Excited-State Dynamics of (SO<sub>2</sub>)<sub>m</sub> Clusters

Te, Dermota; Dp, Hydutsky; Nj, Bianco; Aw, Castleman

doi:10.1021/jp052529u

Cited by 14 publications

(14 citation statements)

References 38 publications

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“…II A͒ is n BSI = N BSI / n and the EII level ͑calculated using the procedure of Sec. [42][43][44][45][46][47] The simulated values of n ii L ͑at t L Ӎ 92 fs͒ exhibit an irregular cluster size dependence at different values of I M . 1, reveals saturation or near saturation of the inner ionization level.…”

Section: B Gross Features Of Inner Ionizationmentioning

confidence: 92%

“…1 The response of elemental and molecular clusters to nearinfrared ultraintense laser fields ͑peak intensity I M =10 15 -10 20 W cm −2 , temporal width = 10-100 fs͒ drives novel ionization processes and manifests new features of electron dynamics 2,3,7,8,[16][17][18][21][22][23][24] on the time scale of Ͻ1 -100 fs. 2,3,10,11,16,17,[21][22][23]26,29,32,33 Extreme multielectron ionization of elemental and molecular clusters, e.g., Ar n , [3][4][5][6][7][37][38][39][40] Xe n , 2,3,5,13,15,26,35,38 ͑H 2 ͒ n , 41 ͑D 2 ͒ n , 42-45 ͑H 2 O͒ n , 34,46 ͑D 2 O͒ n , 27,34 ͑CH 4 ͒ n , 30 ͑CD 4 ͒ n , 20,30,47 and ͑HI͒ n , 46,48,…”

Section: Introductionmentioning

confidence: 99%

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Extreme ionization of Xe clusters driven by ultraintense laser fields

Heidenreich

Last

Jortner

2007

The Journal of Chemical Physics

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We applied theoretical models and molecular dynamics simulations to explore extreme multielectron ionization in Xe(n) clusters (n=2-2171, initial cluster radius R(0)=2.16-31.0 A) driven by ultraintense infrared Gaussian laser fields (peak intensity I(M)=10(15)-10(20) W cm(-2), temporal pulse length tau=10-100 fs, and frequency nu=0.35 fs(-1)). Cluster compound ionization was described by three processes of inner ionization, nanoplasma formation, and outer ionization. Inner ionization gives rise to high ionization levels (with the formation of [Xe(q+)](n) with q=2-36), which are amenable to experimental observation. The cluster size and laser intensity dependence of the inner ionization levels are induced by a superposition of barrier suppression ionization (BSI) and electron impact ionization (EII). The BSI was induced by a composite field involving the laser field and an inner field of the ions and electrons, which manifests ignition enhancement and screening retardation effects. EII was treated using experimental cross sections, with a proper account of sequential impact ionization. At the highest intensities (I(M)=10(18)-10(20) W cm(-2)) inner ionization is dominated by BSI. At lower intensities (I(M)=10(15)-10(16) W cm(-2)), where the nanoplasma is persistent, the EII contribution to the inner ionization yield is substantial. It increases with increasing the cluster size, exerts a marked effect on the increase of the [Xe(q+)](n) ionization level, is most pronounced in the cluster center, and manifests a marked increase with increasing the pulse length (i.e., becoming the dominant ionization channel (56%) for Xe(2171) at tau=100 fs). The EII yield and the ionization level enhancement decrease with increasing the laser intensity. The pulse length dependence of the EII yield at I(M)=10(15)-10(16) W cm(-2) establishes an ultraintense laser pulse length control mechanism of extreme ionization products.

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Section: B Gross Features Of Inner Ionizationmentioning

confidence: 92%

Section: Introductionmentioning

confidence: 99%

Extreme ionization of Xe clusters driven by ultraintense laser fields

Heidenreich

Last

Jortner

2007

The Journal of Chemical Physics

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“…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%

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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“…In addition, in many areas of atmospheric and biological chemistry, one of the basic processes of interest is the acid ionization of HI molecules in aqueous media to form the contact ion-pair I − (H 3 O) + (H 2 O) n−1 [29,30]. Excitation of the HI molecule to the g 3 − Rydberg state and the subsequent transition to the V 1 + valence state is a means of photoinducing the ion-pair formation process that occurs spontaneously in bulk solution [31].…”

Section: Introductionmentioning

confidence: 99%

Study on the (HI)_m(H₂O)_n Clusters by Photofragment Translational Spectroscopy and Ab-Initio Calculation

Bi¹,

Xu²,

Huang³

et al. 2007

Zeitschrift Für Physikalische Chemie

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The photodissociation of the clusters (HI) m (H 2 O) n in the supersonic molecular beam has been investigated at 281.73 nm and 280.99 nm by photofragment translational spectroscopy (PTS). The translational energy distributions of the photofragment I* ( 2 P 1/2 ) show that the photodissociated species is mainly HI(H 2 O) n (n ≥ 4) clusters. In addition, the structures and the relative stability of (HI) m , (H 2 O) n and (HI) m (H 2 O) n (m = 1 ∼ 4, n = 1 ∼ 6) clusters have been obtained by ab initio calculation (the Density Functional Theory). The conclusion of the theoretical analysis is agreeable with the experimental results. So these results indicate that PTS combining theoretical calculation can be used as a new, indirect way to judge the composition of the clusters which are easy to be dissociated and difficult to be detected by mass spectroscopy.

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Excited-State Dynamics of (SO₂)_m Clusters

Cited by 14 publications

References 38 publications

Extreme ionization of Xe clusters driven by ultraintense laser fields

Extreme ionization of Xe clusters driven by ultraintense laser fields

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

Study on the (HI)_m(H₂O)_n Clusters by Photofragment Translational Spectroscopy and Ab-Initio Calculation

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Excited-State Dynamics of (SO2)m Clusters

Cited by 14 publications

References 38 publications

Extreme ionization of Xe clusters driven by ultraintense laser fields

Extreme ionization of Xe clusters driven by ultraintense laser fields

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

Study on the (HI) m (H2O) n Clusters by Photofragment Translational Spectroscopy and Ab-Initio Calculation

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Excited-State Dynamics of (SO₂)_m Clusters

Study on the (HI)_m(H₂O)_n Clusters by Photofragment Translational Spectroscopy and Ab-Initio Calculation