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SESAME workshop 1 New Scientific Opportunities with soft x-ray SR New New Scientific Scientific Opportunities Opportunities with soft x with soft x - - ray SR ray SR Zahid Hussain Scientific Support Group, Leader Scientific Support Group, Leader Advanced Light Source Advanced Light Source Lawrence Berkeley National Laboratory Lawrence Berkeley National Laboratory

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Page 1: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 1

New Scientific Opportunities with soft x-ray SR

New New ScientificScientific Opportunities Opportunities with soft xwith soft x--ray SRray SR

Zahid HussainScientific Support Group, LeaderScientific Support Group, Leader

Advanced Light SourceAdvanced Light SourceLawrence Berkeley National LaboratoryLawrence Berkeley National Laboratory

Page 2: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 2

THE ADVANCED LIGHT SOURCE

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SESAME workshop 3

The mission of the ALS is to

Support Users in doing Outstanding Science

(From 2002 BES review of the ALS)

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SESAME workshop 4

WHAT DOESWHAT DOES SRSR BRIGHTNESSBRIGHTNESS BUY YOU?BUY YOU?

Very High EnergyResolution

SubmicronSpatialResolution Coherence

20 µm

Magnetic structure of LaFeO3 layer on surface oxide.

Page 5: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 5

UNDERSTANDING PRPERTIES OF MATTER

optical, thermal, and structural properties of matter depend on the behavior of electrons.

Ultimately, theelectronic,

magnetic,chemical,

mechanical,

50 µm

288.5 eV

3 µm

Page 6: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 6

What are some of the important areas of science where soft x-ray SR could make big impact ?Where do we stand now ?How could we get there ?

Big ScienceBig Science (large facilities,~5-10 yrs effort$10’sM)

vs.Small ScienceSmall Science (modest experimental effort, big

payoff)

“Science is in the sampleScience is in the sample”, Daniel Chemla, ALS

New Scientific OpportunitiesNew Scientific OpportunitiesNew Scientific Opportunities

Page 7: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 7

New Scientific Opportunities, SummaryNew Scientific Opportunities, New Scientific Opportunities, SummarySummary

Ambient Pressure Photoemission (in situ measurements, catalysis/corrosion, environmental science, biological systems)

Ultra-high Momentum and Energy Resolution ARPES (Scienta electron energy analyzers, strongly correlated electron systems (high temperature superconductors, CMR)

Coherent Scattering (magnetic imaging, dynamics)

Momentum-Resolved Inelastic Scattering (optically forbidden transition, bulk sensitivity)

Spectromicroscopy (SMART/PEEMIII, X-Ray Imaging, STXM)

Ion Spectroscopy (study of positive and negative ions by measurements of ion fragmentation and/or electron spectroscopy)

Time-resolved spectroscopy (f-sec research)

Page 8: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 8

X Rays Are An Important Probe of Matter

Page 9: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 9

X-ray Spectroscopy of Condensed Matter

Quantum Number Selectivity:

Absorption

Angle-integrated photoemission

Angle-resolved photoemission

Spin-polarized photoemission

ω ε2 ⇒ ∆Ε=Εƒ−Ει

(Ν↑ − Ν↓) / (Ν↑ + Ν↓) ⇒ Εƒ,Ει,κ, σ .

Ν(Ε,hω) ⇒ Εƒ,Ει.

Ν(Ε,hω,θ, ϕ) ⇒ Εƒ,Ει,κ.

Page 10: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 10

Photoelectron Spectroscopy

Page 11: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 11

Photoelectron Spectroscopy

Page 12: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 12

Chemical Shift

Page 13: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 13

Chemical Shift

Page 14: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 14

Ambient pressure (in-situ) soft x-ray spectroscopy

Ambient pressure (in-situ) soft x-ray spectroscopy

•Ambient Pressure Photoemission:Pressure ~ (up to 17 torr,vapour Pressure of H2O

@RT)30 years of surface science knowledge for understanding of electronic structure of surfaces/interfaces in UHV (model systems) - Now it is possible to apply under real

conditions ….

•Absorption/emission spectroscopy(photon in/photon out): study of unoccupied and occupied valence bands

Pressure ~ (up to 1-20 atmospheric pressure theoretical analysis a must, (example)Totally new science !!

