High energy radiation femtochemistry of water molecules: early electron-radical pairs processes

The damages triggered by ionizing radiation on chemical and biological targets depend on the survival probability of radicals produced in clusters of ionization-excitation events. In this paper, we report on femtolysis (FEMTOsecond radioLYSIS) of pure liquid water using an innovative laser produced high-energy, ultra-short electron bunches in the 2.5-15 MeV range and high energy radiation femtochemistry (HERF) measurements. The short-time monitoring of a primary reducing radical, hydrated electron e^-_aq^{-}_{aq}, has been performed in confined ionization spaces (nascent spurs). The calculated yield of hydrated electrons at early time, G(e^-_aq)_ETG({\rm e}^{-}_{aq})_{ET}, is estimated to be 6.5 ± 0.5 (number/100 eV) at t ~ 5 ps after the ultrafast energy deposition. This estimated value is high compare to (i) the available data of previous works that used scavenging techniques; (ii) the predictions of stochastic water radiolysis modelling for which the initial behaviour of hydrated electron is investigated in the framework of a classical diffusion regime of independent pairs. The HERF developments give new insights into the early ubiquitous radical escape probability in nascent aqueous spurs and emphasize the importance of short-lived solvent bridged electron-radical complexes [H₃O^+...{\rm H}_{3}{\rm O}^{+...}  e_aq^-{\rm e}_{aq}^{-} ..OH]_nH2O{\rm OH}]_{n{\rm H}_2{\rm O}} (non-independent pairs). A complete understanding of the G(e^-_aq)_ET{\rm e}^{-}_{aq})_{ET} value needs to account for quantum aspects of 1s-like trapped electron ground state and neoformed prototropic radicals that govern ultra-fast recombination processes within these non-independent pair configurations. Femtolysis data emphasize that within a time-dependent non-diffusion regime, spatio-temporal correlations between hydrated electron and nearest neighbours OH radical or hydrated proton (H₃O⁺{\rm H}_{3}{\rm O}^{+}) would assist ultrafast anisotropic 1D recombination within solvent bridged electron-radical complexes. The emerging HERF domain would provide guidance for understanding of ultrashort-lived sub-structure of tracks and stimulate future semi-quantum simulations on prethermal radical reactions.     

Analysis of the <Emphasis Type="Italic">Y</Emphasis>(4140) and related molecular states with QCD sum rules

In this article, we assume that there exist scalar D^*[`(D)]<sup>*</sup>{D}^{\ast}{\bar {D}}^{\ast}, D<sub>s</sub><sup>*</sup>[`(D)]_s^*{D}_{s}^{\ast}{\bar{D}}_{s}^{\ast}, B^*[`(B)]<sup>*</sup>{B}^{\ast}{\bar {B}}^{\ast} and B<sub>s</sub><sup>*</sup>[`(B)]_s^*{B}_{s}^{\ast}{\bar{B}}_{s}^{\ast} molecular states, and study their masses using the QCD sum rules. The numerical results indicate that the masses are about (250–500) MeV above the corresponding D ^*–[`(D)]<sup>*</sup>{\bar{D}}^{\ast}, D <sub>s</sub> <sup>*</sup>–[`(D)]_s^*{\bar {D}}_{s}^{\ast}, B ^*–[`(B)]<sup>*</sup>{\bar{B}}^{\ast} and B <sub>s</sub> <sup>*</sup>–[`(B)]_s^*{\bar {B}}_{s}^{\ast} thresholds, the Y(4140) is unlikely a scalar D_s^*[`(D)]<sub>s</sub><sup>*</sup>{D}_{s}^{\ast}{\bar{D}}_{s}^{\ast} molecular state. The scalar D<sup>*</sup>[`(D)]^*D^{\ast}{\bar{D}}^{\ast}, D_s^*[`(D)]<sub>s</sub><sup>*</sup>D_{s}^{\ast}{\bar{D}}_{s}^{\ast}, B<sup>*</sup>[`(B)]^*B^{\ast}{\bar{B}}^{\ast} and B_s^*[`(B)]<sub>s</sub><sup>*</sup>B_{s}^{\ast}{\bar{B}}_{s}^{\ast} molecular states maybe not exist, while the scalar D￠<sup>*</sup>[`(D)]^￠*{D'}^{\ast}{\bar{D}}^{\prime\ast}, D_s^￠*[`(D)]<sub>s</sub><sup>￠*</sup>{D}_{s}^{\prime\ast}{\bar{D}}_{s}^{\prime\ast}, B<sup>￠*</sup>[`(B)]^￠*{B}^{\prime\ast}{\bar{B}}^{\prime\ast} and B_s^￠*[`(B)]_s^￠*{B}_{s}^{\prime\ast}{\bar{B}}_{s}^{\prime\ast} molecular states maybe exist.     

