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Article: Photodissociation of (SO2)m(H2O)n clusters employing femtosecond pump-probe spectroscopy.

Knappenberger, K L / Castleman, A W

2005 Volume 122, Issue 15, Page(s) 154306

Abstract: ... A. W. Castleman, Jr., J. Chem. Phys. 121, 3540 (2004)]. The E state lifetime increases sequentially ... the dissociation process owing to a steric effect induced by the cluster environment [K. L. Knappenberger, Jr. and ...

Abstract	A femtosecond pump-probe technique was employed to study the photodissociation dynamics of (SO2)m(H2O)n clusters in real time for clusters, where m=1, 2 and n as large as 11. The pump (excitation) step occurs through a multiphoton process which populates the dissociative E state as well as a lower-lying bound state of the sulfur dioxide (SO2) chromophore. Dissociation of the SO2 monomer occurs through the E state and the decay is fit to a lifetime of 230 fs. The present study is in agreement with our previous investigations of homogeneous (SO2)m clusters that have shown that cluster formation inhibits the dissociation process owing to a steric effect induced by the cluster environment [K. L. Knappenberger, Jr. and A. W. Castleman, Jr., J. Chem. Phys. 121, 3540 (2004)]. The E state lifetime increases sequentially as a function of cluster size to as much as 668 fs when 11 water molecules solvate the chromophore. We have employed a method to compare the ratio of amplitude coefficients, which reflect a respective component of the mathematical fit, to determine the nature of the wave packet evolution in binary clusters. An increase of this ratio by as much as 440% was observed for large cluster sizes. A preferential ion state charge transfer, rather than dissociation, was observed in binary clusters. The significance of cluster size on evaporation processes has been investigated.
Language	English
Publishing date	2005-04-15
Publishing country	United States
Document type	Journal Article
ZDB-ID	3113-6
ISSN	1089-7690 ; 0021-9606
ISSN (online)	1089-7690
ISSN	0021-9606
DOI	10.1063/1.1869494
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Article: Superatom spectroscopy and the electronic state correlation between elements and isoelectronic molecular counterparts

Peppernick, Samuel J / Gunaratne, K.D. Dasitha / Castleman, A.W. Jr

Proceedings of the National Academy of Sciences of the United States of America. 2010 Jan. 19, v. 107, no. 3

2010

Abstract: ... heterogeneous diatomic molecules, M-Xâ» (M = Ti,Zr,W; X = O or C). A superposition principle connecting ...

Abstract	Detailed in the present investigation are results pertaining to the photoelectron spectroscopy of negatively charged atomic ions and their isoelectronic molecular counterparts. Experiments utilizing the photoelectron imaging technique are performed on the negative ions of the group 10 noble metal block (i.e. Niâ», Pdâ», and Ptâ») of the periodic table at a photon energy of 2.33 eV (532 nm). The accessible electronic transitions, term energies, and orbital angular momentum components of the bound electronic states in the atom are then compared with photoelectron images collected for isoelectronic early transition metal heterogeneous diatomic molecules, M-Xâ» (M = Ti,Zr,W; X = O or C). A superposition principle connecting the spectroscopy between the atomic and molecular species is observed, wherein the electronic structure of the diatomic is observed to mimic that present in the isoelectronic atom. The molecular ions studied in this work, TiOâ», ZrOâ», and WCâ» can then be interpreted as possessing superatomic electronic structures reminiscent of the isoelectronic elements appearing on the periodic table, thereby quantifying the superatom concept.
Keywords	energy ; image analysis ; ions ; momentum ; spectroscopy
Language	English
Dates of publication	2010-0119
Size	p. 975-980.
Publishing place	National Academy of Sciences
Document type	Article
ZDB-ID	209104-5
ISSN	1091-6490 ; 0027-8424
ISSN (online)	1091-6490
ISSN	0027-8424
DOI	10.1073/pnas.0911240107
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Article: Cluster reactivity experiments: Employing mass spectrometry to investigate the molecular level details of catalytic oxidation reactions

Johnson, Grant E / Tyo, Eric C / Castleman, A.W. Jr

Proceedings of the National Academy of Sciences of the United States of America. 2008 Nov. 25, v. 105, no. 47

2008

Abstract: ... W-O{bullet}) with elongated metal-oxygen bonds. The unique insights gained into bulk-phase oxidation ...

