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  • 1.
    Bain, Colin D.
    et al.
    Univ Durham, Dept Chem, Durham DH1 3LE, England..
    Churchwell, John H.
    Univ Durham, Dept Chem, Durham DH1 3LE, England..
    Tyrode, Eric
    KTH, School of Chemical Science and Engineering (CHE).
    Walker, Robert A.
    Univ Maryland, Dept Chem & Biochem, College Pk, MD 20742 USA..
    TIR Raman spectroscopy of planar supported lipid bilayers2009In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 237Article in journal (Other academic)
  • 2.
    Bain, Colin D.
    et al.
    Univ Durham, Dept Chem, Durham DH1 3LE, England..
    Tyrode, Eric
    KTH, School of Chemical Science and Engineering (CHE).
    Woods, David
    Univ Durham, Dept Chem, Durham DH1 3LE, England..
    Combined Raman and SFG study of the adsorption of cationic surfactants on silica2009In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 237, p. 188-188Article in journal (Other academic)
  • 3.
    Cyran, Jenee
    et al.
    Max Planck Inst Polymer Res, Dept Mol Spect, Mainz, Germany..
    Donovan, Michael
    Max Planck Inst Polymer Res, Dept Mol Spect, Mainz, Germany..
    Tyrode, Eric
    KTH.
    Bonn, Mischa
    Max Planck Inst Polymer Res, Dept Mol Spect, Mainz, Germany..
    Backus, Ellen
    Max Planck Inst Polymer Res, Dept Mol Spect, Mainz, Germany..
    Hydrophobic water at a hydrophilic interface2017In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 254Article in journal (Other academic)
  • 4.
    Dalstein, Laetitia
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Potapova, Elizaveta
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Tyrode, Eric
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    The elusive silica/water interface: isolated silanols under water as revealed by vibrational sum frequency spectroscopy2017In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 19, no 16, p. 10343-10349Article in journal (Refereed)
    Abstract [en]

    It has been long recognized that the surface chemistry of silica, and in particular the type and relative amount of surface bound silanol groups, plays a critical role in many of the properties associated with the material, where a typical example is the discrepant adsorption behavior observed depending on the pretreatment history of the surface. However, in spite of its importance, the direct probing of specific surface silanol groups under water has been hampered by instrumental limitations. Here we make use of vibrational sum frequency spectroscopy (VSFS) to first, identify under water the OH stretch of isolated surface silanols, and second, explore its acid/base behavior and dependence on the surface pretreatment method. The properties of other types of silanol groups (i.e. hydrogen bonded/geminal) are also inferred from the data. The ability to directly probe these functional groups under water represents a crucial step to further improving our understanding of this widely used mineral oxide.

  • 5.
    Hore, Dennis K.
    et al.
    Univ Victoria, Dept Chem, Victoria, BC V8W 3V6, Canada..
    Tyrode, Eric
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Surface and Corrosion Science.
    Probing Charged Aqueous Interfaces Near Critical Angles: Effect of Varying Coherence Length2019In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 123, no 27, p. 16911-16920Article in journal (Refereed)
    Abstract [en]

    Angle-resolved vibrational sum frequency generation experiments have been used to study the silica-water interface as a function of ionic strength. Well below the critical angle, the sum frequency intensity increases up to 10(-4) M NaCl and then drops. However, near the critical angle, a plateau may be observed up to 10(-4) M. We first demonstrate that this is a result of the interaction of a long Debye length at low ionic strength with a long coherence length near the critical angles. In order to account for the behavior at the lowest concentrations where surface potentials are typically large, it is necessary to consider an electrostatic potential that extends into the bulk aqueous phase beyond the Debye-Huckel approximation. Because the extent of second- and third-order contributions to the nonlinear polarization can vary with ionic strength, but not with the angle of incidence, we perform a global fit to the experimental data using our proposed model to extract the relative magnitude of the two susceptibilities. The ionic strength dependence of this ratio points to the critical nature of the silanol deprotonation and the development of surface charge and illustrates how surface water molecules respond. These results highlight the importance of varying the coherence length in order to probe the water structure at charged interfaces.

