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Ultrafast dissociation of ammonia : Auger Doppler effect and redistribution of the internal energy

Travnikova, O. (author)
Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, CNRS, UMR 7614, F-75005 Paris, France.
Kukk, E. (author)
Univ Turku, Dept Phys & Astron, FI-20014 Turku, Finland.
Hosseini, F. (author)
Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, CNRS, UMR 7614, F-75005 Paris, France.;Synchrotron SOLEIL, F-91192 Gif Sur Yvette, France.
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Granroth, S. (author)
Univ Turku, Dept Phys & Astron, FI-20014 Turku, Finland.
Itälä, E. (author)
Univ Turku, Dept Phys & Astron, FI-20014 Turku, Finland.
Marchenko, T. (author)
Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, CNRS, UMR 7614, F-75005 Paris, France.
Guillemin, R. (author)
Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, CNRS, UMR 7614, F-75005 Paris, France.
Ismail, I. (author)
Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, CNRS, UMR 7614, F-75005 Paris, France.
Moussaoui, R. (author)
Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, CNRS, UMR 7614, F-75005 Paris, France.
Journel, L. (author)
Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, CNRS, UMR 7614, F-75005 Paris, France.
Bozek, J. (author)
Univ Turku, Dept Phys & Astron, FI-20014 Turku, Finland.
Püttner, R. (author)
Free Univ Berlin, Fachbereich Phys, D-14195 Berlin, Germany.
Krasnov, Pavel (author)
KTH,Teoretisk kemi och biologi,International Research Center of Spectroscopy and Quantum Chemistry - IRC SQC, Siberian Federal University, Krasnoyarsk, 660041, Russian Federation,KTH Royal Inst Technol, Dept Theoret Chem & Biol, S-10691 Stockholm, Sweden.;Siberian Fed Univ, Int Res Ctr Spect & Quantum Chem IRC SQC, Krasnoyarsk 660041, Russia.
Kimberg, Victor, 1973- (author)
KTH,Teoretisk kemi och biologi,International Research Center of Spectroscopy and Quantum Chemistry - IRC SQC, Siberian Federal University, Krasnoyarsk, 660041, Russian Federation,KTH Royal Inst Technol, Dept Theoret Chem & Biol, S-10691 Stockholm, Sweden.;Siberian Fed Univ, Int Res Ctr Spect & Quantum Chem IRC SQC, Krasnoyarsk 660041, Russia.
Gel'mukhanov, Faris (author)
International Research Center of Spectroscopy and Quantum Chemistry - IRC SQC, Siberian Federal University, Krasnoyarsk, 660041, Russian Federation; Institute for Methods and Instrumentation in Synchrotron Radiation Research FG-ISRR, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Strasse 15, Berlin, 12489, Germany,KTH Royal Inst Technol, Dept Theoret Chem & Biol, S-10691 Stockholm, Sweden.;Siberian Fed Univ, Int Res Ctr Spect & Quantum Chem IRC SQC, Krasnoyarsk 660041, Russia.;Helmholtz Zentrum Berlin Mat & Energie, Inst Methods & Instrumentat Synchrotron Radiat Re, Albert Einstein Str 15, D-12489 Berlin, Germany.
Piancastelli, Maria Novella (author)
Uppsala universitet,Institutionen för fysik och astronomi,Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, CNRS, UMR 7614, F-75005 Paris, France.
Simon, M. (author)
Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, CNRS, UMR 7614, F-75005 Paris, France.
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Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, CNRS, UMR 7614, F-75005 Paris, France Univ Turku, Dept Phys & Astron, FI-20014 Turku, Finland. (creator_code:org_t)
2022
2022
English.
In: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 24:10, s. 5842-5854
  • Journal article (peer-reviewed)
Abstract Subject headings
Close  
  • We study vibrationally-resolved resonant Auger (RAS) spectra of ammonia recorded in coincidence with the NH2+ fragment, which is produced in the course of dissociation either in the core-excited 1s−14a11 intermediate state or the first spectator 3a−24a11 final state. Correlation of the NH2+ ion flight times with electron kinetic energies allows directly observing the Auger-Doppler dispersion for each vibrational state of the fragment. The median distribution of the kinetic energy release EKER, derived from the coincidence data, shows three distinct branches as a function of Auger electron kinetic energy Ee: Ee + 1.75EKER = const for the molecular band; EKER = const for the fragment band; and Ee + EKER = const for the region preceding the fragment band. The deviation of the molecular band dispersion from Ee + EKER = const is attributed to the redistribution of the available energy to the dissociation energy and excitation of the internal degrees of freedom in the molecular fragment. We found that for each vibrational line the dispersive behavior of EKERvs. Ee is very sensitive to the instrumental uncertainty in the determination of EKER causing the competition between the Raman (EKER + Ee = const) and Auger (Ee = const) dispersions: increase in the broadening of the finite kinetic energy release resolution leads to a change of the dispersion from the Raman to the Auger one. 

Subject headings

NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)
NATURVETENSKAP  -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
NATURAL SCIENCES  -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)

Keyword

Ammonia
Degrees of freedom (mechanics)
Dispersions
Dissociation
Excited states
Kinetic energy
Kinetics
Auger-Doppler
Electron kinetic energy
Intermediate state
Internal energies
Kinetic energy release
Molecular band
RAS spectrum
Resonant Auger
Ultrafast dissociation
Vibrationally resolved
Augers

Publication and Content Type

ref (subject category)
art (subject category)

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