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  • 1.
    Elshakre, M.
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Storchi, L.
    Kloda, Tomasz
    Stockholm University, Faculty of Science, Department of Physics.
    Linusson, Per
    Stockholm University, Faculty of Science, Department of Physics.
    Heijkenskjold, F.
    Gengelbach, A.
    Karlsson, L.
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Tarantelli, F.
    Feifel, R.
    A photoelectron and double photoionization study of the valence electronic structure of 1,4-bromofluorobenzene2009In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 131, no 18, p. 184302-Article in journal (Refereed)
    Abstract [en]

    Conventional photoelectron and time-of-flight photoelectron-photoelectron coincidence (TOF-PEPECO) spectra have been measured for the outer valence region of the 1,4-bromofluorobenzene molecule. The photoelectron spectra were recorded using Hela radiation from a resonance Source, and the TOF-PEPECO spectra were recorded using HeII alpha radiation from a pulsed resonance source. The former provide energies of the cationic states and the latter of the dicationic states. The spectra are adequately interpreted with the aid of accurate Green's function calculations, showing very significant correlation effects. The lowest double ionization energy is found at 23.45 eV associated with the (4b(1))X-2 (1)A(1) dicationic state.

  • 2.
    Geng, Ting
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Galván, Ignacio F.
    Schalk, Oliver
    Stockholm University, Faculty of Science, Department of Physics.
    Lindh, Roland
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Time-resolved photoelectron spectroscopy studies on pyrazole and several methylated derivativesManuscript (preprint) (Other academic)
    Abstract [en]

    We present femtosecond time-resolved photoelectron spectra and ab initio studies on pyrazole andits methylated derivatives 1-, 3-, and 5-methylpyrazole. Excitation at 200 nm populates both the two lowest lying states, a 1ππ* state and a mixed 1πσ*/1π3s Rydberg state, from where three relaxation channels are observed: ring puckering, N-H bond cleavage, and ring opening via N-N bond breaking. The N-N bond breaking channel is the fastest process, occurring within one vibrational cycle of the Franc Condon active ring stretching mode. N-H bond cleavage is observed to be aminor channel, and occurs upon direct excitation to the mixed π3s/πσ* state. Finally, ring puckering occurs after a timescale of a few hundred fs because the molecules need time to find the gradient towards this conical intersection. However, this channel is accessed if the initially triggered processes are not successful. The quantum yields of the different channels were found to be very sensitive of the relative positioning of the excited states. In pyrazole and 5-methylpyrazole, N-Nbond cleavage dominates. In 1-, and 3-methylpyrazole, while the 1ππ* state drops in energy the dissociating 1πσ* valence state does not, and this leads to an increased barrier towards ring cleavage and a decreased the quantum yield for N-N bond cleavage. Upon excitation at 267 nm of 1- and 3-methylpyrazole, ring puckering is the only available pathway.

  • 3.
    Geng, Ting
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Schalk, Oliver
    Stockholm University, Faculty of Science, Department of Physics.
    Neville, Simon P.
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Dynamics in higher lying excited states: Valence to Rydberg transitions in the relaxation paths of pyrrole and methylated derivatives2017In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 146, no 14, article id 144307Article in journal (Refereed)
    Abstract [en]

    The involvement of intermediate Rydberg states in the relaxation dynamics of small organic molecules which, after excitation to the valence manifold, also return to the valence manifold is rarely observed. We report here that such a transiently populated Rydberg state may offer the possibility to modify the outcome of a photochemical reaction. In a time resolved photoelectron study on pyrrole and its methylated derivatives, N-methyl pyrrole and 2,5-dimethyl pyrrole, 6.2 eV photons (200 nm) are used to excite these molecules into a bright pi pi* state. In each case, a pi 3p-Rydberg state, either the B-1(pi 3p(y)) or the A(2)(pi 3p(z)) state, is populated within 20-50 fs after excitation. The wavepacket then proceeds to the lower lying A(2)(pi sigma*) state within a further 20 fs, at which point two competing reaction channels can be accessed: prompt N-H (N-CH3) bond cleavage or return to the ground state via a conical intersection accessed after ring puckering, the latter of which is predicted to require an additional 100-160 fs depending on the molecule.

