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  1. Article ; Online: Molecular photodissociation dynamics revealed by Coulomb explosion imaging.

    Crane, Stuart W / Lee, Jason W L / Ashfold, Michael N R / Rolles, Daniel

    Physical chemistry chemical physics : PCCP

    2023  Volume 25, Issue 25, Page(s) 16672–16698

    Abstract: Coulomb explosion imaging (CEI) methods are finding ever-growing use as a means of exploring and distinguishing the static stereo-configurations of small quantum systems (molecules, clusters, ...

    Abstract Coulomb explosion imaging (CEI) methods are finding ever-growing use as a means of exploring and distinguishing the static stereo-configurations of small quantum systems (molecules, clusters,
    Language English
    Publishing date 2023-06-28
    Publishing country England
    Document type Journal Article ; Review
    ZDB-ID 1476244-4
    ISSN 1463-9084 ; 1463-9076
    ISSN (online) 1463-9084
    ISSN 1463-9076
    DOI 10.1039/d3cp01740k
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article ; Online: Initial-site characterization of hydrogen migration following strong-field double-ionization of ethanol.

    Severt, Travis / Weckwerth, Eleanor / Kaderiya, Balram / Feizollah, Peyman / Jochim, Bethany / Borne, Kurtis / Ziaee, Farzaneh / P, Kanaka Raju / Carnes, Kevin D / Dantus, Marcos / Rolles, Daniel / Rudenko, Artem / Wells, Eric / Ben-Itzhak, Itzik

    Nature communications

    2024  Volume 15, Issue 1, Page(s) 74

    Abstract: An essential problem in photochemistry is understanding the coupling of electronic and nuclear dynamics in molecules, which manifests in processes such as hydrogen migration. Measurements of hydrogen migration in molecules that have more than two ... ...

    Abstract An essential problem in photochemistry is understanding the coupling of electronic and nuclear dynamics in molecules, which manifests in processes such as hydrogen migration. Measurements of hydrogen migration in molecules that have more than two equivalent hydrogen sites, however, produce data that is difficult to compare with calculations because the initial hydrogen site is unknown. We demonstrate that coincidence ion-imaging measurements of a few deuterium-tagged isotopologues of ethanol can determine the contribution of each initial-site composition to hydrogen-rich fragments following strong-field double ionization. These site-specific probabilities produce benchmarks for calculations and answer outstanding questions about photofragmentation of ethanol dications; e.g., establishing that the central two hydrogen atoms are 15 times more likely to abstract the hydroxyl proton than a methyl-group proton to form H[Formula: see text] and that hydrogen scrambling, involving the exchange of hydrogen between different sites, is important in H
    Language English
    Publishing date 2024-01-02
    Publishing country England
    Document type Journal Article
    ZDB-ID 2553671-0
    ISSN 2041-1723 ; 2041-1723
    ISSN (online) 2041-1723
    ISSN 2041-1723
    DOI 10.1038/s41467-023-44311-x
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  3. Article ; Online: Differentiating Three-Dimensional Molecular Structures Using Laser-Induced Coulomb Explosion Imaging.

    Lam, Huynh Van Sa / Venkatachalam, Anbu Selvam / Bhattacharyya, Surjendu / Chen, Keyu / Borne, Kurtis / Wang, Enliang / Boll, Rebecca / Jahnke, Till / Kumarappan, Vinod / Rudenko, Artem / Rolles, Daniel

    Physical review letters

    2024  Volume 132, Issue 12, Page(s) 123201

    Abstract: Coulomb explosion imaging (CEI) with x-ray free electron lasers has recently been shown to be a powerful method for obtaining detailed structural information of gas-phase planar ring molecules [R. Boll et al., X-ray multiphoton-induced Coulomb explosion ... ...

