hard x-ray pcs and coherent diffraction at the aps: recent results future directions · 2010. 3....
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Hard X-Ray PCS and Coherent Diffraction at the APS:
Alec Sandy
X-Ray Science Division Argonne National Laboratory
Recent Results &
Future Directions
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Outline
Hard x-ray coherent scattering in the USA (APS)
Beamline 8-ID at the APS – Small angle XPCS – Large angle XPCS
Future Prospects
Conclusions
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Coherent Scattering at the APS Today
Requirement for 3rd (or 4th) generation source means that all such efforts in the USA are currently hosted at the APS
2 major types of programs 1 Coherent x-ray diffraction (imaging) (CXD and CXDI)
• Lensless imaging of thick or buried structures with resolution limited by scattered intensity at large angles
• CXD and CXDI work is distributed across several beamlines—not by design
2 X-ray photon correlation spectroscopy (XPCS) • Probe of nanoscale fluctuations in condensed matter • Mostly dedicated effort at a single beamline at the APS
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Coherent Scattering at the APS Today CXD and CXDI occurs at several beamlines:
– Strain and defects in nanocrystals, nanowires 34-ID-C (50% access) I. Robinson, S. Leake (U. College London) hard x-ray, Bragg R. Harder (ANL) O. Shpyrko, A. Tripathi (UCSD)
– Subcellular organelles, mineral nanostructure 2-ID-B (25% access) B. Abbey, K. Nugent, G. Williams (U. Melbourne) 1-4 keV, small-angle J. Clark, A. Peele, M. Pfeifer (La Trobe U.) H. Jiang, J. Miao, F. Tamanoi (UCLA) C. Song (RIKEN/SPring-8), S. Risbud (UC Davis) L. Graham, M. Glimcher (Children's Hospital Boston)
– Nanostructure of complex materials 26-ID-C (just begun) Isaacs, Nugent, Robinson, and Shpyrko teams hard x-ray, Bragg
– Dealloyed nanofoams, dislocations and strain 8-ID-E/I (0–15% access) K. Chen, D. Dunand (Northwestern U.) hard x-ray, small-angle E. Isaacs (ANL)
M.A. Pfeifer, G.J. Williams, I.A. Vartanyants, R. Harder, I.K. Robinson, Nature 442, 63 (2006)
GaAs nanowire R. Harder
(ANL)
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Coherent Scattering at APS Today
XPCS – Glasses, jamming, aging, polymers, filled polymers, surfaces 8-ID-I (50%)
B. Leheny (JHU) small-angle L. Lurio (NIU) S. Mochrie (Yale) S. Sinha (UCSD) M. Sutton (McGill) …
– CDW’s, martensitic transformations, surface diffraction 8-ID-E (20%) J. Logan and E. Isaacs (U. Chicago and ANL) large-angle K. Ludwig (BU) and M. Sutton (McGill) M. Pierce and H. You (ANL) O. Shpyrko (UCSD) J. Su (ANL)
Near-field speckle (NFS) and ultra-small-angle XPCS (USA XPCS) 8-ID-I (5%) – Technique development, novel form factors, glassy dynamics
S. Mochrie (Yale) ultra-small-angle
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Small Angle XPCS at 8-ID: Dynamics in Glasses
Motivation – Understanding the glass transition
remains a “grand challenge” in condensed matter physics • Are there distinct glassy
phases? • What is the nature of dynamics
in the glassy state?
Even idealized systems are predicted to display complex phase and dynamic behavior:
F. Sciortino, Nature Materials 1, 145 (2002)
Repulsive glass may be melted by switching on a weak attractive interaction Melted glass may be re-vitrified upon further increase in the attraction Density fluctuations decay logarithmically versus time, in the liquid where
attractive and repulsive arrest mechanisms compete
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Small Angle XPCS at 8-ID: Dynamics in Glasses
Glassy dyamics determined via XPCS
Melted phase—liquid-like correlation decays
Repulsive glass
Revitrification—Attractive glass
Melted phase—logarithmic correlation decays
Xinhui Lu, S.G.J. Mochrie, S. Narayanan, A.R. Sandy, M. Sprung, PRL 100, 045701 (2008)
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Small Angle XPCS at 8-ID: Viscous Surface Dynamics
Motivation – Investigate how or if properties of polymer films vary
under confinement (thin films) or at a free surface • Free surface dynamics • Free surface dynamics as h Rg • Free surface dynamics T glass transition
temperature
Ongoing multiyear project • Zhang Jiang and Sunny Sinha (UCSD)
(Ph.D. Thesis 2007) • Hyunjung Kim, Sogang University • Mrinmay Mukhopadhyay and Larry Lurio (NIU) • Suresh Narayanan (ANL)
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Small Angle XPCS at 8-ID: Viscous Surface Dynamics
Overdamped capillary waves investigated on relatively thick entangled PS films on Si at elevated temperatures
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PS Film
H. Kim et al., PRL 90, 68302 (2003)
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Small Angle XPCS at 8-ID: Viscous Surface Dynamics
Previous investigations extended to – Films at temperatures approaching the glass transition
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Z. Jiang, M.K. Mukhopadhyay, S. Song, S. Narayanan, L.B. Lurio, H. Kim, S.K. Sinha, to be published
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Large Angle XPCS at 8-ID-E
Set-up(s) not nearly so polished as small-angle XPCS
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Large Angle XPCS at 8-ID: Cr SDW/CDW’s
Fluctuating charge domains, corresponding to fluctuating spin density domains, in Cr studied as a function of temperature
Transition from higher temperature thermally-activated fluctuations to lower-temperature quantum fluctuations
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λ 2
1
1
1
2 23
3
O.G. Shpyrko, E.D. Isaacs, J.M. Logan, Yejun Feng, G. Aeppli, R. Jaramillo, H.C. Kim, T.F. Rosenbaum, P. Zschack, M. Sprung, S. Narayanan, A.R. Sandy, Nature 447, 68-71 (2007)
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Large Angle XPCS at 8-ID: Martensitic Transformations
Heterogeneous dynamics in the martensic transformation of Co [C. Sanborn, K. Ludwig (BU) and M. Sutton (McGill)]
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C.-S. Yoo et al. J. Phys. Cond. Matt. 10 L311 (1998).
