Structure and dynamics of nanoparticles in intense short … · 2015. 8. 5. · T. Gorkhover et...
Transcript of Structure and dynamics of nanoparticles in intense short … · 2015. 8. 5. · T. Gorkhover et...
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Structure and dynamics of nanoparticles in intense short wavelength light pulses
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Nanoparticles and clusters: scsscienes Issues and Questions
Clusters and nanocrystals are new materials
Size dependent properties• catalytic activity• magnetic properties • photochemical processes• light induced dynamics• geometry and shape
Size dependent colour
Novel pigments in tv-screens
Courtsey: H. Weller, Universität Hamburg
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Atoms / clusters in intense x-ray pulses
What are the differences?
absorption into continuum states
ionization inner ionization: electron removal from a cluster atom
outer ionization: electron removal from the cluster
Plasma formation
Atom Cluster
Last, Jortner, Phys. Rev. A, 62, 013201(2000)
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Properties of clusters / Driving questions
• Shape and structure of individual particles
– Regular shape, non-equilibrium structures ?
• Light induced dynamics– ion motion, electron motion– collective motion, plasma dynamics?– Phase transitions, melting, surface melting
W.Zhu et al, JACS 2013 135 (45), 16833
Curtesy of T. Fennel
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Cluster: Nanolab for laser-matter-interaction
„Three step model“
Experiments Wabnitz Nature 420, 482 (2002) , Laarmann , PRL 92, 143401, PRL 95, 063402 (2005), Bostedt PRL 100, 133401
Theory R. Santra, PRL 91, 233401 (2003), Siedschlag, Rost, PRL 93, 43402 (2004), Ziaja, Phys. Rev. Lett. 102, 205002 (2009)..
Rare gas cluster : simple structure, detailed studies with IR light
Photon energy, size, power densityArbeiter, Fennel, New J. Phys. 13
053022Time scales ?
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Nanoplasma formation
What is a nanoplasma?
Questions:
• internal structure • particle surface / expansion• electron-ion recombination• electron and ion dynamics, consequences for imaging?
r
.
Electrons
Ions
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Outline
• How we got started: initial experiments at TTF-FEL
• Nanoplasma formation – Ar clusters, autoionization of He clusters
• Imaging with soft X-rays– Single clusters, spatial evolution of plasma, shape of
metal clusters, in flight holography
• Time resolved studies – IR –X-ray Pump-probe Xe clusters
• New opportunities
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� size and shape of the clusters
� electronic configuration during interaction
� change of refractive index
� time scale: femtoseconds, during pulse
Ion and electron spectroscopy
� excite cluster with a pump pulse (NIR/XUV)
� probe explosion with a delayed XUV pulse
� time scale: resolve full range from sub-ps to ns
Pump-probe techniques
Soft x-ray scattering
� ionisation and
recombination
� kinetic energies,
expansion process
� time scale: fs up to
hundreds of ps after
the pulse
Complementary methods looking
into different timescales!
Method:Simultaneous imaging and spectroscopy
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Setup: Simultaneous imaging and ion spectroscopy:Single cluster intensity distribution: no averaging
13.5 nm
� clusters with R= 30 nm to >1 µm
� hν = 20 -1500 eV,
� 100 fs pulses, up to 1016 W/cm²
Single cluster single shotwell defined size and power density !
T. Gorkhover et al., Phys. Rev. Lett. 108, 245005 (2 012)C. Bostedt et al., J. Phys. B 43, 194011 (2010)
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200 400 600 800
Xe+
inte
nsity
time of flight [ns]
atom
67
Xe3+
8
Xe++
N~2-20
5
4+
N~80
4 23876 5 1
N~30000
• multiply charged ions from clusters, keV energy
• singly charged atoms
• detailed theoretical workto explain the enhancedabsorption
plasmabsorption (IB)ionisation contiuum lowering
1*1013 W/cm 2
H. Wabnitz et al, Nature 420, 482(2002 )
First results from the TTF -FEL at DESY (98 nm):Ion spectra of Xenon atoms and clusters
