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Background and Present Status from AMO Instrument Team. Team Organization. 2. Proposed Scientific Plan. The First Experiment. 4. Future Plan. Historical Facts. April 2004: LCLS puts out a call for Letters of Intent (LOI) category A: science & end-station construction

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background and present status from amo instrument team
Background and Present Status from AMO Instrument Team
  • Team Organization.

2. Proposed Scientific Plan.

  • The First Experiment.

4. Future Plan.

historical facts
Historical Facts
  • April 2004: LCLS puts out a call for Letters of Intent (LOI)

category A: science & end-station construction

category B: science

category C: instrument design

  • July 2004: LCLS SAC makes recommendation that two AMO proposals of the “category A LOI” collaborative teams merge
  • October 2004: Ultra-fast science workshop

October 2004: Ultra-fast science workshop

  • ►Workshop Objective:
  • solicit input & participation from the AMOP community for the LCLS project
  • - shape the scientific program: Scientists ideas
  • help define the critical XFEL machine parameters
  • help define the designs of an AMOP end-station(s)
  • - interaction of the five collaborative teams
  • ►Five LCLS collaborative teams:
  • Atomic, Molecular & Optical Science
  • Optical pump x-ray probe studies in chemistry, biology & material science
  • Diffraction imaging of single objects approaching atomic scale resolution
  • Coherent x-ray scattering for the study of dynamics
  • High-energy density science

AMO Collaborative Team ( Original Merged LOIs A)

Marriage of Synchrotrons + Ultrafast Communities

  • Lou DiMauro (OSU) & Nora Berrah (WMU) (co-T. Leaders)
  • John Bozek (Instrument Scientist)
  • Pierre Agostini OSUMusahid Ahmed LBL
  • John Bozek LBL Philip H. Bucksbaum SU/SLAC
  • Roy Clarke UM Todd Ditmire UT Austin
  • Paul Fuoss ANL Ernie Glover LBL
  • Chris Greene U Colorado Elliot Kantor ANL
  • Bertold Kraessig ANL Steve Leone UC Berkeley
  • Dan Neumark UC Berkeley Gerhard Paulus Texas A&M
  • Steve Pratt ANL Alexei Sokolov Texas A&M
  • John Reading Texas A&M David Reis UM
  • Steve Southworth ANL Linn Van Woerkom OSU
  • Linda Young ANL

~ Twenty Additional Scientists Expressed Interest at the October 2004 Workshop

update on amo organization activities
Update on AMO Organization/Activities
  • Instrument Scientist, John Bozek, Hired (Jan 2006)
  • Regular Teleconference (Berrah, Bozek, DiMauro, Young)
  • N. Berrah on Sabbatical FY06
  • Periodic visits by DiMauro/Berrah

5. Communication with Broader Team at Conferences (Wisconsin W. 8/04; DOE M. 9/05; DAMOP 5/06)

6. E-mail Updates to Broader Team when Necessary (seek input, communicate news)

Discussions/communication led to determine the instrumentation needs for first experiments!

7. Conceptual Design and Instrument Budget was submitted and Accepted by LCLS.

update on amo activities organization cont
Update on AMO Activities/ Organization (cont..)

8. Synergy between the PULSE Center and AMOS

9. Workshop to Stimulate Theory (ITAMP 06-06)

10. Met with:

-----LCLS Optics Group

------Pump-Probe Team to Explore Common Interest and will Continue to Meet.

11. Plan to Meet with Imaging Group to Explore Shared Experimental System?

12. Held Ultrafast x-ray Summer School June 2007


TeamMajor Scientific Thrusts:

  • Multiphoton and High-Field X-Ray Processes in Atoms, Molecules, Clusters,& Biological Molecules.
  • Time-Resolved Phenomena in Atoms, Molecules (bio-molecules) and Clusters using Ultrafast X-Rays

AMO LOIs Collaborative Team

  • Science:
  • Multiple core excitation in atoms, molecules and clusters
  • 2. Timing experiments: Inner-shell side band experiments Photoionization of aligned molecules
    • Temporal evolution of state-prepared systems
  • 3. Nonlinear physics
  • 4. Ion (positive/negative) studies
  • 5. Pump-probe, X-X or X-laser or X-e
  • 6. Raman processes
  • 7. Cluster dynamics (Diffraction of size-selected clusters)
  • Photoionization dynamics of biomolecules

