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Liu, J. C., Gel'mukhanov, F., Polyutov, S., Krasnov, P. & Kimberg, V. (2024). Complementarity in which-path resonant Auger scattering. Physical Review A: covering atomic, molecular, and optical physics and quantum information, 109(2), Article ID 023116.
Open this publication in new window or tab >>Complementarity in which-path resonant Auger scattering
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2024 (English)In: Physical Review A: covering atomic, molecular, and optical physics and quantum information, ISSN 2469-9926, E-ISSN 2469-9934, Vol. 109, no 2, article id 023116Article in journal (Refereed) Published
Abstract [en]

Different types of Young's double-slit experiments contain a significant amount of both particle and wave information running from full-particle to full-wave knowledge depending on the experimental conditions. We study the Young's double-slit interference in resonant Auger scattering from homonuclear diatomic molecules where opposite Doppler shifts for the dissociating atomic slits provide path information. Different quantitative formulation of Bohr's complementarity principle - path information vs interference - is applied to two types of resonant Auger scattering experiments, with fixed-in-space and randomly oriented molecules. Special attention is paid to the orientational dephasing in conventional Auger experiments with randomly oriented molecules. Our quantitative formulation of the complementarity is compared with the formulation made earlier by Greenberger and Yasin [D. M. Greenberger and A. Yasin, Phys. Lett. A 128, 391 (1988)0375-960110.1016/0375-9601(88)90114-4].

Place, publisher, year, edition, pages
American Physical Society (APS), 2024
National Category
Physical Sciences
Identifiers
urn:nbn:se:kth:diva-344173 (URN)10.1103/PhysRevA.109.023116 (DOI)001172355600001 ()2-s2.0-85185836511 (Scopus ID)
Note

QC 20240307

Available from: 2024-03-06 Created: 2024-03-06 Last updated: 2024-05-03Bibliographically approved
Söderström, J., Ghosh, A., Kjellsson, L., Ekholm, V., Tokushima, T., Såthe, C., . . . Gel'mukhanov, F. (2024). Parity violation in resonant inelastic soft x-ray scattering at entangled core holes. Science Advances, 10(7), 3114
Open this publication in new window or tab >>Parity violation in resonant inelastic soft x-ray scattering at entangled core holes
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2024 (English)In: Science Advances, E-ISSN 2375-2548, Vol. 10, no 7, p. 3114-Article in journal (Refereed) Published
Abstract [en]

Resonant inelastic x-ray scattering (RIXS) is a major method for investigation of electronic structure and dynamics, with applications ranging from basic atomic physics to materials science. In RIXS applied to inversion-symmetric systems, it has generally been accepted that strict parity selectivity applies in the sub-kilo-electron volt region. In contrast, we show that the parity selection rule is violated in the RIXS spectra of the free homonuclear diatomic O2 molecule. By analyzing the spectral dependence on scattering angle, we demonstrate that the violation is due to the phase difference in coherent scattering at the two atomic sites, in analogy with Young's double-slit experiment. The result also implies that the interpretation of x-ray absorption spectra for inversion symmetric molecules in this energy range must be revised.

Place, publisher, year, edition, pages
American Association for the Advancement of Science (AAAS), 2024
National Category
Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-344012 (URN)10.1126/sciadv.adk3114 (DOI)38354244 (PubMedID)2-s2.0-85185243654 (Scopus ID)
Note

QC 20240229

Available from: 2024-02-28 Created: 2024-02-28 Last updated: 2024-02-29Bibliographically approved
Blinov, S. N., Kimberg, V. V., Krasnov, P. O., Gelmukhanov, F. K. & Polyutov, S. P. (2023). Mapping molecular potentials using pump-probe spectroscopy of vibrational wave packets' revival. Physical Review A: covering atomic, molecular, and optical physics and quantum information, 108(1), Article ID 013104.
Open this publication in new window or tab >>Mapping molecular potentials using pump-probe spectroscopy of vibrational wave packets' revival
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2023 (English)In: Physical Review A: covering atomic, molecular, and optical physics and quantum information, ISSN 2469-9926, E-ISSN 2469-9934, Vol. 108, no 1, article id 013104Article in journal (Refereed) Published
Abstract [en]

