1. Materials by Design; Materials for Harsh Environments
John Sarrao
7/19/17

2. The “tree” provides a context with which to address your charge
Description of the technology
Application of the technology for fusion energy, e.g. in a fusion power plant (my read of your planning; NNSA mission need as a proxy)
Expected performance of the technology – what is the critical variable (or variables) that determines or controls the output of the technology?
Design variables – what are the parameters that can be controlled in order to optimize the performance of the technology?
Risks and uncertainties with the technology development and performance
Current maturity of the technology, using e.g. Technical Readiness Levels
Required development for the technology
Other considerations and broader impact

3. …that motivates new capabilities and will demand co-design for success
NNSA’s need to predict and control the microstructure of materials is also a science frontier…
From Quanta to the Continuum: Opportunities for Mesoscale Science
Challenges at the Frontiers of Matter and Energy: Transformative Opportunities for Discovery Science
“In particular, we believe that filling the gap in our ability to ‘predict and control from materials and devices to manufacturing processes’ is especially urgent.”
science.energy.gov/bes/news-and- resources/reports/basic-research-needs/
…that motivates new capabilities and will demand co-design for success

4. Bottom up meets top down at the mesoscale
The Stockpile demands process-aware performance.
Aging
Manufacturing
Material replacement
Safety and surety
integral testing
microstructure-aware
CINT has defined nanoscience integration.
Pulsed laser deposition yields epitaxial metallic nanopillars integrated in oxide matrices
Tunable densities on selected substrates yields controllable anisotropic optical properties
mesoscale
nanoscale

5. (exascaleproject.org)
Exascale Computing & MaRIE-like facilities will accelerate progress IF we emphasize co-design
(exascaleproject.org)
(marie.lanl.gov)
An opportunity for FES is to exploit these capabilities and motivate new ones

6. Imagine…

7. The 2007 Grand Challenges are still compelling AND the landscape has changed as a result of our progress
How Do We Control Material Processes at the Level of Electrons? How do we design and perfect atom- and energy-efficient synthesis of revolutionary new forms of matter with tailored properties? How do remarkable properties of matter emerge from complex correlations of the atomic or electronic constituents and how can we control these properties? How can we master energy and information on the nanoscale to create new technologies with capabilities rivaling those of living things? How do we characterize and control matter away - especially very far away - from equilibrium?

8. New Transformative Opportunities have emerged that have their foundations in the Grand Challenges
“The most exciting phrase to hear in science, the one that heralds new discoveries, is not ‘Eureka!’ but ‘That's funny...’” ―Isaac Asimov
Mastering Hierarchical Architectures and Beyond-Equilibrium Matter Beyond Ideal Materials and Systems: Understanding the Critical Roles of Heterogeneity, Interfaces and Disorder Harnessing Coherence in Light and Matter Crosscutting Opportunities Revolutionary Advances in Models, Mathematics, Algorithms, Data, and Computing Exploiting Transformative Advances in Imaging Capabilities Across Multiple Scales

9. Challenges at the Frontiers of Matter and Energy: Transformative Opportunities for Discovery Science
Instrumentation
& Tools
Human Capital
Synthesis
Beyond Ideal Materials and Systems
Mastering Hierarchical Architectures
Harnessing Coherence in Light and Matter
Imaging Matter across Scales
Data, Algorithms and Computing
Efficient Synthesis for Tailored Properties
Energy and Information on the Nanoscale
Correlated Systems
Systems Away from Equilibrium
Control at the Level of Electrons

10. meso Meso: Beyond atomic, molecular, and nano classical quantum
isolated
interacting
collective
Talking points
Covers quantum to coninuum, rise of collective behavior, interacting degrees of freedom, appearance of defects, heterogeneous systems
Signatures
Diminished atomic granularity & energy quantization
Collective behavior & interacting degrees of freedom
simple
perfect
homogeneous
complex
imperfect
heterogeneous

