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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
Wang, C., Gong, M., Zhao, X., Nan, Q. W., Yu, X. Y., Cheng, Y., . . . Zhang, S. B. (2024). Rebuilding the vibrational wavepacket in TRAS using attosecond X-ray pulses. Communications Physics, 7(1), Article ID 1.
Open this publication in new window or tab >>Rebuilding the vibrational wavepacket in TRAS using attosecond X-ray pulses
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2024 (English)In: Communications Physics, E-ISSN 2399-3650, Vol. 7, no 1, article id 1Article in journal (Refereed) Published
Abstract [en]

Time-resolved X-ray photoelectron spectroscopy (TXPS) is a well-established technique to probe coherent nuclear wavepacket dynamics using both table-top and free-electron-based ultrafast X-ray lasers. Energy resolution, however, becomes compromised for a very short pulse duration in the sub-femtosecond range. By resonantly tuning the X-ray pulse to core-excited states undergoing Auger decay, this drawback of TXPS can be mitigated. While resonant Auger-electron spectroscopy (RAS) can recover the vibrational structures not hidden by broadband excitation, the full reconstruction of the wavepacket is a standing challenge. Here, we theoretically demonstrate how the complete information of a nuclear wavepacket, i.e., the populations and relative phases of the vibrational states constituting the wavepacket, can be retrieved from time-resolved RAS (TRAS) measurements. Thus, TRAS offers key insights into coupled nuclear and electronic dynamics in complex systems on ultrashort timescales, providing an alternative to leverage femtosecond and attosecond X-ray probe pulses.

Place, publisher, year, edition, pages
Springer Nature, 2024
National Category
Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-342178 (URN)10.1038/s42005-023-01507-3 (DOI)001135208000001 ()2-s2.0-85181231041 (Scopus ID)
Note

QC 20240115

Available from: 2024-01-15 Created: 2024-01-15 Last updated: 2024-01-22Bibliographically approved
Barreau, L., Ross, A. D., Kimberg, V., Krasnov, P., Blinov, S., Neumark, D. M. & Leone, S. R. (2023). Core-excited states of Formula Presented probed with soft-x-ray femtosecond transient absorption of vibrational wave packets. Physical Review A: covering atomic, molecular, and optical physics and quantum information, 108(1), Article ID 012805.
Open this publication in new window or tab >>Core-excited states of Formula Presented probed with soft-x-ray femtosecond transient absorption of vibrational wave packets
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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 012805Article in journal (Refereed) Published
Abstract [en]

A vibrational wavepacket in Formula Presented is created by impulsive stimulated Raman scattering with a few-cycle infrared pulse and mapped simultaneously onto five sulfur core-excited states using table-top soft x-ray transient absorption spectroscopy between 170 to 200 eV. The femtosecond vibrations induce real-time energy shifts of the x-ray absorption, whose amplitude depend strongly on the nature of the core-excited state. The pump laser intensity is used to control the number of vibrational states in the superposition, thereby accessing core-excited levels for various extensions of the S-F stretching motion. This enables the determination of the relative core-level potential energy gradients for the symmetric stretching mode, in good agreement with TDDFT calculations. This experiment demonstrates a new means of characterizing core-excited potential energy curves.

Place, publisher, year, edition, pages
American Physical Society (APS), 2023
National Category
Atom and Molecular Physics and Optics Other Chemistry Topics
Identifiers
urn:nbn:se:kth:diva-333875 (URN)10.1103/PhysRevA.108.012805 (DOI)001053004600004 ()2-s2.0-85165536278 (Scopus ID)
Note

QC 20230815

Available from: 2023-08-15 Created: 2023-08-15 Last updated: 2023-09-21Bibliographically 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
Cui, J. J., Cheng, Y., Wang, X., Li, Z., Rohringer, N., Kimberg, V. & Zhang, S. B. (2023). Proposal for Observing XUV-Induced Rabi Oscillation Using Superfluorescent Emission. Physical Review Letters, 131(4), Article ID 043201.
Open this publication in new window or tab >>Proposal for Observing XUV-Induced Rabi Oscillation Using Superfluorescent Emission
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2023 (English)In: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Vol. 131, no 4, article id 043201Article in journal (Refereed) Published
Abstract [en]

Intense x-ray and extreme ultraviolet (XUV) light sources have been available for decades, however, due to weak nonlinear interaction in the XUV photon energy range, observation of Rabi oscillation induced by XUV pulse remains a very challenging experimental task. Here we suggest a scheme where photoionization of a He medium by an intense XUV pump pulse is followed by a strong population inversion and Rabi oscillation at the He+(1s-3p) transition and is accompanied by superfluorescence (SF) of the 7.56 eV pulse at the He+(3p-2s) transition. Our numerical simulations show that the Rabi oscillation at the He+(1s-3p) transition induced by an XUV pulse with photon energy 48.36 eV results in significant signatures in the SF spectra, allowing us to identify and characterize the XUV induced Rabi-oscillatory regime. The proposed scheme provides a sensitive tool to monitor and control ultrafast nonlinear dynamics in atoms and molecules triggered by intense XUV.