In this study, we investigate the nuclear dynamics in nitrogen monoxide after valence ionization by a pump pulse and subsequent probing with a time-delayed x-ray pulse. We calculate the development of the resulting vibrational wave packet, taking into account three different ionization mechanisms: one-photon, multiphoton, and tunneling ionization. Using a two-time propagation method, we solve the nonstationary nuclear Schrödinger equation to obtain time-resolved x-ray absorption spectra (TRXAS), considering the finite duration of the probe pulse. Our simulations show that the TRXAS profile accurately reflects the vibrational wave packets' trajectory in the cationic ground state. Additionally, we find that the TRXAS evolution is highly sensitive to small changes in the probed potential energy curve, making it a useful tool for reconstructing molecular potentials and determining anharmonicity and equilibrium bond length. This method can be applied to other polyatomic molecules and pump mechanisms.

Place, publisher, year, edition, pages
American Physical Society (APS), 2023
National Category
Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-335726 (URN)10.1103/PhysRevA.108.013104 (DOI)001052960000010 ()2-s2.0-85165624202 (Scopus ID)
Note

QC 20230911

Available from: 2023-09-11 Created: 2023-09-11 Last updated: 2023-09-11Bibliographically approved
Gel'mukhanov, F., Liu, J. C., Krasnov, P., Ignatova, N., Rubensson, J. E. & Kimberg, V. (2023). Nonlocal resonant inelastic x-ray scattering. Physical Review A: covering atomic, molecular, and optical physics and quantum information, 108(5), Article ID 052820.
Open this publication in new window or tab >>Nonlocal resonant inelastic x-ray scattering
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2023 (English)In: Physical Review A: covering atomic, molecular, and optical physics and quantum information, ISSN 2469-9926, E-ISSN 2469-9934, Vol. 108, no 5, article id 052820Article in journal (Refereed) Published
Abstract [en]

In the description of resonant inelastic x-ray scattering (RIXS) from inversion-symmetric molecules the small core-level splitting is typically neglected. However, the spacing Δ between gerade and ungerade core levels in homonuclear diatomic molecules can be comparable with the lifetime broadening of the intermediate core-excited state Γ. We show that when Δ∼Γ the scattering becomes nonlocal in the sense that x-ray absorption at one atomic site is followed by emission at the other one. This is manifested in an unusual dependence of the RIXS cross section on the sum of the momenta of incoming and outgoing x-ray photons k+k′, contrary to the normal k-k′ dependence in the conventional local RIXS theory. The nonlocality of the scattering influences strongly the scattering angle and excitation energy dependence of the intensity ratio between parity forbidden and allowed RIXS channels. Numerical simulations for N2 show that this effect can readily be measured at present-day x-ray radiation facilities.

Place, publisher, year, edition, pages
American Physical Society (APS), 2023
National Category
Atom and Molecular Physics and Optics Theoretical Chemistry
Identifiers
urn:nbn:se:kth:diva-340968 (URN)10.1103/PhysRevA.108.052820 (DOI)001110269800001 ()2-s2.0-85178134973 (Scopus ID)
Note

QC 20231218

Available from: 2023-12-18 Created: 2023-12-18 Last updated: 2024-02-29Bibliographically approved
Liu, J.-C., Wang, J., Ignatova, N., Krasnov, P., Gel'mukhanov, F. & Kimberg, V. (2023). Role of the Cohen-Fano interference in recoil-induced rotation. Journal of Chemical Physics, 158(11), Article ID 114304.
Open this publication in new window or tab >>Role of the Cohen-Fano interference in recoil-induced rotation
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2023 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 158, no 11, article id 114304Article in journal (Refereed) Published
Abstract [en]

