Quanta to the Continuum: Opportunities for Mesoscale Science

1. Quanta to the Continuum: Opportunities for Mesoscale Science John Sarrao George Crabtree BESAC, July 2012 meso2012.com

2. The BESAC Charge on Mesoscale Science • Excerpts from Dr. Brinkman’s charge letter of February 14, 2011: • A central theme of these reports is the importance of atomic and molecular scale understanding of how nature works and how this relates to advancing the frontiers of science and innovation. I would now like BESAC to extend this work by addressing the research agenda for mesoscale science, the regime where classical, microscale science and nanoscale science meet. I see two parts to this new study: • 1. Identify mesoscale science directions that are most promising for advancing the Department’s energy mission. • 2. Identify how current and future BES facilities can impact mesoscale science. • This study could prompt a national discussion of mesoscale science at the level heard during the initial formulation of the National Nanotechnology Initiative a decade ago. Report due early Fall 2012

3. The BESAC Meso Subcommittee John Hemminger, Irvine, BESAC chair William Barletta, MIT, BESAC Gordon Brown, Stanford, BESAC Roger French, CWRU, BESAC Laura Greene, UIUC, BESAC Bruce Kay, PNNL, BESAC Mark Ratner, Northwestern, BESAC John Spence, Arizona, BESAC Doug Tobias, Irvine, BESAC John Tranquada, Brookhaven, BESAC John Sarrao, LANL, co-chair George Crabtree, ANL & UIC, BESAC, co-chair Paul Alivisatos, LBNL Frank Bates, Minnesota Marc Kastner, MIT Jennifer Lewis, UIUC Tony Rollett, CMU Gary Rubloff, Maryland

4. Plan for this Meeting Now: Articulate the message that is embodied in the report Later this afternoon: Discuss report in detail and gather your feedback* *we acknowledge some gaps exist now in the report Tomorrow morning: React to your input and propose a path forward Goal: Achieve BESAC approval of report, assuming successful completion of the proposed plan

5. Venues for Community Input: Town Halls and Website APS Boston Wed Feb 29 Marc Kastner and William Barletta (MIT), hosts ACS San Diego Tues Mar 27 John Hemminger, Douglas Tobias (UCI), hosts MRS San Francisco Mon Apr 9 Cynthia Friend, Gordon Brown (Stanford/SLAC) Don DePaolo, Paul Alivisatos (Berkeley/LBNL), hosts ACS Webinar Thu April 12 John Hemminger, Douglas Tobias (UCI), hosts Chicago Mon May 14 George Crabtree (ANL & UIC), host Website Meso2012.com

6. Of the ~ 1000 people that participated in town halls, webinars, and other outreach activities, more than 100 submitted quad charts to meso2012.com Meso-photonics for energy applications Approach Opportunity Meso-scales are exactly compatible with the natural length-scale of the light that is relevant for energy applications: visible and infra-red wavelengths. Tailoring the meso-structure, one can tailor the laws of physics (as far as light is concerned) almost at will. Exploring plasmonics, one can “shrink” length-scales of light to even smaller scales, closer to natural length-scales of electronics, thus bridging the gap in the scales between electronics and photonics. Electro-magnetic phenomena can be modeled exactly, with no approximations apart from the discretization  “numerical experiments” are thus enabled, dramatically speeding-up the scientific progress. Numerous large-scale, cheap meso-fabrication techniques have emerged recently, including: nano-imprint, interference lithography, self-assembly. Impact Meso Challenge 92% of all primary energy sources are converted into electrical and mechanical energy via thermalprocesses  ability to tailor thermal radiation and/or absorption has numerous applications in the energy sector. Solar energy is perhaps the most promising clean-energy source: at the heart of its exploration lies the need to control the behavior of light  meso-photonics promises a wide range of applications: more efficient photo-voltaics, solar-pumped lasers, solar-thermal systems… ~25% of US electricity consumption is due to lighting: meso-photonics could enable dramaticaly more efficient lighting, in terms of: better LEDs, incadescent sources... To enable massive adoption in the energy sector, one needs to have the ability to control meso-structure in macro-scopic objects: novel cheap and reliable mass-fabrication methods are needed. Novel gain materials are needed, compatible with meso-fabrication methods. Plasmonic losses are large: novel plasmonic materials/approaches are needed. We create the laws of physics  large opportunities to explore novel physics emerge: imagination is the limit.

