Molecules and clusters in strong laser fields

Schulz, C. P.; Burnus, T.; Castro, Alberto; Gross, E. K. U.; Heidenreich, Andreas; Hertel, I. V.; Jortner, Joshua; Laarmann, Tim; Last, I.; Levis, Robert J.; Marques, Miguel A. L.; Romanov, Dmitri; Sáenz, Alejandro

doi:10.1007/978-3-540-68038-3_6

Cited by 4 publications

(6 citation statements)

References 291 publications

(487 reference statements)

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“…Hertel et al have systematically investigated time-dependent ionization and fragmentation in C 60 . By the end of the 1990s, the shortest pulse ever used to investigate the ultrafast dynamics in C 60 was 12 fs.…”

Section: Experimental Investigation Of Ultrafast Dynamicsmentioning

confidence: 99%

“…Since the first dipole-allowed transition is between HOMO and LUMO+1, the density accumulates mainly at LUMO+1. These changes can be directly probed experimentally. , As time evolves, the LUMO+1 and HOMO states move closer to the Fermi level (0 eV). This change is a result of lattice relaxation, similar to what we have found in the dark evolution.…”

Section: Theoretical Studymentioning

confidence: 99%

“…Due to our own interest, we emphasize the nonlinear optical response and, in particular, laser-induced dynamics, both of which have received considerable attention. We do not attempt to cover the fragmentation of C 60 , as it has been reviewed recently elsewhere . We refer the reader to other excellent reviews , for other properties.…”

Section: Introductionmentioning

confidence: 99%

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Nonlinear Optical Response and Ultrafast Dynamics in C₆₀

Zhang

George

2009

J. Phys. Chem. A

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Crossed molecular beams experiments were conducted to investigate the chemical dynamics of the reaction of dicarbon molecules, C(2)(X(1)Sigma(g)(+)/a(3)Pi(u)), with diacetylene, C(4)H(2)(X(1)Sigma(g)(+)) at two collision energies of 12.1 and 32.8 kJ mol(-1). The dynamics were found to be indirect, involved C(6)H(2) intermediates, and were dictated by an initial addition of the dicarbon molecule to the carbon-carbon triple bond of diacetylene. The initial collision complexes could isomerize. On the singlet surface, the resulting linear triacetylene molecule (C(6)H(2)(X(1)Sigma(g)(+))) decomposed without an exit barrier to form the linear 1,3,5-hexatriynyl radical (C(6)H(X(2)Pi)). On the triplet surface, the dynamics suggested at least a tight exit transition state involved in the fragmentation of a triplet C(6)H(2) intermediate to yield the 1,3,5-hexatriynyl radical (C(6)H(X(2)Pi)) plus atomic hydrogen. On the basis of the experimental data, we recommend an experimentally determined enthalpy of formation of the 1,3,5-hexatriynyl radical of 1014 +/- 27 kJ mol(-1) at 0 K. Our experimental results and the derived reaction mechanisms gain full support from electronic structure calculations on the singlet and triplet C(6)H(2) potential-energy surfaces. The identification of the 1,3,5-hexatriynyl radical under single collision conditions implies that the neutral-neutral reaction of dicarbon with diacetylene can lead to the formation of 1,3,5-hexatriynyl radicals in the interstellar medium and possibly in the hydrocarbon-rich atmospheres of planets and their moons such as Saturn's satellite Titan.

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Section: Experimental Investigation Of Ultrafast Dynamicsmentioning

confidence: 99%

Section: Theoretical Studymentioning

confidence: 99%

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Nonlinear Optical Response and Ultrafast Dynamics in C₆₀

Zhang

George

2009

J. Phys. Chem. A

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“…5−8 Many postionization techniques utilize photoionization schemes that provide rather small ionization volumeswhich can be of dimensions as small as 10 μm, 9,10 e.g., for ionization in the "strong field regime". 11 In order for SNMS techniques to access a large number of neutral species available in the ejecta plume, the overlap of the confined photoionization volume with the flux of ejecta has to be maximized. This also applies to the timing of sputtering and photoionization steps for schemes utilizing pulsed light sources.…”