We study the rotational dynamics induced by the recoil effect in diatomic molecules using time-resolved two-color x-ray pump-probe spectroscopy. A short pump x-ray pulse ionizes a valence electron inducing the molecular rotational wave packet, whereas the second time-delayed x-ray pulse probes the dynamics. An accurate theoretical description is used for analytical discussions and numerical simulations. Our main attention is paid to the following two interference effects that influence the recoil-induced dynamics: (i) Cohen-Fano (CF) two-center interference between partial ionization channels in diatomics and (ii) interference between the recoil-excited rotational levels manifesting as the rotational revival structures in the time-dependent absorption of the probe pulse. The time-dependent x-ray absorption is computed for the heteronuclear CO and homonuclear N-2 molecules as showcases. It is found that the effect of CF interference is comparable with the contribution from independent partial ionization channels, especially for the low photoelectron kinetic energy case. The amplitude of the recoil-induced revival structures for the individual ionization decreases monotonously with a decrease in the photoelectron energy, whereas the amplitude of the CF contribution remains sufficient even at the photoelectron kinetic energy below 1 eV. The profile and intensity of the CF interference depend on the phase difference between the individual ionization channels related to the parity of the molecular orbital emitting the photoelectron. This phenomenon provides a sensitive tool for the symmetry analysis of molecular orbitals.

Place, publisher, year, edition, pages
AIP Publishing, 2023
National Category
Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-326057 (URN)10.1063/5.0138739 (DOI)000952598200012 ()36948799 (PubMedID)2-s2.0-85150443760 (Scopus ID)
Note

QC 20230425

Available from: 2023-04-25 Created: 2023-04-25 Last updated: 2023-04-25Bibliographically approved
Banerjee, A., Da Cruz, V. V., Ekholm, V., Såthe, C., Rubensson, J. E., Ignatova, N., . . . Odelius, M. (2023). Simulating fluorine K -edge resonant inelastic x-ray scattering of sulfur hexafluoride and the effect of dissociative dynamics. Physical Review A: covering atomic, molecular, and optical physics and quantum information, 108(2), Article ID 023103.
Open this publication in new window or tab >>Simulating fluorine K -edge resonant inelastic x-ray scattering of sulfur hexafluoride and the effect of dissociative dynamics
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2023 (English)In: Physical Review A: covering atomic, molecular, and optical physics and quantum information, ISSN 2469-9926, E-ISSN 2469-9934, Vol. 108, no 2, article id 023103Article in journal (Refereed) Published
Abstract [en]

We report on a computational study of resonant inelastic x-ray scattering (RIXS), at different fluorine K-edge resonances of the SF6 molecule, and corresponding nonresonant x-ray emission. Previously measured polarization dependence in RIXS is reproduced and traced back to the local σ and π symmetry of the molecular orbitals and corresponding states involved in the RIXS process. Also electron-hole coupling energies are calculated and related to experimentally observed spectator shifts. The role of dissociative S-F bond dynamics is explored to model detuning of RIXS spectra at the |F1s-16a1g1) resonance, which shows challenges to accurately reproduce the required steepness for core-excited potential energy surface. We show that the RIXS spectra can only be properly described by considering breaking of the global inversion symmetry of the electronic wave function and core-hole localization, induced by vibronic coupling. Due to the core-hole localization we have symmetry forbidden transitions, which lead to additional resonances and changing width of the RIXS profile.

