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See detailThe Role of Long-Range Forces in the Determination of Translational Kinetic Energy Release. Loss of C4H4+ from Benzene and Pyridine Cations.
Gridelet, E.; Locht, Robert ULg; Lorquet, Andrée ULg et al

in Journal of Physical Chemistry A (2008), 112

Kinetic energy release distributions (KERDs) for the benzene ion fragmenting into C4H4+ and C2H2 have been recorded by double-focussing mass spectrometry in the metastable energy window and by a retarding ... [more ▼]

Kinetic energy release distributions (KERDs) for the benzene ion fragmenting into C4H4+ and C2H2 have been recorded by double-focussing mass spectrometry in the metastable energy window and by a retarding field experiment up to an energy of 5 eV above the fragmentation threshold. They are compared with those resulting from the HCN loss reaction from the pyridine ion. Both reactions display a similar variation of the kinetic energy release as a function of the internal energy: the average release is smaller than statistically expected, with a further restriction of the phase-space sampling for the C5H5N+ dissociation. Ab initio calculations of the potential-energy profile have been carried out. They reveal a complicated reaction mechanism, the last step of which consists in the dissociation of a weakly bound ion-quadrupole or ion-dipole complex. The KERDs have been analyzed by the maximum entropy method. The fraction of phase-space effectively sampled by the pair of fragments has been determined and is similar for both dissociations. Both reactions are constrained by the square root of the released kinetic energy, epsilon1/2. This indicates that in the latter stage of the dissociation process, the reaction coordinate is adiabatically decoupled from the bath of the bound degrees of freedom. For the C6H6+ fragmentation, the analysis of the experimental results strongly suggests that, just as for the symmetric interaction potential, the translational motion is confined to a two-dimensional subspace. This dimensionality reduction of the translational phase space is due to the fact that the Hamiltonian of both weakly bound complexes contains a cyclic coordinate. [less ▲]

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See detailFast multiresponsive micellar gels from a smart ABC triblock copolymer
Willet, Nicolas ULg; Gohy, Jean-François; Lei, Liangcai et al

in Angewandte Chemie (International ed. in English) (2007), 46(42), 7988-7992

The triblock copolymer PS-b-P2VP-b-PEO undergoes simultaneous micellization and gelation, leading to high-storage-modulus materials that have fast responses to pH value, temperature, ionic strength, and ... [more ▼]

The triblock copolymer PS-b-P2VP-b-PEO undergoes simultaneous micellization and gelation, leading to high-storage-modulus materials that have fast responses to pH value, temperature, ionic strength, and shearing. The gel has a hierarchical structure with spherical core-shell-corona micelles, which, in turn, pack closely into an ordered cubic structure. [less ▲]

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See detailpH-responsive micelles in dilute and gel-like media
Willet, Nicolas ULg; Leyh, Bernard ULg; Gohy, Jean-François et al

Conference (2006, June)

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See detailThe VUV Photoabsorption Spectroscopy and Photoionization of Halogenated Etylenes: Bromo-derivatives.
Locht, Robert ULg; Leyh, Bernard ULg; Jochims, H.-W. et al

Book published by Berliner Elektronen Speicherring für Synchrotron Strahlung m.b.H - on CD-ROM (2006)

In this contribution the measurement, by the use of synchrotron radiation, of the V-UV photoabsorption spectrum (PAS) of 1,1-C2H2Br2 and the photoionization efficiency curve (PIC) of 1,1-C2H2Br2+ are ... [more ▼]

In this contribution the measurement, by the use of synchrotron radiation, of the V-UV photoabsorption spectrum (PAS) of 1,1-C2H2Br2 and the photoionization efficiency curve (PIC) of 1,1-C2H2Br2+ are reported. Strong correlations between the PAS and the PIC are shown. The PAS of 1,1-C2F2Br2 is also presented and compared to the PAS of 1,1-C2H2Br2 to show the influence of the fluuorine-substitution. [less ▲]

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See detailThe Photoabsorption and Photoionization of Bromine revisited.
Locht, Robert ULg; Leyh, Bernard ULg; Jochims, H.-W. et al

Book published by Berliner Elektronen Speicherring für Synchrotron Strahlund m.b.H - on CD-ROM (2006)

The V-UV photoabsorption spectrum (PAS) and the photoionization (PIE) efficiency of Br2, Br2+ and Br+ have been measured using synchrotron radiation. At high photon energy a strong correlation between the ... [more ▼]

The V-UV photoabsorption spectrum (PAS) and the photoionization (PIE) efficiency of Br2, Br2+ and Br+ have been measured using synchrotron radiation. At high photon energy a strong correlation between the PAS of Br2 and the PIE of Br2+ is observed. A detailed analysis of the PIE of Br2+ in the threshold region is presented. New data related to the Br+/Br- ion-pair formation are reported. [less ▲]