Abstract	Mass spectrometry is the most widely used tool in the study of the properties and reactivity of clusters in the gas phase. In this article, we demonstrate its use in investigating the molecular-level details of oxidation reactions occurring on the surfaces of heterogeneous catalysts via cluster reactivity experiments. Guided ion beam mass spectrometry (GIB-MS) employing a quadrupole-octopole-quadrupole (Q-O-Q) configuration enables mass-selected cluster ions to be reacted with various chemicals, providing insight into the effect of size, stoichiometry, and ionic charge state on the reactivity of catalyst materials. For positively charged tungsten oxide clusters, it is shown that species having the same stoichiometry as the bulk, WO3+, W2O6+, and W3O9+, exhibit enhanced activity and selectivity for the transfer of a single oxygen atom to propylene (CâHâ), suggesting the formation of propylene oxide (CâHâO), an important monomer used, for example, in the industrial production of plastics. Furthermore, the same stoichiometric clusters are demonstrated to be active for the oxidation of CO to COâ, a reaction of significance to environmental pollution abatement. The findings reported herein suggest that the enhanced oxidation reactivity of these stoichiometric clusters may be due to the presence of radical oxygen centers (W-O{bullet}) with elongated metal-oxygen bonds. The unique insights gained into bulk-phase oxidation catalysis through the application of mass spectrometry to cluster reactivity experiments are discussed.
Keywords	carbon dioxide ; carbon monoxide ; catalysts ; catalytic activity ; gases ; ions ; mass spectrometry ; oxidation ; oxygen ; plastics ; pollution ; pollution control ; propylene ; propylene oxide ; reactive oxygen species ; stoichiometry ; tungsten oxide
Language	English
Dates of publication	2008-1125
Size	p. 18108-18113.
Publishing place	National Academy of Sciences
Document type	Article
ZDB-ID	209104-5
ISSN	1091-6490 ; 0027-8424
ISSN (online)	1091-6490
ISSN	0027-8424
DOI	10.1073/pnas.0801539105
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Journal: Consideration of the Chemistry of Radon Progeny

Castleman, A. W. Jr.

Environmental Science and Technology : Emphasizing, water, air, and waste chemistry

1991 Volume 25, Page(s) 730–735

Abstract: Obwohl die Chemie und Physik der Entstehung von Radon-Spaltprodukten weit davon entfernt ist, voellig verstanden zu sein, steht nun ausreichendes qantitatives Wissen aus Laborexperimenten zur Verfuegung, um bestimmte Beobachtungen zu interpretieren und ... ...

Abstract	Obwohl die Chemie und Physik der Entstehung von Radon-Spaltprodukten weit davon entfernt ist, voellig verstanden zu sein, steht nun ausreichendes qantitatives Wissen aus Laborexperimenten zur Verfuegung, um bestimmte Beobachtungen zu interpretieren und das Verhalten und den Verbleib der Spaltprodukte vorherzusagen. Thema dieses Artikels sind vor allem die zwei Spaltprodukte Blei und Wismut. Ein erheblicher Teil der Spaltprodukte liegen in einfach geladenem Zustand vor. Anfaenglich kann eine Bindung mit O2 aus der Luft vorliegen, der rasch durch andere polare Molekuele ersetzt wird, wodurch die Spaltprodukte rasch mit fuenf bis acht Wassermolekuelen hydriert werden, je nach Temperatur und Feuchtigkeit. Es ist moeglich, dass ein Wassermolekuel durch ein Ammoniak-, Alkohol- oder anderes organisches Molekuel ersetzt werden. Bei Kollisionen dieser Cluster-Ionen mit Aerosolpartikeln koennen verschiedene Mechanismen des Ladungsaustauschs oder die Inkorporierung der Partikel auftreten. Wenn keine Kollision mit einem Aerosolpartikel stattfindet, verbleiben die Cluster waehrend Wachstum und Transport im einfach geladenen Zustand. Als letzter Schritt duerfte dann die Ladungsneutralisierung mittels Rekombination mit Cluster-Anionen in der Luft auftreten, hoechstwahrscheinlich mit NO(ind=3)(xp=-)(H2O)n.
Keywords	Radioaktive Substanz ; Radon ; Blei ; Anionen ; Bismut ; Spaltprodukt ; Kernchemie ; Ammoniak ; Alkohol ; Ionen ; Nitrat ; Lufttemperatur ; Partikel ; Laborversuch ; Inkorporation ; Temperaturabhaengigkeit ; Aerosol ; Hydrierung ; Feuchtigkeit
Language	English
Document type	Journal
Database	OPAC and Environmental database (ULIDAT) of The Federal Environment Agency (UBA)