  • 4.
    Geng, Ting
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Schalk, Oliver
    Stockholm University, Faculty of Science, Department of Physics.
    Neville, Simon P.
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Dynamics in higher lying excited states: Valence to Rydberg transitions in the relaxation paths of pyrrole and methylated derivativesManuscript (preprint) (Other academic)
    Abstract [en]

    The involvement of intermediate Rydberg states in the relaxation dynamics of small organic molecules which, after excitation to the valence manifold, also return to the valence manifold, is rarely observed. We report here that such a transiently populated Rydberg state may offer the possibility to modify the outcome of a photochemical reaction. In a time resolved photoelectron study on pyrrole and its methylated derivatives, N-methyl pyrrole and 2,5-dimethyl pyrrole, 6.2 eVphotons (200 nm) are used to excite these molecules into a bright ππ* state. In each case, a π3p-Rydberg state, either the B1(π3py) or the A2(π3pz) state, is populated within 20-50 fs after excitation. The wave packet then proceeds to the lower lyingA2(πσ*) state within a further 20 fs, at which point two competing reaction channels can be accessed: prompt NH (N-CH3) bond cleavage or ring puckering, the latter of which is predicted to require an additional 100 – 160 fs depending on the molecule.

  • 5.
    Gladh, Jörgen
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Öström, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Electron- and phonon-coupling in femtosecond laser-induced desorption of CO from Ru(0001)2013In: Surface Science, ISSN 0039-6028, E-ISSN 1879-2758, Vol. 615, p. 65-71Article in journal (Refereed)
    Abstract [en]

    We studied femtosecond laser-induced desorption of CO from Ru(0001) using intense near-infrared and visible femtosecond laser pulses. We find a pronounced wavelength dependence with a factor 3-4 higher desorption yield at comparable fluence when desorption is induced via 400 nm light, compared to 800 nm and attribute this difference to the difference in penetration depth of the incident light. All our data can be described using empirical friction-modeling to determine the desorption mechanism with the same mechanism for both wavelengths. We find that both hot electrons and phonons contribute to the desorption process.

  • 6.
    Kloda, Tomasz
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Matsuda, Akitaka
    Karlsson, Hans O.
    Elshakre, Mohamed
    Linusson, Per
    Stockholm University, Faculty of Science, Department of Physics.
    Eland, John H. D.
    Feifel, Raimund
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Strong-field photoionization of O-2 at intermediate light intensity2010In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 82, no 3, p. 33431-Article in journal (Refereed)
    Abstract [en]

    We investigated by electron spectroscopy the strong-field multiphoton ionization of O-2 molecules with ultrashort laser pulses in the intensity range between the multiphoton and tunneling regimes. The ionization proceeds by at least three different mechanisms, in addition to the eight- and nine-photon nonresonant pathways. Transient multiphoton resonances with vibrational Rydberg levels give rise to direct Freeman-type peaks with sublaser linewidth and spin-orbit splitting. Some resonance levels actually become populated and yield extremely narrow lines because of postpulse vibrational autoionization. When the lowest photon order resonance channel for the Rydberg states is closed, a third contribution becomes dominant with a main peak at 0.4 eV that shares its main properties with the recently discovered universal low-energy structure in the electron spectra of atoms and molecules [C. I. Blaga et al., Nat. Phys. 5, 335 (2009); W. Quan et al., Phys. Rev. Lett. 103, 093001 (2009)]. The variation of the Freeman resonance spectrum with the laser peak intensity is well correlated with the vibronic Franck-Condon factors for the overlap of the intermediate Rydberg state with the O-2 ground state. Accordingly, the Freeman peaks could be unambiguously assigned to individual vibronic multiphoton resonances, and the disappearance of the Freeman resonances at a certain laser intensity could be explained. The population of the autoionizing Rydberg states could be assigned similarly to such vibronic resonances.