Study of Light Hypernuclei by the (e,e′K +) Reaction

We have been performing Λ hypernuclear spectroscopic experiments by the (e,e′K ⁺) reaction since 2000 at Thomas Jefferson National Accelerator Facility (JLab). The (e,e′K ⁺) experiment can achieve a few 100 keV (FWHM) energy resolution compared to a few MeV (FWHM) by the (K ^?, π ^?) and (π ⁺, K ⁺) experiments. Therefore, more precise Λ hypernuclear structures can be investigated by the (e,e′K ⁺) experiment. ${^{7}_{\Lambda}{\rm He}}$ , ${^{9}_{\Lambda}{\rm Li}}$ , ${^{10}_{\Lambda}{\rm Be}}$ , ${^{12}_{\Lambda}{\rm B}}$ , ${^{28}_{\Lambda}{\rm Al}}$ , and ${^{52}_{\Lambda}{\rm V}}$ were measured in the experiment at JLab Hall-C. In addition, ${^{9}_{\Lambda}{\rm Li}}$ , ${^{12}_{\Lambda}{\rm B}}$ , and ${^{16}_{\Lambda}{\rm N}}$ were measured in the experiment at JLab Hall-A.     

New experimental limits on violations of the Pauli exclusion principle obtained with the Borexino Counting Test Facility

The Pauli exclusion principle (PEP) has been tested for nucleons (n,p) in and nuclei, using the results of background measurements with the prototype of the Borexino detector, the Counting Test Facility (CTF). The approach consisted of a search for , n, p and/or s emitted in a non-Paulian transition of 1P- shell nucleons to the filled 1S _1/2 shell in nuclei. Similarly, the Pauli-forbidden decay processes were searched for. Due to the extremely low background and the large mass (4.2 tons) of the CTF detector, the following most stringent up-to-date experimental bounds on PEP violating transitions of nucleons have been established: , , , , and , all at C.L.Received: 18 June 2004, Published online: 1 October 2004PACS: 11.30.-j, 24.80. + y, 23.20.-g, 27.20. + nG. Bellini: SpokesmanL. Cadonati: Now at Massachusetts Institute of Technology, NW17-161, 175 Albany St. Cambridge, MA 02139O. Dadoun: Marie Curie fellowship at LNGS Correspondence to: A. Derbin. On leave of absence from St. Petersburg Nuclear Physics Inst. - Gatchina, RussiaM. Deutsch: DeceasedR. Ford: No w at Sudbury Neutrino Observatory, INCO Creighton Mine, P.O.Box 159 Lively, Ontario, Canada, P3Y 1M3B. Freudiger: Marie Curie fellowship at LNGS. Now at Institute for Nuclear Physics, Forschungszentrum Karlsruhe, Postfach 3640, 76021 KarlsruheS. Gazzana: GLIMOSV.V. Kobychev: Now at Institute for Nuclear Research, Prospekt Nauki 47, MSP 03680, Kiev, UkraineG. Korga: On leave of absence from KFKI-RMKI, Konkoly Thege ut 29-33 H-1121 Budapest, HungaryC. Lendvai: Marie Curie fellowship at LNGSP. Lombardi: Detector installation managerA. Martemianov: DeceasedV. Muratova: On leave of absence from St. Petersburg Nuclear Physics Inst. - Gatchina, RussiaL. Niedermeier: Marie Curie fellowship at LNGSL. Papp: On leave of absence from KFKI-RMKI, Konkoly Thege ut 29-33 H-1121 Budapest, HungaryR.S. Raghavan: Present Address: Department of Physics, Virginia Polytechnic Institute and State University, Blacksburg VA 24061G. Ranucci: Project managerC. Salvo: Operational manager Correspondence to: O. SmirnovA. Sonnenschein: Center for Cosmological Physics, University of Chicago, 933 E.56^th St., Chicago, IL 60637     