Place, publisher, year, edition, pages
American Physical Society (APS), 2023
National Category
Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-334790 (URN)10.1103/PhysRevA.108.023103 (DOI)2-s2.0-85167865095 (Scopus ID)
Note

QC 20230901

Available from: 2023-09-01 Created: 2023-09-01 Last updated: 2023-09-04Bibliographically approved
Savchenko, V., Odelius, M., Banerjee, A., Ignatova, N., Foehlisch, A., Gel'mukhanov, F. & Kimberg, V. (2023). Wave packet theory for non-resonant x-ray emission and non-resonant Auger electron emission in molecules. Journal of Chemical Physics, 159(4), Article ID 044110.
Open this publication in new window or tab >>Wave packet theory for non-resonant x-ray emission and non-resonant Auger electron emission in molecules
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2023 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 159, no 4, article id 044110Article in journal (Refereed) Published
Abstract [en]

We present a time-dependent theory for non-resonant x-ray emission spectrum (XES) and normal Auger spectrum (NAS) calculation, based on a fully quantum description of nuclear dynamics using the vibrational wave packet concept. We compare two formulations of the time-dependent theory, either employing a two-time propagation scheme or using spectral integration over the electron energy continuum. We find that the latter formulation is more efficient for numerical simulations, providing a reasonable accuracy when the integration step is shorter than the lifetime broadening of the core-ionized state. We demonstrate our approach using the example of non-resonant x-ray emission from a water molecule, considering the lowest core-ionized K-1 and first core-ionized shake-up (K-1V-1V1) intermediate states. These channels exemplify the developed theory on bound-bound, bound-continuum, continuum-bound, and continuum-continuum transitions. Our results suggest that the time-dependent approach is efficient for simulating XES involving dissociative states, whereas the time-independent approach, based on Franck-Condon factors, is more efficient for bound-bound transitions expressed as discrete frequency dependence in the energy domain. The methods and discussion have general applicability, including both NAS and more complex systems, such as liquid water.

Place, publisher, year, edition, pages
AIP Publishing, 2023
National Category
Theoretical Chemistry
Identifiers
urn:nbn:se:kth:diva-334304 (URN)10.1063/5.0159474 (DOI)001037221300005 ()37493134 (PubMedID)2-s2.0-85165656863 (Scopus ID)
Note

QC 20231122

Available from: 2023-08-18 Created: 2023-08-18 Last updated: 2023-11-27Bibliographically approved
Santos, A. C., Travnikova, O., Boudjemia, N., Marchenko, T., Guillemin, R., Ismail, I., . . . Puettner, R. (2022). Resonant Auger decay induced by the symmetry-forbidden 1a(1g)?: 6a(1g) transition of the SF6 molecule. Journal of Vacuum Science & Technology. A. Vacuum, Surfaces, and Films, 40(4), 042801, Article ID 042801.
Open this publication in new window or tab >>Resonant Auger decay induced by the symmetry-forbidden 1a(1g)?: 6a(1g) transition of the SF6 molecule
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2022 (English)In: Journal of Vacuum Science & Technology. A. Vacuum, Surfaces, and Films, ISSN 0734-2101, E-ISSN 1520-8559, Vol. 40, no 4, p. 042801-, article id 042801Article in journal (Refereed) Published
Abstract [en]

Resonant Auger electron spectroscopic study at the symmetry-forbidden 1 a 1 g -> 6 a 1 g excitation below the S K-shell threshold of SF 6 is reported. Partial electron yield and resonant K L L Auger spectra have been measured by using monochromatized undulator synchrotron radiation. By changing the photon energy in small steps, a so-called 2D map is produced. In this map, the dipole-forbidden transition exhibits spectral features (e.g., an S-shaped dispersion relation), which are well known and understood for dipole-allowed transitions. We validate by a theory that for the case of dipole-forbidden transitions, these spectral features can be analyzed in the same way as previously established for the dipole-allowed ones. This approach grants information on the nuclear dynamics in the K-shell core-excited states of SF 6 on the femtosecond (fs) timescale. In particular, for the potential-energy curves of the states S 1 s(-1) 6(a1g) and S 2p(-2)6a(1g), the slopes at the equilibrium distance of the ground state are derived. Symmetry breaking as a result of ultrafast vibronic coupling is revealed by the population of the electronically forbidden excited state. Published under an exclusive license by the AVS.