Page 15: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 15

Ambient pressure soft x-ray spectroscopy: Concept

e-differentially pumpedelectron transport

synchrotron beam enters through window

controlledgas atmosphere

Photoelectrons from sample surface AND

near-surface gas

Page 16: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 16

Ambient pressure soft x-ray spectroscopy: Basic Concept

P1 P2

P3

Electrostatic Lensescross-over at pumping apertures

Page 17: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 17

• Several groups have used differentially-pumped XPS—K. Siegbahn, H. Siegbahn et al.

• Gas phase photoemission• Surfaces of low vapor-pressure liquidsH. Siegbahn, K. Siegbahn, J. Elec. Spectrosc. Rel. Phen. 2 (1973) 319

—Modified XPS sample holder• Moveable differentially-pumped sample cellR. W. Joyner, M. W. Roberts, K. Yates, Surf. Sci. 87 (1979) 501

—M. Grunze et al.• Surface reactions and catalysisH.J. Ruppender, M. Grunze, C.W. Kong, M. Wilmers, Surf. Interface Anal. 15

(1990) 245

• What’s new?— Differentially-pumped electron optics for higher signals— Synchrotron light-source allows smaller apertures— Pressure range extended 1-2 orders of magnitude

Ambient pressure soft x-ray spectroscopy: History

Page 18: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 18

Prototype Ambient Pressure Photo-Emission System

Modify conventional surface science vacuum

system

HP-PES Differentially Pumped Optics

Page 19: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 19

Ambient Pressure Photoemission: Schematic

Analyzer lens, pumped independently

Experimental cell supplied by gas lines

Sample with Z motion, cold finger and resistive heater

X-rays incident at 15° through a 100 nm Al window

Page 20: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 20

•In situ studies of surface reactions•closing the catalysis “pressure gap”

•Surface science of liquids•Segregation at solution liquid-vapor interfaces•Fundamental Electrochemistry

•Environmental Chemistry•Surfaces exposed to water vapor near ambient conditions•Solvation and ion-transport•Corrosion

•Biological Science•Study in the presence of water (in situ)

Ambient pressure soft x-ray spectroscopy: Possible Applications

Page 21: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 21

In Situ Catalysis

Partial oxidation of methanol to

formaldehyde over copper

CH3OH + O2 → CH2O

Active site exists under reaction conditions

Hendrick Bluhm et al.

540 538 536 534 532 530 528

Cu at 575 K 0.28 Torr O2

0.10 Torr O2 + 0.3 Torr CH3OHCu2O

O2(g)

CO2 (g) CH3OH(g)

CuxO(sub-oxide)

CH2O(g)

Binding Energy (eV)

Page 22: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 22

NEXAFS of Ice Premelting

555550545540535530

Incident photon energy (eV)

-25 ºC-15 ºC-10 ºC-5 ºC-4 ºC

ice, -2 ºC

water, -2 ºC

-39 ºC

560555550545540535530

Incident photon energy (eV)

292 284

Fluorescence Yield,Ice, -25 ºC

cont

amin

atio

n pe

ak

-4 ºC

-25 ºC

XPS C1s-25 ºC

Auger Yield

Page 23: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 23

Highly Correlated Electron SystemsHighly Correlated Electron Systems

Mott Insulator

U

One-electron Band Theory Mott Insulators

Doped Mott Insulators_________________________

High-Tc SuperconductivityCuprates

Colossal MagnetoresistanceManganites

Stripes & Orbital Order(many Oxides)

Anomalous Transport & Spectroscopic propertiesAn unsolved problem in

Many-body physics

Page 24: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 24

Highly Correlated Electron System

uncorrelated system correlated system

ground state

with external perturbation…

The responses are different due to correlation effect!

Page 25: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 25

Colossal Magnetoresistance (CMR) Effect

Novel Electronic PhasesCO : Charge Order (Stripes)FI : Ferromagnetic InsulatorAFI : Antiferro. InsulatorCAF : Canted AFM InsulatorCMR : Colossal MagnetoResis.

negative magneto- resistance

Temperature (K)

Res

istiv

ity (o

hm-c

m)

Susc

eptib

ility

(em

u/m

ol)

ParaFerro

Temperature (K)

H=0TH=1T

H=3TH=5T

H=7T

H=2T

10-1

100

10-2

1000 200 300 1000 200 300

La1.2Sr1.8Mn2O7

O Large drop of resistivityupon relatively small

magnetic fields

O Para Ferromagnetism

O Most dramatic on the insulating phase (short range orbital order)