P (GPa)
T (K
)
ε (hcp) - Co
γ (fcc)
Blaschko et al., PRL 60, 2800 (1988).
Cobalt: fcc → hcp martensitic phase transition Change in stacking sequence: …ABCABC… → …ABABAB… via avalanches
Pixel P
ixel
(013) speckle pattern
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Large Angle XPCS at 8-ID: Martensitic Transformations
Quench from 610 450 °C and observe structural avalanches
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t1 (min)
t 2 (m
in)
Two-Time Correlation Function <I(t1)I(t2)> from the Co martensitic transformation shows avalanches
of structural change.
Fluerasu et al., PRL 94, 055501 (2005)
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XPCS at 8-ID: Summary
Work presented points to expanded future needs: – Time scales probed continuously from
≈ 10 ms >1,000 s • Considerably more coherent flux required – Dynamics with multiple decays,
intermittent dynamics
• Fast small-pixel area detectors [P. Falus and S.G.J. Mochrie (Yale)] – Faster and more reliable required
• On-the-fly compression – Increased robustness and real-time data
reduction required • Robust diffractometer with multiple sample
environments LBNL-ANL Fast CCD Project
Courtesy B. Leheny, JHU
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Future Prospects
Currently the only hard x-ray coherent-scattering beamlines in the USA are at the APS
In the near future, there will be several new and improved facilities • LCLS • NSLS-II • Upgraded APS?
How should coherent scattering work done at these new facilities distinguish and complement each other?
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Future Prospects
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LCLS peak brilliance is another 10 orders of magnitude higher!
Time-averaged brilliance
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Future Prospects
LCLS – Average brilliance 10× greater than that expected from NSLS-II and
1,000× more than the APS today! – Peak brilliance 10 decades beyond these numbers – Time scales
• > 10 ms – LCLS rep rate
• < 1 µs – Delay line XPCS
Coherence-based experiments that take advantage of LCLS peak brilliance and provide access to completely unique time scales are most exciting – Delay-line XPCS
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Future Prospects
NSLS-II – Extraordinary brightness (2 X 1021 ph/s/mm2/mrad2 at ~ 8 keV)
promised (for a 3rd generation source) via • High current (500 mA) • Extremely small emittance (< 1 nm-rad) • Long ID’s
• Coherent hard x-ray (CHX) beamline – – Approved as 1 of 6 facility beamlines – Pros
• Brilliance • Large budget for optimized detector
• ms µs dynamics • Dedicated to small-angle XPCS (and µ-beam SAXS)
– Cons • Lower energy ring • Dedicated to small-angle XPCS (and µ-beam SAXS)
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Future Prospects
NSLS-II – CHX Beamline
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Future Prospects
APS – Many tremendous (coherent scattering) capabilities have been
developed at the APS but these facilities remain significantly under-optimized • Mostly ½-filled “short” straight sections with generic ID’s • Ring current significantly below storage ring design values • Partially dedicated sectors especially for CXD(I) • Lack of optimized detectors
– APS Renewal process has kicked off • (3rd time in 4 years!) • Workshops Monday and Tuesday next week • APS Renewal white paper early 2009 • Full APS Renewal proposal later in 2009 • ???
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Future Prospects
Proposed APS coherent scattering upgrades – CXD and CXDI
• Beamline 34-ID-C (proposed) upgrades – Separation of 34-ID-C (coherent diffraction) from 34-ID-E
(microdiffraction) via canted ID’s and offset monochromator – Markedly improved sample and optics support and positioning
capabilities – Wide dynamic range detectors like Pilatus – Incorporation of hard x-ray CXDI capabilities
• AXI Beamline Letter of Intent – Currently unfunded
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ID-D ID-C
ID-A
200m 70m
II bldg.
200 m beamline for wide-field phase imaging, future CDI hutch
Argonne Imaging Institute Long ID-C hutch for CDI
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Future Prospects
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Proposed APS coherent scattering upgrades – XPCS
• Beamline 8-ID (proposed) upgrades – Long straight section (8 m) with canted shorter-period ID’s to
separate XPCS program from GISAXS – Brilliance-preserving vertical focusing – Higher x-ray-energy XPCS
2X Undulator
8-ID-A FOE
8-ID-D
8-ID-E
8-ID-I
Mono (or pink) beam
0 m
30 m 51 m
65 m
GISAXS, GIWAXS
Small Q and large Q XPCS
Mono beam
8-ID-F
Key White beam Pink beam Mono beam Aperture Mirror Monochromator
8-ID “Tomorrow” via Upgrade
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Conclusions
Coherent beams from LCLS will provide access to totally unprecedented time and length scales
NSLS-II and APS (I hope!) will provide access to – LCLS inaccessible time scales (ms µs) – Hard x-rays (APS) – Extended beam time and more experiments
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Acknowledgements
Beamline 8-ID partner users – Prof. Larry Lurio, Northern Illinois University – Prof. Simon Mochrie, Yale University – Prof. Mark Sutton, McGill University
Graduate Students – Peter Falus, Yale University
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