11. Two Hallmarks of Mesoscale Phenomena are central to the FES challenge
Defects, fluctuations,
statistical variation
Heterogeneity in
structure and dynamics
nanoparticles: single grain, single domain
small molecules
perfect structure
large assemblies
imperfect structure
basis for genetic mutation
and evolution
In mesoscale and larger crystals
defects profoundly affect
• electrical conductivity
• mechanical response
• heat transport
meso and larger particles
heterogeneous grain, domain
and chemical structures
composite parts that cooperate
degrees of freedom interact across interface
enhance performance
steel
degrade performance
infrastructure

12. Cross-cutting Challenges
Opportunities for Mesoscale Tools and Instruments
Synthesis / Assembly
Directed synthesis of complex inorganic materials
Multi-step, multi- component assembly processes
Computational synthesis / assembly
Characterization
In situ, real time dynamic measurements:
4D materials science
Multi-modal experiments, e.g. structure + excitation + energy transfer
Multi-scale energy, time and space
Theory / Simulation
Far from equilibrium behavior
Heterogeneous/disordered systems
Dynamic functionality of composite systems
Cross-cutting Challenges
Co-design/integration of Synthesis  Characterization  Theory/Simulation
Directed Multi-step, multi-component assembly processes that scale
Multi-modal simultaneous and sequential measurements
spanning energy, length & time scales
Predictive theories and simulation of dynamic functionality 12

13. Mastering Hierarchical Architectures and Beyond-Equilibrium Matter
The transformative opportunity is to realize targeted functionality in materials by controlling the synthesis and assembly of hierarchical architectures and beyond‐equilibrium matter, thereby increasing dramatically the exploration space for enhanced function.
To realize this opportunity, several major advances are required:
 1) predictive models, including the incorporation of metastability, to guide the creation of beyond equilibrium matter
2) Mastering synthesis and assembly of hierarchical structures for multi-dimensional hybrid matter
3) in situ characterization of spatial and temporal evolution during their synthesis and assembly

14. Beyond Ideal Materials and Systems: Understanding the Critical Roles of Heterogeneity, Interfaces and Disorder
Developing a fundamental understanding of the roles of heterogeneities, interfacial processes, and disorder in materials behavior represents a transformative opportunity to move from ideal systems to the complexity of real systems under realistic conditions.
Science of scale
Slow and statistically rare events
“epidemiological” studies of heterogeneous populations
Science of degradation and lifetime prediction
geosciences

15. Harnessing Coherence in Light and Matter
The transformative opportunity is the potential ability to realize full control of large-scale quantum-coherent systems… the potential to revolutionize diverse fields through the control of the outcome of chemical reactions or the instantaneous state of a material.
new real‐time quantum microscopes that can visualize and control quantum matter
Long-lived temporally coherent states of quantum wavefunction
Ability to suppress decoherence effects of the environment
Role of symmetry protected states in coherent matter

16. Revolutionary Advances in Models, Mathematics, Algorithms, Data, and Computing
The convergence of theoretical, mathematical, computational, and experimental capabilities are poised to greatly accelerate our ability to find, predict, and control new materials, understand complex matter across a range of scales, and steer experiments towards illuminating deep scientific insights.

17. Exploiting Transformative Advances in Imaging Capabilities Across Multiple Scales
Making and exploiting advances in imaging capabilities emerge as national priorities because of their transformative impacts on materials discovery. … accelerating the introduction of new materials, the understanding of combustion and other chemical processes, and progress in materials synthesis; and solving longstanding challenges in the relationship between the structure of inhomogeneous matter and its behavior.
Attosecond measurements
High resolution, chemically resolved multiscale mapping
4D characterization
Advanced, spatially & temporally resolved spectroscopy

18. Materials behavior limits the performance of advanced energy systems needed for energy independence
Life extension, safety of existing reactor fleet
Improved affordability for new reactors
Sustainable fuel cycles
Fusion Reactor first wall materials t
FES Strategic Goal: “Support the development of the scientific understanding required to design and deploy the materials needed to support a burning plasma environment”

