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LCLS-II-HE “First Experiements ” Meeting AMO, Quantum Materials, Biology Oct 30-31 , 2017

LCLS-II-HE Science Opportunities Overview. LCLS-II-HE “First Experiements ” Meeting AMO, Quantum Materials, Biology Oct 30-31 , 2017. Robert Schoenlein LCLS Deputy for Science. LCLS-II Project – Under Construction 1 st Light - 2020. 10 26. Average Coherent Power. HXU. LCLS-II. 10 25.

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LCLS-II-HE “First Experiements ” Meeting AMO, Quantum Materials, Biology Oct 30-31 , 2017

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  1. LCLS-II-HEScience Opportunities Overview LCLS-II-HE “First Experiements” MeetingAMO, Quantum Materials, BiologyOct 30-31, 2017 Robert Schoenlein LCLS Deputy for Science

  2. LCLS-II Project – Under Construction1st Light - 2020 1026 Average Coherent Power HXU LCLS-II 1025 LCLS SXU x 10,000 1024 LCLS-II 1023 Average Brightness (ph/s/mm2/mrad2/0.1% BW) LCLS-II 4 GeVCW-SCRF 1022 LCLS 1021 LCLS-II CW-SCRF linac (4 GeV) Two new tunable undulators Repetition rate up to 1 MHz Photon energy up to 25 keV (120 Hz) Stability, coherence (seeding) SCRF Cryo-module ~10 msec ~mJ ~fs rings under const. LCLS 1020 Existing Rings EuXFEL (FLASH) ~msec 1019 LCLS-II 102 103 104 Photon Energy (eV)

  3. Proposed LCLS-II-HE Electronic dynamics Atomic-scale structure x 10,000 26 LCLS 10 LCLS-II LCLS-II-HE 25 10 HXU Eu-XFEL SXU 24 10 LCLS-II-HE 23 10 LCLS-II 4 GeVCW-SCRF Average Brightness (ph/s/mm2/mrad2/0.1%BW) DLSR limit 22 10 HXU+Cu-linac (120 Hz) LCLS-II LCLS (120 Hz) 21 LCLS-II-HE CW-SCRF linac (8 GeV) Photon energy up to 20 keV Two tunable undulators Repetition rate up to 1 MHz Stability, coherence (seeding) 10 SCRF Cryo-module ~10 msec ~mJ ~fs DLSR(s) 0.2-1.1 km, 2-6 GeV 6.3 km, 9 GeV LCLS 20 10 EuXFEL (FLASH) ~msec LCLS-II-HE 19 10 2 4 6 8 10 12 14 16 18 20 Photon Energy (keV)

  4. LCLS-II-HE provides new insight to structural dynamics at the atomic scale LCLS-II-HE provides: • Ultrafast coherent X-rays • ~1 Ångstrom (~12 keV) • High repetition rate Structural dynamics at the atomic scale - Atomic and electronic structure - Large momentum (q) transfer Operating environments - X-ray penetration of water ~3 mm @ 12 keV Dynamics excited state non-equilibrium transient structures Fluctuations ground state structure spontaneous evolution 0.12 0.1 Heterogeneity structural complexity ground & excited states Correlated materials strong S-O (5d TM) PX structure via Se phasing 0.08 Earth-abundant3d transition metals Transmission 0.06 1 Å 14.4 keVFe57 (Mossbauer) ~20 keVHigh-resolution IXS >25 keVX-ray scattering, PDF 0.04 0.02 V Cr Mn Fe Co Ni Cu Zn Ir-L3 Se 0 5 6 7 8 9 10 11 12 13 14 15 Photon Energy (keV)

  5. New Experimental Capabilities of LCLS-II-HE (1/3) core-excitedstates X-ray energy hn Q Dynamics near the FT Limit • >300x increase in average spectral flux (ph/s/meV) beyond DLSRs • Spectroscopy & inelastic scattering at high resolution • IXS meV resolution up to 20 keV sub-meV (dispersive spectrometer, ~10 keV) • RIXS ~5 meV (quartz- and sapphire-based analyzers) • Low-energy modes in quasi-elastic energy region • Momentum transfer spanning entire Brillouin zone • Sensitivity (e.g. to electronic vs. lattice modes) • Excited-state dynamics – near-equilibrium perturbations (5 meV 300 fs) • Excited-state potential mapping with element-specificity(e.g. metal-ligand stretch modes) Dt3 Dt2 Dt1