Page 26: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 26

Study of Highly Correlated Electron Systems

Study of Highly Correlated Electron Systems

High Momentum and Energy Resolution Photoemission:A technique of choice for the study of electronic structure of correlated systems•Confirming breakdown of one electron band theory

Splitting of band in NiO due to e-e interaction•Determination of the Fermi Surface (example)•D-wave anisotropy of the super-conducting gap•Static and dynamics stripes in LSCO (example)•Observation of strong e-phonon coupling (example),

Continue photoemission development to achieve:Ultra high momentum resolution ~ 1% of BZ energy resolution ~ 1 meV

Page 27: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 27

The need for ultra-high energy and momentum resolution angle-resolved photoemission (ARPES)

Goal -• Making connections to transport, thermodynamics, and other low-energy scale properties of solids, especially those where these properties are exotic or poorly understood.

• In particular, where these properties are k-dependent, anisotropic, and/or low dimensional.

Page 28: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 28

Key physical properties measurable in ARPES:• Energy vs. wave vector(k) • Fermi Surface• Mean Free Paths• Effective carrier masses• Scattering rates• Electron Self energies • Scattering or nesting vectors• Number of carriers• Pseudogaps and superconducting gaps

ultra-high energy resolution ARPES-Capabilities

The only technique that can get all these in a single self consistent way.

Usually the only way to measure these in a k-resolved way.Only worthwhile if done with energy resolution comparable or better

than other key energy scales, temperatures.

Page 29: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 29

25

20

15

10

5

0

Inte

nsity

(Arb

. Uni

ts) 1.5

1.0

0.5

0.0-0.4 -0.2 0.0

Spectrum near Fermi LevellMost Relevant to

Superconductivity

EF

Valence Band

0-5-10

Energy Relative to EF (eV )

Typical Valence Band Photoemission Spectrum from a High Temperature Superconductor

Intrinsically weak signal experiments

Page 30: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 30

• Mechanism of high-temperature superconductors (HTSCs) unexplained—Electron-phonon interaction underlines

conventional superconductors—Previous experiment and theory suggest a

different mechanism is operative in HTSCs

• Angle-resolved photoemission (ARPES)—High angular resolution at the ALS probes

electron dynamical parameters—Feature at characteristic energies give insight into

operative physical processes•New APRES evidence from three families of HTSCs

•Kink in electron-momentum (dispersion) cureves ubiquitous in all three different classes of samples•Common kink energy and other evidence suggests electron-phonon coupling•Revives question of role of phonons in driving superconductivity inHTSCs

Observation of electron phonon coupling in high Tc superconductors

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SESAME workshop 31

(left) Electro-phonon coupling modifies the electron-momentum dispersion curve near the Fermi energy. (right) Dispersion curves for three families of high-temperature superconductors show a common kink at an energy (arrow) that matches an oxygen lattice vibration. The parameter δ is the doping concentration that determines the transition temperatures in the materials. k' is the reduced momentum (momentum at the Fermi energy kf minus the actual momentum k).

Strong electron phonon coupling in High Tc Superconductors

Lanzara, Hussain, Shen et al.Nature 412,510 (2001)

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SESAME workshop 32

High Energy Resolution Spectroscopy (HERS)Endstation at BL 10.0.1, Advanced Light Source

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SESAME workshop 33

Limitations of photoemission - need of new spectroscopy

Limitations of photoemission - need of new spectroscopy

However Photoemission: Measures single particle spectral function of occupied statesIt is highly surface sensitiveSpectra could become complicated for 3-D systems

Example: YBCO, difficulty due to surface stateLook for additional tools !!Resonant Inelastic soft x-ray scattering

Momentum-resolved provides information about the unoccupied band and anisotropic (direct/indirect) nature of energy gaps in solids.

Great for study of fast Correlated motion of electrons in CMR magnites and HTc cuprate

Page 34: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 34

Techniques of choice:

•Angle resolved photoemission (ARPES) : Single-particle spectrum A(k,ω)

•Inelastic Neutron Scattering (INS) : Spin fluctuation spectrum S(q,ω)

•Inelastic x-ray scattering (IXS) :New info on the Charge Channel : N(q,ω)

This extra experimental info can help understand correlated systems

Spectroscopy's of Correlated Electrons

Page 35: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 35

Manganites Exhibit Interplay of Charge, Spin, lattice and Orbital degrees of freedom

orbital wave excitation

electronic ground state

An unexplored degree of freedom in transition metal oxides:

