Interfacial energy exchange and reaction dynamics in collisions of gases on model organic surfaces

Lu, Jessica W.; Day, Brad; Fiegland, Larry R.; Davis, Erin Durke; Alexander, William N.; Troya, Diego; Morris, John R.

doi:10.1016/j.progsurf.2012.07.002

Cited by 22 publications

(21 citation statements)

References 173 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…SL and RL interface nicely with traditional surface science experiments of non-thermal gas-surface collisions leading to physisorption and chemisorption. [18][19][20][21][22][23] The chemisorption probability has been investigated versus both the projectile's collision energy 18,19 and vibrational energy. 19 Physisorption has been studied experimentally for both translationally [20][21][22] and vibrationally 23 excited projectiles, and in chemical dynamics simulations versus translational energy.…”

Section: Introductionmentioning

confidence: 99%

“…[18][19][20][21][22][23] The chemisorption probability has been investigated versus both the projectile's collision energy 18,19 and vibrational energy. 19 Physisorption has been studied experimentally for both translationally [20][21][22] and vibrationally 23 excited projectiles, and in chemical dynamics simulations versus translational energy. 24,25 SL and RL have important applications including purification of compounds from complex mixtures, [26][27][28] preparation of protein or peptide microarrays, 29 development of biocompatible substrates and biosensors, 30,31 deposition of mass-selected cluster ions, [32][33][34] and preparation of novel synthetic materials, 35,36 including nanomaterials.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Role of Chemical Dynamics Simulations in Mass Spectrometry Studies of Collision-Induced Dissociation and Collisions of Biological Ions with Organic Surfaces

Somer

Macaluso

Barnes

et al. 2019

J. Am. Soc. Mass Spectrom.

View full text Add to dashboard Cite

In this article, a perspective is given of chemical dynamics simulations of collisions of biological ions with surfaces and of collision-induced dissociation (CID) of ions. The simulations provide an atomic-level understanding of the collisions and, overall, are in quite good agreement with experiment. An integral component of ion/surface collisions is energy transfer to the internal degrees of freedom of both the ion and the surface. The simulations reveal how this energy transfer depends on the collision energy, incident angle, biological ion, and surface. With energy transfer to the ion's vibration fragmentation may occur, i.e. surface-induced dissociation (SID), and the simulations discovered a new fragmentation mechanism, called shattering, for which the ion fragments as it collides with the surface. The simulations also provide insight into the atomistic dynamics of soft-landing and reactive-landing of ions on surfaces. The CID simulations compared activation by multiple "soft" collisions, resulting in random excitation, versus high energy single collisions and non-random excitation. These two activation methods may result in different fragment ions. Simulations provide fragmentation products in agreement with experiments, and hence can provide additional information regarding the reaction mechanisms taking place in experiment. Such studies paved the way on using simulations as an independent and predictive tool in increasing fundamental understanding of CID and related processes.

show abstract

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Role of Chemical Dynamics Simulations in Mass Spectrometry Studies of Collision-Induced Dissociation and Collisions of Biological Ions with Organic Surfaces

Somer

Macaluso

Barnes

et al. 2019

J. Am. Soc. Mass Spectrom.

View full text Add to dashboard Cite

show abstract

“…Experimental, theoretical, and computational results are interleaved and discussed throughout. Lu et al (18) have recently reviewed a large body of work on scattering dynamics from self-assembled monolayers (SAMs). Here, we only include SAM studies that are relevant to gas-liquid scattering dynamics.…”

Section: Introductionmentioning

confidence: 99%

Atomic and Molecular Collisions at Liquid Surfaces

Tesa-Serrate

Smoll

Minton

et al. 2016

Annu. Rev. Phys. Chem.

View full text Add to dashboard Cite

The gas-liquid interface remains one of the least explored, but nevertheless most practically important, environments in which molecular collisions take place. These molecular-level processes underlie many bulk phenomena of fundamental and applied interest, spanning evaporation, respiration, multiphase catalysis, and atmospheric chemistry. We review here the research that has, during the past decade or so, been unraveling the molecular-level mechanisms of inelastic and reactive collisions at the gas-liquid interface. Armed with the knowledge that such collisions with the outer layers of the interfacial region can be unambiguously distinguished, we show that the scattering of gas-phase projectiles is a promising new tool for the interrogation of liquid surfaces with extreme surface sensitivity. Especially for reactive scattering, this method also offers absolute chemical selectivity for the groups that react to produce a specific observed product.

show abstract

“…A considerable amount of experimental work has now been directed at interfacial scattering dynamics on surfaces such as polymers, liquid hydrocarbons and self-assembled monolayers. 13 However, the majority of these studies have focused on scattering of nonreactive gas-phase species. Reactive scattering processes have been less extensively investigated.…”

Section: Introductionmentioning

confidence: 99%

Site and bond-specific dynamics of reactions at the gas–liquid interface

Tesa-Serrate

King

Paterson

et al. 2014

Phys. Chem. Chem. Phys.

View full text Add to dashboard Cite

The dynamics of the interfacial reactions of O((3)P) with the hydrocarbon liquids squalane (C30H62, 2,6,10,15,19,23-hexamethyltetracosane) and squalene (C30H50, trans-2,6,10,15,19,23-hexamethyltetracosa-2,6,10,14,18,22-hexaene) have been studied experimentally. Laser-induced fluorescence (LIF) was used to detect the nascent gas-phase OH products. The O((3)P) atoms are acutely sensitive to the chemical differences of the squalane and squalene surfaces. The larger exothermicity of abstraction from allylic C-H sites in squalene is reflected in markedly hotter OH rotational and vibrational distributions. There is a more modest increase in translational energy release. A larger fraction of the available energy is deposited in the liquid for squalene than for squalane, consistent with a more extensive geometry change on formation of the allylic radical co-product. Although the dominant reaction mechanism is direct, impulsive scattering, there is some evidence for OH being accommodated at both liquid surfaces, resulting in thermalised translation and rotational distributions. Despite the H-abstraction reaction being strongly favoured energetically for squalene, the yield of OH is substantially lower than for squalane. This is very likely due to competitive addition of O((3)P) to the unsaturated sites in squalene, implying that double bonds are extensively exposed at the liquid surface.

show abstract

Interfacial energy exchange and reaction dynamics in collisions of gases on model organic surfaces

Cited by 22 publications

References 173 publications

Role of Chemical Dynamics Simulations in Mass Spectrometry Studies of Collision-Induced Dissociation and Collisions of Biological Ions with Organic Surfaces

Role of Chemical Dynamics Simulations in Mass Spectrometry Studies of Collision-Induced Dissociation and Collisions of Biological Ions with Organic Surfaces

Atomic and Molecular Collisions at Liquid Surfaces

Site and bond-specific dynamics of reactions at the gas–liquid interface

Contact Info

Product

Resources

About