F Gel'mukhanov

Shandong Normal University, Chi-nan-shih, Shandong Sheng, China

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Publications (54)202.95 Total impact

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    ABSTRACT: A detailed study of inelastic x-ray scattering from the ground state to the ^{3}Σ_{g}(3σ_{g}^{-1}3s_{g}^{1}) state of the O_{2} molecule is presented. The observed angular anisotropy shows that the vibrational excitations within this final state are strongly dependent on the polarization of the incident radiation. The analysis demonstrates that this is a manifestation of interference between resonant and direct nonresonant inelastic x-ray scattering. This interference provides a new tool to monitor nuclear dynamics by relative rotation of the polarization vectors of the incident and scattered photons.
    Physical Review Letters 05/2013; 110(22):223001. · 7.73 Impact Factor
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    ABSTRACT: This paper reports an advanced study of the excited ionic states of the gas-phase nitrogen molecule in the binding-energy region of 22–34 eV, combining ultrahigh-resolution resonant photoemission (RPE) and ab initio configuration-interaction calculations. The RPE spectra are recorded for nine photon energies within the N 1s→π* absorption resonance of N2 by using a photon bandwidth that is considerably smaller than lifetime broadening, and the dependence on excitation energy of the decay spectra is analyzed and used for the first assignment of 12 highly overlapped molecular states. The effect on the RPE profile of avoided curve crossings between the final N2+ ionic states is discussed, based on theoretical simulations that account for vibronic coupling, and compared with the experimental data. By use of synchrotron radiation with high spectral brightness, it is possible to selectively promote the molecule to highly excited vibrational sublevels of a core-excited electronic state, thereby controlling the spatial distribution of the vibrational wave packets, and to accurately image the ionic molecular potentials. In addition, the mapping of the vibrational wave functions of the core-excited states using the bound final states with far-from-equilibrium bond lengths has been achieved experimentally for the first time. Theoretical analysis has revealed the rich femtosecond nuclear dynamics underlying the mapping phenomenon.
    Physical Review X 01/2013; 3:011017. · 8.39 Impact Factor
  • Q Miao, J-C Liu, H Agren, J-E Rubensson, F Gel'mukhanov
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    ABSTRACT: X-ray lasing is predicted to ensue when molecules are pumped into dissociative core-excited states by a free-electron-laser pulse. The lasing is due to the population inversion created in the neutral dissociation product, and the process features self-trapping of the x-ray pulse at the gain ridge. Simulations performed for the HCl molecule pumped at the 2p_{1/2}→6σ resonance demonstrate that the scheme can be used to create ultrashort coherent x-ray pulses.
    Physical Review Letters 12/2012; 109(23):233905. · 7.73 Impact Factor
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    ABSTRACT: Born–Oppenheimer and Franck–Condon approximations are two major concepts in the interpretation of electronic excitations and modeling of spectroscopic data in the gas and condensed phases. We report large variations of the anisotropy parameter (β) for the fully resolved vibrational sub-states of the X2Πg electronic ground state of O+2 populated by participator resonant Auger decay following excitations of K-shell electrons into the σ☆ resonance by monochromatic x-rays. Decay spectra for light polarization directions parallel and perpendicular to the electron detection axis recorded at four different excitation energies in the vicinity of the O 1s → σ☆ transition are presented. Breakdown of the Born–Oppenheimer approximation is for the first time selectively observed for the lower vibrational sub-states, where two quantum paths—resonant and direct—leading to the same final cationic state exist. The higher vibrational sub-states can only be populated by resonant photoemission; hence no interference between these channels can occur.
    New Journal of Physics 11/2012; 14:113018. · 4.06 Impact Factor
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    ABSTRACT: We experimentally observed interference effects in elastic x-ray scattering from gas-phase HCl in the vicinity of the Cl K edge. Comparison to theory identifies these effects as interference effects between non-resonant elastic Thomson scattering and resonant Raman scattering. The results indicate the non-resonant Thomson and resonant Raman contributions are of comparable strength. The measurements also exhibit strong polarization dependence, allowing an easy identification of the resonant and non-resonant contributions.
    The Journal of Chemical Physics 09/2012; 137(9):094311. · 3.12 Impact Factor
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    ABSTRACT: Resonant inelastic x-ray scattering spectra excited at the O1s−1π* resonance of liquid acetone are presented. Scattering to the electronic ground state shows a resolved vibrational progression where the dominant contribution is due to the C-O stretching mode, thus demonstrating a unique sensitivity of the method to the local potential energy surface in complex molecular systems. For scattering to electronically excited states, soft vibrational modes and, to a smaller extent, intermolecular interactions give a broadening, which blurs the vibrational fine structure. It is predicted that environmental broadening is dominant in aqueous acetone.
