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Photoabsorption Spectroscopy & Imaging with Laser-Plasma X-VUV Continua (Atomic Photoionization with LPP). John T. Costello National Centre for Plasma Science & Technology (NCPST) and School of Physical Sciences, Dublin City University & [email protected] .ie.

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Photoabsorption Spectroscopy & Imaging with Laser-Plasma X-VUV Continua(Atomic Photoionization with LPP)

John T. Costello

National Centre for Plasma Science & Technology (NCPST) and School of Physical Sciences, Dublin City University & [email protected]

Interchannel interaction in photoionization of atoms and photodissociation of molecules, Riezlern, Austria July 12, 2005


Outline of Talk

Part I - Laser Plasma \'Line-Free\' Continuum Sources

  • Origin, Brief History & Update

Part II - Dual Laser Plasma Experiments - Some Case Studies

  • X-VUV Photoabsorption Spectroscopy
  • VUV (Monochromatic) Photoabsorption Imaging

Part III - Next Steps Atomic Photoionization

  • Photoionization of Atoms in Intense Laser Fields - ‘Pump Probe’ Experiments with X-VUV FELs

Collaborators and Contributors

Picosecond X-VUV Continuum Sources

RAL - E Turcu & W Shaikh

QUB - C Lewis, R O\'Rourke and A MacPhee

DCU - O Meighan and C McGuinness

EUV Absorption Spectroscopy

Rostov - P Demekhin, B Lagutin and V Sukhorukov

DCU - P Yeates, A Neogi, C Banahan, D Kilbane, P van Kampen and

E Kennedy

VUV Photoabsorption Imaging Facility - VPIF

Padua - P Nicolosi and L Poletto

DCU - J Hirsch, K Kavanagh, E Kennedy & H de Luna

DESY ‘Pump Probe’ Project

Hasylab- J Feldhaus, E Ploenjes, K Tiedke, S Dusterer & R Treusch

Orsay- Michael Meyer, Denis Cubyannes & Patrick O\'Keefe,

DCU- E Kennedy, P Yeates, J Dardis and P Orr (QUB)

\'Colliding Plasmas\'

DCU - K Kavanagh, H de Luna, J Dardis and M Stapleton


Laser-Plasma/Atomic Phys-NCPST

The LPP node comprises 6 laboratory areas focussed on

pulsed laser matter interactions (spectroscopy/ imaging)

Academic Staff (4):John T. Costello, Eugene T. Kennedy (now VPR),

Jean-Paul Mosnier and Paul van Kampen (on sabbatical)

Post Doctoral Fesearchers (5):

Dr. Deirdre Kilbane (PVK/JC)

Dr. Hugo de Luna (JC)

Dr. Mark Stapleton (JC)

Dr. Jean-Rene Duclere (JPM)

Dr. Pat Yeates (ETK)

Current PhD students (6):

Caroline Banahan (PVK/JC)

Kevin Kavanangh (JC)

Adrian Murphy (JC)

John Dardis (JC)

Rick O\'Hare (JPM),

Eoin O’Leary (ETK)

Visiting PhD students:Domenico Doria (Lecce) and Philip Orr (QUB)

Funded by:

SFI - Frontiers and Investigator

HEA - PRTLI and North-South

IRCSET - Embark & BRGS

Enterprise Ireland - BRGS

EU - Marie Curie and RTD


Laser Plasma Source Parameter Range

Vacuum or

Background Gas





Laser Pulse 1064 nm/

0.01 - 1 J/ 5ps - 10 ns


Spot Size = 50 mm (typ.)

F: 1011 - 1014

Te : 10 - 1000 eV

Ne: 1021 cm-3

Vexpansion 106 cm.s-1

Emitted -





IR - X-ray Radiation


Intense Laser Plasma Interaction

S Elizer, “The Interaction of High Power Lasers with Plasmas”,

IOP Series in Plasma Physics (2002)


Laser Produced ‘Rare Earth’ Continua -

Physical Origin, History & Update

laser plasma rare earth continua
Laser Plasma Rare Earth Continua

P K Carroll et al., Opt.Lett 2, 72 (1978)


What is the Origin of the Continuum ?

Continua emitted from laser produced

rare-earth (and neighbouring elements) plasmas are predominantly free-bound in origin and overlaid by Unresolved Trans- ition Arrays (UTA*) containing many millions of lines which share the available oscillator strength.