  • 7. Oesterling, Sven
    et al.
    Schalk, Oliver
    Stockholm University, Faculty of Science, Department of Physics.
    Geng, Ting
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    de Vivie-Riedle, Regina
    Substituent effects on the relaxation dynamics of furan, furfural and β-furfural: a combined theoretical and experimental approach2017In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 19, p. 2025-2035Article in journal (Refereed)
    Abstract [en]

    For the series furan, furfural and β-furfural we investigated the effect of substituents and their positioning on the photoinduced relaxation dynamics in a combined theoretical and experimental approach. Using time resolved photoelectron spectroscopy with a high intensity probe pulse, we can, for the first time, follow the whole deactivation process of furan through a two photon probe signal. Using the extended 2-electron 2-orbital model [Nenov et al., J. Chem. Phys., 2011, 135, 034304] we explain the formation of one central conical intersection and predict the influence of the aldehyde group of the derivatives on its geometry. This, as well as the relaxation mechanisms from photoexcitation to the final outcome was investigated using a variety of theoretical methods. Complete active space self consistent field was used for on-the-fly calculations while complete active space perturbation theory and coupled cluster theory were used to accurately describe critical configurations. Experiment and theory show the relaxation dynamics of furfural and β-furfural to be slowed down, and together they disclose an additional deactivation pathway, which is attributed to the nO lonepair state introduced with the aldehyde group.

  • 8.
    Schalk, Oliver
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Geng, Ting
    Stockholm University, Faculty of Science, Department of Physics.
    Thompson, Travis
    Baluyot, Noel
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Tapavicza, Enrico
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Cyclohexadiene Revisited: A Time-Resolved Photoelectron Spectroscopy and ab Initio Study2016In: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 120, no 15, p. 2320-2329Article in journal (Refereed)
    Abstract [en]

    We have reinvestigated the excited state dynamics of cyclohexa-1,3-diene (CHD) with time-resolved photoelectron spectroscopy and fewest switches surface hopping molecular dynamics based on linear response time dependent density functional theory after excitation to the lowest lying pi pi* (1B) state. The combination of both theory and experiment revealed several new results: First, the dynamics progress on one single excited state surface. After an incubation time of 35 +/- 10 fs on the excited state, the dynamics proceed to the ground state in an additional 60 +/- 10 fs, either via a conrotatory ring-opening to hexatriene or back to the CHD ground state. Moreover, ring-opening predominantly occurs when the wavepacket crosses the region of strong nonadiabatic coupling with a positive velocity in the bond alternation coordinate. After 100 fs, trajectories remaining in the excited state must return to the CHD ground state. This extra time delay induces a revival of the photoelectron signal and is an experimental confirmation of the previously formulated model of two parallel reaction channels with distinct time constants. Finally, our simulations suggest that after the initially formed cis-Z-cis HT rotamer the trans-Z-trans isomer is formed, before the thermodynamical equilibrium of three possible rotamers is reached after 1 ps.

  • 9.
    Schalk, Oliver
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Stenrup, M.
    Geng, Ting
    Stockholm University, Faculty of Science, Department of Physics.
    Lindh, R.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Feifel, R.
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Influence of Alkoxy Groups on the Photoinduced Dynamics of Organic Molecules Exemplified on Alkyl Vinyl Ethers2015In: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 119, no 45, p. 11105-11112Article in journal (Refereed)
    Abstract [en]

    A series of different alkyl vinyl ethers is investigated to decipher the possible reaction channels upon photoexcitation to the pi 3s-Rydberg and the pi pi*-valence state at 200 nm using time-resolved photoelectron spectroscopy and on-the-fly time-dependent density functional theory dynamics simulations. The results indicate two possible relaxation pathways: (1) a radiationless decay through the pi pi*-state back to the ground state via torsion of the C=C double bond, in accordance with the dynamics found in ethylene; and (2) a fast dissociation of the C-O bond between the alkyl and the vinoxy group in the pi sigma*-state. The latter state can be accessed only after excitation to the pi 3s-Rydberg state (quantum yield of similar to 50% according to the dynamics simulations). Additionally, the excited state barrier leading to formation of a vinyl radical was found to be too high to be crossed. These results indicate that the dynamics of ethers crucially depend on the excitation wavelength and that the pi sigma*-state constitutes an important competitive reaction channel that leads to dissociation of the molecules.

