Ultrafast laser-plasma sources for 50-fs hard x-ray pulse generation and laser pump x-ray probe measurements of solvated transition metal complexes

C. Rose-PetruckDepartment of Chemistry,

Brown University, Providence, R.I.

www.rosepetruck.chem.brown.edu

ERL Workshop, Cornell University June 2006

Outline

50-fs laser-plasma x-ray sources

Ultrafast XANES of Fe(CN)54-

Ultrafast x-ray sources and Cornell ERL-II experiments

Outline

50-fs laser-plasma x-ray sources

Ultrafast XANES of Fe(CN)54-

Ultrafast x-ray sources and Cornell ERL-II experiments

Multiple scattering paths of IPC-Bz at 0 Kelvin

Path 6: 25%Path 8: 153% Path 7: 123% Path 1: 100% Path 23: 11% Path 31: 9%

Path 5: 2%Path 27: 4% Path 35: 4% Path 28: 3%Path 33: 8%Path 20: 9%

Excitation photon wavelength < 270 nm: Charge Transfer To Solvent

Excitation photon wavelength < 400 nm: Photoaquation

CTTS

Photoaquationλ - 400 nm

λ - 266nmCTTS Fe(CN) + eaq6

3- -Fe(CN)4 ∗6-

+H2O Fe(CN)5 H2O( ) + CN-3-

Fe(CN)4 ∗6-

Fe(CN)64 -+ hν

Excited state chemistry of iron hexacyanide in water

Las

erm

etri

cs

Nd:YVO4

OS: 2pcs, 055-0140

NP: 10FC16PB.5

F=50

0mm

Si(111) double crystal spectrometer

Overlap of laser and x-ray beams in liquid sample jet

X-ray lens

CCD camera

Main laser beam for x-ray generation

Pump laser beam

Ultrafast laser for laboratory-based plasma x-ray sources

Laser pulse: 800 nm, 40 fs, 4 mJ, 5 kHzAverage compressed power: 20WLaser intensity: ~ 1017 W/cm2

F=500mm

Honeywell CCDGC-135E24-G

Si(1

11) d

oubl

e cr

ysta

l

spe

ctro

met

er

Ove

rlap

of la

ser a

nd x

-ray

bea

ms

in

liqu

id s

ampl

e je

t

Main laser beam for x-ray generation

X-ra

y le

ns

Pump laser beam

CCD camera

Ultrafast laser-driven XAFS spectrometer

X-ray emission spectrum of 2-kHz source

5

6

7

8

9

5 6 7 8 9 10 11

X-ray photon energy [ keV ]

X-ra

y flu

x [ p

h / (

s 4 π

sr e

V) ]

10

10

10

10

10

Cu-Kα

Zn-Kα

Cu-Kβ

Fe-Kα

Fe-KβV-Kα

Zn-Kβ

Iron K-edge

⎟⎟⎠

⎞⎜⎜⎝

⎛⋅

sph

rangekeV

π4103

1

9⎟⎟⎠

⎞⎜⎜⎝

⎛⋅

sph

KCu

π

α

4105.1 10

Laser plasma x-radiation imaged into sample by x-ray lens

sphotons10x2:KCu

keV1sphotons10x5:lungBremsstrah

5

5

α−

F=500mm

Honeywell CCDGC-135E24-G

Si(1

11) d

oubl

e cr

ysta

l

spe

ctro

met

er

Ove

rlap

of la

ser a

nd x

-ray

bea

ms

in

liqu

id s

ampl

e je

t

Main laser beam for x-ray generation

X-ra

y le

ns

Pump laser beam

CCD camera

Ultrafast laser-driven XAFS spectrometer

Stat

icSt

atic

Pum

pPu

mp

Bac

kgro

und

Fe Kβ Fe K-edge

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1

1.1

1.2

1.3

7110 7120 7130 7140 7150 7160 7170

X-ray photon energy [eV]

Nor

mal

ized

abs

orba

nce

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1

1.1

1.2

1.3

7110 7120 7130 7140 7150 7160 7170

X-ray photon energy [eV]