7. Meso: Background • Why: the need for innovation, as articulated in Science for Energy Technology • Why now: the insights and tools we’ve gained (and are still gaining) from nanoscience, as articulated in New Science for a Secure and Sustainable Energy Future • What: build on basic science challenges, as articulated in Directing Matter and Energy: Five Challenges for Science and the Imagination • 7

8. Meso: Beyond atomic, molecular, and nano meso classical quantum isolated interacting collective simple perfect homogeneous complex imperfect heterogeneous

9. Meso integrates structure, dynamics, and function O2 H2O H+ atomic bulk H2O Sequential catalyzed reactions H2 Groundwater dynamics Carbon sequestration Shale oil and gas Mesoscale assembly Solar water splitting 9

10. Meso is an Opportunity Space • Multiple degrees of freedom interact constructively • Complexity enables new phenomena and functionality • Consilience of systems and architectures • Biological complexity with inorganic materials • Multiple spatial, temporal and energy scales meet • Quantum meets classical • Functional defects and heterogeneous interfaces • Multi-scale dynamics essential for functionality • At the meso scale, new organizing principles are needed • Meso embraces emergent as well as reductionist science • What laws unify top-down and bottom-up assembly?

11. Meso exploits interacting degrees of freedom: Light & Matter 5 µ 1 µ 50 nm 1µ 1µ Metamaterials Photonic crystals • Mesoscale structure • Controls light: • direction, frequency, phase, coherence and intensity • Impacting energy technologies: • Solar electric, solar fuel, light emitting diodes, chemical energy conversion Surface plasmons A broad new horizon as rich as the laser revolution

12. Defects and interfaces are functional at the mesoscale Catalytic reactive surface Superconducting pinning landscape Decorated functional mesopores

13. The hierarchy of architectures, phenomena and functionalities 21st century Constructionist science bottom up nano to meso New architectures, phenomena, functionality and technology 20th century Reductionist science top down to nano/atomic/molecular zero resistivity finite resistivity fracture cracks fossil fuels locomotion photosynthesis Cooper pairs cells chemistry, life vortices mean free path defect aggregation work hardening sedimentary rocks electron-phonon resistivity structural defects superconductors colloids membranes plastics magnetics domains, hysteresis mechanics phonons Electronics insulators - metals solutions polymers Molecules energy transduction Lattices 1D - 3D atoms

14. Six priority research directions (PRDs) for mesoscale science have emerged from our study • Mastering Defect Mesostructure and its Evolution • Regulating Coupled Reactions and Pathway-Dependent Chemical Processes • Optimizing Transport and Response Properties by Design and Control of Mesoscale Structure • Elucidating Non-equilibrium and Many-Body Physics of Electrons • Harnessing Fluctuations, Dynamics and Degradation for Control of MetastableMesoscale Systems • Directing Assembly of Hierarchical Functional Materials 14

15. Mastering Defect Mesostructure and its Evolution Crack Propagation Deformation 3D Coherent Imaging Crack Initiation Failure x-ray tomography New probes enable imaging of damage initiation and evolution at the mesoscale 15

16. Regulating Coupled Reactions and Pathway-Dependent Chemical Processes electrons Aqueous solution surface solid-electrolyte-interface solid-electrolyte-interface anode electrolyte cathode Li+ ions Li ion battery Interfaces control reactivity in the natural and synthetic worlds CO2 sequestration