  • 10.
    Viarbitskaya, Sviatlana
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Kapshai, Valery
    van der Meulen, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Size dependence of second-harmonic generation at the surface of microspheres2010In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 81, no 5, p. 53850-Article in journal (Refereed)
    Abstract [en]

    The resonance-enhanced surface second-harmonic generation (SHG) from a suspension of polystyrene microspheres was investigated as a function of particle size in a range of the order of the fundamental wavelength for two different second-harmonic-enhancing dyes-malachite green and pyridine 1. The two dyes gave the same strongly modulated pattern of the forward second-harmonic scattering efficiency. Direct comparison to the nonlinear Rayleigh-Gans-Debye (NLRGD) and nonlinear Wentzel-Kramers-Brillouin (NLWKB) model predictions showed that the NLWKB model reproduces the overall trend in the size dependence but fails with respect to the strong modulations. The standard NLRGD model was found to fail altogether in the present particle size range, which was well beyond the observed upper particle size for which the NLRGD and NLWKB models give comparable results. A generalization of the NLRGD model to allow for dispersion and to use the particle refractive indices instead of those of the surrounding medium extended its applicability range by almost an order of magnitude in particle size. There is a pronounced maximal SHG efficiency for particles with a radius that is close to the fundamental wavelength inside the particle. The optically soft particle approximation is inadequate to describe the SHG in this particle size range, as refraction and reflection of the waves at the particle surface have a decisive influence. Dispersion of the media plays a negligible role for particle sizes up to about twice the optimal one for SHG.

  • 11.
    Wang, Dong
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Larson, Åsa
    Stockholm University, Faculty of Science, Department of Physics.
    Karlsson, Hans O.
    Larson, Jonas
    Quantum interference structures in trapped ion dynamics beyond the Lamb-Dicke and rotating wave approximations2008In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 77, no 5Article in journal (Refereed)
    Abstract [en]

    We apply wave-packet methods to study an ion-trap system imposing neither the rotating wave nor the Lamb-Dicke approximations. By this approach we show the existence of states with restricted phase-space evolution as a genuine consequence of quantum interference between wave-packet fractions. A particular instance of such a state oscillates between maximal entanglement and pure disentanglement between the constitute subsystems, where the characteristic crossover time is very rapid. Over longer time periods the dynamics of these states exhibits collapse-revival patterns with well-resolved fractional revivals in autocorrelation, inversion, and entanglement.

  • 12.
    Wang, Dong
    et al.
    Stockholm University, Faculty of Science.
    Larson, Åsa
    Stockholm University, Faculty of Science, Department of Physics.
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Karlsson, Hans O.
    Molecular quantum wave-packet splitting and revivals in shared phase space2009In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 79, no 2, p. 23402-Article in journal (Refereed)
    Abstract [en]

    The evolution of a molecular wave packet created by an ultrashort laser pulse in a system of two coupled bound states is investigated by quantum dynamics calculations and semiclassical theory. Under suitable dynamical quantum interference conditions, the wave packet may be split into two separable fractions that move in different but partially overlapping regions of the energetically available phase space. Each wave-packet part can be individually addressed in the divided parts of the molecular phase space, and they are shown to go through separate long-term collapse-revival cycles analogous to those of wave packets moving in single anharmonic potentials. In a pump-probe scheme, the dynamics of the system would look very different depending on what internuclear distances are probed. The regular dynamics observable in the separated parts of the phase space takes on a quite irregular appearance in the regions that are shared by the wave-packet components. The wave-packet regularity is shown to depend sensitively on the pump pulse wavelength, which is a reflection of the energy range over which the quantum interference conditions are maintained. These conditions, as well as the wave-packet fraction revival times, are well reproduced by semiclassical theory.

