Ion/surface collisions at functionalized self-assembled monolayer surfaces

Morris, Michael; Riederer, D. E.; Winger, Brian E.; Cooks, R. Graham; Ast, T.; Chidsey, Christopher E. D.

doi:10.1016/0168-1176(92)87016-8

Cited by 136 publications

(156 citation statements)

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“…Several reports in the literature discuss "hard" versus "soft" surfaces that have been loosely defined by the amount of fragmentation and the resulting scattering angle of the fragments after colliding with the surface. Hard surfaces such as fluorinated self-assembled monolayers (SAMs) generate a population of SID fragments with a narrower angular scattering distribution, whereas softer surfaces such as hydrocarbon SAMs create broader distributions [27]. Fluorinated surfaces have been shown to exhibit unique characteristics when used as collision targets, which can be attributed to their terminal mass [27].…”

Section: Small Molecule Projectiles: Sid and Rissmentioning

confidence: 99%

“…Hard surfaces such as fluorinated self-assembled monolayers (SAMs) generate a population of SID fragments with a narrower angular scattering distribution, whereas softer surfaces such as hydrocarbon SAMs create broader distributions [27]. Fluorinated surfaces have been shown to exhibit unique characteristics when used as collision targets, which can be attributed to their terminal mass [27]. The larger terminal mass of a fluorocarbon SAM, compared to a hydrocarbon SAM, results in a larger amount of laboratory energy conversion into the vibrational en- 193 ergy modes of a projectile ion when colliding on a fluorinated surface, about 20%, as opposed to only 13% on a hydrocarbon surface [28].…”

Section: Small Molecule Projectiles: Sid and Rissmentioning

confidence: 99%

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Surface-induced dissociation of small molecules, peptides, and non-covalent protein complexes

Wysocki

Joyce

Jones

et al. 2008

J. Am. Soc. Mass Spectrom.

130

138

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This article provides a perspective on collisions of ions with surfaces, including surfaceinduced dissociation (SID) and reactive ion scattering spectrometry (RISS). The content is organized into sections on surface-induced dissociation of small ions, surface characterization of organic thin films by collision of well-characterized ions into surfaces, the use of SID to probe peptide fragmentation, and the dissociation of large non-covalent complexes by SID. Examples are given from the literature with a focus on experiments from the authors' laboratory. The article is not a comprehensive review but is designed to provide the reader with an overview of the types of results possible by collisions of ions into surfaces. (J Am Soc Mass Spectrom 2008, 19, 190 -208) © 2008 American Society for Mass Spectrometry T andem mass spectrometry (MS/MS) is an essential tool for elucidating ion structure. The MS/MS experiment involves mass selection of a precursor ion followed by ion activation and subsequent dissociation. The ion activation step is commonly accomplished via collision-induced dissociation (CID) in which the initial kinetic energy of a projectile ion is converted into internal energy through inelastic collisions with a neutral gas. Several alternative activation methods have been used in tandem mass spectrometry, one of which is surfaceinduced dissociation (SID). SID is analogous to CID, except that a surface replaces the neutral gas as the collision target. A typical ion-surface collision event is illustrated in Figure 1.The incorporation of a surface into a mass spectrometer for ion activation was pioneered in the laboratory of R. Graham Cooks in the mid-1970s and early 1980s [1][2][3]. Since that time, collisions of lowenergy (eV) organic ions with surfaces within the tandem mass spectrometer have been valuable for analyzing surface composition, characterizing reactions between organic projectile ions and surface adsorbates, chemically modifying surfaces, and determining projectile ion structure. A major motivation for development of SID is that energy transfer to ionic projectiles can be improved by increasing the mass of the collision target. The total available energy for transfer into the internal modes of the projectile ion is defined by the center-of-mass energy (E COM ) described by eq 1:where E LAB is the laboratory collision energy and M ION and M N are the masses of the projectile ion and neutral, respectively. Energy transfer in CID is limited by the mass of the collision partner, typically inert gases such as helium, argon, or xenon. In SID, if one assumes that the surface is an infinitely large collision partner, E COM becomes independent of mass and approaches the laboratory collision energy. The assumption that the entire surface can be viewed as the collision partner is not always valid, however, and there are instances where the mass of the terminal groups on the surface influence the amount of energy transfer [4,5]. Nonetheless, the use of a massive surface target should, in theory, provide ...

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Section: Small Molecule Projectiles: Sid and Rissmentioning

confidence: 99%

Section: Small Molecule Projectiles: Sid and Rissmentioning

confidence: 99%

Surface-induced dissociation of small molecules, peptides, and non-covalent protein complexes

Wysocki

Joyce

Jones

et al. 2008

J. Am. Soc. Mass Spectrom.

130

138

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“…Parameters for these potentials were determined using CH 4 , NH 4 ϩ , H 2 CO, NH 3 and H 2 O as models representing different types of atoms and functional groups of the peptide ion [17]. This potential accurately describes the short-range, repulsive interactions which determine the collisional energy-transfer, but not the longrange intermolecular potential.…”