Nor

mal

ized

abs

orba

nce

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1

1.1

1.2

1.3

7110 7120 7130 7140 7150 7160 7170

X-ray photon energy [eV]

Nor

mal

ized

abs

orba

nce

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1

1.1

1.2

1.3

7110 7120 7130 7140 7150 7160 7170

X-ray photon energy [eV]

Nor

mal

ized

abs

orba

nce

UXANES at –30 ps, 0 ps, and +40 ps after photoexcitation

NSLS-X11B X 8eV: Fe(CN)64-

+40 ps~0 ps

-30 ps

7045 7050 7055 7060 7065 7070 7075 7080

Fe-Kβ

-30 ps: 7056.95 eV

~0 ps: 7057.39 eV

+40 ps: 7057.48 eV

Peak centroids:

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1.0

1.1

1.2

1.3

1.4

1.5

7110 7120 7130 7140 7150 7160 7170

X-ray photon energy [eV]

Nor

mal

ized

abs

orba

nce

+5 pm[Fe(CN)6]4-

+10 pm

[Fe(CN)5H2O]3-

[Fe2(CN)10]6-

Radial Fe-ligand bond lengths increase of Fe(CN)64-

Outline

50-fs laser-plasma x-ray sources

Ultrafast XANES of Fe(CN)54-

Ultrafast x-ray sources and Cornell ERL-II experiments

New liquid metal x-ray source

Printed circuit board

Ceramic base plate

Piezo actuators

Fused silica membrane, 200 µm thick

4” diameter deformable mirror for focus optimization

200 μm

1.E+07

1.E+08

1.E+09

1.E+10

1.E+11

5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20

X-ray photon energy [ keV ]

X-ra

y so

urce

flux

[ ph

/ (s

4π

sr k

eV) ]

⎟⎟⎠

⎞⎜⎜⎝

⎛π

⋅s4

ph103

rangekeV1

9

Hg-Lα1,2

Hg-Lβ1,2

Hg-Lγ

X-ray emission spectrum of Hg-source

Numerical modeling of laser-produced x-ray emission

Absorption lengths:Fe @ 6.5 keV: 19 μmFe @ 7.2 keV: 3.1 μmHg @ 7.2 keV: 2.7 μm

X-ray absorption in Iron and Mercury

Fe Kα @ 6.5 keV

Fe K-edge

Similar x-ray yields for Fe and Hg @ 7.2 keV

Highest x-ray yield at medium laser

100 fs laserL/λ = 0.2

Temporal x-ray pulse shape from Iron and Mercury

1017 W/cm2

100 fsL/λ = 0.2

solid lines: generated photonsdashed lines: emitted photons

50 fs x-ray pulses are possible

50 fs FWHM

4 x 1015 W/cm2 , 100 fsL/λ = 0.2Mercury target @ 7.2 keV

The continuum pulse can be shorter than the laser pulse

100 fsL/λ = 0.2

X-ray yield and pulsewidth for Fe and Hg target

Outline

50-fs laser-plasma x-ray sources

Ultrafast XANES of Fe(CN)54-

Ultrafast x-ray sources and Cornell ERL-II experiments

6

7

8

9

10

11

12

13

7 8 9 10 11 12 13

Laser peak power (W)

X-ra

y flu

x (p

h/4 π

sr s

)A. Rousse, et al, Phys. Rev. E, 50, 2200 (1994)D. Eder, et al, Appl. Phys. B, 70, 211 (2000)R. Tompkins, et al, Rev. Sci. Instrum. 69, 3113 (1998)M. Yoshida, et al, Appl. Phys. Lett. 73 2393 (1998)B. Soom, et al, J. Appl. Phys. 74, 5372 (1993)Ch. Ziener, et al, Phys. Rev. E 65, 066411 (2002)T. Guo, et al, Rev. Sci. Instrum. 72, 41 (2001)Z. Jiang, et al, Phys Plasmas, 2, 1702, (1995)T. Feurer, at al, Appl. Phys. B, 72, 15, (2001)A. Egbert, et al, Appl. Phys. Let., 81, 2328 (2002)Y. Hironaka, et al, J. Appl. Phys., 74, 165 (1999)G. Korn et al, Opt. Lett. 27, 866-868 (2002)This work 2 kHz, 4.25 mJ, 40 fs,