Orbital Density Waves

Ordering of orbitals produce long-range orbital density waves - a new type of

collective excitation in crystals

E. Saitoh et al. Nature 410, 180 (2001)

Competition among many Energyand Length scales

Determine the physics of these systems

Interacting degrees of freedom (complex electron

systems)

spinlattice

chargeorbital

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SESAME workshop 36

ener

gy

core level

valence band

conduction band

p

d

Resonant Inelastic soft X-ray Scattering(Raman Spectroscopy with finite q)

Energy loss: ω=ω2-ω1Momentum transfer: q=k2-k1Resonance: ω1~ ωedge

hω1,k1,ε1

Photon-in hω2,k2,ε2

Photon-out Optically forbidden d-d excitationOptically forbidden d-d excitation

Finite q transfer allows to study indirect Mott gap

Finite q transfer allows to study indirect Mott gap

Couples to charge density directly (Neutrons couples to spin).

Couples to charge density directly (Neutrons couples to spin).

Energy Resolution not limited by the core hole lifetime: achieve kBT resolution

Energy Resolution not limited by the core hole lifetime: achieve kBT resolution

Can be applied in the presence of magnetic/electric field

Bulk sensitive probe for studying unoccupied electronic states

Can be applied in the presence of magnetic/electric field

Bulk sensitive probe for studying unoccupied electronic states

Why???Why???

Page 37: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 37

Soft x-ray resonances (3p -> 3d) provide the most sensitive channels of excitations to study

orbital wave excitations

Soft x-ray resonances (3p -> 3d) provide the most sensitive channels of excitations to study

orbital wave excitations

Requires study of energy losses with energy resolution

better than 10meV

Requires study of energy losses with energy resolution

better than 10meV

Energy scales of various excitations

Optical Phonons: ~ 40 - 70 meVMagnons: ~ 10 meV - 40 meVOrbital fluctuations (originated

from optically forbidden d-dexcitations): ~ 100 meV - 1.5 eV

0

100meV

X

3 eV

1 eV

Mott Gap,C-T Gap

dd excitations,Orbital Waves

Optical Phonons,Magnons,Local Spin-flips

Page 38: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 38

Previous experiments (@ ALS):

Energy resolution = 200 meVThroughput = low

Need better energy resolutions (<10 meV) and higher throughput

Current State-of-the-ArtStudy of d-d Excitations in Cuprates

Cu d-d excitation at 74eV

200

150

100

50

0

Cou

nts

-2 -1 0 1

Raman shift (eV)

30 degr 40 degr 60 degr

Kuiper, Nordgren, Sawatzky et al., Phys. Rev. Lett. 80, 5204 (1998)Expt carried out @ ALS

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SESAME workshop 39

meV Resolution VLS Spectrograph

• Resolution approaching 1 meV.• Overall length = 2 meters.• Designed for Mn 3p (47 eV)• Source size = 4 microns.

hν = 47 eV ± 5 meV

Ray Traces

Optical Design

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SESAME workshop 40

#1 (5o~35o)#2 (35o~65o)

#3 (65o~95o)

#4 (95o~125o)

#5 (125o~155o)

0o-15o

15o

0.60

0.55

0.50

0.45

0.40

0.35

0.30

0.25

0.20

0.15

0.10

0.05

-15 -10 -5 0 5 10 15

0.75

0.70

0.65

0.60

0.55

0.50

0.45

0.40

0.35

0.30

0.25

0.20

0.15

0.10

0.05

chamber rotation angle

Å-1

mom

entu

m tr

ansf

er ∆

q

fraction of the Brillouin

zone#1

#2

#3

#4

#5

Calculation based on photon energy of 650eV650eV and 3.85 Å lattice constant 10

5

0

-5

-10

50-5

(0,0) (π,0)

(π,π)

Brillouin zone size which can be covered by this spectrometer

Five spectrometers with 30o rotations can cover most of the Brillouin zone

Resonant Inelastic soft X-ray Scattering

Page 41: New Scientific Opportunities Scientific with soft x-ray SRconference.kek.jp/JASS02/PDF_PPT/38_hussain.pdf · 2002. 11. 19. · SESAME workshop 7 New Scientific Opportunities, New

SESAME workshop 41

incoming photon beam

spherical focusing mirror variable line spacing

grating

grating drive mechanism

back-illuminated CCD camera

System with five spectrometers to cover most of the scattering angleswith rotary seal underneath to perform ±15o rotation

Individual spectrometer contains:•Spherical focusing mirror•Variable line spacing grating•High efficiency back-illuminated CCD camera

Resonant Inelastic soft X-ray Scattering

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SESAME workshop 42

Relevant spatial & temporal frequency scales for various physical phenomena

Spatial and temporal frequency sensitivities of various techniques

Combined Nanometer Spatial and Microsecond Temporal Resolution- Coherent Scattering

Intense, transversely coherent soft x-ray beams will allow extension of dynamic laser light scattering to probe temporal fluctuations on the scale of nanometers.