Place, publisher, year, edition, pages
American Vacuum Society, 2022
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-314225 (URN)10.1116/6.0001890 (DOI)000804075400002 ()2-s2.0-85131185508 (Scopus ID)
Note

QC 20220617

Available from: 2022-06-17 Created: 2022-06-17 Last updated: 2022-06-25Bibliographically approved
Liu, J.-C. -., Ignatova, N., Kimberg, V., Krasnov, P., Föhlisch, A., Simon, M. & Gel'mukhanov, F. (2022). Time-resolved study of recoil-induced rotation by X-ray pump - X-ray probe spectroscopy. Physical Chemistry, Chemical Physics - PCCP, 24(11), 6627-6638
Open this publication in new window or tab >>Time-resolved study of recoil-induced rotation by X-ray pump - X-ray probe spectroscopy
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2022 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 24, no 11, p. 6627-6638Article in journal (Refereed) Published
Abstract [en]

Modern stationary X-ray spectroscopy is unable to resolve rotational structure. In the present paper, we propose to use time-resolved two color X-ray pump-probe spectroscopy with picosecond resolution for real-time monitoring of the rotational dynamics induced by the recoil effect. The proposed technique consists of two steps. The first short pump X-ray pulse ionizes the valence electron, which transfers angular momentum to the molecule. The second time-delayed short probe X-ray pulse resonantly excites a 1s electron to the created valence hole. Due to the recoil-induced angular momentum the molecule rotates and changes the orientation of transition dipole moment of core-excitation with respect to the transition dipole moment of the valence ionization, which results in a temporal modulation of the probe X-ray absorption as a function of the delay time between the pulses. We developed an accurate theory of the X-ray pump-probe spectroscopy of the recoil-induced rotation and study how the energy of the photoelectron and thermal dephasing affect the structure of the time-dependent X-ray absorption using the CO molecule as a case-study. We also discuss the feasibility of experimental observation of our theoretical findings, opening new perspectives in studies of molecular rotational dynamics. 

Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC), 2022
Keywords
Angular momentum, Dipole moment, Molecules, Optical pumping, Probes, X ray spectroscopy, Probe spectroscopy, Rotational dynamics, Rotational structures, Time resolved studies, Time-resolved, Transition dipole moments, X ray pulse, X ray pump-probe spectroscopy, X-ray absorptions, X-ray spectroscopy, X ray absorption, article, crystal structure, dipole, excitation, feasibility study, ionization, pump probe spectroscopy, rotation, theoretical study, X ray
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-322580 (URN)10.1039/d1cp05000a (DOI)000762983300001 ()35234760 (PubMedID)2-s2.0-85127334301 (Scopus ID)
Note

QC 20221222

Available from: 2022-12-22 Created: 2022-12-22 Last updated: 2022-12-22Bibliographically approved
Travnikova, O., Kukk, E., Hosseini, F., Granroth, S., Itälä, E., Marchenko, T., . . . Simon, M. (2022). Ultrafast dissociation of ammonia: Auger Doppler effect and redistribution of the internal energy. Physical Chemistry, Chemical Physics - PCCP, 24(10), 5842-5854
Open this publication in new window or tab >>Ultrafast dissociation of ammonia: Auger Doppler effect and redistribution of the internal energy
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2022 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 24, no 10, p. 5842-5854Article in journal (Refereed) Published
Abstract [en]

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. 

Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC), 2022
Keywords
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
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-321875 (URN)10.1039/d1cp05499f (DOI)000759750400001 ()35195639 (PubMedID)2-s2.0-85126072496 (Scopus ID)
Note

QC 20221125

Available from: 2022-11-25 Created: 2022-11-25 Last updated: 2022-11-25Bibliographically approved
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ORCID iD: ORCID iD iconorcid.org/0000-0003-3072-3173

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