17. Optimizing Transport and Response Properties by Design and Control of Mesoscale Structure Phenomena Ionization Ion insertion/extraction Electronic / ionic conduction Volume expansion/contraction Meso Functionality Energy storage Energy delivery Reversibility on demand Degrees of freedom Electronic Ionic Chemical Mechanical

18. Elucidating Non-equilibrium and Many-Body Physics of Electrons Making “contact” with many-body electron states… ~1µ reveals dynamic localization and intrinsic inhomogeneity …to be controlled for electronic functionality 18

19. Harnessing Fluctuations, Dynamics and Degradation for Control of MetastableMesoscale Systems Metastability at the mesoscale control of fluctuation spectra impacts lifetime and aging The opportunity is to emulate nature: smart and self-healing materials for advanced energy technologies 19

20. Directing Assembly of Hierarchical Functional Materials Elements of Assembly compositional structural functional unit connecting functional units architectural connecting sequential steps temporal many interacting degrees of freedom Integration of disparate materials classes by “top down” and “bottom up” approaches is the underpinning focus of directed mesoscale assembly

21. Realizing the meso opportunity requires advances in our ability to observe, characterize, simulate and ultimately control matter. Characterization Synthesis Mesoscale Physics, Materials and Chemistry Theory Simulation Mastering mesoscale materials and phenomena requires the seamless integration of theory, modeling and simulation with synthesis & characterization

22. Opportunities for Mesoscale Tools and Instruments 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 Synthesis / Assembly • Directed synthesis of complex inorganic materials • Multi-step, multi-component assembly processes • Computational synthesis / assembly 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 22

23. Creating the materials, structures, and architectures that access the benefits of mesoscale phenomena is a key challenge Directed synthesis to create complex materials and controlled interfaces Assembly processes and pattering strategies Computational tools for functionality by design In situ observation and control of synthesis processes

24. Exciting new sources (e.g., LCLS, NSLS-II, SNS) are available, but need to advance optics, detectors, environments, and data handling New methods to watch multi-d defect evolution & tracking In situ, in operando measurements Long duration measurements Simultaneous diffraction, Imaging and spectroscopy x-ray tomography Time-correlated probes of local structure, composition, excitation Data mining strategies Notional 3d, in situ, multi-modal measurement 3D Coherent Imaging

25. Theory and simulation need to connect models across scales AND incorporate emergent phenomena to realize functionality by design Well-documented and curated community codes is a key gap years days sec macro ms time scale µs meso Mori-Tanaka, Halpin-Tsai, Lattice Spring, Finite Element atomic molecular nano ns ps Lattice Boltzmann TDGL, DDFT, fs DFT MD, MC,DMFT mm µm m nm Computational materials challenges includes experimental validation length scale 25

26. We lack the needed workforce to fully tap the meso opportunity • New modalities of research necessitate a new generation of mesoscale scientists • Frontier is interdisciplinary, requiring researchers who move across boundaries and interfaces • Need for integrated teams to address large, complex challenges • Foster and grow science of mesoscale synthesis • Complex, multi-modal measurements  enhanced partnering with instrument scientists and large scale facility • Seamless integration of theory and simulation with synthesis and characterization AND translation to common codes • Future mesoscale scientists will fuel broader manufacturing and innovation workforce

27. Perspective • Meso is an opportunity space: • mesoscale phenomena, architectures, and interfaces • New capabilities are needed to discover principles and enable solutions: • directed assembly, in situ dynamics, and multi-modal function • Success will be transformational: • The ability to manufacture at the mesoscale … to yield faster, cheaper, higher performing, and longer lasting products. • The realization of biologically inspired complexity and functionality … to transform energy conversion, transmission, and storage. • The transformation from top-down design … to bottom-up design … producing next-generation technological innovation. • “It is both the magnitude of the challenge in bridging quanta to the continuum and the potential dividend in controlling the mesoscale that have energized the research community and motivated this report.” • Meso2012.com 27