Time-resolved photoelectron spectroscopy on small tungsten cluster anions

We have studied the dynamics of photoexcited tungsten cluster anions W_n^-\mathrm{W}_{n}^{-} (n=3,4,…,14) by means of time-resolved two-photon photodetachment spectroscopy. At an excitation energy of h ν _pump=1.56 eV the photoinduced dynamics is mainly dominated by fast electronic relaxation processes. For the smallest clusters, i.e., W₃^-\mathrm{W}_{3}^{-}, W₄^-\mathrm{W}_{4}^{-}, and W₅^-\mathrm{W}_{5}^{-}, individual relaxation channels have been identified and resolved on a timescale well below 100 fs. The time constants for the decay of nascent and secondary electrons have been deduced from a Bloch model. Complete thermalization takes place for all clusters on a timescale of ∼1 ps.     

Cross section and rate coefficient calculations for electron impact excitation, ionisation and dissociation of the X 1Σg+, c 3Πu, a 3Σ g+, e 3Σu+ and B′1Σu+ states of H2

The weighted total cross section (WTCS) theory has been applied to the electron-H₂ collision to obtain excitation, ionisation and dissociation cross section and rate coefficients of the X ¹S_g⁺^{1}\!\Sigma _{g}^{+}, c ³P_u^{3}\!\Pi _{u}, a ³S_g⁺^{3}\!\Sigma _{g}^{+}, e $^{3}\!\Sigma _{u}^{+}$^{3}\!\Sigma _{u}^{+} and B^{′ 1}S_u⁺^{1}\!\Sigma _{u}^{+} states. Calculation has been performed in the temperature range 1500 K–15000 K. Rate coefficients are calculated from WTCS assuming Maxwellian energy distribution functions for electrons and heavy particles. Thermal equilibrium results are presented and fitting parameters (a, b and c) are given for each reaction rate coefficient: k(θ) = a (θ^b) exp(-c/θ).     

Analysis of the ΛQ baryons in the nuclear matter with the QCD sum rules

In this article, we study the Λ c and Λ b baryons in the nuclear matter using the QCD sum rules, and obtain the in-medium masses M\varLambda c*=2.335 GeVM_{\varLambda _{c}}^{*}=2.335~\mathrm{GeV}, M\varLambda b*=5.678 GeVM_{\varLambda _{b}}^{*}=5.678~\mathrm{GeV}, the in-medium vector self-energies \varSigma \varLambda cv=34 MeV\varSigma ^{\varLambda _{c}}_{v}=34~\mathrm{MeV}, \varSigma \varLambda bv=32 MeV\varSigma ^{\varLambda _{b}}_{v}=32~\mathrm {MeV}, and the in-medium pole residues l\varLambda c*=0.021 GeV3\lambda_{\varLambda _{c}}^{*}=0.021~\mathrm{GeV}^{3}, l\varLambda b*=0.026 GeV3\lambda_{\varLambda _{b}}^{*}=0.026~\mathrm{GeV}^{3}. The mass-shifts are M\varLambda c*-M\varLambda c=51 MeVM_{\varLambda _{c}}^{*}-M_{\varLambda _{c}}=51~\mathrm{MeV} and M\varLambda b*-M\varLambda b=60 MeVM_{\varLambda _{b}}^{*}-M_{\varLambda _{b}}=60~\mathrm{MeV}, respectively.     

Combined constraints on modified Chaplygin gas model from cosmological observed data: Markov Chain Monte Carlo approach