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Article: Complementary Active Sites Cause Size-Selective Reactivity of Aluminum Cluster Anions with Water

Roach, Patrick J / Castleman, A.W. Jr / Khanna, Shiv N / Reber, Arthur C / Woodward, W. Hunter

Science. 2009 Jan. 23, v. 323, no. 5913

2009

Abstract: The reactions of metal clusters with small molecules often depend on cluster size. The selectivity of oxygen reactions with aluminum cluster anions can be well described within an electronic shell model; however, not all reactions are subject to the same ...

Abstract	The reactions of metal clusters with small molecules often depend on cluster size. The selectivity of oxygen reactions with aluminum cluster anions can be well described within an electronic shell model; however, not all reactions are subject to the same fundamental constraints. We observed the size selectivity of aluminum cluster anion reactions with water, which can be attributed to the dissociative chemisorption of water at specific surface sites. The reactivity depends on geometric rather than electronic shell structure. Identical arrangements of multiple active sites in Alâââ», Alâââ», and Alâââ» result in the production of Hâ from water.
Keywords	active sites ; aluminum ; anions ; geometry ; hydrogen ; models ; oxygen
Language	English
Dates of publication	2009-0123
Size	p. 492-495.
Publishing place	American Association for the Advancement of Science
Document type	Article
ZDB-ID	128410-1
ISSN	1095-9203 ; 0036-8075
ISSN (online)	1095-9203
ISSN	0036-8075
DOI	10.1126/science.1165884
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Article: Al₄H{f1} is a resilient building block for aluminum hydrogen cluster materials

Roach, P.J / Reber, A.C / Woodward, W.H / Khanna, S.N / Castleman, A.W. Jr

Proceedings of the National Academy of Sciences of the United States of America. 2007 Sept. 11, v. 104, no. 37

2007

Abstract: The formation and oxygen etching of AlnH[Formula: see text] clusters are characterized in a flow reactor experiment with first-principles theoretical investigations to demonstrate the exceptional stability of Al₄H[Formula: see text]. The origin of the ... ...

Abstract	The formation and oxygen etching of AlnH[Formula: see text] clusters are characterized in a flow reactor experiment with first-principles theoretical investigations to demonstrate the exceptional stability of Al₄H[Formula: see text]. The origin of the preponderance of Al₄H[Formula: see text] in the mass spectra of hydrogenated aluminum anions and its resistance to O₂ etching are discussed. Al₄H[Formula: see text] is shown to have the ability to bond with ionic partners to form stable hydrides through addition of an alkali atom [XAl₄H₇ (X = Li-Cs)]. An intuitive model that can predict the existence of stable hydrogenated cluster species is proposed. The potential synthetic utility of the superatom assemblies built on these units is addressed.
Language	English
Dates of publication	2007-0911
Size	p. 14565-14569.
Publishing place	National Academy of Sciences
Document type	Article
ZDB-ID	209104-5
ISSN	1091-6490 ; 0027-8424
ISSN (online)	1091-6490
ISSN	0027-8424
Database	NAL-Catalogue (AGRICOLA)

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Article: Kinetic analysis of the reaction between (V2O5)n=1,2+ and ethylene.

Moore, Nelly A / Mitrić, Roland / Justes, Dina R / Bonacić-Koutecký, Vlasta / Castleman, A W

The journal of physical chemistry. B

2006 Volume 110, Issue 7, Page(s) 3015–3022

Abstract: ... Koutecký, V.; Castleman, A. W., Jr. J. Am. Chem. Soc., 2003, 125, 6289) provided evidence of the rate ...