  6. New Experimental Capabilities of LCLS-II-HE (2/3) Fluctuations & Heterogeneity Atomic resolution, Ultrafast time scales, Operating conditions Photon Correlation Spectroscopy (XPCS) “Sequential” real-time mode (fast 2D detectors) “Two-pulse” mode (<100 fs) with pulse pairs directly from XFEL “Programmable” time structure encoded in X-ray pulse sequence High rep rate, lower peak power, sample replacement Time-domain (and FT) Inelastic X-ray Scattering Time-resolved (diffuse) X-ray scatteringfollowing impulsive excitation of collective modes Perturbative regime – ground-state fluctuations(fluctuation-dissipation theorem) Non-equilibrium regime, excited-state dynamics High resolution via Fourier-transform of coherent response(1 THz  4 meV) High-brightness hard X-rays – atomic structure (PDF) Dt3 Dt2 Dt1 pump → Trigo et al.,Nature Physics (2013) X-rays →

  7. New Experimental Capabilities of LCLS-II-HE (3/3) How can we exploit the high rep rate and the potential for 108-1010 snapshots/day to: Characterize heterogeneous ensembles, Capture rare transient events, Map spontaneous dynamics operando • Advanced Experimental Approaches • Coherent diffractive imaging (and/or serial crystallography) with spectroscopy • Solution scattering, rapid mixing… • Fluctuation X-ray scattering • Advanced Computational Approaches and Data Science • Mapping reaction landscapes via diffusion maps, manifold embedding and related Bayesian approaches • Capturing rare events via automatic pattern recognition and related machine-learning approaches CXI of heterogeneous nanoparticles in situ Möller et al., Nature Comm. (2014) Potential energy landscape time ~kT

  8. LCLS-II-HEScience Opportunities Chemical dynamics: Reaction dynamics, charge transfer, molecular photocatalysts, natural & artificial photosynthesis Catalysis: Homogeneous and heterogeneous catalysis, interfacial & geo/environmental chemistry Materials Physics:Heterogeneity, spontaneous fluctuations,nonequilibrium dynamics, extreme environments Quantum Materials: Emergent phenomena & collective excitations Biological Function & Structural Dynamics Dynamics in physiological environments

  9. Revealing the full sequence of electronic/atomic structural dynamics & capturing rare events in multi-electron catalysts valence 3p • Scientific Opportunity • Reveal coupling of valence charge structure and subtle changes in molecular structure • Map entire cycle of multi-electron photo-catalysts • Capture rare transient events (transition states) operando • Significance Impact • Directed design of efficient & robust catalysts from abundant elements (3d TM) • LCLS-II-HE Approach • Time-resolved spectroscopy maps excited state valence structure (XES) and potential surfaces (RIXS) • Time-resolved scattering (and PDF), EXAFS map local geometryat the sub-angstrom scale • 108-1010 snapshots/day captures rare transient events Molecular photocatalytic assemblyK. Kjaer, Lund U. 2p Inorganic water oxidation catalyst H. Frei et al. Nature Chem. (2014) Kb2,5 Kb1,3 Ka Requires tunable ultrafast hard X-rays at high rep rate to map dynamics and to capture rare events of functional complexes 1s

  10. LCLS-II-HEScience Opportunities Chemical dynamics: Reaction dynamics, charge transfer, molecular photocatalysts, natural & artificial photosynthesis Catalysis: Homogeneous and heterogeneous catalysis, interfacial & geo/environmental chemistry Materials Physics:Heterogeneity, spontaneous fluctuations,nonequilibrium dynamics, extreme environments Quantum Materials: Emergent phenomena & collective excitations Biological Function & Structural Dynamics Dynamics in physiological environments Peter Paul Ewald Fellows Symposium Oct. 11-13, 2017