  • 13. Yazdi, Milad Ghadami
    et al.
    Moud, Pouya. H.
    Marks, Kess
    Stockholm University, Faculty of Science, Department of Physics.
    Piskorz, Witold
    Östrom, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Kotarba, Andrzej
    Engvall, Klas
    Göthelid, Mats
    Naphthalene on Ni(111): Experimental and Theoretical Insights into Adsorption, Dehydrogenation, and Carbon Passivation2017In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 121, no 40, p. 22199-22207Article in journal (Refereed)
    Abstract [en]

    An attractive solution to mitigate tars and also to decompose lighter hydrocarbons in biomass gasification is secondary catalytic reforming, converting hydrocarbons to useful permanent gases. Albeit that it has been in use for a long time in fossil feedstock catalytic steam reforming, understanding of the catalytic processes is still limited. Naphthalene is typically present in the biomass gasification gas and to further understand the elementary steps of naphthalene transformation, we investigated the temperature dependent naphthalene adsorption, dehydrogenation and passivation on Ni(111). TPD (temperature-programmed desorption) and STM (scanning tunneling microscopy) in ultrahigh vacuum environment from 110 K up to 780 K, combined with DFT (density functional theory) were used in the study. Room temperature adsorption results in a flat naphthalene monolayer. DFT favors the dibridge[7] geometry but the potential energy surface is rather smooth and other adsorption geometries may coexist. DFT also reveals a pronounced dearomatization and charge transfer from the adsorbed molecule into the nickel surface. Dehydrogenation occurs in two steps, with two desorption peaks at approximately 450 and 600 K. The first step is due to partial dehydrogenation generating active hydrocarbon species that at higher temperatures migrates over the surface forming graphene. The graphene formation is accompanied by desorption of hydrogen in the high temperature TPD peak. The formation of graphene effectively passivates the surface both for hydrogen adsorption and naphthalene dissociation. In conclusion, the obtained results on the model naphthalene and Ni(111) system, provides insight into elementary steps of naphthalene adsorption, dehydrogenation, and carbon passivation, which may serve as a good starting point for rational design, development and optimization of the Ni catalyst surface, as well as process conditions, for the aromatic hydrocarbon reforming process.

  • 14.
    Öberg, Henrik
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Nestsiarenka, Yuliya
    Stockholm University, Faculty of Science, Department of Physics.
    Matsuda, A.
    Stockholm University, Faculty of Science, Department of Physics.
    Gladh, Jörgen
    Stockholm University, Faculty of Science, Department of Physics.
    Hansson, Tony
    Stockholm University, Faculty of Science, Department of Physics.
    Pettersson, Lars G.M.
    Stockholm University, Faculty of Science, Department of Physics.
    Öström, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Adsorption and Cyclotrimerization Kinetics of C2H2 at a Cu(110) Surface2012In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 116, no 17, p. 9550-9560Article in journal (Refereed)
    Abstract [en]

    The kinetics of acetylene adsorption and cyclotrimerization was studied by vibrational sum-frequency generation spectroscopy (SFG) and density functional theory (DFT) calculations. At low temperature, SFG shows two resonances corresponding to acetylene adsorbed in two different sites. Upon heating, two new vibrational resonances appear. We interpret these resonances as being due to C2H2 island formation and adsorbed C4H4, which is the intermediate in the subsequent cyclotrimerization reaction to form benzene. A kinetic model is applied, which allows determination of the relevant activation barriers. The barrier for C2H2 diffusion is determined to be 43 +/- 1 kJ/mol. The activation barrier for formation of the C4H4 intermediate is found to be 84 +/- 6 kJ/mol and the barrier for benzene formation 5 +/- 3 kJ/mol lower. Barriers to diffusion and formation of C4H4 and C6H6 obtained from DFT calculations are in quantitative agreement with the experiments once the locally high coverage in C2H2 islands is included.

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