Infrared photofragmentation spectra of size-selected Krn+SF6 cluster ions

Atrill, S.; Stace, A. J.

doi:10.1039/a907634d

Cited by 6 publications

(4 citation statements)

References 25 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Using these methods, Eyler showed that IR spectra of covalently bound ions could be recorded (Baykut et al, 1985) and Beauchamp applied it to negative ions (Shin & Beauchamp, 1990). In addition to CO 2 lasers (Atrill & Stace, 2000), Stace and co-workers used CO lasers to access different parts of the IR spectrum (Odeneye & Stace, 2005). Unfortunately, gas-discharge lasers, such as CO 2 and CO lasers have a limited and discontinuous tuning range, which constrains their spectroscopic usefulness.…”

Section: Introductionmentioning

confidence: 99%

Vibrational spectroscopy of bare and solvated ionic complexes of biological relevance

Polfer

Oomens²

2009

Mass Spectrometry Reviews

402

393

View full text Add to dashboard Cite

The low density of ions in mass spectrometers generally precludes direct infrared (IR) absorption measurements. The IR spectrum of an ion can nonetheless be obtained by inducing photodissociation of the ion using a high-intensity tunable laser. The emergence of free electron lasers (FELs) and recent breakthroughs in bench-top lasers based on nonlinear optics have now made it possible to routinely record IR spectra of gas-phase ions. As the energy of one IR photon is insufficient to cause dissociation of molecules and strongly bound complexes, two main experimental strategies have been developed to effect photodissociation. In infrared multiple-photon dissociation (IR-MPD) many photons are absorbed resonantly and their energy is stored in the bath of vibrational modes, leading to dissociation. In the "messenger" technique a weakly bound van der Waals atom is detached upon absorption of a single photon. Fundamental, historical, and practical aspects of these methods will be presented. Both of these approaches make use of very different methods of ion preparation and manipulation. While in IR-MPD ions are irradiated in trapping mass spectrometers, the "messenger" technique is generally carried out in molecular beam instruments. The main focus of this review is the application of IR spectroscopy to biologically relevant molecular systems (amino acids, peptides, proteins). Particular issues that will be addressed here include gas-phase zwitterions, the (chemical) structures of peptides and their collision-induced dissociation (CID) products, IR spectra of gas-phase proteins, and the chelation of metal-ligand complexes. Another growing area of research is IR spectroscopy on solvated clusters, which offer a bridge between the gas-phase and solution environments. The development of state-of-the-art computational approaches has gone hand-in-hand with advances in experimental techniques. The main advantage of gas-phase cluster research, as opposed to condensed-phase experiments, is that the systems of interest can be understood in detail and structural effects can be studied in isolation. It will be shown that IR spectroscopy of mass-selected (bio)molecular systems is now well-placed to address specific questions on the individual effect of charge carriers (protons and metal ions), as well as solvent molecules on the overall structure.

show abstract

Section: Introductionmentioning

confidence: 99%

Vibrational spectroscopy of bare and solvated ionic complexes of biological relevance

Polfer

Oomens²

2009

Mass Spectrometry Reviews

402

393

View full text Add to dashboard Cite

show abstract

“…[23][24][25][26][27][28][29][30][31] Earlier, the structures of rare gas clusters mixed with SF 6 were investigated. [32][33][34][35][36] Mixed argon-nitrogen clusters are easily formed due to the small difference in inter-molecular potentials. 37,38 The structure and electronic properties of mixed Ar-N 2 clusters were investigated by electron diffraction, 39 surface scattering, 40 X-ray absorption spectroscopy, and zero kinetic energy photoelectron spectroscopy.…”

Section: Introductionmentioning

confidence: 99%

Structures of mixed argon-nitrogen clusters

Nagasaka

Serdaroglu

Flesch

et al. 2012

The Journal of Chemical Physics

View full text Add to dashboard Cite

The structures of mixed argon-nitrogen clusters of different compositions are investigated by analyzing core level shifts and relative intensities of surface and bulk sites in the Ar 2p(3/2) regime in soft X-ray photoelectron spectroscopy. These structures are confirmed by core level shift calculations taking induced dipole interactions into account, in which several model structures of the mixed clusters are considered by Monte Carlo simulations. These results suggest that the mixed argon-nitrogen clusters show partial core-shell structures, where an argon core is partially covered by nitrogen molecules.

show abstract

“…Since the dissociation requires the absorption of many infrared photons, powerful lasers need to be used and historically, mainly CO 2 lasers have been applied. [20][21][22][23][24] Recently, the use of CO lasers, covering the interesting wavelength range between roughly 1500 and 1900 cm À1 , for IRMPD spectroscopy has also been reported. 25 (Note that the term IRMPD is commonly used in MS applications as a method to induce molecular dissociation, see, e.g., ref.…”

Section: Introductionmentioning

confidence: 99%

Reaction products in mass spectrometry elucidated with infrared spectroscopy

Polfer

Oomens

2007

Phys. Chem. Chem. Phys.

221

178

View full text Add to dashboard Cite

Determining the structure and dynamics of large biologically relevant molecules is one of the key challenges facing biology. Although X-ray crystallography (XRD) and nuclear magnetic resonance (NMR) yield accurate structural information, they are of limited use when sample quantities are low. Mass spectrometry (MS) on the other hand has been very successful in analyzing biological molecules down to atto-mole quantities and has hence begun to challenge XRD and NMR as the key technology in the life sciences. This trend has been further assisted by the development of MS techniques that yield structural information on biomolecules. Of these techniques, collision-induced dissociation (CID) and hydrogen/deuterium exchange (HDX) are among the most popular. Despite advances in applying these techniques, little direct experimental evidence had been available until recently to verify their proposed underlying reaction mechanisms. The possibility to record infrared spectra of mass-selected molecular ions has opened up a novel avenue in the structural characterization of ions and their reaction products. On account of its high pulse energies and wide wavelength tunability, the free electron laser for infrared experiments (FELIX) at FOM Rijnhuizen has been shown to be ideally suited to study trapped molecular ions with infrared photo-dissociation spectroscopy. In this paper, we review recent experiments in our laboratory on the infrared spectroscopic characterization of reaction products from CID and HDX, thereby corroborating some of the reaction mechanisms that have been proposed. In particular, it is shown that CID gives rise to linear fragment ion structures which have been proposed for some time, but also yields fully cyclical ring structures. These latter structures present a possible challenge for using tandem MS in the sequencing of peptides/proteins, as they can lead to a scrambling of the amino acid sequence information. In gas-phase HDX of an amino acid it is shown that the structure can be changed from a charge solvated to a zwitterionic structure, thereby demonstrating that HDX can be an invasive technique, in fact changing the structure of the analyte. These results emphasize that more fundamental work is required in order to understand the underlying mechanisms in two of the most important structural techniques in MS.

show abstract

Infrared photofragmentation spectra of size-selected Krn+SF6 cluster ions

Cited by 6 publications

References 25 publications

Vibrational spectroscopy of bare and solvated ionic complexes of biological relevance

Vibrational spectroscopy of bare and solvated ionic complexes of biological relevance

Structures of mixed argon-nitrogen clusters

Reaction products in mass spectrometry elucidated with infrared spectroscopy

Contact Info

Product

Resources

About