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  1. Article ; Online: Efficient generation of the 7th harmonic of Ti:sapphire (114.6 nm) vacuum ultraviolet pulses with 60 fs duration by non-collinear four-wave mixing in argon.

    Forbes, Ruaridh / Hockett, Paul / Lausten, Rune

    Optics letters

    2021  Volume 47, Issue 10, Page(s) 2410–2413

    Abstract: The recent advances in femtosecond vacuum UV (VUV) pulse generation, pioneered by the work of Noack et al., has enabled new experiments in ultrafast time-resolved spectroscopy. Expanding on this work, we report the generation of 60 fs VUV pulses at the ... ...

    Abstract The recent advances in femtosecond vacuum UV (VUV) pulse generation, pioneered by the work of Noack et al., has enabled new experiments in ultrafast time-resolved spectroscopy. Expanding on this work, we report the generation of 60 fs VUV pulses at the 7th harmonic of Ti:sapphire with more than 50 nJ of pulse energy at a repetition rate of 1 kHz. The 114.6 nm pulses are produced using non-collinear four-wave difference-frequency mixing in argon. The non-collinear geometry increases the phase-matching pressure, and results in a conversion efficiency of ∼10
    Language English
    Publishing date 2021-10-19
    Publishing country United States
    Document type Journal Article
    ISSN 1539-4794
    ISSN (online) 1539-4794
    DOI 10.1364/OL.457070
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article ; Online: Auger electron angular distributions following excitation or ionization from the Xe 3d and F 1s levels in xenon difluoride.

    Forbes, Ruaridh / Hockett, Paul / Powis, Ivan / Bozek, John D / Pratt, Stephen T / Holland, David M P

    Physical chemistry chemical physics : PCCP

    2022  Volume 24, Issue 3, Page(s) 1367–1379

    Abstract: Linearly polarized synchrotron radiation has been used to record polarization dependent, non-resonant Auger electron spectra of ... ...

    Abstract Linearly polarized synchrotron radiation has been used to record polarization dependent, non-resonant Auger electron spectra of XeF
    Language English
    Publishing date 2022-01-19
    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/d1cp04797c
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  3. 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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  4. Article ; Online: Ultrafast Molecular Frame Quantum Tomography.

    Morrigan, Luna / Neville, Simon P / Gregory, Margaret / Boguslavskiy, Andrey E / Forbes, Ruaridh / Wilkinson, Iain / Lausten, Rune / Stolow, Albert / Schuurman, Michael S / Hockett, Paul / Makhija, Varun

    Physical review letters

    2023  Volume 131, Issue 19, Page(s) 193001

    Abstract: We develop and experimentally demonstrate a methodology for a full molecular frame quantum tomography (MFQT) of dynamical polyatomic systems. We exemplify this approach through the complete characterization of an electronically nonadiabatic wave packet ... ...

    Abstract We develop and experimentally demonstrate a methodology for a full molecular frame quantum tomography (MFQT) of dynamical polyatomic systems. We exemplify this approach through the complete characterization of an electronically nonadiabatic wave packet in ammonia (NH_{3}). The method exploits both energy and time-domain spectroscopic data, and yields the lab frame density matrix (LFDM) for the system, the elements of which are populations and coherences. The LFDM fully characterizes electronic and nuclear dynamics in the molecular frame, yielding the time- and orientation-angle dependent expectation values of any relevant operator. For example, the time-dependent molecular frame electronic probability density may be constructed, yielding information on electronic dynamics in the molecular frame. In NH_{3}, we observe that electronic coherences are induced by nuclear dynamics which nonadiabatically drive electronic motions (charge migration) in the molecular frame. Here, the nuclear dynamics are rotational and it is nonadiabatic Coriolis coupling which drives the coherences. Interestingly, the nuclear-driven electronic coherence is preserved over longer timescales. In general, MFQT can help quantify entanglement between electronic and nuclear degrees of freedom, and provide new routes to the study of ultrafast molecular dynamics, charge migration, quantum information processing, and optimal control schemes.
    Language English
    Publishing date 2023-11-24
    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.131.193001
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  5. Article ; Online: Filming enhanced ionization in an ultrafast triatomic slingshot.

    Howard, Andrew J / Britton, Mathew / Streeter, Zachary L / Cheng, Chuan / Forbes, Ruaridh / Reynolds, Joshua L / Allum, Felix / McCracken, Gregory A / Gabalski, Ian / Lucchese, Robert R / McCurdy, C William / Weinacht, Thomas / Bucksbaum, Philip H

    Communications chemistry

    2023  Volume 6, Issue 1, Page(s) 81

    Abstract: Filming atomic motion within molecules is an active pursuit of molecular physics and quantum chemistry. A promising method is laser-induced Coulomb Explosion Imaging (CEI) where a laser pulse rapidly ionizes many electrons from a molecule, causing the ... ...