Science discussed at 2004 October AMOS forum

Ken Taylor (Ireland) Possibilities for few- and many-electron atoms & ions in XFEL pulses

David Reis (UM) Synchronization issues for pump-probe experiments at LCLS

Robin Santra (ITAMP) Cluster physics at high photon energies

Anders Nielsson (SSRL) Time resolved spectroscopy for studies in surface chemistry and electron driven processes in aqueous systems

Chris Greene (UCB) Multiphoton ionization processes in free atoms and clusters

John Bozek (ALS, LBNL) Atoms, molecules, clusters and their ions studied with two or more Photons

Ali Belkacem (LBNL) Inner-shell ionization and de-excitation pathways of laser-dressed atoms and molecules

Keith Nelson (MIT) Give him 10 minutes max and then let's get back to reality

Ernie Glover (LBNL) X-ray/optical wave mixing

Elliott Kanter (ANL) Hollow neon atoms

lcls characteristics
LCLS Characteristics
  • The LCLS beam intensity (~1013 x-rays/200 fs) is greater than the current 3rd generation sources (104 x-rays/100 ps).
  • Extreme focusing (KB pairs) leads to intensity ~1035 photons/s/cm2 (~ 1020 W/cm2 for 800 eV x- rays)
  • Nonlinear and strong-field effects are expected when the LCLS beam is focused to a spot diameter of 1μm.
  • BUT, electron’s ponderomotive (quiver motion) important at low frequencies IS negligible in the x-ray regime (λ2).
amos inst team short long range plans
AMOS Inst.Team Short-Long Range Plans:
  • High Field: Using the extremely high brightness of the LCLS we propose to study:
    • multiple ionization atoms & simple molecules with angle-resolved spectroscopy and ion imaging to understand basic phenomena in highly excited matter
    • High-field photoionization in clusters (of various types)
    • Low density ionic targets: atoms, molecules, fragments, clusters, biomolecules by photoelectron and ion imaging techniques
  • Time-Resolved: Temporal resolution will be used to perform:
    • Inner-shell photoelectron spectroscopy of molecules (pump-probe using lasers) into specific states.
    • Inner-shell photoelectron imaging of isolated biomolecules to follow their chemistry in natural time scale
double k vacancy in gas phase systems possible consequences
Double K Vacancy in Gas-Phase Systems → Possible Consequences
  • The decay of the KK-vacancy state will produce higher charge states
  • This process → extensive fragmentation in molecules
  • This process → damage consideration in experiments on Bio-molecules?
lcls high field beam will probe

Auger Decay

Auger Decay

LCLS High Field Beam will Probe:

Sequential(or “Cascade”) Multi-Auger Decay


(or Ionization)

SimultaneousDouble-Auger Decay

( 3-10% of single Auger)


Some Examples

High Field Studies in Atoms

x ray strong field experiment


correlated ionization



2-photon, 2-electron

X-Ray Strong Field Experiment

x-ray multiphoton ionization

low frequency physics high frequency

- Ip

- Ip

10x20 W/cm2

1015 W/cm2

- Ip

1013 W/cm2

Low-Frequency Physics → High Frequency


Low frequency regime


Intense photon source


Highly ionizing source

  • Angstrom wavelength
  • Direct multiphoton ionisation
  • Secondary processes
  • Keldysh parameter >>1
  • Multi-photon ionisation
  • Ponderomotive energy 10 meV
  • Keldysh parameter <<1
  • Tunnel / over the barrier ionisation
  • Ponderomotive energy 10 – 100 eV

  Optical Frequency = (Ip/2Up)1/2 -1; Up=I/4ω2 (au)

Tunneling Frequency


FLASH Experiments

PRL 94, 023001 (2005)

Theory Available! Calculate the rate of production of highly charged Xei+ ions produced by direct multiphoton absorption, to compare with experiment.


