Multiphoton dissociation of molecules with low power continuous wave infrared laser radiation

Woodin, R. L.; Bomse, David S.; Beauchamp, J. L.

doi:10.1021/ja00478a065

Cited by 213 publications

(151 citation statements)

References 4 publications

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“…The complementary a/z ions are radical ions. Such a⅐/z⅐ ions are observed at low abundance in the mass spectra following ECD of dC 5 -dC 7 . Their lower abundance may be attributed to the lower stability of radical ions, in analogy with the previous observation that the abundance of z⅐ ions is typically about half of that of even-electron c ions in ECD of peptides [28].…”

Section: Pathways and Mechanisms For Ecd Cleavage Of Dnamentioning

confidence: 99%

“…For dC 4 , the isotopic distribution corresponding to base loss from the reduced parent ion shows the presence of both ([M ϩ 2H] ϩ⅐ Ϫ CH) and ([M ϩ H] ϩ Ϫ CH), in which CH denotes a neutral cytosine base [73] (mass 111.0432). For dC 6 and dC 7 , the corresponding distributions show the presence of ([M ϩ 2H] ϩ⅐ Ϫ CH) and ([M ϩ 2H] ϩ⅐ Ϫ C⅐), in which C⅐ is a radical cytosine base of mass, 110.0354. No base loss from the reduced parent ion was seen from ECD of dC 5 .…”

Section: Pathways and Mechanisms For Ecd Cleavage Of Dnamentioning

confidence: 99%

“…These ions could also be d-type fragment ions (see text). One radical "sequence" ion (labeled a n ⅐) is seen in the spectra of dC 5 -dC 7 , respectively. Cytosine neutral base (CH) loss is observed from the w/d ions and, to a low degree, from the reduced parent ions.…”

Section: Pathways and Mechanisms For Ecd Cleavage Of Dnamentioning

confidence: 99%

“…A biomolecule sequence is generally obtained by tandem mass spectrometry (MS/MS) [5], in which a parent ion is first isolated from other ions of different mass-to-charge (m/z) ratio and then dissociated into sequence-specific fragment ions. The fragmentation technique (e.g., collision induced dissociation (CID) [6], infrared multiphoton dissociation (IRMPD) [7,8], blackbody infrared radiative dissociation (BIRD) [9,10], surface induced dissociation (SID) [11], or ultraviolet photodissociation [12,13]) as well as the nature of the parent ion charge (singly versus multiply charged, protonation versus metal cation attachment, cation versus anion, etc.) play key roles in determining the major fragmentation processes.…”

mentioning

confidence: 99%

“…A unique fragmentation of adenine-containing oligonucleotides was explained by interaction between the adenine base and the phosphate backbone, lowering the proton affinity of the base. Here, we present ECD results for doubly protonated and protonated/cationized homodeoxynucleotides, dC 4 -dC 7 , dG 5 , dG 7 , and dA 6 , as well as d(GCATGC), which contains all four kinds of nucleotides. We chose to investigate both protonated and protonated/cationized oligonucleotides because we had observed earlier that such precursor ions fragment very differently in ECD of O-glycosylated peptides [55].…”

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confidence: 99%

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Electron capture dissociation and infrared multiphoton dissociation of oligodeoxynucleotide dications