We use the Markov Chain Monte Carlo method to investigate a global constraints on the modified Chaplygin gas (MCG) model as the unification of dark matter and dark energy from the latest observational data: the Union2 dataset of type supernovae Ia (SNIa), the observational Hubble data (OHD), the cluster X-ray gas mass fraction, the baryon acoustic oscillation (BAO), and the cosmic microwave background (CMB) data. In a flat universe, the constraint results for MCG model are, W_bh² = 0.02263^+0.00184_-0.00162 (1s)^+0.00213_-0.00195 (2s){\Omega_{b}h^{2}\,{=}\,0.02263^{+0.00184}_{-0.00162} (1\sigma)^{+0.00213}_{-0.00195} (2\sigma)}, B_s = 0.7788^+0.0736_-0.0723(1s)^+0.0918_-0.0904 (2s){B_{s}\,{=}\,0.7788^{+0.0736}_{-0.0723}(1\sigma)^{+0.0918}_{-0.0904} (2\sigma)}, a = 0.1079^+0.3397_-0.2539 (1s)^+0.4678_-0.2911 (2s){\alpha\,{=}\,0.1079^{+0.3397}_{-0.2539} (1\sigma)^{+0.4678}_{-0.2911} (2\sigma)}, B = 0.00189^+0.00583_-0.00756(1s)^+0.00660_-0.00915 (2s){B\,{=}\,0.00189^{+0.00583}_{-0.00756}(1\sigma)^{+0.00660}_{-0.00915} (2\sigma)}, and H₀=70.711^+4.188_-3.142 (1s)^+5.281_-4.149(2s){H_{0}=70.711^{+4.188}_{-3.142} (1\sigma)^{+5.281}_{-4.149}(2\sigma)}.     

Lifetime vibrational interference during the NO 1s-1π* resonant excitation studied by the NO+(A 1Π → X 1Σ+) fluorescence

Dispersed fluorescence from fragments formed after the de-excitation of the 1s^-1π^* resonances of N^*O and NO^* has been measured in the spectral range of 118–142 nm. This range is dominated by lines of atomic nitrogen and oxygen fragments and by the bands in the NO⁺ ion which result from the participator Auger decay of the 1s^-1π^* resonances. Ab-initio calculations of the transition probabilities between vibrational levels during the reaction NO N^*O ⇒ NO were used to explain the observed intensity dependence for the fluorescence bands on the exciting-photon energy across the resonances and on both v^′ and v^′′ vibrational quantum numbers. The multiplet structure of the 1s^-1π^* resonance and lifetime vibrational interference explain the observed exciting-photon energy dependence of the fluorescence intensity. A strong spin-orbit coupling between singlet and triplet states of NO⁺ is proposed to reduce additional cascade population of the state via radiative transitions from the and states and to explain remaining differences between measured and calculated integral fluorescence intensities.     

Fougerite FeII − III oxyhydroxycarbonate in environmental chemistry and nitrate reduction

The identification of the fougerite mineral responsible for the bluish-green shade of gleysols in aquifers as being the Fe^II???III oxyhydroxycarbonate $\text{GR}(\text{CO}_{3}^{2-})^*$ of formula, $[\text{Fe}^{\rm II}_{6x}\text{Fe}^{\rm III}_{6(1 - x)}\text{O}_{12}\text{H}_{2(7-3x)}]^{2+}\bullet[\text{CO}_{3}^{2-}\bullet3\text{H}_{2}\text{O}]^{2-}$ where the ferric molar ratio x = [Fe^III/Fe_total] is restricted to the domain [1/3–2/3] induces to study the reactivity of the synthetic green rust for reducing some major pollutants. The oxidation within the solid compound $\text{GR}(\text{CO}_{3}^{2-})^*$ in the presence of nitrates is followed by miniaturized Mössbauer spectrometer (MIMOS). Ratio x = [Fe^III/Fe_total] increases up to 0.67 where $\text{GR}(\text{CO}_{3}^{2-})^*$ transforms gradually into magnetite. This could well explain the composition variability of fougerite occurrences.     

Multireference calculation of lifetime of A~2Π_u state in nitrogen-molecule cation

This paper utilizes multireference configuration interaction theory to calculate the lifetime of A2Πu state for nitrogen molecular ion N+2.It obtains the transition moment function for A2Πu→X2Σ+ g,Franck-Condon factors between vibrational levels of the two states.The calculated lifetimes are 16.81,14.62,13.10,12.18,11.40,and 11.64 μs forv'= 0,1,2,3,4,5 vibrational levels of A2Πu state,respectively,which are in excellent agreement with available experimental values.     