  • 6.
    Okur, Halil I.
    et al.
    Ecole Polytech Fed Lausanne, Inst Bioengn IBI, Sch Engn STI, Lab Fundamental BioPhoton LBP, CH-1015 Lausanne, Switzerland.;Ecole Polytech Fed Lausanne, Inst Mat Sci IMX, Sch Engn STI, CH-1015 Lausanne, Switzerland.;Ecole Polytech Fed Lausanne, Lausanne Ctr Ultrafast Sci LACUS, CH-1015 Lausanne, Switzerland..
    Drexler, Chad I.
    Penn State Univ, Dept Chem, University Pk, PA 16802 USA..
    Tyrode, Eric
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry. Ecole Polytech Fed Lausanne, Inst Bioengn IBI, Sch Engn STI, Lab Fundamental BioPhoton LBP, CH-1015 Lausanne, Switzerland.;Ecole Polytech Fed Lausanne, Inst Mat Sci IMX, Sch Engn STI, CH-1015 Lausanne, Switzerland.;Ecole Polytech Fed Lausanne, Lausanne Ctr Ultrafast Sci LACUS, CH-1015 Lausanne, Switzerland..
    Cremer, Paul S.
    Penn State Univ, Dept Chem, University Pk, PA 16802 USA.;Penn State Univ, Biochem & Mol Biol, University Pk, PA 16802 USA..
    Roke, Sylvie
    Ecole Polytech Fed Lausanne, Inst Bioengn IBI, Sch Engn STI, Lab Fundamental BioPhoton LBP, CH-1015 Lausanne, Switzerland.;Ecole Polytech Fed Lausanne, Inst Mat Sci IMX, Sch Engn STI, CH-1015 Lausanne, Switzerland.;Ecole Polytech Fed Lausanne, Lausanne Ctr Ultrafast Sci LACUS, CH-1015 Lausanne, Switzerland..
    The Jones-Ray Effect Is Not Caused by Surface-Active Impurities2018In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 9, no 23, p. 6739-6743Article in journal (Refereed)
    Abstract [en]

    Pure aqueous electrolyte solutions display a minimum in surface tension at concentrations of 2 +/- 1 mM. This effect has been a source of controversy since it was first reported by Jones and Ray in the 1930s. The Jones Ray effect has frequently been dismissed as an artifact linked to the presence of surface-active impurities. Herein we systematically consider the effect of surface-active impurities by purposely adding nanomolar concentrations of surfactants to dilute electrolyte solutions. Trace amounts of surfactant are indeed found to decrease the surface tension and influence the surface chemistry. However, surfactants can be removed by repeated aspiration and stirring cycles, which eventually deplete the surfactant from solution, creating a pristine surface. Upon following this cleaning procedure, a reduction in the surface tension by millimolar concentrations of salt is still observed. Consequently, we demonstrate that the Jones Ray effect is not caused by surface-active impurities.

  • 7.
    Sengupta, Sanghamitra
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Moberg, Daniel R.
    Univ Calif San Diego, Dept Chem & Biochem, Mat Sci & Engn, La Jolla, CA 92093 USA..
    Paesani, Francesco
    Univ Calif San Diego, Dept Chem & Biochem, Mat Sci & Engn, La Jolla, CA 92093 USA.;Univ Calif San Diego, San Diego Supercomp Ctr, La Jolla, CA 92093 USA..
    Tyrode, Eric
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Neat Water-Vapor Interface: Proton Continuum and the Nonresonant Background2018In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 9, no 23, p. 6744-6749Article in journal (Refereed)
    Abstract [en]

    Whether the surface of neat water is "acidic" or "basic" remains an active and controversial field of research. Most of the experimental evidence supporting the preferential adsorption of H3O+ ions stems from nonlinear optical spectroscopy methods typically carried out at extreme pH conditions (pH < 1). Here, we use vibrational sum frequency spectroscopy (VSFS) to target the "proton continuum", an unexplored frequency range characteristic of hydrated protons and hydroxide ions. The VSFS spectra of neat water show a broad and nonzero signal intensity between 1700 and 3000 cm-' in the three different polarization combinations examined. By comparing the SF response of water with that from dilute HCl and NaOH aqueous solutions, we conclude the intensity does not originate from either adsorbed H3O+ or OH- ions. Contributions from the nonresonant background are then critically considered by comparing the experimental results with many-body molecular dynamics (MB-MD) simulated spectra.

  • 8.
    Sthoer, Adrien
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Surface and Corrosion Science. kth.
    Interactions of Na+ Cations with a Highly Charged Fatty Acid Langmuir Monolayer: Molecular Description of the Phase Transition2019In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455Article in journal (Other (popular science, discussion, etc.))
    Abstract [en]