    Physical review. B, Condensed matter 10/2011; 84(13). · 3.77 Impact Factor
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    ABSTRACT: Resonant inelastic soft x-ray scattering spectra excited at the dissociative 1σg → 3σu resonance in gas-phase O2 are presented and discussed in terms of state-of-the-art molecular theory. A new selection rule due to internal spin coupling is established, facilitating a deep analysis of the valence excited final states. Furthermore, it is found that a commonly accepted symmetry selection rule due to orbital parity breaks down, as the core hole and excited electron swap parity, thereby opening the symmetry forbidden 3σg decay channel.
    Journal of Physics B Atomic Molecular and Optical Physics 07/2011; 44(16):161002. · 2.03 Impact Factor
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    ABSTRACT: Resonant inelastic soft x-ray scattering (RIXS) spectra excited at the 1σ(g) → 3σ(u) resonance in gas-phase O2 show excitations due to the nuclear degrees of freedom with up to 35 well-resolved discrete vibronic states and a continuum due to the kinetic energy distribution of the separated atoms. The RIXS profile demonstrates spatial quantum beats caused by two interfering wave packets with different momenta as the atoms separate. Thomson scattering strongly affects both the spectral profile and the scattering anisotropy.
    Physical Review Letters 04/2011; 106(15):153004. · 7.73 Impact Factor
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    ABSTRACT: We report both experimental and theoretical studies on x-ray absorption measured using partial Auger yields of gas phase nitrogen, carbon monoxide, and oxygen molecules near the N 1s ->pi(*), O 1s ->pi(*), and O 1s ->pi(*) regions, respectively. The main tool of our study is a two-dimensional map in which resonant Auger yields are plotted as a function of photon and kinetic energy. The partial yields of the three molecules are analyzed in detail by extracting profiles along various directions in the map. Narrowing of the absorption resonances is observed along the direction of constant kinetic energy. It is shown that such profiles are similar to the conventional x-ray-absorption spectrum for a broad class of molecules whose potential energy surfaces of the final and core-excited states are almost parallel. However, substantial differences with the conventional x-ray-absorption profiles are observed in the general case of nonparallel surfaces due to the lifetime vibrational interference. Here, we suggest a systematic way to eliminate the lifetime vibrational interference.
    Physical Review A 01/2009; 79(2). · 3.04 Impact Factor
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    ABSTRACT: We report both experimental and theoretical studies on x-ray absorption measured in the resonant Auger scattering mode of gas phase carbon monoxide near the O1s-->2pi region. Both experiment and theory display a crucial difference between the x-ray absorption profiles obtained in the conventional and resonant scattering modes. Lifetime vibrational interference is the main source of the difference. It is demonstrated that such interference, which arises from a coherent excitation to overlapping intermediate levels, ruins the idea for obtaining x-ray absorption spectra in a lifetime broadening free regime.
    Physical Review Letters 08/2008; 101(7):073001. · 7.73 Impact Factor
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    ABSTRACT: A detailed dynamical theory of photobleaching by periodical sequences of laser pulses is presented. The theory is used for interpretation of recent experiments with pyrylium salts. Our simulations are based on first-principles simulations of photoabsorption cross-sections and on empirical rate constants. Two competitive channels of photobleaching, namely, photobleaching from the lowest excited singlet and triplet states and from higher excited states, are found to explain different intensity dependences of the photobleaching rates in different samples. The process includes two-photon excitation from the ground state to the first or second excited singlet states and one-photon excitation from the first singlet or triplet states to higher excited states. The fluorescence follows double-exponential dynamics with two characteristic times. The first and the shorter one is the equilibrium settling time between the ground and the lowest triplet states. The second characteristic time, the time of photobleaching, is responsible for the long-term dynamics. The effective rate of photobleaching from the first excited singlet and lowest triplet states depends differently on the irradiance in comparison with the photobleaching in higher states. The first channel is characterized by a quadratic intensity dependence in contrast to the second channel that shows a cubic dependence. The competition between these photobleaching channels is very sensitive to the rate constants as well as to the repetition rate, the pulse duration, and the peak intensity. The double-exponential decay of the fluorescence is explained by the spatial inhomogeneity of the light beam. The findings in this work are discussed in terms of the possibility of using many-photon-induced photobleaching for new three-dimensional read-write devices.