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See detailHydrogen atom loss from the benzene cation. Why is the kinetic energy release so large?
Gridelet, E.; Lorquet, Andrée ULg; Locht, Robert ULg et al

in Journal of Physical Chemistry A (2006), 110(27), 8519-8527

The kinetic energy release distributions (KERDs) associated with the hydrogen loss from the benzene cation and the deuterium loss from the perdeuteriobenzene cation have been remeasured on the metastable ... [more ▼]

The kinetic energy release distributions (KERDs) associated with the hydrogen loss from the benzene cation and the deuterium loss from the perdeuteriobenzene cation have been remeasured on the metastable time scale and analyzed by the maximum entropy method. The experimental kinetic energy releases are larger than expected statistically, in contradistinction to what has been observed for the C-X fragmentations of the halogenobenzene cations. H(D) loss from C6H6+ (C6D6+) occurs via a conical intersection connecting the (2)A(2) and (2)A(1) electronic states. Two models are proposed to account for the experimental data: (i) a modified orbiting transition state theory (OTST) approach incorporating electronic nonadiabaticity; (ii) an electronically nonadiabatic version of the statistical adiabatic channel model ( SACM) of Quack and Troe. The latter approach is found to be preferable. It leads to the conclusion that the larger the energy stored in the transitional modes, which partly convert to the relative interfragment motion, the shorter the value of the reaction coordinate at which the adiabatic channels cross, and the larger the probability of undergoing the (2)A(2) -> (2)A(1) transition required for hydrogen loss. [less ▲]

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See detailAnalysis of kinetic energy release distributions by the maximum entropy method.
Leyh, Bernard ULg; Gridelet, E.; Locht, Robert ULg et al

in International Journal of Mass Spectrometry (2006), 249-250

Energy is not always fully randomized in an activated molecule because of the existence of dynamical constraints. An analysis of kinetic energy release distributions (KERDs) of dissociation fragments by ... [more ▼]

Energy is not always fully randomized in an activated molecule because of the existence of dynamical constraints. An analysis of kinetic energy release distributions (KERDs) of dissociation fragments by the maximum entropy method (MEM) provides information on the efficiency of the energy flow between the reaction coordinate and the remaining degrees of freedom during the fragmentation. For example, for barrierless cleavages, large translational energy releases are disfavoured while energy channeling into the rotational and vibrational degrees of freedom of the pair of fragments is increased with respect to a purely statistical partitioning. Hydrogen atom loss reactions provide an exception to this propensity rule. An ergodicity index, F, can be derived. It represents an upper bound to the ratio between two volumes of phase space: that effectively explored during the reaction and that in principle available at the internal energy E. The function F(E) has been found to initially decrease and to level off at high internal energies. For an atom loss reaction, the orbiting transition state version of phase space theory (OTST) is especially valid for low internal energies, low total angular momentum, large reduced mass of the pair of fragments, large rotational constant of the fragment ion, and large polarizability of the released atom. For barrierless dissociations, the major constraint that results from conservation of angular momentum is a propensity to confine the translational motion to a two-dimensional space. For high rotational quantum numbers, the influence of conservation of angular momentum cannot be separated from effects resulting from the curvature of the reaction path. The nonlinear relationship between the average translational energy <epsilon > and the internal energy E is determined by the density of vibrational-rotational states of the pair of fragments and also by non-statistical effects related to the incompleteness of phase space exploration. The MEM analysis of experimental KERDs suggests that many simple reactions can be described by the reaction path Hamiltonian (RPH) model and provides a criterion for the validity of this method. Chemically oriented problems can also be solved by this approach. A few examples are discussed: determination of branching ratios between competitive channels, reactions involving a reverse activation barrier, nonadiabatic mechanisms, and isolated state decay. (c) 2005 Elsevier B.V. All rights reserved. [less ▲]

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See detailAbout the Photoionization of Methyl Bromide (CH3Br). Photoelectron and Photoionization Mass Spectrometric Investigation.
Locht, Robert ULg; Leyh, Bernard ULg; Dehareng, Dominique ULg et al

in Chemical Physics (2006), 323

The threshold photoelectron (TPES) and the photoionization mass spectrometric (PIMS) study of CH3Br in the 8-20 eV photon energy range is presented. The interpretation and assignments are supported by ab ... [more ▼]

