Vibrational predissociation spectroscopy of the H2-tagged mono- and dicarboxylate anions of dodecanedioic acid

Kamrath, Michael Z.; Relph, Rachael A.; Guasco, Timothy L.; Leavitt, Christopher M.; Johnson, Mark A.

doi:10.1016/j.ijms.2010.10.021

Cited by 140 publications

(184 citation statements)

References 45 publications

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“…The experimentally estimated binding of a given H 2 molecule to a negatively charged cluster is around 7 kJ/mol (∼600 cm −1 ). 64 The Journal of Physical Chemistry A In all of the hydrated clusters, water seems to be acting like a tag in the sense that the high %RMS H peaks above 1200 cm −1 are observed (e.g., the peaks at ∼1400 cm −1 ) and their intensities are qualitatively comparable to the simulated results. This inference is in agreement with (a) the calculated binding energy of water to bisulfate, which is less than one-third that of sulfuric acid to bisulfate (Table 1), and (b) the observed fragmentation pattern of the larger clusters, in which significant water loss occurs with only small contributions of the total fragment ion signal coming from acid loss.…”

Section: Analysis and Discussionsupporting

confidence: 64%

Vibrational Spectroscopy of Bisulfate/Sulfuric Acid/Water Clusters: Structure, Stability, and Infrared Multiple-Photon Dissociation Intensities

et al. 2013

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ABSTRACT:The structure and stability of mass-selected bisulfate, sulfuric acid, and water cluster anions, HSO 4 − (H 2 SO 4 ) m (H 2 O) n , are studied by infrared photodissociation spectroscopy aided by electronic structure calculations. The triply hydrogen-bound HSO 4 − (H 2 SO 4 ) configuration appears as a recurring motif in the bare clusters, while incorporation of water disrupts this stable motif for clusters with m > 1. Infrared-active vibrations predominantly involving distortions of the hydrogenbound network are notably missing from the infrared multiplephoton dissociation (IRMPD) spectra of these ions but are fully recovered by messenger-tagging the clusters with H 2 . A simple model is used to explain the observed "IRMPD transparency".

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Section: Analysis and Discussionsupporting

confidence: 64%

Vibrational Spectroscopy of Bisulfate/Sulfuric Acid/Water Clusters: Structure, Stability, and Infrared Multiple-Photon Dissociation Intensities

et al. 2013

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“…The ions were stored for ∼90 ms, during which they are collisionally cooled by helium buffer gas. The buffer gas was doped with about 10% D 2 , which condensed onto the cluster of interest at these cold temperatures and acted as the spectroscopic messenger (34). The cold clusters were ejected from the trap into the extraction region of a Wiley-McLaren TOF mass spectrometer.…”

Section: Methodsmentioning

confidence: 99%

Site-specific vibrational spectral signatures of water molecules in the magic H ₃ O ⁺ (H ₂ O) ₂₀ and Cs ⁺ (H ₂ O) ₂₀ clusters

Fournier

Wolke

Johnson

et al. 2014

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

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Theoretical models of proton hydration with tens of water molecules indicate that the excess proton is embedded on the surface of clathrate-like cage structures with one or two water molecules in the interior. The evidence for these structures has been indirect, however, because the experimental spectra in the critical H-bonding region of the OH stretching vibrations have been too diffuse to provide band patterns that distinguish between candidate structures predicted theoretically. Here we exploit the slow cooling afforded by cryogenic ion trapping, along with isotopic substitution, to quench water clusters attached to the H 3 O + and Cs + ions into structures that yield well-resolved vibrational bands over the entire 215-to 3,800-cm −1 range. The magic H 3 O + (H 2 O) 20 cluster yields particularly clear spectral signatures that can, with the aid of ab initio predictions, be traced to specific classes of network sites in the predicted pentagonal dodecahedron H-bonded cage with the hydronium ion residing on the surface.water clusters | cryogenic vibrational spectroscopy | hydrogen bonding O ver the last decade, the cooperative mechanics underlying the microhydration of simple ions has undergone a renaissance due to rapid advances in experimental and theoretical methods. On the experimental side, it is routine to capture and study size-selected species cooled to cryogenic temperatures (1-5), and theoretical techniques are now capable of handling tens of atoms with all-electron, "supermolecule" approaches, where complex hydration networks are treated in the ansatz of polyatomic molecular physics (6). A dramatic example of the new insights afforded by this combined approach is the recent elucidation of the spectral signature associated with the hydronium ion when it is accommodated on the surface of a pentagonal dodecahedral cage formed by the "magic" H 3 O + (H 2 O) 20 cluster (7). The theoretical structure proposed earlier (8) (denoted I) is illustrated in Fig. 1, and the recently reported D 2 predissociation spectrum of the cryogenically cooled, D 2 tagged H 3 O + (H 2 O) 20 cluster is compared with that observed for the H 3 O + (H 2 O) 3 Eigen cation (9, 10) in Fig. 1 A and B, respectively. The key bands derived from the OH stretching motions of the surface-embedded hydronium (denoted ν a H3O +) were assigned (7) to the broad features in the experimental spectrum about 500 cm −1 below the corresponding bands in the free Eigen cation. The intramolecular HOH bending and OH stretching modes of the surface water molecules are not strongly shifted by introduction of the ion, however, where the latter appear as a broad envelope spanning the 3,000-to 3,700-cm −1 range typical of liquid water. An interesting aspect of the D 2 tagged spectrum obtained with cryogenic cooling (as opposed to that reported on the same ion generated under the more rapid quenching conditions at play in a supersonic jet ion source) (8, 11) is that distinct features begin to emerge above the continuous background absorption in the OH stretchin...