19. An outsider’s take on FES Materials Needs
Materials science as it relates to plasma and fusion sciences will provide the scientific foundations for greatly improved plasma confinement and heat exhaust. (FES Ten-Year Perspective)
A high-priority objective during this decade is to combine research on materials effects on plasma confinement (e.g., edge pedestal formation, and transport in the open field lines), high heat flux effects on materials, and neutron irradiation effects. The overall motivation is to gain entry into a new class of fusion materials science wherein the combined effects of fusion-relevant heat, particle, and neutron fluxes can be studied for the first time anywhere.
FES will explore development of a new research platform that can study how material samples are impacted by neutron irradiation with high rates of atomic displacements and an energy spectrum similar to that of a fusion energy system
Understand the science of evolving materials at reactor-relevant plasma conditions and how novel materials and manufacturing methods enable improved plasma performance (Maingi-Zinkle workshop)
Plasma-material interaction (PMI) and high heat flux (HHF) research for plasma-facing components during long pulse operation; (FESAC Strat Plan)
Materials science research to understand and mitigate property degradation phenomena associated with intense D-T fusion neutron-irradiation and to design new high- performance materials to enable practical fusion energy; (FESAC Strat Plan)

20. LANL’s materials strategy emphasizes performance prediction and controlled functionality in key areas of leadership
Goals
Performance Prediction and Controlled Functionality
Themes
Defects & Interfaces
Extreme Environments
Emergent Phenomena
Areas of Leadership
Materials
Dynamics
Energetic Materials
Integrated Nano-materials
Complex Functional Materials
Actinides & Correlated Electron Materials
Materials in Harsh Env.
Mfg. Science
Cross Cuts
Making
Measuring
Modeling

21. In situ, dynamic measurements
Materials research is on the brink of a new era – from observation of performance to control of properties
The confluence of unprecedented experimental capabilities (e.g. 4th generation light sources, controlled synthesis and characterization, …) and simulation advances are providing remarkable insights at length and time scales previously inaccessible
New capabilities will be needed to realize this vision:
In situ, dynamic measurements
simultaneous scattering & imaging
of well-controlled and characterized materials
advanced synthesis and characterization
in extreme environments
dynamic loading, irradiation
coupled with predictive modeling and simulation
materials design & discovery
MaRIE will provide a transformational facility for NNSA: simultaneous, multi-probe measurements of in situ transient phenomena in relevant dynamic extremes to understand the behavior of interfaces, defects, and microstructure

22. Petascale simulations are revealing key mechanisms at the nano-/molecular scale
Accurate description of catalytic processes requires modeling intricate reaction networks using realistic models
Competing dislocations, twinning and/or phases determine dynamic response of materials
Impact example: these are ‘billion atom –class simulations’
-stress corrosion cracking – a key degradation mechanism and the inverse of reactive catalytic surfaces; preventing or controlling this could lead to several % impacts on $B industries
>>I will say that petascale simulations clearly demonstrate that getting
>>the electrons right matters. You can't get solvation (bulk or
>>interfacial) and reactivity correct without explicit treatment of
>>electrons, and you can't get relaibale, accurate treatment of
>>electrons in molecular systems without petascale. Also, petascale computing puts us at
>>the threshold of "catalysis by design" (see attached slide).
>> 
>>Exascale will allow us to treat mesoscale systems, coupling transport
>>and reactivity, and to accurately simulate directed self-assembly of
>>mesoscale systems because, based on petascale, we know how to
>>accurately treat electrons at interfaces and in solutions.
Direct non-equilibrium molecular dynamics simulation can match time and length scales of APS & LCLS experiments
Ab initio molecular dynamics simulations for accurate free energy estimate of thermal and electro processes in complex environments
Petascale computation enabled first simulations at scale of relevant unit processes controlling materials structure and function