* J. Bauche, C. Bauche-Arnoult & M. Kalpisch, Phys. Scr 37, 659 (1988)


But why is no line emission observed ?

  • Line emission is due to complex 4d-4f arrays in (typically) 7 - 20 times ionized atoms
  • 4dn5sq5ps4fm 4dn-15sr5pt 4fm+1, q+s = r+t
  • Furthermore 4f/5p and 4f/5s level crossing gives rise to overlapping bands of low lying configurations, most of which are populated in the ~100 eV plasma
  • Result - the summed oscillator strength for each 4d - 4f (XUV) and 5p - 5d (VUV) array is spread out over a supercomplex of transitions producing bands of unresolved pseudo continua (so called ‘UTA’) superimposed on the background continuum
  • Even expectedly strong lines from simple 4f - 4f arrays are washed out by plasma opacity

There are up to 0.5 million allowed transitions in

LS couplingover the ~10 eV bandwidth of a UTA

In fact this is a lower bound since many additional LS forbidden transitions are ‘switched on’ by the breakdown in LS coupling here - G O’Sullivan et al., J.Phys.B 32, 1893 (1999)


Brief History/ Highlights of Laser Plasma Rare-Earth’ Continua -1990

First report of line free continua - P K Carroll et al., Opt.Lett 2, 72 (1978)

First full study/ applications - P K Carroll et al., Appl.Opt. 19, 1454 (1980)

VUV Radiometric Transfer Standard - G O’Sullivan et al., Opt.Lett 7, 31 (1982)

Absolute Calibration with Synchrotron - J Fischer et al, Appl.Opt. 23, 4252 (1984)

Photoelectron Spectroscopy - Ch. Heckenkamp et al., J.Phys.D 14, L203 (1981)

First Study for XUV lithography - D J Nagel et al., Appl.Opt. 19, 1454 (1980)

7. XUV Reflectometer - S Nakayama et al., Physica Scripta 41, 754 (1990)

8. First Industrial Application - DuPont - Insulator Band Structure

VUV Reflectance Spectroscopy - R H French, Physica.Scripta 41, 404 (1990) -

System subsequently made available commercially from ARC

For a review of the early years (1,2) and more recent work (3)

including applications in photoabsorption spectroscopy see :

1. J T Costello et al., Physica Scripta T34, 77 (1991)

2. P Nicolosi et al., J.Phys.IV 1, 89 (1991)

3. E Kennedy et al., Radiat. Phys. Chem 70, 291 (2004)


Recent Developments in LP Continua I


O Meighan et al., Appl.Phys.Lett 70, 1497 (1997)

O Meighan et al., J.Phys.B:AMOP 33, 1159 (2000)


Summary - LP Continuum Light Sources

Table-top continuum light source now well established

Covers Deep-UV to soft X-ray spectral range

Pulse duration can be < 100 ps !

Continuum flux ~ 1014 photons/pulse/sr/nm (0.8J/10ns)

Low cost laboratory source - needs greater awareness

6. Recent work on (100 ps) + (6ns) Pre-plasma source -

we already see a flux gain of up to X4 with Cu-

A Murphy et al., Proc SPIE, 4876, 1202 (2003)

Problem of plasma debris for work in clean environments - proposals to solve, Michette, O’Sullivan, Attwood,…


Part II- Dual Laser Plasma

Photoabsorption Experiments


Part II - Section A

Photoabsorption Spectroscopy of Ions


Photoionization of Atomic Ions

Still a lot of work to be done here-

Nice review by John West in:

J.Phys.B:AMOP 34, R45 (2001)

Covers DLP Experiments &

Merged Synchrotron + Ion Beams


Dual Laser Plasma Principle






No tuning required

No vapour required

Backlighting Plasma Io

Both Plasmas I = Ioe-snL

Relative Absorption Cross Section

sNL =Ln(Io/I)

Isonuclear Sequences

Isoelectronic Sequences

Dx, DT, I(W/cm2)

 Species choice


XUV DLP Specifications

  • Time resolution:~20 ns (LP Continuum duration)
  • Inter-plasma delay range:0 - 10 sec
  • Delay time jitter:± 1ns
  • Monochromator:McPherson™ 2.2m GI
  • X-VUV photon energy: 25 - 170 eV
  • Resolving power:~2000 @25 eV (20mm slits)
  • ~1200 @ 170 eV
  • Detector:Galileo CEMA with PDA readout
  • Spatial resolution:~250 m (H) x 250 m (V)

Some sample DLP case studies

Kr-like ions

Mn ions



Have published upwards of 100 papers on DLP photoabsorption experiments on selected atoms and ions from all rows of the periodic table.

