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Aug 17, 2022 559 likes •1.09k views

Intro to SR & FEL spectroscopy; interaction between radiation & matter (2) Maria Novella Piancastelli Sorbonne Universits, UPMC Univ Paris 06, CNRS, Laboratoire de Chimie Physique-Matire et Rayonnement, France Department of Physics

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Intro to SR & FEL spectroscopy; interaction between radiation & matter (2)

Maria Novella Piancastelli Sorbonne Universités, UPMC Univ Paris 06, CNRS, Laboratoire de Chimie Physique-Matière et Rayonnement, France Department of Physics and Astronomy, Uppsala University, SE-75120 Uppsala, Sweden

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The Physics of Free Electron Lasers By Evgeny Saldin, Evgeny A. Schneidmiller, M.V. Yurkov Springer, 2000 Classical Theory of Free-Electron Lasers By Eric B. Szarmes Morgan & Claypool Publishers, 2014 Insertion Devices for Synchrotron Radiation and Free Electron Laser By F. Ciocci , G. Dattoli, A. Torre, A. Renieri World Scientific, 2000

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FLASH

DESY, Hamburg, Germany

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Pump-probe experiments

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  • Y. H. Jiang et al., PRL 105, 263002 (2010)
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Mean isomerization time: 52 ± 15 fs

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LCLS

SLAC, Stanford, CA, USA

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L.Young et al., Nature 466, 56 (2010)

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B.Erk et al., Science 345, 288 (2014)

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L.S.Cederbaum et al, J.Chem.Phys. 85, (1986) 6513

DCH Single-Site (SS) DCH Two-Site (TS)

Substantially enhanced chemical sensitivity

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Double (multiple) ionisation energy (DIP, …)

EB1 + EB2 (+ …) = h - Ekin1 - Ekin2 (- …)

Single Photon – Multiple Ionisation

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Time-Of-Flight Magnetic Bottle Multi-Electron Spectrometer

J.H.D. Eland et al., Phys. Rev. Lett. 90, 053003 (2003)

฀ t  D EKin

Pulsed light source: He-lamp, SR, fs-laser system, FEL

e-

e-

e-

e- “4π” correlation device

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P.Lablanquie, F.Penent,J.Palaudoux, L.Andric, P.Selles, S.Carniato, K.Buĉar, M.Žitnik, M. Huttula, J.H.D.Eland, E.Shigemasa, K.Soejima, Y.Hikosaka, I.H.Suzuki, M.Nakano and K.Ito, PRL 106, 063003 (2011)

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J.H.D.Eland, M.Tashiro, P.Linusson, M.Ehara, K.Ueda and R. Feifel, PRL 105, 213005 (2010)

NH3 CH4

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  • P. Lablanquie,T. P. Grozdanov, M. Žitnik, S. Carniato, P. Selles, L. Andric, J. Palaudoux, F. Penent, H. Iwayama,
  • E. Shigemasa, Y. Hikosaka, K. Soejima, M. Nakano, I. H. Suzuki and K. Ito, PRL 107, 193004 (011)

C2H2

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Few Photon – Multiple Ionisation

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DCH measurements: CO

  • N. Berrah, ……M.N.Piancastelli et al., PNAS

108, 16912 (2011) Challenge remains: TS-DCH  CVV/VVVV Auger and Auger from other channels overlap

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80 90 100 110 120 500 1000 1500

80 90 100 110 120 2000 4000 Foc Unfoc Foc-unfoc Kinetic energy (eV) Counts / eV

N2O (N 1s)

PAP tsDCH Nt

  • 1Nc
  • 1

tsDCH Nc

  • 1Nt
  • 1

(b)

SCH Nc

  • 1

SCH Nt

  • 1

Kinetic energy (eV) 80 100 120 140 160 180 200 200 400 600

80 120 160 200 1500 3000 Foc Unfoc Foc-unfoc Kinetic energy (eV) Counts / eV

ssDCH N

  • 2

tsDCH N

  • 1N
  • 1

PAP

N2 (a)

SCH N

  • 1

Counts / eV Kinetic energy (eV) 80 90 100 110 120 500 1000 1500

80 90 100 110 120 2000 4000 Foc Unfoc Foc-unfoc Kinetic energy (eV) Counts / eV

N2O (N 1s)

PAP tsDCH Nt

  • 1Nc
  • 1

tsDCH Nc

  • 1Nt
  • 1

(b)

SCH Nc

  • 1

SCH Nt

  • 1

Kinetic energy (eV) 80 100 120 140 160 180 200 200 400 600

80 120 160 200 1500 3000 Foc Unfoc Foc-unfoc Kinetic energy (eV) Counts / eV

ssDCH N

  • 2

tsDCH N

  • 1N
  • 1

PAP

N2 (a)

SCH N

  • 1

Counts / eV Kinetic energy (eV)

  • P. Salén, P. van der Meulen, H.T. Schmidt, R.D. Thomas, M. Larsson, R. Feifel, M.N. Piancastelli, L.Fang, B.

Murphy, T. Osipov, N. Berrah, E. Kukk, K. Ueda, J.D. Bozek, C. Bostedt, S. Wada, R. Richter, V. Feyer and K.C. Prince, PRL 108, 153003 (2012)

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High performances of the GALAXIES beam line: high flux and high resolution Single-channel measurements Immediate identification of states of the type:

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R.Püttner, G. Goldsztejn, D. Céolin, J.-P.Rueff, T. Moreno, R. K. Kushawaha, T. Marchenko,

  • R. Guillemin, L.Journel, D. W. Lindle, M.N. Piancastelli and M. Simon, Phys. Rev. Lett. 114, 093001 (2015)
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Double core hole (DCH) in Neon

Ground state : 1s22s22p6

1s 2s 2p E(eV) hν

Intermediate state : 1s02s22p6 First Auger decay : 1s12s22p4

870.2 eV

Second Auger decay : 1s22s22p2 Ne Ne2+ Ne3+ Ne4+

  • K-2 in Neon.
  • Double Ionization

Potential = 1863 eV.

  • The two photoelectrons

share the energy

  • First Auger electron =

Hypersatellite.

  • Second Auger electron

= satellite. Ground state : 1s22s22p6

1s 2s 2p E(eV) hν

Intermediate state : 1s02s22p6nl1 Spectator Auger decay : 1s12s22p4nl1

870.2 eV

Participator Auger decay : 1s22s22p5 Ne Ne+ Ne2+ Ne2+

  • r
  • K-2V in Neon.
  • Photoelectrons

well separated and easy to identify.

  • Different type of

decays at different energies.

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Photon energy dependence of DCH

hν = 2300 eV hν = 3000 eV hν = 4000 eV hν = 7000 eV

1s-23s 1s-23p 1s-24s 1s-24p 1s-25s

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The hypersatellite spectra

  • K-1 ≈ 1000 times more intense than K-2
  • Thanks to much better resolution we were able to identify K-1 satellites

Southworth et al. PRA 67, 062712 (2003) Svensson et al. J. Electron Spectrosc. Relat. Phenom. 47, 327 (1988)

Southworth et al. 2003 HAXPES 2014 K-1 Rydberg serie

820 840 860 880

K-2 K-2V

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Aerial view Beam transport and beamlines

FERMI

Elettra, Trieste, Italy

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FERMI

Variable polarization Negligible photon energy jitter Negligible time jitter

First seeded FEL

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Low Density Matter (LDM)

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Probing keto-enol tautomerism in acetylacetone

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Keto form Enol form

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  • J. Dyke, N. Jonathan, E. Lee and A. Morris
  • J. Chem. Soc., Faraday Trans. 2 72, (1976) 1385

CH3

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