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“…The H 2 -tagged molecules are then extracted from the trap and intersected with a tunable infrared OPO 2 μs after extraction. Resonant absorption with subsequent intramolecular vibrational redistribution leads to photo-evaporation of H 2, which has a typical binding energy of 370-600 cm -1 [50][51][52]. This is detected as a dip in the H + GPGG ·H 2 signal in the time-of-flight analysis.…”

Section: Infrared Spectroscopymentioning

confidence: 99%

“…We acquire infrared spectra through H 2 predissociation as first demonstrated by Okumura et al [47][48][49] and later generalized by Johnson [50]. In this process, H 2 adducts are formed with the molecule of interest in the planar ion trap through threebody collisions involving the cold ions and H 2 molecules.…”

Section: Infrared Spectroscopymentioning

confidence: 99%

Infrared Spectroscopy of Mobility-Selected H⁺-Gly-Pro-Gly-Gly (GPGG)

Masson

Kamrath

Perez

et al. 2015

J. Am. Soc. Mass Spectrom.

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109

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Abstract. We report the first results from a new instrument capable of acquiring infrared spectra of mobility-selected ions. This demonstration involves using ion mobility to first separate the protonated peptide Gly-Pro-Gly-Gly (GPGG) into two conformational families with collisional cross-sections of 93.8 and 96.8 Å 2 . After separation, each family is independently analyzed by acquiring the infrared predissociation spectrum of the H 2 -tagged molecules. The ion mobility and spectroscopic data combined with density functional theory (DFT) based molecular dynamics simulations confirm the presence of one major conformer per family, which arises from cis/trans isomerization about the proline residue. We induce isomerization between the two conformers by using collisional activation in the drift tube and monitor the evolution of the ion distribution with ion mobility and infrared spectroscopy. While the cis-proline species is the preferred gas-phase structure, its relative population is smaller than that of the trans-proline species in the initial ion mobility drift distribution. This suggests that a portion of the trans-proline ion population is kinetically trapped as a higher energy conformer and may retain structural elements from solution.

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Vibrational predissociation spectroscopy of the H2-tagged mono- and dicarboxylate anions of dodecanedioic acid

Cited by 140 publications

References 45 publications

Vibrational Spectroscopy of Bisulfate/Sulfuric Acid/Water Clusters: Structure, Stability, and Infrared Multiple-Photon Dissociation Intensities

Vibrational Spectroscopy of Bisulfate/Sulfuric Acid/Water Clusters: Structure, Stability, and Infrared Multiple-Photon Dissociation Intensities

Site-specific vibrational spectral signatures of water molecules in the magic H ₃ O ⁺ (H ₂ O) ₂₀ and Cs ⁺ (H ₂ O) ₂₀ clusters

Infrared Spectroscopy of Mobility-Selected H⁺-Gly-Pro-Gly-Gly (GPGG)

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Vibrational predissociation spectroscopy of the H2-tagged mono- and dicarboxylate anions of dodecanedioic acid

Cited by 140 publications

References 45 publications

Vibrational Spectroscopy of Bisulfate/Sulfuric Acid/Water Clusters: Structure, Stability, and Infrared Multiple-Photon Dissociation Intensities

Vibrational Spectroscopy of Bisulfate/Sulfuric Acid/Water Clusters: Structure, Stability, and Infrared Multiple-Photon Dissociation Intensities

Site-specific vibrational spectral signatures of water molecules in the magic H 3 O + (H 2 O) 20 and Cs + (H 2 O) 20 clusters

Infrared Spectroscopy of Mobility-Selected H+-Gly-Pro-Gly-Gly (GPGG)

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Product

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Site-specific vibrational spectral signatures of water molecules in the magic H ₃ O ⁺ (H ₂ O) ₂₀ and Cs ⁺ (H ₂ O) ₂₀ clusters

Infrared Spectroscopy of Mobility-Selected H⁺-Gly-Pro-Gly-Gly (GPGG)