Section: Potential Energy Functionmentioning

confidence: 99%

“…In SID, a fraction of the ion's kinetic energy is converted into vibrational excitation resulting in its dissociation. The efficiency of this translational to vibrational energy-transfer strongly depends on the properties of the surface [2][3][4][5]. SID occurs via two mechanisms known as non-shattering and shattering [6].…”

mentioning

confidence: 99%

Importance of shattering fragmentation in the surface-induced dissociation of protonated octaglycine

Park

Deb

Song

et al. 2009

J. Am. Soc. Mass Spectrom.

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A QM ϩ MM direct chemical dynamics simulation was performed to study collisions of protonated octaglycine, gly 8 -H ϩ , with the diamond {111} surface at an initial collision energy E i of 100 eV and incident angle i of 0°and 45°. The semiempirical model AM1 was used for the gly 8 -H ϩ intramolecular potential, so that its fragmentation could be studied. Shattering dominates gly 8 -H ϩ fragmentation at i ϭ 0°, with 78% of the ions dissociating in this way. At i ϭ 45°shattering is much less important. For i ϭ 0°there are 304 different pathways, many related by their backbone cleavage patterns. For the i ϭ 0°fragmentations, 59% resulted from both a-x and b-y cleavages, while for i ϭ 45°70% of the fragmentations occurred with only a-x cleavage. For i ϭ 0°, the average percentage energy transfers to the internal degrees of freedom of the ion and the surface, and the energy remaining in ion translation are 45%, 26%, and 29%. For 45°these percentages are 26%, 12%, and 62%. The percentage energy-transfer to ⌬E int for i ϭ 0°is larger than that reported in previous experiments for collisions of des-Arg 1 -bradykinin with a diamond surface at the same i . This difference is discussed in terms of differences between the model diamond surface used in the simulations and the diamond surface prepared for the experiments. (J Am Soc Mass Spectrom 2009, 20, 939 -948)

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“…Organic thin films on metal substrates substantially reduce neutralization of projectile ions. Surfaces commonly used in SID experiments include self-assembled monolayers of n-alkanethiols (HSAM) and their fluorinated analogs (FSAM) on gold or silver (Morris et al, 1992;Cooks et al, 1994;Dongre, Somogyi, & Wysocki, 1996), thin films of a liquid perfluoropolyether (Koppers et al, 1997), Langmuir-Blodgett (L-B) films (Gu et al, 1999) or highly oriented pyrolytic graphite (Beck et al, 1996a). Thin films of insulating materials (such as metal halides or diamond) on metal substrates have a great potential for efficient dissociation of large molecules (Laskin & Futrell, 2003b).…”

Section: Choice Of the Sid Targetmentioning

confidence: 99%

Activation of large lons in FT‐ICR mass spectrometry

Laskin

Futrell

2004

Mass Spectrometry Reviews

177

146

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The advent of soft ionization techniques, notably electrospray and laser desorption ionization methods, has enabled the extension of mass spectrometric methods to large molecules and molecular complexes. This both greatly extends the applications of mass spectrometry and makes the activation and dissociation of complex ions an integral part of these applications. This review emphasizes the most promising methods for activation and dissociation of complex ions and presents this discussion in the context of general knowledge of reaction kinetics and dynamics largely established for small ions. We then introduce the characteristic differences associated with the higher number of internal degrees of freedom and high density of states associated with molecular complexity. This is reflected primarily in the kinetics of unimolecular dissociation of complex ions, particularly their slow decay and the higher energy content required to induce decomposition-the kinetic shift (KS). The longer trapping time of Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) significantly reduces the KS, which presents several advantages over other methods for the investigation of dissociation of complex molecules. After discussing general principles of reaction dynamics related to collisional activation of ions, we describe conventional ways to achieve single-and multiple-collision activation in FT-ICR MS. Sustained off-resonance irradiation (SORI)-the simplest and most robust means of introducing the multiple collision activation process-is discussed in greatest detail. Details of implementation of this technique, required control of experimental parameters, limitations, and examples of very successful application of SORI-CID are described. The advantages of high mass resolving power and the ability to carry out several stages of mass selection and activation intrinsic to FT-ICR MS are demonstrated in several examples. Photodissociation of ions from small molecules can be effected using IR or UV/vis lasers and generally requires tuning lasers to specific wavelengths and/ or utilizing high flux, multiphoton excitation to match energy levels in the ion. Photodissociation of complex ions is much easier to accomplish from the basic physics perspective. The quasi-continuum of vibrational states at room temperature makes it very easy to pump relatively large amounts of energy into complex ions and infrared multiphoton dissociation (IRMPD) is a powerful technique for characterizing large ions, particularly biologically relevant molecules. Since both SORI-CID and IRMPD are slow activation methods they have many common characteristics. They are also distinctly different because SORI-CID is intrinsically selective (only ions that have a cyclotron frequency close to the frequency of the excitation field are excited), whereas IRMPD is not (all ions that reside on the optical path of the laser are excited). There are advantages and disadvantages to each technique and in many applications they complement each other. In contrast wi...

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Ion/surface collisions at functionalized self-assembled monolayer surfaces

Cited by 136 publications

References 47 publications

Surface-induced dissociation of small molecules, peptides, and non-covalent protein complexes

Surface-induced dissociation of small molecules, peptides, and non-covalent protein complexes

Importance of shattering fragmentation in the surface-induced dissociation of protonated octaglycine

Activation of large lons in FT‐ICR mass spectrometry

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