    Abstract Filming atomic motion within molecules is an active pursuit of molecular physics and quantum chemistry. A promising method is laser-induced Coulomb Explosion Imaging (CEI) where a laser pulse rapidly ionizes many electrons from a molecule, causing the remaining ions to undergo Coulomb repulsion. The ion momenta are used to reconstruct the molecular geometry which is tracked over time (i.e., filmed) by ionizing at an adjustable delay with respect to the start of interatomic motion. Results are distorted, however, by ultrafast motion during the ionizing pulse. We studied this effect in water and filmed the rapid "slingshot" motion that enhances ionization and distorts CEI results. Our investigation uncovered both the geometry and mechanism of the enhancement which may inform CEI experiments in many other polyatomic molecules.
    Language English
    Publishing date 2023-04-27
    Publishing country England
    Document type Journal Article
    ZDB-ID 2929562-2
    ISSN 2399-3669 ; 2399-3669
    ISSN (online) 2399-3669
    ISSN 2399-3669
    DOI 10.1038/s42004-023-00882-w
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  6. 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
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  7. Article ; Online: A quantum molecular movie: polyad predissociation dynamics in the VUV excited 3pσ

    Makhija, Varun / Boguslavskiy, Andrey E / Forbes, Ruaridh / Veyrinas, Kevin / Wilkinson, Iain / Lausten, Rune / Schuurman, Michael S / Grant, Edward R / Stolow, Albert

    Faraday discussions

    2021  Volume 228, Page(s) 191–225

    Abstract: The optical formation of coherent superposition states, a wavepacket, can allow the study of zeroth-order states, the evolution of which exhibit structural and electronic changes as a function of time: this leads to the notion of a molecular movie. ... ...

    Abstract The optical formation of coherent superposition states, a wavepacket, can allow the study of zeroth-order states, the evolution of which exhibit structural and electronic changes as a function of time: this leads to the notion of a molecular movie. Intramolecular vibrational energy redistribution, due to anharmonic coupling between modes, is the molecular movie considered here. There is no guarantee, however, that the formed superposition will behave semi-classically (e.g. Gaussian wavepacket dynamics) or even as an intuitively useful zeroth-order state. Here we present time-resolved photoelectron spectroscopy (TRPES) studies of an electronically excited triatomic molecule wherein the vibrational dynamics must be treated quantum mechanically and the simple picture of population flow between coupled normal modes fails. Specifically, we report on vibronic wavepacket dynamics in the zeroth-order 3pσ2Σu Rydberg state of NO2. This wavepacket exemplifies two general features of excited state dynamics in polyatomic molecules: anharmonic multimodal vibrational coupling (forming polyads); nonadiabatic coupling between nuclear and electronic coordinates, leading to predissociation. The latter suggests that the polyad vibrational states in the zeroth-order 3p Rydberg manifold are quasi-bound and best understood to be scattering resonances. We observed a rapid dephasing of an initially prepared 'bright' valence state into the relatively long-lived 3p Rydberg state whose multimodal vibrational dynamics and decay we monitor as a function of time. Our quantum simulations, based on an effective spectroscopic Hamiltonian, describe the essential features of the multimodal Fermi resonance-driven vibrational dynamics in the 3p state. We also present evidence of polyad-specificity in the state-dependent predissociation rates, leading to free atomic and molecular fragments. We emphasize that a quantum molecular movie is required to visualize wavepacket dynamics in the 3pσ2Σu Rydberg state of NO2.
    Language English
    Publishing date 2021-02-24
    Publishing country England
    Document type Journal Article
    ISSN 1364-5498
    ISSN (online) 1364-5498
    DOI 10.1039/d0fd00128g
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  8. Article ; Online: Multi-Particle Three-Dimensional Covariance Imaging: "Coincidence" Insights into the Many-Body Fragmentation of Strong-Field Ionized D

    Allum, Felix / Cheng, Chuan / Howard, Andrew J / Bucksbaum, Philip H / Brouard, Mark / Weinacht, Thomas / Forbes, Ruaridh

    The journal of physical chemistry letters

    2021  Volume 12, Issue 34, Page(s) 8302–8308

    Abstract: We demonstrate the applicability of covariance analysis to three-dimensional velocity-map imaging experiments using a fast time stamping detector. Studying the photofragmentation of strong-field doubly ionized ... ...

    Abstract We demonstrate the applicability of covariance analysis to three-dimensional velocity-map imaging experiments using a fast time stamping detector. Studying the photofragmentation of strong-field doubly ionized D
    Language English
    Publishing date 2021-08-24
    Publishing country United States
    Document type Journal Article
    ISSN 1948-7185
    ISSN (online) 1948-7185
    DOI 10.1021/acs.jpclett.1c02481
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  9. Article ; Online: Vacuum Ultraviolet Excited State Dynamics of the Smallest Ketone: Acetone.

    Forbes, Ruaridh / Neville, Simon P / Larsen, Martin A B / Röder, Anja / Boguslavskiy, Andrey E / Lausten, Rune / Schuurman, Michael S / Stolow, Albert

    The journal of physical chemistry letters

    2021  Volume 12, Issue 35, Page(s) 8541–8547

    Abstract: We combined tunable vacuum-ultraviolet time-resolved photoelectron spectroscopy (VUV-TRPES) with high-level quantum dynamics simulations to disentangle multistate Rydberg-valence dynamics in acetone. A femtosecond 8.09 eV pump pulse was tuned to the ... ...

    Abstract We combined tunable vacuum-ultraviolet time-resolved photoelectron spectroscopy (VUV-TRPES) with high-level quantum dynamics simulations to disentangle multistate Rydberg-valence dynamics in acetone. A femtosecond 8.09 eV pump pulse was tuned to the sharp origin of the A
    Language English
    Publishing date 2021-08-31
    Publishing country United States
    Document type Journal Article
    ISSN 1948-7185
    ISSN (online) 1948-7185
    DOI 10.1021/acs.jpclett.1c02612
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  10. 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
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