Materials Design and Discovery, and the Challenges of the Materials Genome Nicola Marzari, EPFL

Materials Design and Discovery, and the Challenges of the Materials Genome Nicola Marzari, EPFL

The good news: Europe at the forefront in codes for materials simula@ons To name just a few: Quantum- ESPRESSO (Trieste/ Cineca/EPFL), CP2K (UZH), CPMD (IBM Zurich), Abinit (Louvain), VASP (Wien), Castep and Onetep (Cambridge), SIESTA (Madrid), Wien2K (Wien), FLEUR (Julich), ExciUng/ELK (Berlin/Halle) E.g. 700 papers published in 2012 using Q- E

Accelera@ng materials design

Digging for gold

5 or shopping for diamonds?

Some background on first- principles (i.e. quantum mechanical) materials simula@ons

AROSA, CANTON DES GRISONS, 27 DECEMBER 1925 at the moment i am struggling with a new atomic theory. i am very optimistic about this thing and expect that if I can only solve it, it will be very beautiful. e. schrödinger

A lab that doubles every 14 months Total computing power in TOP500 10 16 Computing power (FLOPs) 10 15 10 14 10 13 10 12 6/1993 6/1994 6/1995 6/1996 6/1997 6/1998 6/1999 6/2000 6/2001 6/2002 6/2003 6/2004 6/2005 6/2006 6/2007 6/2008 6/2009 6/2010 11/1993 11/1994 11/1995 11/1996 11/1997 11/1998 11/1999 11/2000 11/2001 11/2002 11/2003 11/2004 11/2005 11/2006 11/2007 11/2008 11/2009 Jack Dongarra, CCP 2011

! Most cited papers in the history of APS! Journal! #!cites! Title! Author(s)! 1! PRB!(1988)! 39190! Development!of!the!ColleBSalvetti!CorrelationBEnergy!! Lee,!Yang,!Parr! 2! PRL!(1996)! 25452! Generalized!Gradient!Approximation!Made!Simple! Perdew,!Burke,!Ernzerhof! 3! PRA!(1988)! 22904! DensityBFunctional!ExchangeBEnergy!Approximation!...! Becke! 4! PR!(1965)! 20142! SelfBConsistent!Equations!Including!Exchange!and!Correlation!! Kohn!and!Sham! 5! PRB!(1996)!!!13731! Efficient!Iterative!Schemes!for!Ab!Initio!TotalBEnergy!! Kresse!and!Furthmuller! 6! PRB!(1976)! 13160!!!!Special!Points!for!BrillouinBZone!Integrations! Monkhorst!and!Pack! 7! PRB!(1992)! 10876! Accurate!and!Simple!Analytic!Representation!of!the!Electron!! Perdew!and!Wang! 8! PRB!(1999)! 10007! From!Ultrasoft!Pseudopotentials!to!the!Projector!Augmented!! Kresse!and!Joubert! 9! PRB!(1990)! 9840! Soft!SelfBConsistent!Pseudopotentials!in!a!Generalized!! Vanderbilt! 10! PR!(1964)! 9789! Inhomogeneous!Electron!Gas! Hohenberg!and!Kohn! 11! PRB!(1981)! 9787! SelfBInteraction!Correction!to!DensityBFunctional!Approx.!! Perdew!and!Zunger! 12! PRB!(1992)! 9786! Atoms,!Molecules,!Solids,!and!Surfaces!B!Applications!of!the!! Perdew,!Chevary,!! 13! PRB!(1986)! 9313! DensityBFunctional!Approx.!for!the!CorrelationBEnergy!! Perdew! 14! PR!(1934)! 9271! Note!on!an!Approximation!Treatment!for!ManyBElectron!Systems! Moller!and!Plesset! 15! PRB!(1994)! 9100! Projector!AugmentedBWave!Method! Blochl! 16! PRL!(1980)! 7751! GroundBState!of!the!ElectronBGas!by!a!Stochastic!Method! Ceperley!and!Alder! 17! PRL!(1987)!!!!!!7663! Inhibited!Spontaneous!Emission!in!Solid>State!Physics!! Yablonovitch! 18! PRL!(1986)! 7589! Atomic!Force!Microscope! Binnig,!Quate,!Gerber! 19! PRB!(1991)! 7425! Efficient!Pseudopotentials!for!PlaneBWave!Calculations! Troullier!and!Martins! 20! PRB!(1993)! 6925! Ab!initio!Molecular!Dynamics!for!Liquid!Metals! Kresse!and!Hafner! 21! PR!(1961)! 6467! Effects!of!Configuration!Interaction!on!Intensities!and!Phase!Shifts! Fano! 22! PR!(1957)! 6260! Theory!of!Superconductivity! Bardeen,!Cooper,!Schrieffer!!