Fock-Space Projector Studied in Weyl Ordering Approach

We find that the Fock space projector |n〉〈n| is a Weyl ordered Laguerre polynomial 2 ^:_:(-)ⁿL_n ( 4a^fa ) e^-2afa :_:2{\,}^{:}_{:}(-)^{n}L_{n} ( 4a^{\dagger}a ) e^{-2a^{\dagger}a}{\,}^{:}_{:}, where a ^† a is the number operator,^:_: ^:_:,{}^{:}_{:}\ {}^{:}_{:} denotes the Weyl ordering symbol. This brings convenience to derive the Wigner functions of many other quantum states.     

Charge-transfer reactions in clusters excited with synchrotron radiation

Charge-transfer reactions are observed in a photoluminescence study of NF₃\rm NF_3-doped free krypton clusters. They show up in emissions from Kr⁺F^-\rm Kr^{+}F^{-}free excimers ejected from the clusters, and from excited Kr₂⁺F^-\rm Kr_2^{+}F^{-}and Kr₂⁺(NF₃)_m^-{\rm Kr}_2^{+}({\rm NF}_3)_m^{-} (m 3(m\geq 1) solvated in the clusters. The results show that reaction dynamics in clusters differs considerably from that in the gas and solid phases.     

Analysis of the <Emphasis Type="Italic">Y</Emphasis>(4140) with QCD sum rules

In this article, we assume that there exists a scalar D_s^*[`(D)]<sub>s</sub><sup>*</sup>D_{s}^{\ast}{\bar{D}}_{s}^{\ast} molecular state in the J/ψ φ invariant mass distribution, and we study its mass using the QCD sum rules. The predictions depend heavily on the two criteria (pole dominance and convergence of the operator product expansion) of the QCD sum rules. The value of the mass is about M<sub>Ds<sup>*</sup>[`(D)]s^*</sub>=(4.43±0.16)M_{D_{s}^{\ast}{\bar{D}}_{s}^{\ast}}=(4.43\pm0.16)  GeV, which is inconsistent with the experimental data. The D_s^*[`(D)]_s^*D_{s}^{\ast}{\bar{D}}_{s}^{\ast} is probably a virtual state and is not related to the meson Y(4140). Another possibility, such as a hybrid charmonium, is not excluded.     

Spectroscopy study of air plasma induced by IR CO2 laser pulses

A spectroscopic study of ambient air plasma, initially at room temperature and pressures ranging from 32 to 101 kPa, produced by high-power transverse excitation atmospheric (TEA) CO₂ laser (λ=9.621 and 10.591 μm; τ _FWHM≈64 ns; power densities ranging from 0.29 to 6.31 GW cm⁻²) has been carried out in an attempt to clarify the processes involved in laser-induced breakdown (LIB) air plasma. The strong emission observed in the plasma region is mainly due to electronic relaxation of excited N, O and ionic fragments N⁺. The medium-weak emission is due to excited species O⁺, N²⁺, O²⁺, C, C⁺, C²⁺, H, Ar and molecular band systems of N ₂⁺(_{2}^{+}( B ²\varSigma _u⁺^{2}\varSigma _{\mathrm{u}}^{+} –X ²\varSigma _g⁺)^{2}\varSigma _{\mathrm{g}}^{+}) , N₂(C³ Π _u–B³ Π _g), N ₂⁺(_{2}^{+}( D² Π _g–A² Π _u) and OH(A² Σ ⁺–X² Π). Excitation temperatures of 23400±700 K and 26600±1400 K were estimated by means of N⁺ and O⁺ ionic lines, respectively. Electron number densities of the order of (0.5–2.4)×10¹⁷ cm⁻³ and (0.6–7.5)×10¹⁷ cm⁻³ were deduced from the Stark broadening of several ionic N⁺ and O⁺ lines, respectively. Estimates of vibrational and rotational temperatures of N ₂⁺_{2}^{+} electronically excited species are reported. The characteristics of the spectral emission intensities from different species have been investigated as functions of the air pressure and laser irradiance. Optical breakdown threshold intensities in air at 10.591 μm have been measured.     

Effect of isospin-dependent cross-section on fragment production in the collision of charge asymmetric nuclei

To understand the role of isospin effects on fragmentation due to the collisions of charge asymmetric nuclei, we have performed a complete systematical study using isospin-dependent quantum molecular dynamics model. Here simulations have been carried out for $^{124}{\rm X}_{n}+^{124}{\rm X}_{n}$ , where n varies from 47 to 59 and for $^{40}{\rm Y}_{m}+^{40}{\rm Y}_{m}$ , where m varies from 14 to 23. Our study shows that isospin-dependent cross-section shows its influence on fragmentation in the collision of neutron-rich nuclei.     