Place, publisher, year, edition, pages
American Physical Society (APS), 2023
Keywords
Extreme Ultraviolet, Extreme ultraviolet light sources, Extreme ultraviolet pulse, Nonlinear interactions, Photon energy, Photon energy range, Population inversions, Pump pulse, Rabi oscillations, Ultraviolet photon
National Category
Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-335306 (URN)10.1103/PhysRevLett.131.043201 (DOI)001062108700009 ()37566830 (PubMedID)2-s2.0-85166741216 (Scopus ID)
Note

QC 20230905

Available from: 2023-09-05 Created: 2023-09-05 Last updated: 2023-11-08Bibliographically 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
Wang, C., Gong, M., Cheng, Y., Kimberg, V., Liu, X. J., Vendrell, O., . . . Zhang, S. B. (2023). Time-Resolved Resonant Auger Scattering Clocks Distortion of a Molecule. Journal of Physical Chemistry Letters, 14(24), 5475-5480
Open this publication in new window or tab >>Time-Resolved Resonant Auger Scattering Clocks Distortion of a Molecule
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2023 (English)In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 14, no 24, p. 5475-5480Article in journal (Refereed) Published
Abstract [en]

Resonant Auger scattering (RAS) provides information on the core-valence electronic transition and impresses a rich fingerprint of the electronic structure and nuclear configuration at the time-initiating RAS process. Here, we suggest using a femtosecond X-ray pulse to trigger RAS in a distorted molecule, which is generated from the nuclear evolution on a valence excited state pumped by a femtosecond ultraviolet pulse. With the time delay varied, the amount of molecular distortion can be controlled and the RAS measurements imprint both their electronic structures and changing geometries. This strategy is showcased in H2O prepared in an O-H dissociative valence state, where molecular and fragment lines appear in RAS spectra as signatures of ultrafast dissociation. Given the generality of this approach for a broad class of molecules, this work opens a new alternative pump-probe technique for mapping the core and valence dynamics with ultrashort X-ray probe pulses.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2023
National Category
Atom and Molecular Physics and Optics Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-334854 (URN)10.1021/acs.jpclett.3c01347 (DOI)001006208500001 ()37289034 (PubMedID)2-s2.0-85163477600 (Scopus ID)
Note

QC 20230829

Available from: 2023-08-28 Created: 2023-08-28 Last updated: 2023-08-29Bibliographically 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
Dong, X. X., Liu, Y. R., Kimberg, V., Vendrell, O., Wu, Y., Wang, J. G., . . . Zhang, S. B. (2022). Carrier-envelope-phase measurement of sub-cycle UV pulses using angular photofragment distributions. Communications Physics, 5(1), Article ID 181.
Open this publication in new window or tab >>Carrier-envelope-phase measurement of sub-cycle UV pulses using angular photofragment distributions
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2022 (English)In: Communications Physics, E-ISSN 2399-3650, Vol. 5, no 1, article id 181Article in journal (Refereed) Published
Abstract [en]

Carrier-envelope-phase (CEP) of sub-cycle ultraviolet (UV) pulse strongly influences the dynamics of quantum systems, but its characterization is not accessible experimentally. Here we investigate photodissociation of a diatomic molecule from its ground-rovibrational state in a linearly polarized weak sub-cycle UV pulse with a controlled CEP. The angular distribution of photofragments shows an asymmetric profile deviating from the well-known cos(2-) or sin(2)-like ones, which can be identified as a way to imprint CEP. We unveil that such an effect stems from the temporal neighboring rotational excitation by molecular permanent dipole interaction through the joint contributions between counter-rotating and rotating terms. This in turn, opens different pathways in photodissociation dynamics. Given that the temporal excitation between various states with close energies can be manipulated by CEP of subcycle UV pulses, our results pave ways for understanding and manipulating electron, nuclear and their joint dynamics with variation of CEP of attosecond pulses.

Place, publisher, year, edition, pages
Springer Nature, 2022
National Category
Theoretical Chemistry
Identifiers
urn:nbn:se:kth:diva-315930 (URN)10.1038/s42005-022-00959-3 (DOI)000825408500001 ()2-s2.0-85134251779 (Scopus ID)
Note

QC 20220728

Available from: 2022-07-28 Created: 2022-07-28 Last updated: 2023-02-09Bibliographically approved
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ORCID iD: ORCID iD iconorcid.org/0000-0003-1269-8760

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