Ephot = 12.8 eVIpXe = 12.1 eV
N~ 90000
R. Santra, Ch. H. Green PRL 91, 233401 (2003),
C. Siedschlag, J. M. Rost , PRL 93, 43402 (2004)
B. Ziaja et. al PRL 102, 205002 (2009).
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Cluster ionisation and nanoplasma formation: Electron spectra of Ar clusters :
First electron
C. Bostedt et al. Phys. Rev. Letters 100, 133401 (2008)
sequential emission of electrons
only a small percentage of generatedphotoelectrons can leave the cluster
→ nanoplasma
- experiment....theory
Ar 150 clusters, 38 eV, a few 10 11 ~ 1014 W/cm2
Theory T. Fennel
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Direct photo emission42.8 eV (2x 21.4 eV)
ICD, 1s → 2p, 21.4 eV
Collective autoionisation
Y. Ovcharenko et al. PRL 112, 073401 (2014)
FERMI
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ICD type Autoionisation
• With intense light sources, multiple atoms in the cluster can be excited, 2p> 3s
• ICD between neighboring atoms leads to ionization of one of the atoms• Ionization rate through ICD sequential one photon absorption (linear process) >> 2 photon ionization (nonlinear)
Proposed for Ne clusters
A. Kuleff et. al.
Phys. Rev. Lett. 105, 043004 (2010 )
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• A new type of nanoplasma is formed• Many excited atoms are involved at the same time
Different autoionisation processes
Inelastic collision betweenelectrons and excited atoms
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Collective autoionization extremely efficient
• electron yield linear at ‘low‘ power density
• saturation at high powerdensity
• much more efficient thandirect photoemission at least two photon process
A. LaForge et al. Scientific Reports 4, 3621 (2014)
Y. Ovcharenko et al. PRL 112, 073401 (2014)
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Transition from ICD type to collective autoionizatio n
He 1s > 2p, collective autoionisation, network, plasma
Time scalesub fs?
ICD,two atomsNext to eachother, isolated
Y. Ovcharenko, M. Mudrich, A. LaForge,et al. in preparation
He cluster N= 50000
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Morphology of large xenon clusters
R= 30-50 nm
R= 150- 300 nm
R= 600nm
R= 1µm
?
� Direct imaging of growth by coagulation� Non-spherical shapes freeze out (“hailstones”)
Growth by coagulation
Experimental pattern 2D-projection 2D-Fourier transformation
D.Rupp et. al, J. Pys.B 43,194011(2010).JCP 141, 044306 (2014)
sph
eri
cals
twin
s/tr
iple
s ha
ilston
es
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Focal density distributionHit in focus
Hit in side
Hit in wing
max
min
Xe1+Xe2+
Xe5+
R=400nm
Single cluster intensity distribution: no averaging
1014 W/cm2
5x 1012 W/cm2
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Single cluster ion spectra: Signatures of strong recombination
electron spill out
partially
screened
surface
quasi-neutral
nanoplasma
surface
explodescore
recombines
Very sharp lines; narrow kinetic energy distribution
-homogeneous
hydrodynamic
expansion
D. Rupp
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Single cluster scattering patterns• Exposure power density (Intensity at position of the cluster)
• Ultrafast electronic changesduring the 100 fs light pulse
400 nm radius
Scattering angle
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•R
•d
•R From bottom to top:Weakly absorbing outer shellIncreasing thickness 25-50nmDecreasing real part of the refractive
index
•d
Nanoplama-shell with different refractive index
D. Rupp PhD thesis
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Time resolved imaging of exploding clusters
IR pump + FEL probe pulse (LCLS),
CAMP
Scattering sensitive to both, changes in electronic and geometric structure
L. Strüder et al. Nucl. Instr. Meth. A 610, 483 (2010)
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cluster source
FEL
Experimental setup in CAMP
+
-
MCP
ions
ion spectroscopyIR
λ = 0.8 nmE = 1.5 mJt = 70 fsup to 10 17 W/cm2
λ = 800 nmE = 1.5 mJt = 70 fsup to 10 15 W/cm2
X-ray only: T. Gorkhover et al., Phys. Rev. Lett. 108 , 245005 (2012)S. Schorb, T. Gorkhover, et al., Appl. Phys. Lett. 100, 121107 (2012)
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500 fs
Delay dependent X-ray diffraction
up to 5 ps up to 500 fs
T.Gorkhover, PhD. thesis,Xe clusters 20 nm radiusX-ray pulse 1.5 mJ, 1.5 nm
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Comparison with simulation
250 fs
500 fs
0 fs
100 fs
T. Gorkhover et al., Nature photonics, under review
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New imaging approaches
Holography: overcoming the phase problem
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„In-flight“ holography
High resolution imaging of single gas phase nanoparticles
M. M. Seibert et al., Nature 470, 78 (2011)Eisebitt,S., et al., Nature 432, 885 (2004)
X-ray Fourier holography Single nanoparticle imaging
+
?????