Abstract	A systematic experimental and theoretical investigation of the influence of reactant energy on the reactivity of (V(2)O(5))(n)=1,2(+) clusters with ethylene (Justes, D. R.; Mitrić, R.; Moore, N. A.; Bonacić-Koutecký, V.; Castleman, A. W., Jr. J. Am. Chem. Soc., 2003, 125, 6289) provided evidence of the rate controlling steps in the reaction. Herein, we present further experimental and theoretical evidence for our recently proposed radical cation mechanism for oxygen atom transfer from (V(2)O(5))(n)=1,2(+) clusters to ethylene. In particular the results of ab initio molecular dynamics simulations are found to further support the radical cation mechanism. Experimental reaction cross sections at the zero pressure limit and rate coefficients show that the energy dependence of the reaction cross section is in accord with the Langevin formula. Evidence is presented that ion-molecule association is the rate determining step, whereas subsequent hydrogen transfer and formation of acetaldehyde proceed without significant barriers. We propose a kinetic model for the reaction cross section that fully accounts for the experimental findings. The model offers the prospect of elucidating the details of the general reaction mechanisms through a study of the energy dependence of the reaction cross sections.
Language	English
Publishing date	2006-02-23
Publishing country	United States
Document type	Journal Article
ISSN	1520-6106
ISSN	1520-6106
DOI	10.1021/jp055652u
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Article: Theoretical and experimental consideration of the reactions between VxOy+ and ethylene.

Justes, Dina R / Mitrić, Roland / Moore, Nelly A / Bonacić-Koutecký, Vlasta / Castleman, A Welford

Journal of the American Chemical Society

2003 Volume 125, Issue 20, Page(s) 6289–6299

Abstract: ... Castleman, A. W., Jr. J. Phys. Chem. A 2001, 105, 10237). The lowest-energy structures for the V(2)O(2)(-)(6 ... to corroborate the experimental results obtained by Castleman and co-workers (Zemski, K. A.; Justes, D. R ...

Abstract	We present joint theoretical and experimental results which provide evidence for the selectivity of V(x)O(y)(+) clusters in reactions toward ethylene due to the charge and different oxidation states of vanadium for different cluster sizes. Density functional calculations were performed on the reactions between V(x)O(y)(+) and ethylene, allowing us to identify the structure-reactivity relationship and to corroborate the experimental results obtained by Castleman and co-workers (Zemski, K. A.; Justes, D. R.; Castleman, A. W., Jr. J. Phys. Chem. A 2001, 105, 10237). The lowest-energy structures for the V(2)O(2)(-)(6)(+) and V(4)O(8)(-)(10)(+) clusters and the V(2)O(3)(-)(6)(+)-C(2)H(4) and V(4)O(10)(+)-C(2)H(4) complexes, as well as the energetics for reactions between ethylene and V(2)O(4)(-)(6)(+) and V(4)O(10)(+) are presented here. The oxygen transfer reaction pathway was determined to be the most energetically favorable one available to V(2)O(5)(+) and V(4)O(10)(+) via a radical-cation mechanism. The association and replacement reaction pathways were found to be the optimal channels for V(2)O(4)(+) and V(2)O(6)(+), respectively. These results are in agreement with the experimental results reported previously. Experiments were also conducted for the reactions between V(2)O(5)(+) and ethylene to include an energetic analysis at increasing pressures. It was found that the addition of energy depleted the production of V(2)O(4)(+), confirming that a more involved reaction rather than a collisional process is responsible for the observed phenomenon. In this contribution we show that investigation of reactions involving gas-phase cationic vanadium oxide clusters with small hydrocarbons is suitable for the identification of reactive centers responsible for selectivity in heterogeneous catalysis.
Language	English
Publishing date	2003-05-21
Publishing country	United States
Document type	Journal Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/ja021349k
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Article: Attenuation of virus-induced airway dysfunction in rats treated with imiquimod.

Stokes, J R / Sorkness, R L / Kaplan, M R / Castleman, W L / Tomai, M A / Miller, R L / Lemanske, R F

The European respiratory journal

1998 Volume 11, Issue 2, Page(s) 324–329

Abstract: Viral respiratory infections cause acute airway abnormalities consisting of inflammation and physiological dysfunction in both animals and humans. It is likely that inflammatory cell products, such as cytokines, contribute substantially to viral-induced ... ...