Motivation - almost always exploration of some \'quirk\' of the photoionization process in a many electron atom !

Kr-like ions - Rb+, Sr2+, Y3+


Why Specifically Kr-like Ions ?

Electronic Configuration


1. Prototypical high-Z closed shell atom - beyond simple Fano theory

2. 30+ years of research in both single and multiphoton ionization

3. Will the photoionization dynamics (q/G) change (a little or a lot ?)

4. How will current many-electron photoionization theory stand up ?


XUV Photoabsorption along Isoelectronic (Kr-like) Sequence (Rostov/ DCU)

4s24p6 + hnVUV 4s4p6np + 4s64p4nln’l’  Kr+(4s24p5) + e’l

A Neogi et al., Phys.Rev.A 67, Art. No. 042707 (2003)

P Yeates et al., J. Phys. B: At. Mol. Opt. Phys. 37, 4663 (2004)


It\'s a plasma with an ionization balance-

how do we know that we have Y3+ say ?

4p - nd, Epstein and Reader , J. Opt. Soc. Am 72, 476 (1982)

4s - 5p assigned using Clark et al., J. Opt. Soc. Am. B 3, 371 (1986)


What about

cross sections ?


\'Mirroring Resonances\'

r2q2 0  complete cancellation - no resonances


An update from Aarhus !

Bizau, West & Kilbane (DCU)


Kr-like ions - Summary

1. It is clear that the ‘Fano’ profile parameters for the main 4s – np

resonances in each spectrum are very sensitive to degree of ionization and

that complex doubly excited resonances persist (at least in the early members

of the isoelectronic sequence).

2. Computed cross sections show good agreement with measured spectra.

3. Rescaling the Coulomb interaction is needed to better fit the 4s-5p

resonance in Sr2+

4. We observe that the complex doubly excited resonances straddling the

first 4s-5p in Kr moves to higher photon energy blending with higher energy

4s-np (n>6) resonances and that the 4s-5p drops below the 4p threshold for Y3+

For Y3+ the resonance q values become quite large and the spectrum

consists mainly of almost symmetric absorption features

We see that a number of features are suppressed in Rb+ and Sr2+ since

they are built from exactly (or almost exactly) cancelling \'mirroring resonances\'


DLP XUV Photoabsorption along isonuclear

sequences - Mn2+ (and Mn3+) Ions

Mn+, 3p63d54s + hn  3p5(3d64s + 3d54s2)

Mn2+, 3p63d5 + hn  3p5(3d6 + 3d54s)

\'duplicity of the 3d orbital\' - "valence-like by energy but inner shell-like by radial distribution" (Dolmatov, JPB 29, L687 1996)


3p-subshell photoabsorption - Mn2+

Overall we see a good match with

Dolmatov at least at the low energy

side of the main resonance

But why does the experimental

trace fall off much more quickly

than the theory -

Excitation from metastable states ?


Metastables and their effect on 3p-subshell

photoabsorption of iron group ions - Mn3+

Mn3+, 3p63d4 + hn  3p5(3d5 + 3d44s)





What do simple Cowan code calculations give ?

First Step

Compute \'cross sections\' for photoabsorption from ground and low-lying terms of Mn3+ (3d4) - 5D, 3P, 3F, 3G, and 3H


Next Step

To \'reproduce\' the experimental plasma spectrum, take a weighted sum over each such cross section


Mn ions - Summary

Clear that we are going to have problems with excited state absorption

since we have a hot sample. In fact the plasma temperature at will vary from

~10 eV at 20 ns to 2 eV at 150 ns and hence we will have significant

populations of low lying 3dn and 3dn-14s states

3. Same is also true of the ion beams used in the synchtotron experiments

4. So we need a combined atomic physics and plasma physics approach

-some codes available (HULLAC) but complex and expensive

5. Contrast with Kr-like ions - closed shell - stable - ions tend to converge

and stay on this favoured configuration - nice to work with

Same problem will occur in 4d, 5d, 4f and 5f metals

However, electronic structure of Mn2+ and Mn3+ ions important in

manganites (recent Nature papers), biology (DNA),.....