Geilhufe,J. et al., Nature Communications 5, 3008 (2014)
Tais Gorkhover, C. Bostedt et al
T. Gorkhover
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reference
measured
Inverse FFTdiffraction pattern
X-rays
sample
X-ray Fourier holography
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reference
Inverse FFTdiffraction pattern
X-rays
sample
„In-flight“ X-ray Fourier holography
Gas phase single particle holography: instead of a fixed mask, use randomly injected Xe clusters
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FEL,1nm, 3mJ, 80 fs
scatteringpattern
Experimental setup in LAMP
Xe cluster source
bio injector (Uppsala) pnCCD
collaboration with J. Hajdu, H. Chapman teams
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Holograms of twin particles
diffraction pattern inverse 2D FFTex
perim
ent
sim
ulat
ion
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Imaging of metal clusters
• Regular shape, non-equilibrium structures ?
• Nanoplasma effects ?
W.Zhu et al, JACS 2013 135 (45), 16833
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Morphology of large gas-phase silver clusters
I. Barke, et. al, Nature
Communications 7187 (2015)
collaboration with Rostock 7/15
� Diversity of (metastable) structural
motives
� 3D information in a single-shot image
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Key to 3D sensitivity: large angle scattering
small angle large angle
Born 2D projected
Born 3D
Born 3D
+ effective absorption
(used for quick identification)
full solution of continuum
Maxwell Eq. via FDTD
(used for refinement)
trunc. oct., r=120, λ=13.5nm
(single shot tomography)
I. Barke et. al,
Nature communications 7187 (2015)
Wide angle scattering, no inversion symmetry: → 3D Structure
I.Barke
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Outlook
Novel approach for time resolved imaging
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Two images from a single clusters at different time s
D. Rupp, TU-Berlin
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Collective oscillations/dynamics in nanoparticles,surface melting
Damping?
Size selected
Vis /XUV pump probe
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Summary and outlook: Clusters in intense X -ray pulses
� Scattering pattern: ultrafast
electronic changes due to plasma
generation
� electron and ion spectra: nanoplasma
formation explosion of a thin surface, strong
recombination in the quasi-neutral plasma
� Time-resolved: image surface melting after
tens of ps, debris after ps-ns
Imaging structure and dynamics of clusters :A lot of exciting physics ahead of us!
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Experiments at FERMI / LDM collaboration: He cluster
Carlo Callegari, Aron Laforge, Y. Ovcharenko, Paolo Piseri, Victor Layamayev, RavaelKatzky, Paola Finetti, Oksana Plekan, Marcello Coreno, Robert Richter, Marcel Drabbels, Kevin Prince, Thomas Möller, Frank Stienkemeier , from ERMI FlavioCapotondi, Gerardo D’Auria, Giuseppe Penco,Emiliano Principi, Marco Zangrando.
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Acknowledgement
TU Berlin:D. Rupp,
L. Flückiger
T. Gorkhover
B. Langbehn
M. Müller
E. Ovcharenko
M. Sauppe
A. Ulmer
M. Adolph,
M.Krikunova
SLAC
C. Bostedt,
T. Gorkhover
S. Schorb
TU Berlin
CAMP Team
B. Erk, S. Epp
L. Foucar,
A. Rudenko,
R. Hartmann,
D. Rolles,
I. Schlichting, L. Strüder, J. Ullrich
Funding by BMBF and DFGForschungsschwerpunkt FLASH/FEL
FLASH, LCLS, FERMI TeamsCFEL, H. Chapman
Cooperation with theory
T. Fennel (Rostock)
U. Saalman, J. Rost (Dresden)
B. Ziaja, R. Santra (CFEL/DESY)
I. Barke, K.H. Meiwes-Broer,
J. Tiggesbäumker, T. Laarmann,
J, Hajdu M. Handke, F. Maia, M. Seibert
LDM Team
C. Calagari, K. Prince, O. Plekan,
P. Finetti, F. Stienkemeier