    The Journal of Physical Chemistry A 12/2007; 111(47):11961-75. · 2.77 Impact Factor
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    Journal of Electron Spectroscopy and Related Phenomena 01/2007; · 1.71 Impact Factor
  • F F Guimarães, F Gel'mukhanov
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    ABSTRACT: Pump-probe spectra of molecules driven by strong infrared (IR) field in both ground and excited states are studied theoretically. The role of the final state interaction becomes important when pump and probe pulses overlap, and the Rabi frequency is comparable with the lifetime broadening of the excited state and the duration of the pump pulse. Our theoretical approach is applied to x-ray absorption of nitrogen molecule and valence photoionization of carbon monoxide. It is shown that IR-x-ray pump-probe spectroscopy can directly evidence the delocalization of core hole.
    The Journal of Chemical Physics 12/2006; 125(20):204313. · 3.12 Impact Factor
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    ABSTRACT: The theory of IR-X-ray pump-probe spectroscopy beyond the Born-Oppenheimer approximation is developed and applied to the study of the dynamics of intramolecular proton transfer in glyoxalmonoxime leading to the formation of the tautomer 2-nitrosoethenol. Due to the IR pump pulses the molecule gains sufficient energy to promote a proton to a weakly bound well. A femtosecond X-ray pulse snapshots the wave packet route and, hence, the dynamics of the proton transfer. The glyoxalmonoxime molecule contains two chemically nonequivalent oxygen atoms that possess distinct roles in the hydrogen bond, a hydrogen donor and an acceptor. Core ionizations of these form two intersecting core-ionized states, the vibronic coupling between which along the OH stretching mode partially delocalizes the core hole, resulting in a hopping of the core hole from one site to another. This, in turn, affects the dynamics of the proton transfer in the core-ionized state. The quantum dynamical simulations of X-ray photoelectron spectra of glyoxalmonoxime driven by strong IR pulses demonstrate the general applicability of the technique for studies of intramolecular proton transfer in systems with vibronic coupling.
    The Journal of Physical Chemistry A 12/2006; 110(47):12805-13. · 2.77 Impact Factor
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    ABSTRACT: The core-level photoelectron spectra of N2 molecules are observed at high energy resolution, resolving the 1σg and 1σu components as well as the vibrational components in the extended energy region from the threshold up to 1 keV. The σg/σu cross section ratios display modulation as a function of photoelectron momentum due to the two-centre interference, analogous to the classical Young's double-slit experiment, as predicted by Cohen and Fano a long time ago. The Cohen–Fano interference modulations display different phases depending on the vibrational excitations in the core-ionized state. Extensive ab initio calculations have been performed within the Hartree–Fock and random phase approximations in prolate spheroidal coordinates. The dependence of photoionization amplitudes on the vibrational states was taken into account using the Born–Oppenheimer approximation. The ab initio results are in reasonable agreement with the experimental data. The theoretical analysis allows the modulation to be connected with the onset of transitions to the states of increasing orbital angular momentum which occurs at increasing photon energies. Deviation from the Cohen–Fano formula is found for both the experimental and the ab initio results and is attributed to electron scattering by the neighbouring atom. A new formula for the interference modulation is derived within the framework of the multiple scattering technique. It differs from the classical Cohen–Fano formula by the addition of twice the scattering phase of the photoelectron by the neighbouring atom. We demonstrate that one can measure directly the scattering phase by fitting our formula to the experimental results.
    Journal of Physics B Atomic Molecular and Optical Physics 11/2006; 39(23):4801. · 2.03 Impact Factor
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    ABSTRACT: The ratios of photoionization cross sections of the 1σg and 1σu shells of the N2 molecule for the vibrational transitions to the v' = 0 and v' = 1 core-ionized states in the photon energy region between 440 and 550 eV have been measured. The calculations in the random phase approximation well reproduce the experimental data. The variation of the ratio with photon energy is attributed to the interference modulation that is caused by coherent photoemission from the two atoms, as an analogue of the Young's double-slit experiment. The calculations extended up to 1.8 keV allow connecting the modulation with the onset of transitions to the states of increasing orbital angular momentum which occurs at increasing photon energies and demonstrate that the main contribution to these modulations comes from the σ continuum states.