First LCLS Experiment: K-Shell in Ne1.Photoionization2. Auger Decay3. Sequential Multiphoton Ionization4. Direct Multiphoton IonizationTheory:Double-K ionization in Ne due to absorption of 2-photons by 1 atom for hγ>932 eV is predicted to be 100%



Ne K-edge ~ 870 eV

2 e-out

The probability of two-photon absorption by 1s2 -shell accompanied by the creation of double 1s-vacancies predominates over the probability of the process of two-photon one-electron excitation/ionization of the 1s2 shell in the range of x-ray photon energies ≥ 930 eV.


ne charge state vs intensity
Ne Charge State vs Intensity

Rohringer & Santra, PRA 76, 033416 (2007)

@1050 eV

probable ne charge state with hv
Probable Ne Charge State with hv

@1μm beamsize

Rohringer & Santra, PRA 76, 033416 (2007)


Power of TOFs: Inner-Shell Resonances in Ar; 2 p Excitation to Rydberg States(ALS)

LCLS: K-Shell ArHow would the ratio of Doubly Ionized Ions (Auger decay) Compares to Singly Ionized Ions due to spectator Auger decay?

Resonant shake-off of two electrons.

resonant auger electron spectroscopy
Resonant Auger Electron Spectroscopy
  • Interesting in molecules too – CO resonant Auger:

Ion Imaging : Fragmentation Decay Channels of CO22+ Subsequent to K-Shell Photoionization and Auger Decay of CO2.

Identify different fragmentation mechanisms


Fragment Momentum Correlation Plots: Fragmentation Decay Channels of CO22+ Subsequent to K-shell Photoionization and Auger Decay of CO2.

cluster studies flash
Cluster Studies, FLASH

Xenon Cluster size 2500 atoms

Tpuls=50 fs

lFEL=98 nm

  • Unusually high energy absorption in cluster
  • Fragmentation starting at 1011 W/cm2

Wabnitz et al, Nature 420, 482 (2002)


Molecular dynamics simulations indicate

that standard collisional heating cannot fully account for the strong energy absorption.


In contrast with earlier studies in IR and VUV spectral regime, we find NO evidence for electron emission from plasma heating processes; Multistep ionization process is dominant

hν=37.8 eV, <N>~100, I=3x1013W/cm2 @25 fs

proposed at lcls ion e and scattering experiments on clusters
Proposed at LCLS: Ion, e-, and Scattering Experiments on Clusters
  • Study the Dynamics of Cluster Explosion as a Function of Cluster Size, Wavelengths, Intensity:

Is it a Coulomb Explosion Picture(as in intense optical or near IR ultrafast laser pulses) OR

Explosion due to Hot Nanoplasma(multiple scattering from the cluster atoms can confine electrons yielding a nanoplasma); Explosion Time can be Different

OR, New mechanisms??

  • Will Collective Electron Effects be important as in the dynamics of IR irradiated large clusters?

Velocity Map Imaging Coincidence System (PEPIPICO) @ ALS

Ion Detection

Electron Detection

80 mm position-sensitive multi-hit hex-anode detector (Roentdek)

Rolles et al. Nucl. Instr. and Meth. B 261, 170 (2007).


Movable Ion-Photon Beamline for ions & size-selected clusters

Size Selected Production

Size and Charge Selected Detection

Absolute cross sections: measurements of overlaps, photon & ion fluxes and detector efficiencies.


High Charge State Formation Following 2p Photodetachment of S- (ALS)

S2+/S+ 60%

LCLS: S K-shell


PR A 72, 050701(R), 05

H, S-Off; S-Up+Seq-Aug

Int, K-Out

Th, Sim-Auger

photoionization dynamics of clusters or biomolecules
Photoionization Dynamics of Clusters or Biomolecules
  • Biomolecules injected via electrospray

Time-Resolved Studies of Molecules

Pump-probe experiments of molecules (state-selected): - Launch a molecule on a particular potentially energy surface - Watch temporal evolution with angle-resolved inner-shell PES


Photodissociation Dynamics of I2-: Pump-Probe Experiments

  • Short delay times photodetachment
  • accesses bound vibrational levels
  • of I2 states
  • Longer times,
  • dissociation to I- + I
  • Complete dissociation
  • ≡ photodetaching free I-


LCLS, Probe with >800 eV photons



Photodissociation Dynamics of I2-

2P1/2 and 2P3/2 spin-orbit states of I.

I- photoelectron spectrum

Neumark et al. Chem. Phys. Lett, 258 (1996) 523.


Photodissociation Dynamics of I2-

I 2P3/2

Dissociation Time scale: Rise time of electron signal reaches 50% of its maximum value by 100 fs.

I 2P1/2