23. Exascale will provide needed resolution and fidelity for realistic mesoscale systems & coupled interactions
Discovery and exploitation of collective, multi-scale phenomena that emerge from complex assemblies of molecular and nanoscale building blocks
Here we will focus on a different problem in the same general area, but one that require exascale computing power
Again, the problem must be DOE-relevant
We need to specifically explain why we need exascale simulation.
What does the extra 1000X computing power allow us to do that we canNOT do at the petascale
Do not give the ensemble answer here (although that could be part of the UQ story later)
It is important that we give enough evidence of analysis that the audience will believe that we really need exascale
And the problem has to be compelling enough that we want to solve it
We should be able to say that “At exascale, we will be able to show X and that is important because of Y.”
We also need to tie this to our theme of UQ and predictivity
What physical phenomena will we be able to predict with higher (and quantified) confidence because of exascale?
As in the previous slide, ideally, we will have a science result and an application
We also should make the “urgency” argument in terms of the “first to benefit” approach
Ensembles of high-throughput microstructures by design with in situ, ab initio force constants
Accurate description of transport and reactivity in catalytic processes with interfaces by design
Exascale computation will enable understanding, design and predictive synthesis of materials at the mesoscale, with bounded uncertainty

24. MaRIE with LANL’s integrated co-design approach will couple multi-scale theory and multi-probe experiment on next-generation computing architectures for future integrated codes
Variable-resolution models are synergistic with multi-probe, in-situ, transient measurements
Mesoscale materials phenomena
need extreme-scale computing

25. Additively Manufactured 316L Stainless Steel
MaRIE will provide critical data to inform and validate advanced modeling and simulation to accelerate qualification of advanced manufacturing – move from “process-” to “product-based”
Damage under shock loading unable to coalesce leading to a tougher, more shock resistant material
Additively Manufactured 316L Stainless Steel
microns
X-ray
Laser
pRad beam
Prototype Gas Bottle
Need clearer labels, and explanations in notes of what these are.
Changed “additive” to “advanced” in title now that Cook is gone.
Trying to have phrases match the most recent MNS.
In the future stockpile, we may be changing to components with different principles of operation[1], or have components that are expected to be reliable in a wider range of Stockpile-to-Target-Sequence conditions[2], that will be beyond the nuclear test experience.  It will be essential to have an experimental capability that can discover if physical mechanisms, different than previously assumed and not presently captured in design codes, are important to model and to provide validation in that new domain of operation.
[1] Classified examples could be provided.
[2] Consider increased emphasis on safety during production or on hostile environments.
From left to right on bottom:
1. TRUCHAS ASC code modified for directed energy additive manufacturing (J. Gibbs, A. Clarke, N. Carlson) It is a model of a metal wire being heated for deposition in such an AM application.
2. Multiscale dendritic needle network (DNN) model (D. Tourret and A. Clarke) Calculations of freezing from melt in casting.
3. Polycrystalline plasticity model (C. Bronkhorst, V. Livescu) The model is 3D, you are seeing a 2D slice so the tetrahedral zones look triangular.  Stress along the three principle axes of the polycrystal is determined in another code and applied at boundary of this calculation cube.  The various phases and orientations of the polycrystals then affect the transmitted stress.
4. You are seeing a bi-crystal, left and right of a hockey-puck cylinder, same material different orientation of the crystal.  Stress is applied at the boundary but results in very different internal von Mises stresses (in GPa) in the two-different crystals (C. Bronkhorst and D.J. Luscher)
Microstructure Modeling
Performance Modeling
Process Modeling
Properties Modeling
MaRIE and Exascale will enable rapid and confident deployment of new concepts and components through more cost-effective and more rigorous science-based approaches.

26. Summary
Mesoscale science is a scientific frontier, where quantum meets that continuum, that will only yield to integrated, multi-disciplinary efforts.
For Los Alamos (and FES?), this is not only a good idea but also a mission imperative.
Computing at the exascale will enable progress, if we emphasize co-design.
Experiment-Simulation Integration
Data Science, Machine Learning, Scientific Computing