Dissociation pathways of sulfur dioxide clusters and mixed sulfur dioxide-water clusters

Zhong, Qun; Hurley, S. M.; Castleman, A. W.

doi:10.1016/s1387-3806(98)14211-2

Cited by 17 publications

(24 citation statements)

References 28 publications

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“…12,13,21 Nonetheless, results presented in the present work ͑Fig. 6͒ lead to the conclusion that ͑H 2 O͒ n−1 H + arise from ͑H 2 O͒ n neutrals.…”

Section: Generation Of Mixed "Sosupporting

confidence: 55%

“…Femtosecond ionization spectra show that the ͑SO 2 ͒H + ion is detected from the ionization of the mixed neutral dimer ͑SO 2 ͒͑H 2 O͒. 12,13,21 In the present experiment with 26.5 eV ionization, obvious signals of the unprotonated mixed dimer ion ͑SO 2 ͒ ϫ͑H 2 O͒ + ͑Fig. 5͒ and mixed ͑SO 2 ͒ n ͑H 2 O͒ + ions ͑1 ഛ n ഛ 5͒ ͑Fig.…”

Section: Generation Of Mixed "Somentioning

confidence: 53%

“…Multiphoton ionization of ͑SO 2 ͒ n by femtosecond laser excitation shows much more extensive fragmentation, with ͑SO 2 ͒ n−1 SO + features being more intense than parent ͑SO 2 ͒ n + features. [19][20][21] One advantage of femtosecond versus nanosecond multiphoton ionization is that up pumping to the ion state typically precludes dissociation reactions for the neutral cluster during the ultrafast ionization process. Apparently, single photon, even 26.5 eV, ionization imparts much less final energy "excess energy" over that required for vertical ionization.…”

Section: Discussionmentioning

confidence: 99%

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Single photon ionization of van der Waals clusters with a soft x-ray laser: (SO2)n and (SO2)n(H2O)m

Dong

Heinbuch

Rocca

et al. 2006

The Journal of Chemical Physics

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van der Waals cluster ͑SO 2 ͒ n is investigated by using single photon ionization of a 26.5 eV soft x-ray laser. During the ionization process, neutral clusters suffer a small fragmentation because almost all energy is taken away by the photoelectron and a small part of the photon energy is deposited into the ͑SO 2 ͒ n cluster. The distribution of ͑SO 2 ͒ n clusters decreases roughly exponentially with increasing cluster size. The photoionization dissociation fraction of I͓͑SO 2 ͒ n−1 SO + ͔ / I͓͑SO 2 ͒ n + ͔ decreases with increasing cluster size due to the formation of cluster. The metastable dissociation rate constants of ͑SO 2 ͒ n + are measured in the range of ͑0.6-1.5͒ ϫ 10 4 s −1 for cluster sizes 5 ഛ n ഛ 16. Mixed SO 2 -H 2 O clusters are studied at different experimental conditions. At the condition of high SO 2 concentration ͑20% SO 2 partial pressure͒, ͑SO 2 ͒ n + cluster ions dominate the mass spectrum, and the unprotonated mixed cluster ions ͑SO 2 ͒ n H 2 O + ͑1 ഛ n ഛ 5͒ are observed. At the condition of low SO 2 concentration ͑5% SO 2 partial pressure͒ ͑H 2 O͒ n H + cluster ions are the dominant signals, and protonated cluster ions ͑SO 2 ͒͑H 2 O͒ n H + are observed. The mixed clusters, containing only one SO 2 or H 2 O molecule, SO 2 ͑H 2 O͒ n H + and ͑SO 2 ͒ n H 2 O + are observed, respectively.