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SESAME workshop 43

Coherent Soft X-Ray Science

CohOptcsBL.ppt

• Coherent scattering from dynamic systems• Fourier optics at soft x-ray wavelengths

From Attwood

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SESAME workshop 44

Magnetic Structure and Fluctuations in a Co:Pt Multilayer

• Candidate for future magnetic recording media

• Perpendicular magnetic anisotropy

• Magnetic domains ~ 100 nm

• ‘Tunable’ magnetization loop

Ptsubstrate

Co:Pt

50 repeats (7Å Pt + 4Å Co)

M

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SESAME workshop 45

Imaging Magnetic Domains with a Soft X-ray Microscope

0012105100121051rect

1 µ

• Contrast provided by huge magnetic circular dichroism near the Co L23

absorption edge [2p3/2 - 3d] at hν ~ 780 eV

• Wavelength λ ~ 15.8 Å allows good spatial resolution

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SESAME workshop 46

Return Point Memory Effect

Macroscopic (Madelung, 1905):

• The ‘major magnetization loop’ is well-defined - it reproduces after saturation;• Excursion onto a ‘minor magnetization loop’ leaves from and reconnects to the major loop at a single point.Microscopic:• Is the magnetic domain structure reproducible around such major and minor loops?

major loop

minor loop

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SESAME workshop 47

• Speckle pattern ≡ diffraction pattern of the magnetic domain structure;

• Domain sized inversely related to angular width of the ‘doughnut’;

• Contrast provided by x-ray magneto-optic effects near the Co L-edge.

• New apparatus will enable us to measure the individual Fourier components fluctuating at MHz time scales;

• We will measure domain flipping (Barkhausen noise) and domain wall motion with a combined spatial and temporal resolution not available with other techniques.

Soft X-ray Speckle Pattern of a Pt:Co Multilayer

00121051rect

1 µ

Real Space Reciprocal Space

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Dynamic Light Scattering

I(t)

t

C(τ)=( ) ( )∫ + dttItI

Tτ1

τ

τdecay ~ 1µs - 1hr

correlator

I(t)

Ar-Ion Laserλ = 3511Å

Spatial Filter

Fluctuatingsample

I(t)

Undulatorλ = 16Å

Monochromator:λ/∆λ ~ 103

Spatial Filter

Fluctuatingsample

Fcoh~1010-11/s

Fcoh~1017/s

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The combination of the large soft x-ray magnetic contrast with high coherent flux of the new CSX beamline will enable many experiments that probe spatiotemporal magnetic fluctuations. Flangosaurus

Flangosauruswith yoke

Octapolar Flangosaurus

Coherent Soft X-ray Magnetic Scattering End Station• Applied field to 0.52 T of arbitrary orientation • ‘Continuous’ scattering angle from 0o to ~ 165o

• Functional prototype for higher field device

Coherent soft-X ray Scattering

Speckle-diffraction Pattern through a Co:Pt film.

major loopminor loop

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Why dynamic soft X-rays coherent scattering ?Why dynamic soft XWhy dynamic soft X--rays coherent scattering ?rays coherent scattering ?

o More coherent flux - Scales like λ2 x brightness(2000 times more coherent flux for λ = 4.4nm than for 0.1nm)

o High sensitivity for 3d metals: Resonant 2p-3d transitions(excited electrons into spin polarized empty 3d states)

o Wide range of Spatial resolution:1 nm (wavelength of rad.) - 40 µm (transverse coherence length)

o Time resolution: > µs - 5ns) limited by time correlator

o No multiple scattering complications (photons are weak scatters).

o Bulk sensitivity

o Can be applied in the presence of magnetic/electric field

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Time-Resolved X-Ray SpectroscopyTime-Resolved X-Ray Spectroscopy

• Ultra-fast time regime: < 200fs• Electron excitation/de-excitation (fs)• Bond breaking• Carrier-carrier scattering• Hole-optical phonon scattering• Charge density wave/charge transfer

