Sum frequency generation surface spectra of ice, water, and acid solution investigated by an exciton model

Buch, V.; Tarbuck, Teresa L.; Richmond, Geraldine L.; Groenzin, Henning; Li, I.; Shultz, Mary Jane

doi:10.1063/1.2790437

Cited by 104 publications

(127 citation statements)

References 96 publications

(130 reference statements)

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“…We calculated SFG spectra of the ice surface for the striped phase and, by comparison, for the fully disordered dangling atom pattern, using the recently developed exciton-based method (33). Fig.…”

Section: Resultsmentioning

confidence: 99%

Proton order in the ice crystal surface

Buch

Groenzin

et al. 2008

Proc. Natl. Acad. Sci. U.S.A.

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131

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The physics of the ice crystal surface and its interaction with adsorbates are not only of fundamental interest but also of considerable importance to terrestrial and planetary chemistry. Yet the atomic-level structure of even the pristine ice surface at low temperature is still far from well understood. This computational study focuses on the pattern of dangling H and dangling O (lone pairs) atoms at the basal ice surface. Dangling atoms serve as binding sites for adsorbates capable of hydrogen-and electrostatic bonding. Extension of the well known orientational disorder (''proton disorder'') of bulk crystal ice to the surface would naturally suggest a disordered dangling atom pattern; however, extensive computer simulations employing two different empirical potentials indicate significant free energy preference for a striped phase with alternating rows of dangling H and dangling O atoms, as suggested long ago by Fletcher [Fletcher NH (1992) Philos Mag 66:109 -115]. The presence of striped phase domains within the basal surface is consistent with the hitherto unexplained minor fractional peaks in the helium diffraction pattern observed 10 years ago. Compared with the disordered model, the striped model yields improved agreement between computations and experimental ppp-polarized sum frequency generation spectra.ice surface ͉ Monte Carlo simulations ͉ surface order ͉ dangling atoms ͉ ice-adsorbate interaction W ater ice is an intellectually challenging and fundamentally important solid. Ice and ice particles play a basic role in terrestrial, atmospheric, planetary, and interstellar phenomena (1-3). The remarkable properties of ice are determined by the unique ability of H 2 O to form four relatively strong hydrogen bonds to four neighboring water molecules, in an approximately tetrahedral arrangement. This gives rise to a rich bulk phase diagram comprising a variety of crystalline phases, in addition to muchdebated amorphous phases (1).Under ambient conditions, hexagonal ice is the dominant solid form of H 2 O. Here we focus on the surface structure of hexagonal ice, which hosts a variety of chemical reactions in natural environments; perhaps the most famous example being the sequence of reactions leading to ozone-hole formation, which is initiated by HCl and ClO adsorption on frozen stratospheric cloud particles (4). The interaction of ice with molecules, ions, and electrons is affected by the solvating properties of its surface. It has long been recognized that these properties are directly related to the structure and dynamics of the surface H-bond network, which has consequently received considerable attention in past research (see, for example, refs. 1, 3, and 5-16).Here, we address a feature of the ice surface that has not received extensive attention but that is expected to significantly influence its properties, including its interaction with adsorbates. Specifically, we argue that the pattern of dangling H (d-H) and dangling O (d-O) atoms on the ice surface is composed of ordered striped domains, with a...

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Section: Resultsmentioning

confidence: 99%

Proton order in the ice crystal surface

Buch

Groenzin

et al. 2008

Proc. Natl. Acad. Sci. U.S.A.

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131

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“…The calculations of the vibrational band shapes of the OH stretching mode involved in H-bond interactions have a long history and have captured the attention of a number of papers [43][44][45][46][47][48][49][50][51][52][53][54][55][56][57][58][59][60][61]. In order to explain spectacular features in frequency shifts, band shapes, and bandwidths of the components the OH stretching modes the linear and nonlinear response theory [43][44][45], quantum ab inito calculations for possible cluster structures [62][63][64][65][66][67][68], classical [69][70][71][72][73] and mixed quantum/classical molecular dynamics simulations [74][75][76] have been used.…”

Section: Discussionmentioning

confidence: 99%

Hydrogen bonds of interfacial water in human breast cancer tissue compared to lipid and DNA interfaces

Abramczyk¹,

Brożek-Płuska²,

Surmacki³

et al. 2011

JBPC

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The paper presents the results for water confined in a human breast cancerous tissue, a single stranded DNA, a double stranded DNA and in phospholipids (DPPC-D--Phosphatidylcholine, dipalmitoyl). The interfacial water in DNA and lipids is represented by a double band in the region of the OH stretching mode of water corresponding to the symmetric and asymmetric vibrational modes, in contrast to water confined in the cancerous breast tissue where only one band at 3311 cm -1 has been recorded. The marked red-shift of the maximum peak position of the OH stretching mode confirms that the vibrational properties of the interfacial water observed in restricted biological environment differ drastically from those in bulk water. The change of vibrational pattern of behavior may be due to the decoupling of the vibrations of the OH bonds in water molecule or change of the vibrational selection rules at biological interfaces. According to our knowledge Raman vibrational properties of water confined in the normal and cancerous breast tissue of the same patient have not been reported in literature yet. Here we have also presented the first Raman 'optical biopsy' images of the non-cancerous and cancerous (infiltrating ductal cancer) human breast tissues.

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“…158,161,163,[172][173][174][175][176][177] Experimental studies using surface sensitive methods at liquid water and ice surfaces provide important complementary information. 176,[178][179][180] However, modeling heterogeneous reactions in these complex environments remains a challenge. The ionization of acids and proton recombination are important processes in environmental waters at water and ice surfaces.…”

Section: Cluster Models For Condensed Phases Aerosols and Interfacesmentioning

confidence: 99%

Perspective: Water cluster mediated atmospheric chemistry

Vaida

2011

The Journal of Chemical Physics

279

249

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The importance of water in atmospheric and environmental chemistry initiated recent studies with results documenting catalysis, suppression and anti-catalysis of thermal and photochemical reactions due to hydrogen bonding of reagents with water. Water, even one water molecule in binary complexes, has been shown by quantum chemistry to stabilize the transition state and lower its energy. However, new results underscore the need to evaluate the relative competing rates between reaction and dissipation to elucidate the role of water in chemistry. Water clusters have been used successfully as models for reactions in gas-phase, in aqueous condensed phases and at aqueous surfaces. Opportunities for experimental and theoretical chemical physics to make fundamental new discoveries abound. Work in this field is timely given the importance of water in atmospheric and environmental chemistry.

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Sum frequency generation surface spectra of ice, water, and acid solution investigated by an exciton model

Cited by 104 publications

References 96 publications

Proton order in the ice crystal surface

Proton order in the ice crystal surface

Hydrogen bonds of interfacial water in human breast cancer tissue compared to lipid and DNA interfaces

Perspective: Water cluster mediated atmospheric chemistry

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