Interfacial Molecular Organization at Aqueous Solution Surfaces of Atmospherically Relevant Dimethyl Sulfoxide and Methanesulfonic Acid Using Sum Frequency Spectroscopy and Molecular Dynamics Simulation

Chen, Xiangke; Minofar, Babak; Jungwirth, Pavel; Allen, Heather C.

doi:10.1021/jp1078339

Cited by 37 publications

(47 citation statements)

References 56 publications

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“…Since the DMSO contains a large amount of water, it is expected that silicon nanocrystal after formation reacts with the water and produce oxide layer on its surface [27,28]. Interestingly, the UV-VIS optical absorption spectrum shows stability of the SiNCs colloid.…”

Section: Resultsmentioning

confidence: 99%

Blue-green luminescent silicon nanocrystals fabricated by nanosecond pulsed laser ablation in dimethyl sulfoxide

Mansour¹,

Momeni²,

Karimzadeh³

et al. 2012

Opt. Mater. Express

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In this work, stable blue-green luminescent colloidal silicon nanocrystals (SiNCs) are fabricated by nanosecond pulsed laser ablation of a silicon target in dimethyl sulfoxide (DMSO). Transmission electron microscopy and X-ray diffraction analysis have shown the formation of spherical silicon nanocrystals in the colloid with size range of 2-5 nm. Our results show that the DMSO stabilizes the silicon nanocrystals via oxide formations on the nanocrytals surfaces by a simple route of laser ablation and a schematic representation of the process is suggested. The colloid exhibits strong blue luminescent emissions in the spectral range of 455-465 nm when excited at wavelengths near the direct band gap of the silicon nanocrystal. The luminescent emission band shifts to longer wavelengths (green light) if the excitation wavelength increases toward the indirect band gap of the SiNCs. The oxidized SiNCs with quantum confinement effects are shown to be responsible for visible photoluminescence of the colloid. The observed blue-green emission of the colloid makes it a good candidate for display, solid-state lighting and biological luminescent based devices.

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Section: Resultsmentioning

confidence: 99%

Blue-green luminescent silicon nanocrystals fabricated by nanosecond pulsed laser ablation in dimethyl sulfoxide

Mansour¹,

Momeni²,

Karimzadeh³

et al. 2012

Opt. Mater. Express

View full text Add to dashboard Cite

show abstract

“…[166][167][168][169][170][171] Molecular dynamics simulations of the structural and thermodynamic properties of acids and salts at the surface of water have been effective in studying aqueous surfaces. 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.…”

Section: Cluster Models For Condensed Phases Aerosols and Interfacesmentioning

confidence: 99%

“…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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“…Although this challenge has been well-known for more than a decade, [22][23][24][25] no general solutions to it have been proposed, to the best of our knowledge. Details about this function are described in the supporting information.…”

Section: Introductionmentioning

confidence: 99%

Solving the “Magic Angle” Challenge in Determining Molecular Orientation Heterogeneity at Interfaces

Xiong

2016

J. Phys. Chem. C

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It is critical to determine conformations of molecular monolayers in order to understand and control their functions and properties, such as efficiencies of self-assembly-based biosensors and turnover frequency of surface-bound electrocatalysts. However, surface molecules of the monolayers can adopt conformations with many different orientations. Thus, it is necessary to describe the orientations of surface molecular monolayers using both mean tilt angle and orientational distribution, which together we refer as orientation heterogeneity. Orientation heterogeneity is difficult to measure. In most cases, in order to calculate the mean tilt angle, it is assumed that the orientational distribution is narrow. This assumption causes ambiguities in determining the mean tilt angle, and loss of orientational distribution information, which is known as the "magic angle" challenge. Using heterodyne two-dimensional vibrational sum frequency generation (HD 2D VSFG) spectroscopy, we report a novel method to solve the "magic angle" challenge, by simultaneously measuring mean tilt angle and orientational distribution of molecular monolayers. We applied this new method to a CO2 reduction catalyst/gold interface and found that the catalysts formed a monolayer with a mean tilt angle between its quasi-C3 symmetric axis and the surface normal of 53°, with 5° orientational distribution. The narrow orientational distribution indicates that the surface molecules are rigid, which sample only limited configurations for facilitating a reaction, because of the short anchoring groups. Although applied to a specific system, this method is a general way to determine the orientation heterogeneity of an ensemble-averaged molecular interface.3

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Interfacial Molecular Organization at Aqueous Solution Surfaces of Atmospherically Relevant Dimethyl Sulfoxide and Methanesulfonic Acid Using Sum Frequency Spectroscopy and Molecular Dynamics Simulation

Cited by 37 publications

References 56 publications

Blue-green luminescent silicon nanocrystals fabricated by nanosecond pulsed laser ablation in dimethyl sulfoxide

Blue-green luminescent silicon nanocrystals fabricated by nanosecond pulsed laser ablation in dimethyl sulfoxide

Perspective: Water cluster mediated atmospheric chemistry

Solving the “Magic Angle” Challenge in Determining Molecular Orientation Heterogeneity at Interfaces

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