Part II - Section B (short)

VUV Photoabsorption Imaging

Collaboration between DCU & Univ. Padua


VUV Absorption Imaging Principle

Hirsch et al, J.Appl.Phys. 88, 4953 (2000) - QUB/DCU Collaboration






Pass a collimated VUV beam through the plasma sample

and measure the spatial distribution of the absorption. Convert

to \'Equivalent Width\' images and extract column density (NL)

maps - see Rev.Sci. Instrum. 74, 2992 (2003) for details


VUV Photoaborption Imaging

  • Time resolution: ~10 ns (200 ps - EKSPLA)
  • Spectral range:10 - 35 eV (120 - 35 nm)
  • VUV bandwidth:0.025 [email protected] eV (50mm slits)
  • Spatial resolution:~120 m (H) x 150 m (V)

J Hirsch, E Kennedy, J T Costello, L Poletto & P Nicolosi

Rev.Sci. Instrum. 74, 2992 (2003)


Advantages of using a VUV beam

1. VUV light can probe the higher (electron) density regimes not

accessible in visible absorption experiments

2. The refraction of the VUV beam in a plasma is reduced

compared to visible light with deviation angles scaling as l2

3. Image analysis is not complicated by interference patterns

since the VUVcontiuum source has a small coherence length

4. VUV light can be used to photoionize ions -

simplified equation of radiative transfer (no bound states).

5. Fluorescence to electron emission branching ratio for inner

shell transitions can be 10-4 or even smaller => almost all photons

are converted to electrons


VUV absorption Imaging- Ca+ - 33.2 eV

3p64s (2S) - 3p54s3d (2P)


Plume Expansion Profile -

Singly Charged Calcium & Barium Ions

Plume COG Position (cm)

Delay (ns)

Ca+ plasma plume velocity

experiment: 1.1 x 106 cms-1

simulation: 9 x 105 cms-1

Ba+ plasma plume velocity

experiment: 5.7 x 105 cms-1

simulation: 5.4 x 105 cms-1


Advantages of using a VUV beam

1. VUV light can probe the higher (electron) density regimes not

accessible in visible absorption experiments

2. The refraction of the VUV beam in a plasma is reduced

compared to visible light with deviation angles scaling as l2

3. Image analysis is not complicated by interference patterns

since the VUVcontiuum source has a small coherence length

4. VUV light can be used to photoionize ions -

simplified equation of radiative transfer (no bound states).

5. Fluorescence to electron emission branching ratio for inner

shell transitions can be 10-4 or even smaller => almost all photons

are converted to electrons


What do we extract from I and Io images ?








You can also extracts maps of column density,

e.g.,Singly Ionized Barium

Since we measure resonant photoionization, e.g.,

Ba+(5p66s 2S)+h Ba+*(5p56s6d2P)  Ba2+ (5p61S)+e-

h = 26.54 eV (46.7 nm) and

the ABSOLUTE VUV photoionization cross-section

for Ba+ has been measured:

Lyon et al., J.Phys.B 19, 4137 (1986)

We should be able to extract maps of column density -

\'NL\' = ∫n(l)dl


Maps of equivalent width of Ba+ using

the 5p-6d resonance at 26.55 eV (46.7 nm)


Convert from WE to NL

Compute WE for a range of NL and fit a function f(NL) to a plot of NL .vs. WE

Apply pixel by pixel




Result - Column Density [NL] Maps

100 ns

150 ns

(C) 200 ns

(D) 300 ns

(E) 400 ns

(F) 500 ns


VPIF - Summary

VPIF - Provides pulsed, collimated and tuneable VUV

beam for probing dynamic and static samples

Spectral (1000) & spatial (<100 mm) resolution and

divergence (< 0.2 mrad) all in excellent agreement

with ray tracing results

Extracted time and space resolved maps of

column density for various time delays

Measured plume velocity profiles compare quite well

with simple simulations based on adibatic expansion


Current & Future Applications

Space Resolved Thin Film VUV Transmission

and Reflectance Spectroscopy - PVK

‘Colliding-Plasma’ Plume Imaging

Non-Resonant Photoionization Imaging

VUV Projection Imaging ?