1017W/cm2, Brass wire

10 Hz, 200 mJ, 200 fs,1017W/cm2, Cu slab

1 kHz, 0.5 mJ, 100 fsliquid jet Cu(NO)3

20 Hz, 80 mJ, 35 fs,1018W/cm2, Cu wire

10 Hz, 240 mJ, 60 fs,1017W/cm2, Co0.016 Hz, 13 mJ, 1.3 ps,

4x1015W/cm2, Al coat on Si

250 kHz, 3 μJ, 160 fs,X-ray diode, Cu anode

0.0016 Hz, 900 mJ, 300 fs, 4x1018W/cm2, Ta

10 Hz, 60 mJ, 42 fs,1017W/cm2, Cu disk

1 kHz, 30 μJ, 120 fs

10 Hz, 200 mJ,42 fs, 3x1017W/cm2,4th shot, Cu

1st shot

estgimated future flux:2 kHz, 4.25 mJ, 40 fs,

3x1018W/cm2, liquid Hg

10

10

10

10

10

10

10

10

10 10 10 10 10 10 10

10 Hz, 60 mJ, 80 fs,5x1017W/cm2, Si

10 Hz, 1.5 mJ, 100 fs, 3x1016W/cm2, Al 1 kHz, 1.8 mJ, 100 fs,

3x1016W/cm2, liquid Ga

Comparison of laboratory-based hard x-ray sources

Comparison of x-ray sources

X-ray absorption spectrometer with …

Repetition rate[kHz]

Pulse length[ps]

Peak x-ray flux[ph / s ps]

12 kW rotating anode tube 6 x 109 6 x 10-3

APS, sector 7ID, @ 1kHz pump laser rep. rate,

special-timing-mode1 80 unfocused: 2x109

KB-focused: 5x107unfocused: 2 x 107

KB-focused: 5 x 105

APS, sector 11ID-D, @ 1kHz pump laser rep. rate,

special-timing-mode1 80 108 106

Old Source: 106

New Source: 108

+ crystal optics: 1010

Old Source: 107

New Source: 109

+ crystal optics: 1011

At

dete

ctor Old Source: 100

New Source: 104

+ crystal optics: 106

Old Source: 1000New Source: 105

+ crystal optics: 107

c.w.

Average x-ray flux[ph / s]

At s

ampl

eTabletop ultrafast x-ray sources

(8 - 15 W) 4 0.1

Prospective ERL parameters

The I2-reflectron

B. Kohler, J.L. Krause, F. Ráksi, C. Rose-Petruck, R.M. Whitnell, K.R. Wilson, V.V. Yakovlev, Y. Yan, S. Mukamel,J. Phys. Chem. 97, 12602 (1993)

optimal chirp

200 600 1000 1400 1800

250300350400450

positive chirp

250300350400450

I-I d

ista

nce

[pm

]

time delay [fs]

0

5

10

15

20

Ψ Ψ*

I-I distance probability distributions

optimal chirp

positive chirp

time delay [fs]

diffr

actio

n an

gle

[deg

ree]

2050

80

110

140

170

200 600 1000 1400 1800

2050

80

110

140

170

counts0

100

200

300

400

500

Simulated diffraction pattern for Cu-Kα x-ray pulses

Funding

National Science Foundation, Chemistry

Department of Energy, BES

Army Medical Res. and Material Command

Argonne National Laboratory

Andrew W. Mellon Foundation

Research Corporation

www.rosepetruck.chem.brown.edu

Nuclear motions and ultrafast x-ray diffraction off I2

250300350400450

diffr

actio

n an

gle

[deg

ree]

I-I d

ista

nce

[pm

]

200 600 1000 1400 1800

time delay [fs]200 600 1000 1400 1800

2050

80

110

140

170

optimal chirpoptimal chirp

0.00

0.20

0.40

0.60

0.80

1.00

1.20

8.32

8.33

8.34

8.35

8.36

8.37

8.38

8.39

8.40

8.41

8.42

8.43

8.44

8.45

8.46

8.47

8.48

8.49

8.50

8.51

8.52

8.53

8.54

8.55

8.56

8.57

8.58

8.59

8.60

X-ray photon energy [keV]

Nor

m. A

bsor

ptio

n [a

.u.]