Abstract	Viral respiratory infections cause acute airway abnormalities consisting of inflammation and physiological dysfunction in both animals and humans. It is likely that inflammatory cell products, such as cytokines, contribute substantially to viral-induced airway dysfunction. We hypothesized that imiquimod, an immune response enhancing agent that induces interferon-alpha, would attenuate the development of airway dysfunction during acute viral illness in rats. Adult Brown Norway rats were inoculated with parainfluenza type 1 (Sendai) virus or sterile vehicle, and treated with either imiquimod or water. Respiratory system resistance (Rrs), arterial oxygen tension (Pa,O2), lung viral titres and bronchoalveolar lavage (BAL) leucocyte counts were measured in anaesthetized, paralysed, ventilated rats. Virus-infected, water-treated rats had a significant decrease in Pa,O2 and had significant increases in leucocyte count and Rrs when compared to both the virus-infected, imiquimod-treated, (Pa,O2, p = 0.03; leucocyte count, p = 0.02; and Rrs, p = 0.009) and noninfected, water-treated rats (Pa,O2, p = 0.007; leucocyte count, p = 0.001; and Rrs, p = 0.01). In addition, imiquimod suppressed BAL eosinophils in both virus-infected (p = 0.02) and noninfected (p = 0.001) groups, and lowered overall virus titres (p = 0.03). Thus, both virus-induced airway inflammation and physiological dysfunction were attenuated significantly by imiquimod treatment in this animal model. By further delineating mechanisms by which infections induce airway dysfunction in animal models, more specific pharmacological interventions can be developed for the treatment of virus-induced asthma.
MeSH term(s)	Adjuvants, Immunologic/therapeutic use ; Aminoquinolines/therapeutic use ; Animals ; Body Weight/drug effects ; Bronchoalveolar Lavage Fluid/cytology ; Imiquimod ; Inflammation/pathology ; Inflammation/virology ; Interferons/blood ; Male ; Rats ; Respiratory Tract Diseases/pathology ; Respiratory Tract Diseases/virology ; Respirovirus/isolation & purification ; Respirovirus Infections/complications ; Respirovirus Infections/drug therapy ; Respirovirus Infections/virology
Chemical Substances	Adjuvants, Immunologic ; Aminoquinolines ; Interferons (9008-11-1) ; Imiquimod (P1QW714R7M)
Language	English
Publishing date	1998-02
Publishing country	England
Document type	Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, P.H.S.
ZDB-ID	639359-7
ISSN	1399-3003 ; 0903-1936
ISSN (online)	1399-3003
ISSN	0903-1936
DOI	10.1183/09031936.98.11020324
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Journal: Kinetics of the association reaction of SO2 with the hydroxyl radical

Castleman, A.W. jr. / Tang, I.N.

Journal of Photochemistry : An International Journal devoted to the Study of the Quantitative Aspects of Photochemistry and Energy Transfer

1977 Volume 6, Page(s) 349–354

Abstract: Der Vorgang der chemischen SO2 Oxidation und der nachfolgenden Bildung von stratosphaerischem und troposphaerischem Aerosol wurde mittels Photolyse untersucht. Die Oxidation von SO2 ueber das Hydroxylradikal wurde bei Druecken von 20 bis 1000 Torr undbei ...

Abstract	Der Vorgang der chemischen SO2 Oxidation und der nachfolgenden Bildung von stratosphaerischem und troposphaerischem Aerosol wurde mittels Photolyse untersucht. Die Oxidation von SO2 ueber das Hydroxylradikal wurde bei Druecken von 20 bis 1000 Torr undbei Temperaturen zwischen -20 Grad Celsius und +24 Grad Celsius gemessen. In Gegenwart von Stickstoff ergab sich bei 297 Grad Kelvin eine Reaktionskonstante dritter Ordnung von 1,6 x 10 hoch minus31 cm hoch 6 Molekuel hoch minus2 / s hoch minus 1. Beiderselben Temperatur und einem Gesamtdruck von 760 Torr ist die Reaktionskonstante zweiter Ordnung 6,0 x 10 hoch minus13 cm3/Molekuel hoch minus 1 s hoch minus 1. Die Reaktionskonstante dritter Ordnung steigt mit sinkender Temperatur. Eine Energie von -2,8 kcal/mol. ist zur Anregung der Reaktion noetig.
Keywords	Stratosphaere ; Reaktionskinetik ; Aerosolentstehung ; Troposphaere ; Oxidation ; Photolyse ; Schwefeldioxid
Language	English
Document type	Journal
Database	OPAC and Environmental database (ULIDAT) of The Federal Environment Agency (UBA)

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