Photoion Spectroscopy of Ion Beams ?


Photoionization Mass Spectrometry

R Flesch et al., Rev.Sci.Instrum 71, 1319 (2000)

VUV Photoionizationof O2

Laser on

Laser off


‘Colliding Stars Model System\' -

\'Colliding Plasmas\'

NGC2346 -

Planetary Nebula

Distance - 2,000 light years

Extent ~ 0.4 light years

Result of the collision of two stars - believed that one became a red giant

and swallowed its partner in the binary system.

Credit: Hubble Wide Field & Planeary Camera - Massimo Stiavelli (NASA)

NGC 2346


Colliding Laser Plasma Generation

Laser Pulse Energy: 10 -150 mJ/ beam

Laser Pulse duration: 12 - 15 ns

Focal Spot Size: ~ 100 mm

Irradiance: 1010 - 1011


Ca - Emission Imaging @ 423 nm

Stagnation for angled target geometry

Tight point focus on each Ca face/ 120 mJ per beam


How about hetero-atomic collisions ?

- Li + Ca Plasmas

  • Should be able to track each plume species individually
  • so we could look for crossover at the stagnation layer










Hetero-atomic collisions-Li+Ca Plasmas

Ca -

420 nm

Ca+ -

390 nm

Li -

670 nm

Li+ -

548 nm

Delay = 300 ns & Gate time = 50 ns

3O wedge, ~ 10mm Plume - Plume Separation


\'Collisionality Parameter\'

Collisionality (z) will be determined by both the mean free path

(lii) and colliding plasma experimental scale length\' (L).

z = D/lii = D/Cstii = D.nii/Cs

Cs= Ion sound speed,nii = ion-ion collision frequency

Expect to strong stagnation for counter streaming plasmas

where the mfp is small in comparison to the ablation front

separation - Rambo and Denavit, Phys. Plasmas 1 4050 (1994)


What have we learned to date ?

Strong stagnation in table top colliding plasmas

due to large value of the collisionality parameter (z)

Degree of confinement/ hardness of the stagnation

layer can be controlled by designing the value of z

Stagnation layer becomes quite uniform after 100s ns

and so looks attractive for investigation as alternative

pulsed laser materials deposition source

For this reason it also looks a good bet for atomic

physics experiments using laser probing/excitation.....


Part III - Next steps in fundamental

photoionization studies ?

Atoms and Molecules in Laser Fields

1. Attosecond pulse generation/ HHG

2. Photoionization of ‘state prepared’ species

(a) Weak Optical + Weak X-VUV

(b) Intense Optical + Weak (Intense) X-VUV

3. Atoms, Molecules, Cluster & Ions in Intense Fields (Multiple-Photon and Optical Field/Tunnel-Ionization)


Free Electron Laser at

Hasylab, DESY, Hamburg

\'Laser-like\' radiation

in the VUV and EUV


Free electron radiation sources

Josef Feldhaus, DESY, Hamburg

Bending magnet, broad band

 NW x bending magnet

 NU2 x bending magnet


 NU2 x Ne x bending magnet

NU , NW = # magnetic periods

Ne = # electrons in a bunch


Schematic layout of a SASE FEL

LINAC Tunnel

Experimental Hall


Timetable EUV FEL - TTF2

February 2004: - complete linac vacuum

- install photon diagnostics in FEL tunnel

Mar.-July 2004: - injector commissioning

- completion of LINAC

Aug.-Dec. 2004: - LINAC and FEL commissioning with short bunch trains

- installation of first two FEL beamlines (~20 µm focus direct beam and high resolution PGM)

Jan.-March 2005: - commissioning of first FEL beamlines and gas ionisation monitor

- photon beam diagnostics

Spring 2005: - first user experiments


Femtosecond X-VUV + IR

Pump-Probe Facility,Hasylab, DESY



Pump-probe experiments in the gas phase (project: II-02-037-FEL)

M. Meyer et al, LIXAM, Orsay, France

Participating groups:

HASYLAB, Hamburg, Germany

J. Feldhaus, S. Dusterer, R. Treusch, Kai Tiedke, Elke Ploenjes

LIXAM, Orsay, France

M. Meyer, D. Cubannes

NCPST, Dublin City University, Ireland

J. T. Costello, Philip Orr (QUB), P Yeates


Two subsets of experiments


Direct photoionization in a non-resonant laser field


Resonant photoionization in a resonant laser field


Let\'s first look at II-A -

‘Direct photoionization\'

in a non-resonant laser field*

*Slides provided by Patrick O’Keefe and Michael Meyer,




Ar+ 3p5


Ar 3p6

Ponderomotive streaking of the ionization potential as a method for measuring pulse durations in the XUV domain with fs resolution

E.S. Toma, H.G. Muller, P.M. Paul, P. Berger, M. Cheret, P. Agostini,C. LeBlanc, G. Mullot, G. Cheriaux

Phys. Rev. A 62, Art. No. 061801 (2000)

presence of IR:

- shift of IP

- broadening of PES peaks

- sidebands

Test-experiments at LLC:M. Meyer, P. O’Keefe (LURE), A. L’Huillier (LLC)

fs-laser system: Ti:Saph. 800 nm, 50 fs, 1 kHz

VUV --> HHG, DT ≈ 30 fs, 1 kHz,

IR --> up to 0.5 mJ --> 1-10 TW/cm2

PES: magnetic bottle spectrometer

- high angular acceptance

- high energy resolution for Ekin < 10 eV


Cross correlation experiments using high order harmonics
















Ekin (eV)



(laser) = 800nm

H11 = 17 eV

H13 = 20 eV

H15 = 23 eV




E = 15.8 eV


Ar+ 3p5


Ar 3p6


But also very interesting are:

Type IIB-Experiments-

\'Resonant photoionization\'

in an intense/resonant fields

=>Study intensity controlled autoionization !!


Proposed (approved) experiment at the FEL

Exp.:Two-photon double-resonant excitation

FEL : hn = 65.1 eV (tunable) Laser : l = 750 - 800 nm (tunable)

Coupling of He Doubly Excited States


2s2p 1P – 2s3d 1D

Intense Laser


20 fs (34 meV)

A. I. Magunov, I. Rotter and S. I. Strakhova

J. Phys. B32, 1489 (1999)

H. Bachau, Lambropoulos and Shakeshaft

PRA 34, 4785 (1986)


He 1s2


Bachau, Lambropoulos and Shakeshaft, PRA 34, 4785 (1986)

Laser on Resonance (d2 = 0)

& scan the XUV photon energy

1s2(1S) + hnXUV -

{2s2p (1P) + hnLaser

<=> 2s3d (1D)}


Could this be done with a

laser plasma X-VUV source

and a table top OPA ?



In principle YES

You just cross the sample with intense

laser (OPA) and weak XUV beams

Need wavelength selection and high (average)

X-VUV intensity

Count rate low -

~ 1 ion/laser shot for He with Volint ~ 10 -3 cm-3


But - the Ca+ 3p-subshell resonances have:

1. Cross sections up to 2500 MB .vs. < 0.1MB for He

2. Excitation widths up to 100 meV

3. A VUV excitation energy (31 eV)


Scheme- Ca+:

3p64s (2S) + hnXUV (33.2 eV) 

{3p53d4s (2P) + hnLaser (3 eV) <=> 3p53d5p (2D)}

Exploratory study in DCU -

Summer 2005


Photoionization Summary

Single VUV - X-ray photon photoionization (and concomitant

correlation) in atoms and ions is still a rich source of physics

Photoionization of atoms (much less so ions) in intense IR/VIS

laser fields is now well established also (MPI .vs. Tunnelling)

New things to so - Cross-over of the above two ?

Atoms in intense VUV/XUV (high frequency) fields -

first result - Nature 2002

Resonant/ non-resonant photoionization of atoms in intense

resonant/non-resonant laser fields

Why bother ?

Pushing limits - exploring new spaces - new science & technol.


Ideas that come to mind

at this workshop

FEL Opportunities

PIFS on weak resonances

PIFS on ion beams - Kr-like ions


Exploring Xe-like, 5s-subshell excitation

Table Top PIFS

PIFS with laser plasma source

Or with tuneable (upconverted) VUV