What can first- principles do for me? Fairly straightorward, but *fundamental*: equilibrium structures, thermodynamic stability, thermomechanical properues, electronic structure, energeucs and reacuons Harder: vibrauonal and magneuc spectroscopies (IR, Raman, NMR, EPR), XPS/XANES, BCS superconducuvity, opucal absorpuon, phase diagrams Jedi master: thermal and electrical conducuviues, photoemission spectroscopies Predic@ve accuracy is a key challenge

Electrical and thermal transport from first- principles Nanoscale devices for microelectronics (either silicon or carbon based) Bulk or nanostructured thermoelectrics (harvesung waste energy, cooling) Source: Nature Materials

Microscopic origin of transport Density- func@onal perturba@on theory hxp://www.quantum- espresso.org

Valida@on through spectroscopies P.H. Tan et al., Nature Materials (2012)

Thermal conduc@vity: Si 1- x Ge x J. Garg, N. Bonini, B. Kozinsky and N. Marzari, Phys. Rev. LeX. (2011)

Mean free paths: Si 1- x Ge x J. Garg, N. Bonini, B. Kozinsky and N. Marzari, Phys. Rev. LeX. (2011)

Engineering high- performance thermoelectrics

Making sense of experiments: graphene Simula@ons: A. Cepellob, N. Bonini, and N. Marzari (2013) expts from A. Balandin (Nature Materials 2011)

ρ e ph (Ω) 25 0 100 10 1 Theory Experiment (Efetov & Kim) Upper bounds on intrinsic mobility 100 200 300 400 T (K) n (10 13 cm 2 ) 1.36 2.86 4.65 6.85 10.8 (c) 100 200 300 400 T (K) n (10 13 cm 2 ) 1.36 2.86 4.65 6.85 10.8 (d) 0.1 10 100 T (K) Theory 10 100 T (K) Experiment (Efetov & Kim) C. H. Park, N. Bonini, G. Samzonides, B. Kozinsky, and N. Marzari (2013)

How many materials do we know? ICSD (InternaUonal Crystallographic Structure Database): 143,000 entries Very lixle is known for the vast majority of these Basic properues for all of them can be calculated in a few hours on petaflop- class machines

Materials design: Once a material property can be calculated accurately from quantum simula@ons, it becomes straightorward to explore rapidly and systema@cally thousands of compounds for improved performance.

Proper@es/performance è descriptors è high- throughput searches Courtesy of S. Curtarolo / Nature Materials (2013)

Novel ferroelectric perovskites G. Pizzi, A. Cepellob, S. Halilov and in collabora@on with M. Fornari, G. Ceder, R. Armiento, B. Kozinsky

Ferroelectric phase transi@ons Cubic Orthorhombic Tetragonal Rhombohedral Preliminary results F(T) of rhombohedral phase taken as reference Crossing points where phase transitions occur T (K) DFT Exp T-C 670 403 O-T 309 278 R O T C R-O 102 183

Run computer laboratories with a materials informa@cs platorm: prepare, organize, run, store, datamine, share, repeat Developing AIDA ( Automated Infrastructure and Database for Ab- ini@o calcula@ons - EPFL+Robert Bosch RTC) a librarian: job tracking and organizauon of all present and future acuviues of a group a library: databases of jobs and job results a network of connected libraries: possibility to share databases with of other groups

User interface Select: Structure Codes Desired proper@es AIDA server Backed up data storage and databases Codes database Structures Database Calcula@on Database: History Permanent results storage Calcula@on Data analysis CSCS Input file genera@on Output parser Work submission Execu@on on clusters User interface

AIDA network Clusters Users Group 1 AIDA server Databases Private data Public/shared data Permissions for access to each entry (calcula@on, structure,...) UUIDs associated to each entry Scripts to download/upload entries from/to remote DBs or sync two AIDA DBs Some data shared AIDA server AIDA server Group 2 Some data shared Group 3

Rapid and long- term reproducibility of calcula@ons: workflows and dependencies

Conclusions First- principles calcula@ons have reached predic@ve accuracy for many (but not all!) materials and materials proper@es Intelligent high- throughput searches are the next, natural step, and lead to materials design and discovery Computa@onal laboratories can and should be organized with an informa@cs infrastructure to organize, run, store, datamine, share, and repeat calcula@ons