    Journal of Physics B Atomic Molecular and Optical Physics 06/2006; 39(12):L261. · 2.03 Impact Factor
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    S Polyutov, V Kimberg, A Baev, F Gel'mukhanov, H Å gren
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    ABSTRACT: Temporal oscillations of amplified spontaneous emission of molecules are studied theoretically. From the proposed theory and numerical simulations, it is found that the self-pulsations originate in an interplay between stimulated emission and saturable absorption. A stability analysis demonstrates the crucial role of the photoabsorption in this process, which can be regulated by a proper choice of buffer molecules. Variations in the saturable absorption mediate a transition from damped oscillations to self-sustained pulsations. The role of propagation effects as well as of the interaction of co- and counter-propagating pulses is also investigated. Numerical simulations, demonstrating the theoretical findings, are performed for a model 3-level system and for an organic chromophore; 4-[N-(2-hydroxyethyl)-N-(methyl)amino phenyl]-4'-(6-hydroxyhexyl sulphonyl) stilbene.
    Journal of Physics B Atomic Molecular and Optical Physics 01/2006; 39(2):215-227. · 2.03 Impact Factor
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    S Polyutov, I Minkov, F Gel'mukhanov, H Agren
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    ABSTRACT: We present a theory of two-photon absorption that addresses the formation of spectral shapes taking the vibrational degrees of freedom into account. The theory is used to rationalize the observed differences between the spectral shapes of one- and two-photon absorption. We find that the main cause of these differences is that the two-step and coherent two-photon spectral bands are different even considering a single final state. Our formalism is applied to the N101 molecule (p-nitro-p'-diphenylamine stilbene), which was recently studied experimentally. Simulations show that the two-step two-photon electrovibrational absorption results in a blue shift of the absorption spectrum in agreement with the measurements.
    The Journal of Physical Chemistry A 11/2005; 109(42):9507-13. · 2.77 Impact Factor
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    ABSTRACT: We have studied the spectral features of resonant inelastic x-ray scattering of condensed ethylene with vibrational selectivity both experimentally and theoretically. Purely vibrational spectral loss features and coupled electronic and vibrational losses are observed. The one-step theory for resonant soft x-ray scattering is applied, taking multiple vibrational modes and vibronic coupling into account. Our investigation of ethylene underlines that the assignment of spectral features observed in resonant inelastic x-ray scattering of polyatomic systems requires an explicit description of the coupled electronic and vibrational loss features.
    Physical Review Letters 11/2005; 95(16):163002. · 7.73 Impact Factor
  • V C Felicíssimo, A Cesar, Y Luo, F Gel'mukhanov, H Agren
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    ABSTRACT: Carbon and oxygen near-edge X-ray absorption fine structure (NEXAFS) spectra of 1,4-cyclohexadiene, p-benzoquinone, norbornadiene, norbornadienone, and cis-cis-[4,4,2]propella-3,8-diene-11,12-dione were calculated by means of Hartree-Fock and hybrid density functional theory using the static-exchange (STEX) approximation. The NEXAFS spectra are used as a probe to identify weak molecular interactions between the two non-conjugated ethylenic pi* orbitals present in these molecules. We show that the X-ray absorption spectrum of 1,4-cyclohexadiene exhibits some particular spectral structures in the discrete energy region that evidence diene through-bond orbital interaction, whereas absorption peaks are identified in the norbornadiene and norbornadienone spectra that indicate effective through-space orbital interactions. The molecular structure of the cis-cis-[4,4,2]propella-3,8-diene-11,12-dione isomer is such that the indirect through-bond or through-space diene orbital interactions are too weak to be assigned by its C1s NEXAFS spectrum.
    The Journal of Physical Chemistry A 09/2005; 109(33):7385-95. · 2.77 Impact Factor

Publication Stats

754 Citations
202.95 Total Impact Points


  • 2012
    • Shandong Normal University
      Chi-nan-shih, Shandong Sheng, China
  • 2000–2012
    • KTH Royal Institute of Technology
      • Division of Theoretical Chemistry and Biology
      Tukholma, Stockholm, Sweden
  • 2011
    • Lund University
      • MAX-Lab
      Lund, Skane, Sweden
  • 2006
    • Tohoku University
      • Institute of Multidisciplinary Research for Advanced Materials (IMRAM)
      Sendai-shi, Miyagi-ken, Japan
  • 2003–2006
    • Sophia University
      • Division of Physics
      Edo, Tōkyō, Japan
  • 2000–2002
    • Uppsala University
      • Department of Physics and Astronomy
      Uppsala, Uppsala, Sweden
  • 1996–2000
    • Linköping University
      Linköping, Östergötland, Sweden