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Title: From atoms to aerosols: probing clusters and nanoparticles with synchrotron based mass spectrometry and X-ray spectroscopy

Abstract

Tunable synchrotron radiation provides a universal yet selective scalpel to decipher molecular information in complex chemical systems when coupled to mass spectrometry and X-ray spectroscopy. At the Chemical Dynamics Beamline, the radiation emanating from the Advanced Light Source at Berkeley has been utilized by physical chemists and chemical physicists to probe chemical reactivity, energetics and spectroscopy for over two decades. Emerging themes are the study of molecular growth mechanisms, solvation, electronic structure and reactivity in clusters, complexes and nanoparticles. The ion-induced and neutral growth mechanisms in methanol and acetylene clusters are revealed by vacuum ultraviolet (VUV) single photon ionization mass spectrometry. The photoionization dynamics of glycerol show signatures of strong ionic hydrogen bonds, non-covalent interactions are explored in naphthalene water clusters, proton transfer pathways are revealed in acetaldehyde water clusters, and exciton charge transfer is probed in argon water clusters. X-ray spectroscopy provides a local probe of a sample's electronic structure with elemental and site-specificity and is thus ideally suited for probing solvation. Velocity map imaging X-ray photoelectron spectroscopy coupled to nanoparticle beams that allows for the visualization of dynamic processes in solvation and molecular growth processes is described. This technique is used to probe reactivity in aerosol chemistry, obtainmore » phase and pH dependent information on aqueous nanoparticles and electron scattering cross-sections from hydrocarbon nanoparticles. Here, we describe future opportunities in probing elusive radicals such as the cyclic 3,5-dehydroxyphenyl radical cation and excited states in water clusters formed in VUV photoionization, explore reactivity in confined spaces via X-ray spectroscopy and elucidate time dynamics with laser-synchrotron pump probe experiments.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]
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  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1608279
Alternate Identifier(s):
OSTI ID: 1592797
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 22; Journal Issue: 5; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ahmed, Musahid, and Kostko, Oleg. From atoms to aerosols: probing clusters and nanoparticles with synchrotron based mass spectrometry and X-ray spectroscopy. United States: N. p., 2020. Web. doi:10.1039/c9cp05802h.
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Ahmed, Musahid, & Kostko, Oleg. From atoms to aerosols: probing clusters and nanoparticles with synchrotron based mass spectrometry and X-ray spectroscopy. United States. https://doi.org/10.1039/c9cp05802h
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Ahmed, Musahid, and Kostko, Oleg. Mon . "From atoms to aerosols: probing clusters and nanoparticles with synchrotron based mass spectrometry and X-ray spectroscopy". United States. https://doi.org/10.1039/c9cp05802h. https://www.osti.gov/servlets/purl/1608279.
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@article{osti_1608279,
title = {From atoms to aerosols: probing clusters and nanoparticles with synchrotron based mass spectrometry and X-ray spectroscopy},
author = {Ahmed, Musahid and Kostko, Oleg},
abstractNote = {Tunable synchrotron radiation provides a universal yet selective scalpel to decipher molecular information in complex chemical systems when coupled to mass spectrometry and X-ray spectroscopy. At the Chemical Dynamics Beamline, the radiation emanating from the Advanced Light Source at Berkeley has been utilized by physical chemists and chemical physicists to probe chemical reactivity, energetics and spectroscopy for over two decades. Emerging themes are the study of molecular growth mechanisms, solvation, electronic structure and reactivity in clusters, complexes and nanoparticles. The ion-induced and neutral growth mechanisms in methanol and acetylene clusters are revealed by vacuum ultraviolet (VUV) single photon ionization mass spectrometry. The photoionization dynamics of glycerol show signatures of strong ionic hydrogen bonds, non-covalent interactions are explored in naphthalene water clusters, proton transfer pathways are revealed in acetaldehyde water clusters, and exciton charge transfer is probed in argon water clusters. X-ray spectroscopy provides a local probe of a sample's electronic structure with elemental and site-specificity and is thus ideally suited for probing solvation. Velocity map imaging X-ray photoelectron spectroscopy coupled to nanoparticle beams that allows for the visualization of dynamic processes in solvation and molecular growth processes is described. This technique is used to probe reactivity in aerosol chemistry, obtain phase and pH dependent information on aqueous nanoparticles and electron scattering cross-sections from hydrocarbon nanoparticles. Here, we describe future opportunities in probing elusive radicals such as the cyclic 3,5-dehydroxyphenyl radical cation and excited states in water clusters formed in VUV photoionization, explore reactivity in confined spaces via X-ray spectroscopy and elucidate time dynamics with laser-synchrotron pump probe experiments.},
doi = {10.1039/c9cp05802h},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 5,
volume = 22,
place = {United States},
year = {Mon Jan 13 00:00:00 EST 2020},
month = {Mon Jan 13 00:00:00 EST 2020}
}
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Reaction Dynamics in Astrochemistry: Low-Temperature Pathways to Polycyclic Aromatic Hydrocarbons in the Interstellar Medium
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The Statistical Mechanics of Dynamic Pathways to Self-Assembly
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Ion-induced nucleation of pure biogenic particles
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Size-Resolved Photoelectron Anisotropy of Gas Phase Water Clusters and Predictions for Liquid Water
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Synthesis of microporous silica nanoparticles to study water phase transitions by vibrational spectroscopy
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The effect of microhydration on ionization energies of thymine
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To Be or Not To Be a Molecular Ion: The Role of the Solvent in Photoionization of Arginine
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Photoelectron Spectroscopy of CdSe Nanocrystals in the Gas Phase: A Direct Measure of the Evanescent Electron Wave Function of Quantum Dots
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Dyson orbitals within the fc-CVS-EOM-CCSD framework: theory and application to X-ray photoelectron spectroscopy of ground and excited states
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Direct Observation of Hierarchic Molecular Interactions Critical to Biogenic Aerosol Formation
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Low-energy electron-induced reactions in condensed matter
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Effective attenuation length of an electron in liquid water between 10 and 600 eV
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Observation of the fastest chemical processes in the radiolysis of water
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Vacuum Ultraviolet Photoionization Studies of PtCH 2 and H-Pt-CH 3 : A Potential Energy Surface for the Pt+CH 4 Reaction
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Hydrogen-Abstraction/Acetylene-Addition Exposed
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Ultrafast extreme ultraviolet photoemission without space charge
journal, January 2019

