| 1. |
- Savchenko, Viktoriia, et al.
(författare)
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Hydrogen bond effects in multimode nuclear dynamics of acetic acid observed via resonant x-ray scattering
- 2021
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 154:21
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Tidskriftsartikel (refereegranskat)abstract
- A theoretical and experimental study of the gas phase and liquid acetic acid based on resonant inelastic x-ray scattering (RIXS) spectroscopy is presented. We combine and compare different levels of theory for an isolated molecule for a comprehensive analysis, including electronic and vibrational degrees of freedom. The excitation energy scan over the oxygen K-edge absorption reveals nuclear dynamic effects in the core-excited and final electronic states. The theoretical simulations for the monomer and two different forms of the dimer are compared against high-resolution experimental data for pure liquid acetic acid. We show that the theoretical model based on a dimer describes the hydrogen bond formation in the liquid phase well and that this bond formation sufficiently alters the RIXS spectra, allowing us to trace these effects directly from the experiment. Multimode vibrational dynamics is accounted for in our simulations by using a hybrid time-dependent stationary approach for the quantum nuclear wave packet simulations, showing the important role it plays in RIXS.
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| 2. |
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| 3. |
- Savchenko, Viktoriia, et al.
(författare)
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Vibrational resonant inelastic X-ray scattering in liquid acetic acid : a ruler for molecular chain lengths
- 2021
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Ingår i: Scientific Reports. - : Springer Nature. - 2045-2322. ; 11:1
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Tidskriftsartikel (refereegranskat)abstract
- Quenching of vibrational excitations in resonant inelastic X-ray scattering (RIXS) spectra of liquid acetic acid is observed. At the oxygen core resonance associated with localized excitations at the O-H bond, the spectra lack the typical progression of vibrational excitations observed in RIXS spectra of comparable systems. We interpret this phenomenon as due to strong rehybridization of the unoccupied molecular orbitals as a result of hydrogen bonding, which however cannot be observed in x-ray absorption but only by means of RIXS. This allows us to address the molecular structure of the liquid, and to determine a lower limit for the average molecular chain length.
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| 4. |
- Söderström, Johan, et al.
(författare)
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Parity violation in resonant inelastic soft x-ray scattering at entangled core holes
- 2024
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Ingår i: Science Advances. - : American Association for the Advancement of Science (AAAS). - 2375-2548. ; 10:7, s. 3114-
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 5. |
- Barreau, Lou, et al.
(författare)
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Core-excited states of Formula Presented probed with soft-x-ray femtosecond transient absorption of vibrational wave packets
- 2023
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Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society (APS). - 2469-9926 .- 2469-9934. ; 108:1
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 6. |
- Cui, Jun Jie, et al.
(författare)
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Proposal for Observing XUV-Induced Rabi Oscillation Using Superfluorescent Emission
- 2023
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Ingår i: Physical Review Letters. - : American Physical Society (APS). - 0031-9007 .- 1079-7114. ; 131:4
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 7. |
- da Cruz, Vinicius Vaz, et al.
(författare)
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Anomalous polarization dependence in vibrationally resolved resonant inelastic x-ray scattering of H2O
- 2018
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Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society. - 2469-9926 .- 2469-9934. ; 98:1
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Tidskriftsartikel (refereegranskat)abstract
- It is well established that different electronic channels, in resonant inelastic x-ray scattering (RIXS), display different polarization dependences due to different orientations of their corresponding transition dipole moments in the molecular frame. However, this effect does not influence the vibrational progression in the Franck-Condon approximation. We have found that the transition dipole moments of core excitation and deexcitation experience ultrafast rotation during dissociation in the intermediate core-excited state. This rotation makes the vibrational progression in RIXS sensitive to the polarization of the x-ray photons. We study the water molecule, in which the effect is expressed in RIXS through the dissociative core-excited state where the vibrational scattering anisotropy is accompanied also by violation of parity selection rules for the vibrations.
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| 8. |
- da Cruz, Vinicius Vaz, et al.
(författare)
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Nuclear dynamics in resonant inelastic X-ray scattering and X-ray absorption of methanol
- 2019
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Ingår i: Journal of Chemical Physics. - : American Institute of Physics (AIP). - 0021-9606 .- 1089-7690. ; 150:23
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Tidskriftsartikel (refereegranskat)abstract
- We report on a combined theoretical and experimental study of core-excitation spectra of gas and liquid phase methanol as obtained with the use of X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). The electronic transitions are studied with computational methods that include strict and extended second-order algebraic diagrammatic construction [ADC(2) and ADC(2)-x], restricted active space second-order perturbation theory, and time-dependent density functional theory-providing a complete assignment of the near oxygen K-edge XAS. We show that multimode nuclear dynamics is of crucial importance for explaining the available experimental XAS and RIXS spectra. The multimode nuclear motion was considered in a recently developed "mixed representation" where dissociative states and highly excited vibrational modes are accurately treated with a time-dependent wave packet technique, while the remaining active vibrational modes are described using Franck-Condon amplitudes. Particular attention is paid to the polarization dependence of RIXS and the effects of the isotopic substitution on the RIXS profile in the case of dissociative core-excited states. Our approach predicts the splitting of the 2a RIXS peak to be due to an interplay between molecular and pseudo-atomic features arising in the course of transitions between dissociative core- and valence-excited states. The dynamical nature of the splitting of the 2a peak in RIXS of liquid methanol near pre-edge core excitation is shown. The theoretical results are in good agreement with our liquid phase measurements and gas phase experimental data available from the literature. (C) 2019 Author(s).
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| 9. |
- da Cruz, Vinicius Vaz, et al.
(författare)
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Probing hydrogen bond strength in liquid water by resonant inelastic X-ray scattering
- 2019
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 10
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Tidskriftsartikel (refereegranskat)abstract
- Local probes of the electronic ground state are essential for understanding hydrogen bonding in aqueous environments. When tuned to the dissociative core-excited state at the O1s pre-edge of water, resonant inelastic X-ray scattering back to the electronic ground state exhibits a long vibrational progression due to ultrafast nuclear dynamics. We show how the coherent evolution of the OH bonds around the core-excited oxygen provides access to high vibrational levels in liquid water. The OH bonds stretch into the long-range part of the potential energy curve, which makes the X-ray probe more sensitive than infra-red spectroscopy to the local environment. We exploit this property to effectively probe hydrogen bond strength via the distribution of intramolecular OH potentials derived from measurements. In contrast, the dynamical splitting in the spectral feature of the lowest valence-excited state arises from the short-range part of the OH potential curve and is rather insensitive to hydrogen bonding.
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| 10. |
- Dong, Xiao Xia, et al.
(författare)
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Carrier-envelope-phase measurement of sub-cycle UV pulses using angular photofragment distributions
- 2022
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Ingår i: Communications Physics. - : Springer Nature. - 2399-3650. ; 5:1
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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