    Vibrational sum frequency spectroscopy has been used to study the molecular properties upon compression of a highly charged arachidic acid Langmuir monolayer, which displays a first-order phase transition plateau in the surface pressure - molecular area (π-A) isotherm. By targeting vibrational modes from the carboxylic acid headgroup, alkyl chain, and interfacial water molecules, information regarding the surface charge, surface potential, type of ion pair formed, and conformational order of the monolayer could be extracted. The monolayer was found to be fully charged before reaching the 2D-phase transition plateau, where partial reprotonation, as well as the formation of COO⎺ Na+ contact-ion pairs, started to take place. After the transition, three headgroup species, mainly hydrated COO⎺, COOH, and COO⎺ Na+ contact-ion pairs could be identified and their proportions quantified. Comparison with theoretical models shows that predictions from the Gouy Chapman model are only adequate for the lowest surface charge densities (<-0.1 C/m2). In contrast, a modified Poisson-Boltzmann (MPB) model that accounts for finite-size of the cation, captures many of the experimental observables, including the partial reprotonation, and surface potential changes upon compression. The experimental results provide a quantitative molecular insight that could be used to test potential extensions to the theory.

  • 9.
    Sthoer, Adrien
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Hladilkova, Jana
    Lund Univ, Theoret Chem, Lund, Sweden..
    Lund, Mikael
    Lund Univ, Theoret Chem, Lund, Sweden..
    Tyrode, Eric
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Molecular insight into the carboxylic acid - alkali metal cations interactions: Reversed affinity and ion pair formation2018In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 256Article in journal (Other academic)
  • 10.
    Tyrode, Eric
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Corkery, Robert
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Charging of Carboxylic Acid Monolayers with Monovalent Ions at Low Ionic Strengths: Molecular Insight Revealed by Vibrational Sum Frequency Spectroscopy2018In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 122, no 50, p. 28775-28786Article in journal (Refereed)
    Abstract [en]

    The charging of arachidic acid Langmuir monolayers as a function of subphase pH and monovalent ion concentration below 100 mM was investigated using vibrational sum frequency spectroscopy. Molecular information was obtained by targeting the vibrational modes of the carboxylic acid headgroups, alkyl chains, and water molecules in the immediate surface and diffuse double layers. The surface charge in the monolayer was experimentally determined by monitoring the hydrated carboxylate stretching modes. The charging behavior was found to be in excellent agreement with that predicted by Gouy-Chapman theory using a thermodynamic pK(a) of 5.1 +/- 0.2. This resulted in an apparent pK(a) of similar to 10.8 when the only ions present in solution were those associated with adjusting the pH. Water molecules with a preferred orientation in the immediate surface region were found to primarily interact with the uncharged carboxylic acid moiety, decreasing in number as the monolayer further deprotonated. Contributions from water molecules in the diffuse double layer, partly aligned by the exponentially decaying surface electric field, closely followed the predictions of a recently proposed theoretical framework that accounts for interference and screening effects. Finally, the charging of the monolayer was experimentally found to be independent of the identity of either the monovalent cation (i.e., Li+, Na+, Rb+) or anion (i.e., F-, Cl-, I-) at low salt concentrations.

  • 11.
    Tyrode, Eric
    et al.
    KTH, Superseded Departments (pre-2005), Chemistry.
    Johnson, C M
    KTH, Superseded Departments (pre-2005), Chemistry.
    Kumpulainen, A
    KTH, Superseded Departments (pre-2005), Chemistry.
    Rutland, Mark W.
    KTH, Superseded Departments (pre-2005), Chemistry.
    Claesson, Per M.
    KTH, Superseded Departments (pre-2005), Chemistry.
    Hydration state of non-ionic surfactant monolayers at the liquid/vapor interface: Structure determination by vibrational sum frequency spectroscopy (VSFS)2005In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 230, p. U2904-U2905Article in journal (Other academic)
  • 12.
    Tyrode, Eric
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Johnson, C. Magnus
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Surface and Corrosion Science.
    Claesson, Per M.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Rutland, Mark W.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    COLL 153-Molecular ordering at the liquid/air interface and hydration of surfactants2006In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 232Article in journal (Other academic)
  • 13.
    Tyrode, Eric
    et al.
    KTH, Superseded Departments (pre-2005), Chemistry.
    Johnson, C. Magnus
    KTH, Superseded Departments (pre-2005), Chemistry.
    Leygraf, Christopher
    KTH, Superseded Departments (pre-2005), Chemistry.
    Studies of the liquid/vapor interface of aqueous formic acid solutions by vibrational sum frequency spectroscopy (VSFS)2005In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 230, p. U2905-U2905Article in journal (Other academic)
  • 14.
    Tyrode, Eric
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Sengupta, Sanghamitra
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Sthoer, Adrien
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Surface and Corrosion Science.
    Vibrational Spectral Signature of Eigen-like hydrated protonsat negatively charged surfacesManuscript (preprint) (Other academic)
1 - 14 of 14
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