    Abstract Coulomb explosion imaging (CEI) with x-ray free electron lasers has recently been shown to be a powerful method for obtaining detailed structural information of gas-phase planar ring molecules [R. Boll et al., X-ray multiphoton-induced Coulomb explosion images complex single molecules, Nat. Phys. 18, 423 (2022).NPAHAX1745-247310.1038/s41567-022-01507-0]. In this Letter, we investigate the potential of CEI driven by a tabletop laser and extend this approach to differentiating three-dimensional structures. We study the static CEI patterns of planar and nonplanar organic molecules that resemble the structures of typical products formed in ring-opening reactions. Our results reveal that each molecule exhibits a well-localized and distinctive pattern in three-dimensional fragment-ion momentum space. We find that these patterns yield direct information about the molecular structures and can be qualitatively reproduced using a classical Coulomb explosion simulation. Our findings suggest that laser-induced CEI can serve as a robust method for differentiating molecular structures of organic ring and chain molecules. As such, it holds great promise as a method for following ultrafast structural changes, e.g., during ring-opening reactions, by tracking the motion of individual atoms in pump-probe experiments.
    Language English
    Publishing date 2024-04-05
    Publishing country United States
    Document type Journal Article
    ZDB-ID 208853-8
    ISSN 1079-7114 ; 0031-9007
    ISSN (online) 1079-7114
    ISSN 0031-9007
    DOI 10.1103/PhysRevLett.132.123201
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  4. Article ; Online: Multiparticle Cumulant Mapping for Coulomb Explosion Imaging.

    Cheng, Chuan / Frasinski, Leszek J / Moğol, Gönenç / Allum, Felix / Howard, Andrew J / Rolles, Daniel / Bucksbaum, Philip H / Brouard, Mark / Forbes, Ruaridh / Weinacht, Thomas

    Physical review letters

    2023  Volume 130, Issue 9, Page(s) 93001

    Abstract: We extend covariance velocity map ion imaging to four particles, establishing cumulant mapping and allowing for measurements that provide insights usually associated with coincidence detection, but at much higher count rates. Without correction, a ... ...

    Abstract We extend covariance velocity map ion imaging to four particles, establishing cumulant mapping and allowing for measurements that provide insights usually associated with coincidence detection, but at much higher count rates. Without correction, a fourfold covariance analysis is contaminated by the pairwise correlations of uncorrelated events, but we have addressed this with the calculation of a full cumulant, which subtracts pairwise correlations. We demonstrate the approach on the four-body breakup of formaldehyde following strong field multiple ionization in few-cycle laser pulses. We compare Coulomb explosion imaging for two different pulse durations (30 and 6 fs), highlighting the dynamics that can take place on ultrafast timescales. These results have important implications for Coulomb explosion imaging as a tool for studying ultrafast structural changes in molecules, a capability that is especially desirable for high-count-rate x-ray free-electron laser experiments.
    Language English
    Publishing date 2023-02-24
    Publishing country United States
    Document type Journal Article
    ZDB-ID 208853-8
    ISSN 1079-7114 ; 0031-9007
    ISSN (online) 1079-7114
    ISSN 0031-9007
    DOI 10.1103/PhysRevLett.130.093001
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  5. Article ; Online: Single- and multi-photon-induced ultraviolet excitation and photodissociation of CH

    Ziaee, Farzaneh / Borne, Kurtis / Forbes, Ruaridh / P, Kanaka Raju / Malakar, Yubaraj / Kaderiya, Balram / Severt, Travis / Ben-Itzhak, Itzik / Rudenko, Artem / Rolles, Daniel

    Physical chemistry chemical physics : PCCP

    2023  Volume 25, Issue 14, Page(s) 9999–10010

    Abstract: The UV-induced photodissociation dynamics of iodomethane ( ... ...

    Abstract The UV-induced photodissociation dynamics of iodomethane (CH
    Language English
    Publishing date 2023-04-05
    Publishing country England
    Document type Journal Article
    ZDB-ID 1476244-4
    ISSN 1463-9084 ; 1463-9076
    ISSN (online) 1463-9084
    ISSN 1463-9076
    DOI 10.1039/d3cp00498h
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  6. Article ; Online: Hydrogen migration in inner-shell ionized halogenated cyclic hydrocarbons.

    Abid, Abdul Rahman / Bhattacharyya, Surjendu / Venkatachalam, Anbu Selvam / Pathak, Shashank / Chen, Keyu / Lam, Huynh Van Sa / Borne, Kurtis / Mishra, Debadarshini / Bilodeau, René C / Dumitriu, Ileana / Berrah, Nora / Patanen, Minna / Rolles, Daniel

    Scientific reports

    2023  Volume 13, Issue 1, Page(s) 2107

    Abstract: We have studied the fragmentation of the brominated cyclic hydrocarbons bromocyclo-propane, bromocyclo-butane, and bromocyclo-pentane upon Br(3d) and C(1s) inner-shell ionization using coincidence ion momentum imaging. We observe a substantial yield of ... ...