Håkansson

Hudgins

Marshall

et al. 2003

J. Am. Soc. Mass Spectrom.

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We report electron capture dissociation (ECD) and infrared multiphoton dissociation (IRMPD) of doubly protonated and protonated/alkali metal ionized oligodeoxynucleotides. Mass spectra following ECD of the homodeoxynucleotides polydC, polydG, and polydA contain w or d "sequence" ions. For polydC and polydA, the observed fragments are even-electron ions, whereas radical w/d ions are observed for polydG. Base loss is seen for polydG and polydA but is a minor fragmentation pathway in ECD of polydC. We also observe fragment ions corresponding to w/d plus water in the spectra of polydC and d(GCATGC). Although the structure of these ions is not clear, they are suggested to proceed through a pentavalent phosphorane intermediate. The major fragment in ECD of d(GCATGC) is a d ion. Radical a-or z-type fragment ions are observed in most cases. IRMPD primarily results in base loss, but backbone fragmentation is also observed. IRMPD provides more sequence information than ECD, but the spectra are more complex due to extensive base and water losses. It is proposed that the smaller degree of sequence coverage in ECD, with fragmentation mostly occurring close to the ends of the molecules, is a consequence of a mechanism in which the electron is captured at a P¢O bond, resulting in a negatively charged phosphate group. Consequently, at least two protons (or alkali metal cations) must be present to observe a w or d fragment ion, a requirement that is less likely for small fragments. , in which a parent ion is first isolated from other ions of different mass-to-charge (m/z) ratio and then dissociated into sequence-specific fragment ions. The fragmentation technique (e.g., collision induced dissociation (CID) [6], infrared multiphoton dissociation (IRMPD) [7,8], blackbody infrared radiative dissociation (BIRD) [9,10], surface induced dissociation (SID) [11], or ultraviolet photodissociation [12,13]) as well as the nature of the parent ion charge (singly versus multiply charged, protonation versus metal cation attachment, cation versus anion, etc.) play key roles in determining the major fragmentation processes.To date most attention has focused on the fragmentation reactions of even-electron ions, but electrospray ionization in combination with ion-ion reactions, ionelectron reactions, or ion-neutral reactions have opened up new opportunities to examine the fragmentation reactions of odd-electron ions. Examples include electron capture dissociation (ECD) of [M ϩ nH] nϩ ions of peptides and proteins [14,15], polymers [16,17] [24], and CID of a Cu(II)-amine-peptide complex [25]. In each case, the formation of the radical cation (or anion) results in new fragmentation pathways, which are complementary to those observed for even-electron fragmentation. For example, disulfide bond cleavage is observed as a major fragmentation pathway in ECD [26], whereas such cleavage is not observed in CID or IRMPD. In other instances, novel fragmentation chem-

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Section: Pathways and Mechanisms For Ecd Cleavage Of Dnamentioning

confidence: 99%

Section: Pathways and Mechanisms For Ecd Cleavage Of Dnamentioning

confidence: 99%

Section: Pathways and Mechanisms For Ecd Cleavage Of Dnamentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

See 3 more Smart Citations

Electron capture dissociation and infrared multiphoton dissociation of oligodeoxynucleotide dications

Håkansson

Hudgins

Marshall

et al. 2003

J. Am. Soc. Mass Spectrom.

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Gas phase activation energy for unimolecular dissociation of biomolecular ions determined by Focused RAdiation for Gaseous Multiphoton ENergy Transfer (FRAGMENT)

Freitas

Hendrickson

Marshall

1999

Rapid Commun. Mass Spectrom.

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We present a novel approach for the determination of activation energy for the unimolecular dissociation of a large (>50 atoms) ion, based on measurement of the unimolecular dissociation rate constant as a function of continuous-wave CO(2) laser intensity. Following a short ( approximately 1 s) induction period, CO(2) laser irradiation produces an essentially blackbody internal energy distribution, whose 'temperature' varies inversely with laser intensity. The only currently available method for measuring such activation energies is blackbody infrared radiative dissociation (BIRD). Compared with BIRD, FRAGMENT: (a) eliminates the need to heat the surrounding ion trap and vacuum chamber to each of several temperatures (each requiring hours for temperature equilibration); (b) offers a three-fold wider range of effective blackbody temperature; and (c) extends the range of applications to include initially cold ions (e.g., gas-phase H/D exchange). Our FRAGMENT-determined activation energy for dissociation of protonated bradykinin, 1.2 +/- 0.1 eV, agrees within experimental error to the value, 1.3 +/- 0.1 eV, previously reported by Williams et al. from BIRD experiments. Copyright 1999 John Wiley & Sons, Ltd.

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Fourier transform ion cyclotron resonance mass spectrometry: A primer

Marshall

Hendrickson

Jackson

1998

Mass Spectrom. Rev.

1,851

1,541

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Multiphoton dissociation of molecules with low power continuous wave infrared laser radiation

Cited by 213 publications

References 4 publications

Electron capture dissociation and infrared multiphoton dissociation of oligodeoxynucleotide dications

Electron capture dissociation and infrared multiphoton dissociation of oligodeoxynucleotide dications

Gas phase activation energy for unimolecular dissociation of biomolecular ions determined by Focused RAdiation for Gaseous Multiphoton ENergy Transfer (FRAGMENT)

Fourier transform ion cyclotron resonance mass spectrometry: A primer

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