Section: ■ Introductionmentioning

confidence: 99%

“…Secondary neutral mass spectrometry (SNMS) techniques aim to access a part of the large fraction of neutral species in the cloud of sputtered material by postionization in a dedicated ionization step subsequent to the sputtering event. − Many postionization techniques utilize photoionization schemes that provide rather small ionization volumeswhich can be of dimensions as small as 10 μm, , e.g., for ionization in the “strong field regime” . In order for SNMS techniques to access a large number of neutral species available in the ejecta plume, the overlap of the confined photoionization volume with the flux of ejecta has to be maximized.…”

Section: Introductionmentioning

confidence: 99%

Angular Distribution of Molecules Sputtered by Gas Cluster Ion Beams and Implications for Secondary Neutral Mass Spectrometry

Lorenz

Shard

Counsell³

et al. 2016

J. Phys. Chem. C

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We present experimental data on the angular distribution of Irganox 1010 organic molecules sputtered by large argon gas cluster projectiles (E/n = 5 eV, 10 keV Ar2000). Ejection probability distributions as derived from deposit patterns on planar collector surfaces were recorded at various angles of incidence of the primary cluster ion beam. The sputtered material is ejected at polar angles, on average, greater than 45° from the surface normal. At normal incidence there is no azimuthal dependence in the ejecta distribution, but the ejecta are forward directed even at incidence angles as low as 15°. After this initial rapid change, the ejecta distribution shows a rather weak dependence on the incidence angle of the primary ion beam and the polar, and azimuthal angles of preferred ejection remain relatively constant. Ejecta distributions agree with previously published results from molecular dynamics simulations for organic molecules sputtered with large argon gas cluster projectiles and are consistent with the picture derived from experimental data for metal target species. The close chemical resemblance of collector and target materials as identified by secondary ion mass spectrometry, and the large total volume of deposits accounting for over 75% of the sputtered material as inferred from symmetry considerations, indicate that a large fraction of the sputtered material is intact molecules. Findings are discussed with respect to the utilization of large cluster projectiles as primary ion beams in secondary neutral mass spectrometry.

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Femtosecond pulse shaping as analytic tool in mass spectrometry of complex polyatomic systems

Laarmann

Shchatsinin

Singh

et al. 2008

J. Phys. B: At. Mol. Opt. Phys.

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An additional dimension to mass spectrometric studies on building blocks of proteins is discussed in this paper. The present approach is based on tailored femtosecond laser pulses, using the concept of strong-field pulse shaping in an adaptive feedback loop. We show that control strategies making use of coherent properties of the electromagnetic wave allow one to break pre-selected backbone bonds in amino acid complexes that may be regarded as peptide model systems. Studies on different chromophores, such as phenylalanine and alanine, while keeping the backbone structure unchanged elucidates the effect of the excitation dynamics on the relaxation pathways. The observation of protonated species in the corresponding mass spectra indicates that optimal control of ultrafast laser pulses may even be useful to study intramolecular reactions such as hydrogen- or proton-transfer in particular cases. This opens new perspectives for biophysical and biochemical research, since these photochemical reactions are suggested to explain, e.g. photostability of DNA.

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Molecules and clusters in strong laser fields

Cited by 4 publications

References 291 publications

Nonlinear Optical Response and Ultrafast Dynamics in C₆₀

Nonlinear Optical Response and Ultrafast Dynamics in C₆₀

Angular Distribution of Molecules Sputtered by Gas Cluster Ion Beams and Implications for Secondary Neutral Mass Spectrometry

Femtosecond pulse shaping as analytic tool in mass spectrometry of complex polyatomic systems

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Molecules and clusters in strong laser fields

Cited by 4 publications

References 291 publications

Nonlinear Optical Response and Ultrafast Dynamics in C60

Nonlinear Optical Response and Ultrafast Dynamics in C60

Angular Distribution of Molecules Sputtered by Gas Cluster Ion Beams and Implications for Secondary Neutral Mass Spectrometry

Femtosecond pulse shaping as analytic tool in mass spectrometry of complex polyatomic systems

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Nonlinear Optical Response and Ultrafast Dynamics in C₆₀

Nonlinear Optical Response and Ultrafast Dynamics in C₆₀