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“…12,13,21 Nonetheless, results presented in the present work ͑Fig. 6͒ lead to the conclusion that ͑H 2 O͒ n−1 H + arise from ͑H 2 O͒ n neutrals.…”

Section: Generation Of Mixed "Sosupporting

confidence: 55%

Section: Generation Of Mixed "Somentioning

confidence: 53%

Section: Discussionmentioning

confidence: 99%

See 1 more Smart Citation

Single photon ionization of van der Waals clusters with a soft x-ray laser: (SO2)n and (SO2)n(H2O)m

Dong

Heinbuch

Rocca

et al. 2006

The Journal of Chemical Physics

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“…Castleman and co-workers have studied protonated sulfur dioxide-water clusters experimentally and characterized them mass-spectroscopically. 22,23 Clusters of constitution H 3 SO 3 + indicated that SO(OH) 2 does not form in aqueous environment. Other studies investigated SO 2 and water mixtures showing the structure and stability of this complex.…”

Section: Introductionmentioning

confidence: 99%

On the Formation of the Sulfonate Ion from Hydrated Sulfur Dioxide

et al. 2004

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In solutions of hydrated SO 2 it is well-known that both the bisulfite ion HOSO 2 -and the sulfonate ion HSO 3 -are present whereas the sulfonate form prevails in some salts. Here we show by ab initio and transition state theory considerations how the mechanism of sulfonate formation works. In aqueous solution, dissolved SO 2 first forms a bisulfite ion which is in a next step converted into the sulfonate ion. Direct formation of the sulfonate ion is kinetically hindered due to a very high reaction barrier for this process. Tautomerization of the bisulfite ion into the sulfonate ion is catalyzed by water molecules. Insight into this process is vital in understanding the formation of sulfonate salts upon crystallization from aqueous solution.

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“…This catalytic effect not only accelerates the rate of decomposition but also explains why attempts to isolate sulfurous acid from aqueous SO 2 solutions failed. Castleman and co‐workers have studied protonated sulfur dioxide–water clusters experimentally and characterized them mass‐spectroscopically 23, 24. Clusters of constitution H 3 SO 3 + are composed of two isomers, namely H 2 OH + ⋅ SO 2 and SO 2 H + ⋅ H 2 O, but not of S(OH) 3 + ; this shows that H 2 SO 3 does not form in an aqueous environment.…”

Section: Introductionmentioning

confidence: 99%

About the Stability of Sulfurous Acid (H2SO3) and Its Dimer

Voegele¹,

Tautermann²,

Loerting³

et al. 2002

Chem. Eur. J.

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A series of optically active helical polyphosphazene block copolymers of general formula R[NP(O2C20H12)]n‐b‐[NPMePh]m (R‐7 a–c) was synthesized and characterized. The polymers were prepared by sequential living cationic polycondensation of N‐silylphosphoranimines using the mono‐end‐capped initiator [Ph3PNPCl3][PCl6] (5) and exhibit a low polydispersity index (ca. 1.3). The temperature dependence of the specific optical activity ([α]D) of R‐7 a,b relative to that for the homopolymers R‐[NP(O2C20H12)]n (R‐8 a) and the R/S analogues (R/S‐7 a,b), revealed that the binaphthoxy–phosphazene segments induce a preferential helical conformation in the [NPMePh] blocks through a “sergeant‐and‐soldiers” mechanism, an effect that is unprecedented in polyphosphazenes. The self‐assembly of drop‐cast thin films of the chiral block copolymer R‐7 b (bearing a long chiral and rigid R[NP(O2C20H12)] segment) evidenced a transfer of helicity mechanism, leading to the formation of twisted morphologies (twisted “pearl necklace”), not observed in the nonchiral R/S‐7 b. The chiral R‐7 a and the nonchiral R/S‐7 a, self‐assemble by a nondirected morphology reconstruction process into regular‐shaped macroporous films with chiral‐rich areas close to edge of the pore. This is the first nontemplate self‐assembly route to chiral macroporous polymeric films with pore size larger than 50 nm. The solvent annealing (THF) of these films leads to the formation of regular spherical nanostructures (ca. 50 nm), a rare example of nanospheres exclusively formed by synthetic helical polymers.

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Dissociation pathways of sulfur dioxide clusters and mixed sulfur dioxide-water clusters

Cited by 17 publications

References 28 publications

Single photon ionization of van der Waals clusters with a soft x-ray laser: (SO2)n and (SO2)n(H2O)m

Single photon ionization of van der Waals clusters with a soft x-ray laser: (SO2)n and (SO2)n(H2O)m

On the Formation of the Sulfonate Ion from Hydrated Sulfur Dioxide

About the Stability of Sulfurous Acid (H2SO3) and Its Dimer

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