• Time regime: < 2ps• Carrier acoustic phonon scattering• Relaxation of biological system after light absorption

(Rhodopsin); Phase transition (diamond graphite)• Time regime: > 1-100ps

• Stripe fluctuation in High Temp Superconductor• Magnetic recording• Protein folding (ps-s)

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Time-Resolved X-Ray SpectroscopyTechniques

Time-Resolved X-Ray SpectroscopyTechniques

• Laser Time Slicing of SR, τ ~ 100 - 200fs • Bending Magnet ~ 105 photons/s

• Undulator ~ 108 photons/s• Phase transition

• Streak Camera; τ ~ 1-2 ps,limited by detector• Could use dispersive methods in time and energy• Ultrafast lattice dynamics (coherent phonons)

• Polarons in condensed matter (magnites)

• Dynamics Coherent Soft X-Ray Scattering, τ > 1ns - µs • Stripe fluctuation in High Temp Superconductor (ns-µs)• Magnetic recording (ns)• Protein folding (ps-s)

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wiggler

Femtosecond Electron Bunch

Bend-MagnetBeamline

30 ps ElectronBunch

FemtosecondLaser Pulse

Spatial SeparationDispersive Bend

λW

Electron-PhotonInteraction in Wiggler

FemtosecondX-Rays

CalculatedElectronDensityDistribution

-1000 -500 0 500 1000 0

.2

.4

.6

.8

1.0

01234

-4-3-2-1

time (fs)

x/σx

GENERATION OF FEMTOSECONDX-RAYS FROM THE ALS

Zholents and Zolotorev, Phys. Rev. Lett., 76, 916,1996. Schoenlein et al., Science, 287, 2237, 2000

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Science of Heterogeneous systems, Interfaces, heteromagnetism

Science of Heterogeneous systems, Interfaces, heteromagnetism

• Real Space Microscopy (transmission, scanning or imaging)• Biological systems (water window, in-situ conditions,

resolution ~20-30 nm, Tomography (Larabell et al)• Environmental Science

• Spectromicroscopy of interfaces down to nm resolution(PEEM III,SMART, abberation corrected optics )?• Exchange bias in magnetic layers (Co/LaFeO3), (example)

• Reciprocal space Imaging with Coherent Soft x-ray Scattering; Spatial resolution ~ 1nm - 40µm

• Magnetic domains (Co/Pt multilayer), (example)• Stripe fluctuation in High Temp Superconductor

Development of these techniques necessary for Nanotechnology; “shape the world atom by atom” Ronald Hoffmann

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HIGH SPATIAL RESOLUTION MICROSCOPY OF HYDRATED MATERIALS

1 µm

S. Myneni et al., Science 278, p.1107

pH 9.5

pH 7.5 pH 9.5

0.5 µm

K. Kurtis, P. Monteiro et al.Cement & Concrete Research

B. Tonner K. Nealson et al.

C. Larabell, S. Lelièvre, D. Hamamoto, M. Bissell

646 eV 517 eV

C. Magowan et al.PNAS 94, 6222

Malaria Cell Nucleus Labeled for Splicing Factor Alkali-Aggregate Reaction

Manganese-Eating BacteriaReactions at Fe-oxides

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Linear dichroism at Fe L edge images AFM domains (left). Circular dichroism at Co L edge images FM domains (right). Comparison of images shows that the Co domains align with the AFM domains (light and dark regions inside outlined areas).

Exchange bias in magnetic nanostructures

F. Nolting et al, Nature, 405, 767(2000)

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AcknowledgementsAcknowledgementsAcknowledgements

o Daniel Chemla, Neville Smith, Howard Padmore, Eli Rotenberg, Mike Martin, John Bozek, Wayne McKinney, Phil Heimann, Ernie Glover, Elke Arenholtz, Andres Scholl (ALS, LBNL)

o Zahid Hasan (Princeton)ZX Shen, Xingjiang Zhou, Pasha Bogdanov, SSRL/StanfordA. Lanzara (UC Berkeley/LBNL), Dan Dessau (Univ of Colorado)

o Dave Attwood, Jim Underwood, Jeff Kortright, Miquel Salmeron, Hendrik Bluhm, Chuck Fadley, Frank Ogleoree, Bob Schoenlein, Roger Falcone, MSD, LBNL

o Steve Kevan (Univ of Oregon) and Larry Sorensen (Univ of Washington)

o Satish Mynenei (Princeton)

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Conclusions

We may need to look harder buta lot of new physics still to come!!