Calculated XAFS spectrum of NiCO4

S/N calculation for EXAFS of solute at “ultrafast” Cornell ERL-II

Beam thickness [um] 500 # of pump photons / pulse 1.34E+11Pumped beam width (time axis) [mm] 0.01 Transmitted pulse energy [mJ] 1.78E-05Pumped beam height (wavelength axis) [mm] 0.01 Absorbed pulse energy [mJ] 8.22E-05Pumped beam height restriction factor (for measuring a restricted wavelength range with increased pump laser fluence) [%] 100.00% Transmittance 17.78%

Beam area [mm²] 0.0001 Absorbance 82.22%Solute number in "Solutes" Worksheet 4 # of absorbed pump photons 1.11E+11Solute concentration [mol / L] 0.030 Pumped beam volume [mm^3] 0.00005Solute name Ni(CO)4 Concentration of exited molecules [mol / L] 3.67E-03Molar absorption coefficient [L / (mol cm)] 500 Concentration of unexcited molecules [mol / L] 2.63E-02Pump wavelength [nm] 267 Excitation fraction [%] 12.23%Pump pulse energy [mJ] 1.E-04Pump repetition rate [kHz] 1000Average laser power [W] 100Pump pulse fluence [mJ / cm²] 100.0Pump pulselength [fs] 100Pump pulse intensity [W / cm²] 1.0E+12

Solvent parametersX-ray transmission by solvent [%] 45.8% X-ray transmission by solvent [%] 45.83%

X-ray absorbance by excited molecules [%] 0.35%

X-ray absorbance by unexcited molecules [%] 2.50%

Edge type Ni-K Total x-ray absorbance due to solute molecules [%] 2.85%Post-edge x-ray mass absorption coefficient [cm² / g] 328.6 Total x-ray transmittance due to solute molecules [%] 97.15%Pre-edge x-ray mass absorption coefficient [cm² / g] 44.24 Transmission modulation due to exited molecules 0.35%Molar mass of x-ray absorbing solute atom [g / mol] 58.693 Total x-ray transmittance due to solute and solvent [%] 44.52%EXAFS modulation depth [%] 5.00% Required accuracy of measurement 8.72E-06Accuracy of measurement for excited solutes [%] 5.00% Min. S/N of x-ray measurement 114663.90X-ray fluorescence efficiency [%] 30.00% Min. required # of x-ray ph. on sample / wave-time step 5.91E+10

Min. required # of x-ray ph. on sample / (all times full spectral range) 5.91E+15

Total data acquisition time (all times 1000eV) [s] 16846.479

Detection efficiency for transmission detection [%] 50.00% Total data acquisition time (all times 1000eV) [min] 280.77

Detection efficiency for fluorescence detection [%] 10.00% Number of wave-channels measured simultaneously for full spectral range 1

# of x-ray photons on sample [1 / eV s] 7.65E+11 Number of time-channels measured simultaneously 1

Desired spectral resolution (i.e. wave step) [eV] 1 Total data acquisition time [h : m : s] 4:40:46

Numer of desired time-steps 100Spectral range over which the measurements are done [eV] 1000

X-ray spectrometer parameters

Solute parameters

Liquid beam parameters Results for sample excitation

Results for transmission detection

Acknowledgments:

Dr. Christian ReichDr. Chris LaperleDr. Taewoo LeeDr. Yan JiangXiaodi LiBrian AhrJoshua LessingEmma WelchMargaret GrantFrank Benesch

Dr. Claude BailatDr. Guohua CaoProf. Gerald Diebold Theron HamiltonDr. Philip Wintermeyer, M.D., Dr. Stephan Gehring, M.D.,

Liver Research Center, Brown Medical SchoolProf. Jack R. Wands, M.D., Liver Research Center, Brown Medical School,

Rhode Island Hospital