  11. Structural Dynamics, Interfaces, & Electrochemical Energy Storage • Scientific Opportunity • Unravel chemical, structural, & electronic dynamics of the electrical double layer (interface) • Atomic resolution,operando • Significance and Impact • Critical input for electronic structure theory & directed design of advanced batteries, electro-catalysts, solar fuel cells etc. • Contaminant & elemental cycling in enviro-geochemistry • LCLS-II-HE Approach • Dynamic X-ray scattering methods span many decades in time and space, to fs and Å • XPCS characterizes statistically dynamic systems without long-range order, measuring S(q,t) • Time-resolved X-ray scattering (20 keV, large-q)with Pair Distribution Function (PDF) analysis S. Lapiduset al., PCCP (2014) XPCS/CXI H. Ogasawara • Requires hard X-rays at high repetition rate & programmable pulse structure • to capture dynamics of local changes in structure

  12. Coupled electronic & nuclear dynamics are fundamental to heterogeneous catalysis and interfacial chemistry • Scientific Opportunity • Correlate catalytic reactivity & structure nanoparticle-by-nanoparticle • Characterize evolving heterogeneous catalyst in real-time and operando withchemical specificity & atomic resolution • Significance and Impact • Input for theory for directed design & synthesis of efficient, selective and robust systems based on earth-abundant elements • LCLS-II-HE Approach • Coherent scattering and spectroscopy measured simultaneously provides electronic & atomic structure(shape) of each nanoparticle • ~108-1010 independent measurements/day characterizes heterogeneous ensembles PtnSnm/γ-Al2O3 Ab Initio MD & XAS J. Rehret al. J. Phys. Chem. (2013) CXI hn hn e- XPS Requires tunable ultrafast hard X-rays at high repetition rate to sample large ensembles CXI of heterogeneous nanoparticles in situ Möller et al., Nature Comm. (2014)

  13. LCLS-II-HEScience Opportunities Chemical dynamics: Reaction dynamics, charge transfer, molecular photocatalysts, natural & artificial photosynthesis Catalysis: Homogeneous and heterogeneous catalysis, interfacial & geo/environmental chemistry Materials Physics:Heterogeneity, spontaneous fluctuations,nonequilibrium dynamics, extreme environments Quantum Materials: Emergent phenomena & collective excitations Biological Function & Structural Dynamics Dynamics in physiological environments

  14. Imaging of ion diffusion and fluctuating material structures • Scientific Opportunity • Characterize local atomic distortions and long-range strain fields • Resulting from ion diffusion in real materials under operating conditions • Significance and Impact • Inform directed design and synthesis of energy conversion and storage materials • LCLS-II-HE Approach • Dynamic X-ray scattering methods span many decades in time and space,down to fs and Å • XPCS characterizes statistically dynamic systemswithout long-range order, measuring S(q,t) discharge ion 3d metal-oxide electrode ion 100 fs ~1 Å/vsound M. Toney 5 µm t3 t2 LiCoO2 Co t1 Understanding ion diffusion at atomic level is central to performance improvements in electro-chemical energy storage materials Requires hard X-rays at high repetition rate & programmable pulse structure to capture dynamics of local changes in structure delay Dt

  15. LCLS-II-HEScience Opportunities Chemical dynamics: Reaction dynamics, charge transfer, molecular photocatalysts, natural & artificial photosynthesis Catalysis: Homogeneous and heterogeneous catalysis, interfacial & geo/environmental chemistry Materials Physics:Heterogeneity, spontaneous fluctuations,nonequilibrium dynamics, extreme environments Quantum Materials: Emergent phenomena & collective excitations Biological Function & Structural Dynamics Dynamics in physiological environments

  16. The uniquely high spectral brightness opens a long-sought window into emergent phenomena in complex materials • Scientific Opportunity • Characterize collective modes in materials • Correlated materials - multiple strong interactionscharge, spin, orbital, lattice • Resonant: RIXS, non-resonant: IXS • New insight from >300x ph/s/meV • Significance and Impact • Fundamental material description: S(q,w)~c(q, w) • Limited resolution and precision to date • Direct link to theory predictions for collective modes • LCLS-II-HE Approach • Collective modes at ~1 meVscale and beyond • Continuum charge modes, e-ph coupling • Span entire Brillouin zone: k-dependent coupling • Complex materials, high-Z elements, weak signals lattice elastic peak charge spin orbital Average spectral brightness of LCLS-II-HE will be ~1000x beyond existing X-ray sources