Generation and characterization of ultrathin free-flowing liquid sheets
text, January 2018

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Size-Resolved Photoelectron Anisotropy of Gas Phase Water Clusters and Predictions for Liquid Water
text, January 2017

Attosecond chronoscopy of electron scattering in dielectric nanoparticles
text, January 2017

Decomposing electronic and lattice contributions in optical pump – X-ray probe transient inner-shell absorption spectroscopy of CuO
text, January 2019

  • Mahl, Johannes; Neppl, Stefan; Roth, Friedrich
  • Deutsches Elektronen-Synchrotron, DESY, Hamburg
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Ion-induced nucleation of pure biogenic particles
text, January 2016

Velocity of a Molecule Evaporated from a Water Nanodroplet: Maxwell–Boltzmann Statistics versus Non‐Ergodic Events
journal, October 2015

  • Abdoul‐Carime, Hassan; Berthias, Francis; Feketeová, Linda
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Efficient charge generation from triplet excitons in metal-organic heterojunctions
text, January 2019

  • Roth, Friedrich; Neppl, Stefan; Shavorskiy, Andrey
  • Deutsches Elektronen-Synchrotron, DESY, Hamburg
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HACA's Heritage: A Free-Radical Pathway to Phenanthrene in Circumstellar Envelopes of Asymptotic Giant Branch Stars
journal, March 2017

  • Yang, Tao; Kaiser, Ralf I.; Troy, Tyler P.
  • Angewandte Chemie, Vol. 129, Issue 16
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10 years of pioneering X-ray science at the Free-Electron Laser FLASH at DESY
text, January 2019

  • Rossbach, Jörg; Schneider, Jochen R.; Wurth, Wilfried
  • Deutsches Elektronen-Synchrotron, DESY, Hamburg
  • DOI: 10.3204/pubdb-2019-02680

Molecular transport through capillaries made with atomic-scale precision
text, January 2016

Size-Resolved Photoelectron Anisotropy of Gas Phase Water Clusters and Predictions for Liquid Water
text, January 2016

Ultrafast extreme ultraviolet photoemission without space charge
text, January 2018

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