Elementary Processes in Peptides: Electron Mobility and Dissociation in Peptide Cations in the Gas Phase

Weinkauf, R.; Schanen, P.; Yang, Daoshan; Soukara, Stella; Schlag, E. W.

doi:10.1021/j100028a029

Cited by 162 publications

(214 citation statements)

References 13 publications

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“…On a longer (tens of femtoseconds) time scale, nuclear motion results in electron hole localization at a particular molecular site that can be different from the site of initial ionization. This has been observed in mass spectrometric measurements and in pump-probe experiments with femtosecond time resolution [12], including the most recent ones [13] which suggest that faster dynamics may well be occurring. However, experimental verification of the critical short-time electron correlation driven dynamics is still lacking.…”

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confidence: 71%

“…Even in the case of such relatively involved dynamics, the delay-dependent spLEAD transition probability mimics the survival probability of the sudden ionization state well over the first two revivals. One has to keep in mind that the fixed-nuclei approximation adopted here is not expected to be valid on the time scale beyond several tens of femtoseconds [12,13]. However, the demonstrated ability of the spLEAD signal to reproduce the dynamics over longer time scales can be used to track the onset of the nuclear motion effects in time by comparing the experimental and the theoretical (fixed-nuclei) signals.…”

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confidence: 99%

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Single-Photon Laser-Enabled Auger Spectroscopy for Measuring Attosecond Electron-Hole Dynamics

Cooper

Averbukh

2013

Phys. Rev. Lett.

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We propose and simulate a new type of attosecond time-resolved spectroscopy of electron hole dynamics, applicable particularly to ultrafast hole migration. Attosecond ionization in the innervalence region is followed by a VUV probe inducing single-photon laser-enabled Auger decay, a onephoton two-electron transition filling the inner-valence vacancy. The double ionization probability as a function of the attosecond pump-VUV probe delay captures efficiently the ultrafast innervalence hole dynamics. Detailed ab initio calculations are presented for inner-valence hole migration in glycine.

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confidence: 71%

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confidence: 99%

Single-Photon Laser-Enabled Auger Spectroscopy for Measuring Attosecond Electron-Hole Dynamics

Cooper

Averbukh

2013

Phys. Rev. Lett.

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“…Unlike DNA, these studies do not dispute the fact that the polypeptide can conduct current, but instead they try to find out the exact mechanism of conduction; whether the conduction is done by protons, holes, or direct electron transfer, and then to try and speculate on what exactly is the method of carrier transport by studying the dynamics of the peptide in question. The earlier work by Weinkauf et al [26] showed that charge transfer processes in suspended amino acids in the gas phase is directly related to their chemical reactivity. This study was done by laser photoexcitation of specific amino acids and measurements of the radiation of their chromophore sidechains.…”

Section: Protein Conductance Experimentsmentioning

confidence: 99%

Electrical Conductance in Biological Molecules

Shinwari

Deen

Starikov

et al. 2010

Adv Funct Materials

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Nucleic acids and proteins are not only biologically important polymers: They have recently been recognized as novel functional materials surpassing in many aspects the conventional ones. Although Herculean efforts have been undertaken to unravel fine functioning mechanisms of the biopolymers in question, there is still much more to be done. This particular paper presents the topic of biomolecular charge transport, with a particular focus on charge transfer/transport in DNA and protein molecules. Here the experimentally revealed details, as well as the presently available theories, of charge transfer/transport along these biopolymers are critically reviewed and analyzed. A summary of the active research in this field is also given, along with a number of practical recommendations.)Received: ((will be filled in by the editorial staff))Revised: ((will be filled in by the editorial staff))

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“…Particularly interesting for applications are hydrocarbon molecules. It has been shown previously that dissociation of these molecules is accompanied by extraordinarily rich internal electronic dynamics [7,8] that are still far from being understood.We study the fragmentation of acetylene, C 2 H 2 , subject to fully determined few-cycle laser electric fields. In our experiments we generate 4.5 fs laser pulses by spectral broadening of ≈ 25 fs laser pulses from a Titanium-Sapphire laser amplifier system in a 1 m long hollow-core glass capillary filled with argon and subsequent recompression by several bounces from chirped mirrors.…”

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confidence: 99%

mentioning

confidence: 99%

Fragmentation Control of a Polyatomic Molecule by fully determined Laser-Fields

Xie

Roither

Schöffler

et al. 2013

EPJ Web of Conferences

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Abstract. Strong-field control of acetylene fragmentation by fully determined fewcycle laser pulses is demonstrated. The control mechanism is shown to be based on electron recollision and inelastic ionization from inner-valence molecular orbitals.Chemistry is usually perceived as breaking and making molecular bonds. These processes that typically occur on the timescale of tens of femtoseconds (fs) to nanoseconds are preceded and ultimately governed by the much faster intra-molecular motion of electrons that proceeds on the sub-femtosecond timescale [1,2]. This timescale matches the light oscillations of laser pulses carried at frequencies in the visible and near-infrared. As the electric field of strong laser pulses is capable of exerting forces onto the electrons that are comparable to those of the binding forces, it becomes possible to drive the intra-molecular electron density by light. Deterministic steering, however, requires fully controlled laser electric fields, for example few-cycle pulses with a locked carrier-envelope (CE) offset frequency. Using such pulses it has been shown that the localization of an electron during dissociation of D + 2 [3, 4] and CO + [5], as well as the directionality of multiple dissociative channels of CO [6] can be controlled.In this submission we extend this scheme from simple diatomics studied so far to chemically more relevant polyatomic molecules. Particularly interesting for applications are hydrocarbon molecules. It has been shown previously that dissociation of these molecules is accompanied by extraordinarily rich internal electronic dynamics [7,8] that are still far from being understood.We study the fragmentation of acetylene, C 2 H 2 , subject to fully determined few-cycle laser electric fields. In our experiments we generate 4.5 fs laser pulses by spectral broadening of ≈ 25 fs laser pulses from a Titanium-Sapphire laser amplifier system in a 1 m long hollow-core glass capillary filled with argon and subsequent recompression by several bounces from chirped mirrors. The pulses, with a spectrum centered around 750 nm are directed into an ultrahigh vacuum chamber where they are focused onto a cold supersonic jet of randomly aligned acetylene molecules. The three-dimensional momenta of the resulting ionic fragments from a single molecule are recorded as described previously [9]. As at maximum only one molecule interacts with one laser pulse it becomes possible to measure the duration and the carrier-envelope (CE) phase of each of the few-cycle pulses delivered at the repetition rate of 5 kHz on a single-shot basis [10][11][12] instead of actively stabilizing it, leading to improved accuracy. The peak intensity of the laser pulses on target was 1.5×10 14 W/cm 2 , as determined from a separate calibration measurement using single ionization of argon atoms in circularly polarized light [13]. a

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Elementary Processes in Peptides: Electron Mobility and Dissociation in Peptide Cations in the Gas Phase

Cited by 162 publications

References 13 publications

Single-Photon Laser-Enabled Auger Spectroscopy for Measuring Attosecond Electron-Hole Dynamics

Single-Photon Laser-Enabled Auger Spectroscopy for Measuring Attosecond Electron-Hole Dynamics

Electrical Conductance in Biological Molecules

Fragmentation Control of a Polyatomic Molecule by fully determined Laser-Fields

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