Temperature dependence of the quenching of N<Subscript>2</Subscript> (C <Superscript>3</Superscript>Π<Subscript>u</Subscript>) by N<Subscript>2</Subscript> (X) and O<Subscript>2</Subscript> (X)

The temperature dependences of the quenching rate constants of the states N₂ (${\rm C} \ {^{3}{ \rm \Pi }_{u}}${\rm C} \ {^{3}{ \rm \Pi }_{u}} v^′=0,1) by N₂ (X) and of the state N₂ (${\rm C} \ {^{3}{ \rm \Pi }_{u}} \ v^{\prime}=0${\rm C} \ {^{3}{ \rm \Pi }_{u}} \ v^{\prime}=0) by O₂ (X) are studied. Time-resolved light emission from the gas was analyzed in the temperature range from 300 K to 210 K keeping the gas at constant density. In case of quenching by N₂ (X), the quenching rate constant for the vibrational level v^′= 0 increases by (13 ±3)% with gas cooling whereas the quenching rate constant for v^′= 1 decreases by (5.0 ±2.5)% in this temperature range. For quenching by O₂ (X), the quenching rate constant decreases by (3 ±2)% with gas cooling. The temperature variation of the N₂ (C ³Π_u v^′=0) emission intensity for pure nitrogen and dry air are calculated using the obtained quenching rate constants and is compared with the experimental data available in the literature.     

Ultrafast delocalization of hydrogen atoms in allene in intense laser fields

Ultrafast delocalization of hydrogen atoms in allene (CH₂=C=CH₂) induced by intense laser fields was investigated by the Coulomb explosion coincidence momentum imaging method. On the basis of the kinetic energy distributions of the fragment ions produced through the two three-body Coulomb explosion pathways, C₃H₄³⁺ ? H⁺ + CH⁺ + C₂H₂⁺\mathrm{C}_{3}\mathrm{H}_{4}^{3+} \rightarrow \mathrm{H}^{+} + \mathrm{CH}^{+} + \mathrm{C}_{2}\mathrm{H}_{2}^{+} and C₃H₄³⁺ ? H⁺ + C₂H⁺ +CH₂⁺\mathrm{C}_{3}\mathrm{H}_{4}^{3+} \rightarrow \mathrm{H}^{+} + \mathrm{C}_{2}\mathrm{H}^{+} +\mathrm{CH}_{2}^{+}, and the proton maps for both pathways, it was shown that the decomposition proceeds in a stepwise manner as well as in a concerted manner. The time scale of the hydrogen migration within an allene molecule was estimated to be ∼20 fs.     

Physisorption and dissociative chemisorption of H2 on sub-nanosized Al$_{13}^{-}$ anion cluster: ab initio study

We have studied the interaction of Al₁₃^-_{13}^{-} anion cluster with H₂. Both the long range interaction and dissociative adsorption have been examined using the established correlated ab initio methods, MP2 and CCSD(T), in conjunction with the augmented correlation consistent basis sets up to aug-cc-pVTZ. The formation of the weakly bound (physisorbed) end-on anion complex Al₁₃^-_{13}^{-}...H₂ is predicted for the interacting Al...H distances of 3.95 ? with the H-H axis pointing towards the ‘hollow’ site of Al₁₃^-_{13}^{-} and binding energy (D_e)D_{e}) of 0.7 kcal/mol at the estimated complete basis set (CBS) limit of CCSD(T). The barrier height for H₂ dissociation on Al₁₃^-_{13}^{-} of 41.6 (42.9) kcal/mol calculated at the ZPVE-corrected CCSD(T)/aug-cc-pVTZ (estimated CCSD(T)/CBS) level is at least twice as large as that evaluated by us for a dissociative adsorption of H₂ on an open-shell Al₁₃ neutral cluster. To our knowledge, this report presents the first “benchmark” quality study of the physisorption and dissociative chemisorption of molecular hydrogen on Al₁₃^-_{13}^{-} anion cluster.