2019)
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C.-H. Park et al., Nano Letters (2014)

  • T. Y. Kim, C.-H. Park, and N. Marzari, Nano Letters (2016)

THEORY EXPTS (Kim 2010)

HOW WELL CAN WE REPRODUCE THE REAL WORLD?

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COMPUTATIONAL EXFOLIATION OF ALL KNOWN INORGANIC MATERIALS COMPUTATIONAL EXFOLIATION OF ALL KNOWN INORGANIC MATERIALS

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PHYSICS AND CHEMISTRY IN LOW DIMENSIONS

von Klitzing 1985 Laughlin, Störmer, Tsui 1989 Fert, Grünberg 2007 Bednorz and Müller 1987 Geim and Novoselov 2010 Ertl 2007 Binnig, Rohrer 1986

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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.

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External databases (ICSD, COD) Geometrically layered VdW-DFT electronic structure, binding energies Magnetic Electronic Mechanical Photocatalysis Membranes ……. Exfoliation Characterization Applications

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).

HIGH-THROUGHPUT COMPUTATIONAL EXFOLIATION

Plasmonics CDW, spintronics Topological High e/h mobility

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AUTOMATIC WORKFLOWS: FROM STRUCTURE TO PROPERTY

Input: Structure Relaxation of input structure 20 DFT calculations

  • f deformed structures

Fits Output: Elastic tensor

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Automation Data Environment Sharing

http://www.aiida.net (MIT BSD, with Robert Bosch)

  • G. Pizzi et al., Comp. Mat. Sci. 111, 218 (2016)
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  • G. Pizzi et al., Comp. Mat. Sci. 111, 218 (2016)

AN OPERATING SYSTEM FOR COMPUTATIONAL SCIENCE

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AN OPERATING SYSTEM FOR COMPUTATIONAL SCIENCE

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ALL DATA FROM COMPLEX WORKFLOWS AS DIRECTED ACYCLIC GRAPHS Nodes: Calculations Codes Data

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LET’S START FROM A MATERIAL (VOBr2)

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FROM ICSD TO A WORKING STRUCTURE

Primitive cell & structure symmetry refinement

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3D RELAXATION

Lowdimfinder on relaxed structure Individual DFT calculations Quantum ESPRESSO Workflow

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MAGNETIC SCREENING OF THE 2D MONOLAYER

Electronic & magnetic workflow

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REMOVING MECHANICAL INSTABILITIES

Stabilization procedure

Phonon calculation

Displace atoms along unstable eigenvectors Final atomic/cellr elaxation

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Band structures Phonon dispersions

  • T. Sohier et al., Nano Letters (2017)

STABILITY ANALYSIS

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FINALLY…

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INFRASTRUCTURE AND DISSEMINATION

http://materialscloud.org

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GEOMETRIC IDENTIFICATION OF LAYERED MATERIALS

𝒆𝒋,𝒌 < 𝒔𝒋

𝒘𝒆𝒙 + 𝒔𝒌 𝒘𝒆𝒙 − ∆

  • S. Alvarez, Dalton Transactions (2013)
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HOW RELIABLE ARE THE FUNCTIONALS?

RPA from T. Björkman et al., PRL 108, 235502 (2012)`

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HOW MANY CANDIDATES? GEOMETRIC SCREENING

*At this level unicity is not tested

Unique to COD Unique to ICSD Common to both

Total

Entries analyzed 307616 172370 479986* CIF inputs 99212 87070 186282* Unique 3D structures 60354 34548 13521 108423 Layered 3D structures 1180 3257 1182 5619

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Difference in interlayer distance when computed with/without vdW functionals (%)

  • Eb < 30 meV/Å2 (DF2-C09) or Eb < 35 meV/Å2 (rVV10) → 2D, easily exfoliable
  • In-between→ 2D, potentially exfoliable
  • Eb > 130 meV/Å2 → not 2D (discarded)

HOW MANY CANDIDATES? QUANTUM SCREENING

Easily exfoliable Potentially exfoliable

1036 monolayers 789 monolayers

Not exfoliable

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2D PROTOTYPES

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ELECTRICAL TRANSPORT: AN AiiDA MOBILITY WORKFLOW

  • FET-doping explicitly

included

  • Open-boundary conditions
  • Automation: Identification
  • f 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)
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UNDERSTANDING

Material P4(h) P4(e) MoS2(e) WS2(e) As(e) WSe2(e) Mobility 612 307 139 61 45 24

(300 K, cm2/Vs) Mobility increases <-> number of valleys decreases

  • T. Sohier et al., Phys. Rev. Materials (2018)
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ENGINEERING

Arsenene

  • T. Sohier et al., arXiv (2019)
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SOME FERMIOLOGY…

Magnetic metals and insulators Half-semiconductors

In collaboration with K. Thygesen (DTU)

Plasmonics and TC

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Z2 TOPOLOGICAL INSULATORS

  • A. Marrazzo et al., in preparation (2019)
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THE DISCOVERY OF JACUTINGAITE

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THE DISCOVERY OF JACUTINGAITE

Classified as potentially exfoliable (binding energy of 60 meV Å-2)

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THE DISCOVERY OF JACUTINGAITE

Classified as potentially exfoliable (binding energy of 60 meV Å-2)

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THE KANE-MELE PHYSICS OF JACUTINGAITE

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THE KANE-MELE PHYSICS OF JACUTINGAITE

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THE KANE-MELE PHYSICS OF JACUTINGAITE

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THE KANE-MELE PHYSICS OF JACUTINGAITE

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THE KANE-MELE PHYSICS OF JACUTINGAITE

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arXiv

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  • A. Tamai and F. Baumberger

(U. of Geneva)

K K K K M M G

SINGLE CRYSTAL ARPES, EXFOLIATION

Pt2HgSe3 single crystals,

  • E. Giannini (U. of Geneva)

Transport, A. Morpurgo (U. of Geneva)

  • A. Murello, F. Stellacci (EPFL)
  • A. Vymazalová (Czech

Geological Survey)

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  • 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

THERE IS PLENTY OF ROOM AT THE TOP

  • 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)

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Andrea Cepellotti Andrius Merkys Philippe Schwaller Ivano E. Castelli Davide Campi Antimo Marrazzo Thibault Sohier Marco Gibertini Nicolas Mounet Giovanni Pizzi

2D ACKNOWLEDGMENTS

CERN U. of Geneva IBM/Cambridge Vilnius DTU Harvard U.