  17. The uniquely high spectral brightness opens a long-sought window into emergent phenomena in complex materials • Scientific Opportunity • Characterize collective modes in materials • Correlated materials - multiple strong interactionscharge, spin, orbital, lattice • Resonant: RIXS, non-resonant: IXS • New insight from >300x ph/s/meV • Significance and Impact • Fundamental material description: S(q,w)~c(q, w) • Limited resolution and precision to date • Direct link to theory predictions for collective modes • LCLS-II-HE Approach • Collective modes at ~1 meVscale and beyond • Continuum charge modes, e-ph coupling • Span entire Brillouin zone: k-dependent coupling • Complex materials, high-Z elements, weak signals Sr2IrO4 DE=130 meV DE=30 meV Kim et al. PRL (2012) Kim et al. Nature Com. (2014) Average spectral brightness of LCLS-II-HE will be ~1000x beyond existing X-ray sources

  18. The uniquely high spectral brightness opens a long-sought window into emergent phenomena in complex materials • Scientific Opportunity • Characterize collective modes in materials • Correlated materials - multiple strong interactionscharge, spin, orbital, lattice • Resonant: RIXS, non-resonant: IXS • New insight from >300x ph/s/meV • Significance and Impact • Fundamental material description: S(q,w)~c(q, w) • Limited resolution and precision to date • Direct link to theory predictions for collective modes • LCLS-II-HE Approach • Collective modes at ~1 meVscale and beyond • Continuum charge modes, e-ph coupling • Span entire Brillouin zone: k-dependent coupling • Complex materials, high-Z elements, weak signals • Dynamic response to tailored excitations Order Parameter of Pseudo-gap Phase? THz-Driven Superconductivity Enhanced Tc ? Magnetoelectricquadrupole via magnon- phonon coupling 20 THz modulationofOxygen out-of-plane mode in YBCO U. Staub Average spectral brightness of LCLS-II-HE will be ~1000x beyond existing X-ray sources cuprate superconductor A. Cavalleri

  19. LCLS-II-HEScience Opportunities Chemical dynamics: Reaction dynamics, charge transfer, molecular photocatalysts, natural & artificial photosynthesis Catalysis: Homogeneous and heterogeneous catalysis, interfacial & geo/environmental chemistry Materials Physics:Heterogeneity, spontaneous fluctuations,nonequilibrium dynamics, extreme environments Quantum Materials: Emergent phenomena & collective excitations Biological Function & Structural Dynamics Dynamics in physiological environments

  20. Imaging Biological Function - Biology in Action • Scientific Opportunity • Reveal structural dynamics of bio-molecules & molecular machines on fundamental scales • Near physiological conditions – room temperature • Significance and Impact • Dynamics (e.g. low-energy collective motions) are key missing link between biological structure & function • Beyond “model” complexes with large photolysis to biologically relevant processes • LCLS-II-HE Approach • Serial nano-crystallography complete time sequences at atomic scale • Larger-scale conformational changes:Solution scattering (SAXS, fluctuation SAXS) Photo-triggered Dynamics CO-myoglobin ligand dissociation dynamics I. Schlichting et al., Science(2015) Trans to cis isomerization in PYP M. Schmidt et al., Science (2016) Phytochrome– light sensing kinasecontrols cellular function in bacteria & plants Understanding heterogeneous ensembles & dynamics under physiological conditions requires hard X-rays at high repetition rate

  21. Imaging Biological Function - Biology in Action AChEenzyme – synaptic transmission • Scientific Opportunity • Reveal structural dynamics of bio-molecules & molecular machines on fundamental scales • Near physiological conditions – room temperature, solution • Significance and Impact • Dynamics (e.g. low-energy collective motions) are the key missing link between biological structure & function • Beyond “model” complexes with large photolysis to biologically relevant processes • LCLS-II-HE Approach • Solution scattering (SAXS, fluctuation SAXS)complete time sequences of structural dynamics • Rapid mixing (~10 msec, <1 mm crystals, room temp.) • Activated substrates (small molecules, <10 msec) • Optogenetic & biological photo-actuators - trigger • 108-1010 snapshots/spectra per day  rare transient events reaction turnover ~50,000/sec (20 msec) active site Understanding heterogeneous ensembles & dynamics under physiological conditions requires hard X-rays at high repetition rate Conformational (PE) landscape ~kT

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