    Abstract We have studied the fragmentation of the brominated cyclic hydrocarbons bromocyclo-propane, bromocyclo-butane, and bromocyclo-pentane upon Br(3d) and C(1s) inner-shell ionization using coincidence ion momentum imaging. We observe a substantial yield of CH
    Language English
    Publishing date 2023-02-06
    Publishing country England
    Document type Journal Article
    ZDB-ID 2615211-3
    ISSN 2045-2322 ; 2045-2322
    ISSN (online) 2045-2322
    ISSN 2045-2322
    DOI 10.1038/s41598-023-28694-x
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  7. Article ; Online: An Experimental Protocol for Femtosecond NIR/UV - XUV Pump-Probe Experiments with Free-Electron Lasers.

    Rolles, Daniel / Boll, Rebecca / Erk, Benjamin / Rompotis, Dimitrios / Manschwetus, Bastian

    Journal of visualized experiments : JoVE

    2018  , Issue 140

    Abstract: This protocol describes key steps in performing and analyzing femtosecond pump-probe experiments that combine a femtosecond optical laser with a free-electron laser. This includes methods to establish the spatial and temporal overlap between the optical ... ...

    Abstract This protocol describes key steps in performing and analyzing femtosecond pump-probe experiments that combine a femtosecond optical laser with a free-electron laser. This includes methods to establish the spatial and temporal overlap between the optical and free-electron laser pulses during the experiment, as well as important aspects of the data analysis, such as corrections for arrival time jitter, which are necessary to obtain high-quality pump-probe data sets with the best possible temporal resolution. These methods are demonstrated for an exemplary experiment performed at the FLASH (Free-electron LASer Hamburg) free-electron laser in order to study ultrafast photochemistry in gas-phase molecules by means of velocity map ion imaging. However, most of the strategies are also applicable to similar pump-probe experiments using other targets or other experimental techniques.
    MeSH term(s) Electrons/therapeutic use ; Lasers
    Language English
    Publishing date 2018-10-23
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't ; Video-Audio Media
    ISSN 1940-087X
    ISSN (online) 1940-087X
    DOI 10.3791/57055
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  8. Article ; Online: Valence shell electronically excited states of norbornadiene and quadricyclane.

    Cooper, Joseph C / Holland, David M P / Ingle, Rebecca A / Bonanomi, Matteo / Faccialà, Davide / De Oliveira, Nelson / Abid, Abdul R / Bachmann, Julien / Bhattacharyya, Surjendu / Borne, Kurtis / Bosch, Michael / Centurion, Martin / Chen, Keyu / Forbes, Ruaridh J G / Lam, Huynh V S / Odate, Asami / Rudenko, Artem / Venkatachalam, Anbu S / Vozzi, Caterina /
    Wang, Enliang / Weber, Peter M / Ashfold, Michael N R / Kirrander, Adam / Rolles, Daniel

    The Journal of chemical physics

    2024  Volume 160, Issue 6

    Abstract: The absolute photoabsorption cross sections of norbornadiene (NBD) and quadricyclane (QC), two isomers with chemical formula C7H8 that are attracting much interest for solar energy storage applications, have been measured from threshold up to 10.8 eV ... ...

    Abstract The absolute photoabsorption cross sections of norbornadiene (NBD) and quadricyclane (QC), two isomers with chemical formula C7H8 that are attracting much interest for solar energy storage applications, have been measured from threshold up to 10.8 eV using the Fourier transform spectrometer at the SOLEIL synchrotron radiation facility. The absorption spectrum of NBD exhibits some sharp structure associated with transitions into Rydberg states, superimposed on several broad bands attributable to valence excitations. Sharp structure, although less pronounced, also appears in the absorption spectrum of QC. Assignments have been proposed for some of the absorption bands using calculated vertical transition energies and oscillator strengths for the electronically excited states of NBD and QC. Natural transition orbitals indicate that some of the electronically excited states in NBD have a mixed Rydberg/valence character, whereas the first ten excited singlet states in QC are all predominantly Rydberg in the vertical region. In NBD, a comparison between the vibrational structure observed in the experimental 11B1-11A1 (3sa1 ← 5b1) band and that predicted by Franck-Condon and Herzberg-Teller modeling has necessitated a revision of the band origin and of the vibrational assignments proposed previously. Similar comparisons have encouraged a revision of the adiabatic first ionization energy of NBD. Simulations of the vibrational structure due to excitation from the 5b2 orbital in QC into 3p and 3d Rydberg states have allowed tentative assignments to be proposed for the complex structure observed in the absorption bands between ∼5.4 and 7.0 eV.
    Language English
    Publishing date 2024-02-13
    Publishing country United States
    Document type Journal Article
    ZDB-ID 3113-6
    ISSN 1089-7690 ; 0021-9606
    ISSN (online) 1089-7690
    ISSN 0021-9606
    DOI 10.1063/5.0187707
    Database MEDical Literature Analysis and Retrieval System OnLINE

