Journal: Faraday Discussions

Abbreviation

Faraday Discuss.

Publisher

Royal Society of Chemistry

Journal Volumes

ISSN

1359-6640
1364-5498

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Publications1 - 10 of 91
  • Vibrational and condensed phase dynamics: general discussion
    Item type: Journal Article
    Orr-Ewing, Andrew J.; Kornilov, Oleg; Sølling, Theis I.; et al. (2016)
    Faraday Discussions
  • Modelling the stochastic behaviour of primary nucleation
    Item type: Journal Article
    Maggioni, Giovanni; Mazzotti, Marco (2015)
    Faraday Discussions
  • Electrochemical characterization of individual oil micro-droplets by high-frequency nanocapacitor array imaging
    Item type: Journal Article
    Renault, Christophe Jacques; Laborde, Cecilia; Cossettini, Andrea; et al. (2022)
    Faraday Discussions
    CMOS-based nanocapacitor arrays allow locally probing the impedance of an electrolyte in real time and with sub-micron spatial resolution. Here we report on the physico-chemical characterization of individual microdroplets of oil in a continuous water phase using this new tool. We monitor the sedimentation and wetting dynamics of individual droplets, estimate their volume and infer their composition based on their dielectric constant. From measurements before and after wetting of the surface, we also attempt to estimate the contact angle of individual micron-sized droplets. These measurements illustrate the capabilities and versatility of nanocapacitor array technology.
  • XUV pump-XUV probe transient absorption spectroscopy at FELs
    Item type: Journal Article
    Ding, Thomas; Rebholz, Marc; Aufleger, Lennart; et al. (2021)
    Faraday Discussions
    The emergence of ultra-intense extreme-ultraviolet (XUV) and X-ray free-electron lasers (FELs) has opened the door for the experimental realization of non-linear XUV and X-ray spectroscopy techniques. Here we demonstrate an experimental setup for an all-XUV transient absorption spectroscopy method for gas-phase targets at the FEL. The setup combines a high spectral resolving power of E/ΔE ≈ 1500 with sub-femtosecond interferometric resolution, and covers a broad XUV photon-energy range between approximately 20 and 110 eV. We demonstrate the feasibility of this setup firstly on a neon target. Here, we intensity- and time-resolve key aspects of non-linear XUV-FEL light-matter interactions, namely the non-resonant ionization dynamics and resonant coupling dynamics of bound states, including XUV-induced Stark shifts of energy levels. Secondly, we show that this setup is capable of tracking the XUV-initiated dissociation dynamics of small molecular targets (oxygen and diiodomethane) with site-specific resolution, by measuring the XUV transient absorption spectrum. In general, benefitting from a single-shot detection capability, we show that the setup and method provides single-shot phase-locked XUV pulse pairs. This lays the foundation to perform, in the future, experiments as a function of the XUV interferometric time delay and the relative phase, which enables advanced coherent non-linear spectroscopy schemes in the XUV and X-ray spectral range.
  • Ab initio instanton rate theory made efficient using Gaussian process regression
    Item type: Journal Article
    Laude, Gabriel; Calderini, Danilo; Tew, David P.; et al. (2018)
    Faraday Discussions
    Ab initio instanton rate theory is a computational method for rigorously including tunnelling effects into the calculations of chemical reaction rates based on a potential-energy surface computed on the fly from electronic-structure theory. This approach is necessary to extend conventional transition-state theory into the deep-tunnelling regime, but it is also more computationally expensive as it requires many more ab initio calculations. We propose an approach which uses Gaussian process regression to fit the potential-energy surface locally around the dominant tunnelling pathway. The method can be converged to give the same result as from an on-the-fly ab initio instanton calculation but it requires far fewer electronic-structure calculations. This makes it a practical approach for obtaining accurate rate constants based on high-level electronic-structure methods. We show fast convergence to reproduce benchmark H + CH4 results and evaluate new low-temperature rates of H + C2H6 in full dimensionality at a UCCSD(T)-F12b/cc-pVTZ-F12 level.
  • Applications and serious games: From docking to protein folding
    Item type: Other Journal Item
    Reiher, Markus (2014)
    Faraday Discussions
  • How do organic vapors contribute to new-particle formation?
    Item type: Journal Article
    Donahue, Neil M.; Ortega, Ismael K.; Chuang, Wayne; et al. (2013)
    Faraday Discussions
  • On experiments to detect parity violation in chiral molecules (Discussion Contribution)
    Item type: Other Journal Item
    Quack, Martin (2011)
    Faraday Discussions
  • Terrestrial and marine sources of ice nucleating particles in the Eurasian Arctic
    Item type: Journal Article
    Li, Guangyu; Welti, André; Rocchi, Arianna; et al. (2025)
    Faraday Discussions
    Ice nucleating particles (INPs) catalyze primary ice formation in Arctic low-level mixed-phase clouds, influencing their persistence and radiative properties. Knowledge of the abundance and sources of INP over the remote Arctic Ocean is scarce due to limited data coverage, particularly in the Eurasian Arctic. This study presents summertime measurements of INP concentrations in seawater, fog water and air from the ship-based Arctic Century Expedition, exploring the Barents, Kara, and Laptev Seas, and the adjacent high Arctic islands and archipelagos in August and September 2021. Heat sensitivity tests of ambient aerosols revealed that heat-liable, biogenic INPs make up the majority of Arctic INP populations at temperatures above -20 degrees C, and to a lesser extent down to -25 degrees C. INP content in fog water is found to be similar to ambient aerosol, indicating that INP in marine air could also act as cloud condensation nuclei. Measurements of aerosolized INPs using an on-board sea-spray aerosol bubble tank generator exhibit a positive correlation with ambient INP concentrations, but not with INP abundance in seawater samples. INP concentrations in air derived from sea water samples (using a NaCl conversion factor representative for the Arctic) were significantly lower than those measured in ambient air or bubble tank experiments. INP concentrations in bubble tank experiments positively correlated with the phosphate and fluorescence signals in the water. This suggests an important role of the aerosolization mechanism for preferentially partitioning biogenic INPs to the atmosphere.
  • Designing refractive index fluids using the Kramers-Kronig relations
    Item type: Journal Article
    Sai, Tianqi; Saba, Matthias; Dufresne, Eric; et al. (2020)
    Faraday Discussions
    For a number of optical applications, it is advantageous to precisely tune the refractive index of a liquid. Here, we harness a well-established concept in optics for this purpose. The Kramers-Kronig relation provides a physical connection between the spectral variation of the (real) refractive index and the absorption coefficient. In particular, a sharp spectral variation of the absorption coefficient gives rise to either an enhancement or reduction of the refractive index in the spectral vicinity of this variation. By using bright commodity dyes that fulfil this absorption requirement, we demonstrate the use of the Kramers-Kronig relation to predictively obtain refractive index values in water solutions that are otherwise only attained with toxic specialised liquids.
Publications1 - 10 of 91