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    In stock of ZB MED Bonn / Germany

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  9. Article: An experimental protocol for femtosecond nir/uv - xuv pump-probe experiments with free-electron lasers

    Rolles, Daniel / Boll, Rebecca / Erk, Benjamin / Rompotis, Dimitrios / Manschwetus, Bastian

    Journal of visualized experiments. 2018 Oct. 23, , no. 140

    2018  

    Abstract: This protocol describes key steps in performing and analyzing femtosecond pump-probe experiments that combine a femtosecond optical laser with a free-electron laser. This includes methods to establish the spatial and temporal overlap between the optical ... ...

    Abstract This protocol describes key steps in performing and analyzing femtosecond pump-probe experiments that combine a femtosecond optical laser with a free-electron laser. This includes methods to establish the spatial and temporal overlap between the optical and free-electron laser pulses during the experiment, as well as important aspects of the data analysis, such as corrections for arrival time jitter, which are necessary to obtain high-quality pump-probe data sets with the best possible temporal resolution. These methods are demonstrated for an exemplary experiment performed at the FLASH (Free-electron LASer Hamburg) free-electron laser in order to study ultrafast photochemistry in gas-phase molecules by means of velocity map ion imaging. However, most of the strategies are also applicable to similar pump-probe experiments using other targets or other experimental techniques.
    Keywords data collection ; gases ; image analysis ; lasers ; photochemistry
    Language English
    Dates of publication 2018-1023
    Size p. e57055.
    Publishing place Journal of Visualized Experiments
    Document type Article
    ZDB-ID 2259946-0
    ISSN 1940-087X
    ISSN 1940-087X
    DOI 10.3791/57055
    Database NAL-Catalogue (AGRICOLA)

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  10. Article ; Online: Multiple-core-hole resonance spectroscopy with ultraintense X-ray pulses.

    Rörig, Aljoscha / Son, Sang-Kil / Mazza, Tommaso / Schmidt, Philipp / Baumann, Thomas M / Erk, Benjamin / Ilchen, Markus / Laksman, Joakim / Music, Valerija / Pathak, Shashank / Rivas, Daniel E / Rolles, Daniel / Serkez, Svitozar / Usenko, Sergey / Santra, Robin / Meyer, Michael / Boll, Rebecca

    Nature communications

    2023  Volume 14, Issue 1, Page(s) 5738

    Abstract: Understanding the interaction of intense, femtosecond X-ray pulses with heavy atoms is crucial for gaining insights into the structure and dynamics of matter. One key aspect of nonlinear light-matter interaction was, so far, not studied systematically at ...

    Abstract Understanding the interaction of intense, femtosecond X-ray pulses with heavy atoms is crucial for gaining insights into the structure and dynamics of matter. One key aspect of nonlinear light-matter interaction was, so far, not studied systematically at free-electron lasers-its dependence on the photon energy. Here, we use resonant ion spectroscopy to map out the transient electronic structures occurring during the complex charge-up pathways of xenon. Massively hollow atoms featuring up to six simultaneous core holes determine the spectra at specific photon energies and charge states. We also illustrate how different X-ray pulse parameters, which are usually intertwined, can be partially disentangled. The extraction of resonance spectra is facilitated by the possibility of working with a constant number of photons per X-ray pulse at all photon energies and the fact that the ion yields become independent of the peak fluence beyond a saturation point. Our study lays the groundwork for spectroscopic investigations of transient atomic species in exotic, multiple-core-hole states that have not been explored previously.
    Language English
    Publishing date 2023-09-15
    Publishing country England
    Document type Journal Article
    ZDB-ID 2553671-0
    ISSN 2041-1723 ; 2041-1723
    ISSN (online) 2041-1723
    ISSN 2041-1723
    DOI 10.1038/s41467-023-41505-1
    Database MEDical Literature Analysis and Retrieval System OnLINE

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