The threshold photoelectron (TPES) and the photoionization mass spectrometric (PIMS) study of CH3Br in the 8-20 eV photon energy range is presented. The interpretation and assignments are supported by ab initio calculations. The TPES shows several new discrete features in the Jahn-Teller split ground state X2E(2A'-2A") of CH3Br+. An additional continuous band starts at about 11.8 eV. These observations are both correlated with direct ionization and autoionizing transitions. This is supported by constant ion state (CIS) spectroscopy. A large enhancement of the transitions to the A2A and B2E states is ascribed to important autoionizing contributions. Based on the present calculations, the weak to very weak bands in the 17.5-22.0 eV photon energy range were mainly assigned to 2a1 ionization and to double excitations described essentially by the 2e-24a11 and 1e-12e-14a11 configurations. The photoionization mass spectrometric study allows us to investigate in detail the ionization and dissociation of CH3Br+ leading to CH2+, CH3+, Br+ and CH2Br+ from threshold up to 20 eV photon energy. The experimental data are compared to ab initio dissociation energies. At the onset, the CH3+ and CH2Br+ fragment ion production is correlated with the ground state of CH3Br+ and both fragment ions have to appear through dissociative autoionization from the (3a11/1e1)6s or 5s Rydberg state. This interpretation is supported by the photoabsorption spectrum measured recently in the same photon energy range. At higher energies, beside a likely direct (pre)dissociation of the A2A1 and B2E states of CH3Br+, autoionization also contributes to the fragmentation in all decay channels. Avoided crossings in a manyfold of 2A' states are likely to be involved. This is supported by ab initio calculations. For CH3+ the photoion-pair process is analyzed and detailed assignments are proposed on the basis of our latest VUV photoabsorption spectroscopic data. [less ▲]

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See detailThe vacuum UV photoabsorption spectrum of methyl bromide (CH3Br) and its perdeuterated isotopomer CD3Br: a Rydberg series analysis
Locht, Robert ULg; Leyh, Bernard ULg; Jochims, H.-W. et al

in Chemical Physics (2005), 317(1), 73-86

The vacuum UV photoabsorption spectrum of CH3Br has been recorded between 6 and 25 eV. A large number of vibronic bands are observed. They were partly ascribed to vibrationless Rydberg transitions. In the ... [more ▼]

The vacuum UV photoabsorption spectrum of CH3Br has been recorded between 6 and 25 eV. A large number of vibronic bands are observed. They were partly ascribed to vibrationless Rydberg transitions. In the high photon energy range of 12-25 eV, very weak diffuse bands are mostly assigned to transitions from the 3a(1), 1e and (2a(1) + 1a(1)) to 3s orbitals. In the 6-12 eV photon energy range, numerous weak to strong bands are observed. The sharpness is very variable over the entire spectral region. In a first step, the interpretation of the spectrum and the assignment of the Rydberg transitions is based on the simple Rydberg formula. The observed features are classified in two groups of four series, each converging to one of the two spin-orbit components of the (X) over tilde E-2 state of CH3Br+. Rydberg series of nsa(1), npa(1), npe, nd and possibly nf characters are observed. The same measurements have been made for the first time on CD3Br in the 6-12 eV photon energy range. The observed features are classified into the same Rydberg series characterized by nearly the same delta values. Ionization energies for CD3Br (X) over tilde (2) E-3/2 at 10.565 eV and (X) over tilde (2) E-1/2 at 10.902 eV are deduced. In a second step, we fitted the experimental data to an energy expression taking into account both the exchange interaction and the spin-orbit coupling. Already states with n = 6 are found to correspond to Hund's case (c). Constant values of the quantum defects are deduced. (C) 2005 Elsevier B.V. All rights reserved. [less ▲]

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See detailConcomitant adsorption of poly(ethylene oxide)-b-poly(epsilon-caprolactone) copolymers and sodium dodecyl sulfate at the silica-water interface
Vangeyte, Patrick; Leyh, Bernard ULg; De Clercq, C. et al

in Langmuir (2005), 21(17), 7710-7716

Upon addition of silica to aqueous solutions of poly(ethylene oxide)-b-poly(epsilon-caprolactone) copolymers (PEO-b-PCL) and sodium dodecyl sulfate (SDS), adsorption of the solutes occurs at the silica ... [more ▼]

Upon addition of silica to aqueous solutions of poly(ethylene oxide)-b-poly(epsilon-caprolactone) copolymers (PEO-b-PCL) and sodium dodecyl sulfate (SDS), adsorption of the solutes occurs at the silica-water interface. The amount of the adsorbed constituents has been measured by the total concentration depletion method. Small-angle neutron scattering experiments (SANS) have been carried out to investigate the structure of the adsorbed layer. Although SDS is not spontaneously adsorbed onto hydrophilic silica, adsorption is observed in the presence of PEO-b-PCL diblocks, in relation to the relative concentration of the two compounds. Conversely, SDS has a depressive effect on the adsorption of the copolymer, whose structure at the interface is modified. Copolymer desorption is however never complete at high SDS content. These observations have been rationalized by the associative behavior of PEO-b-PCL and SDS in water. [less ▲]

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See detailAdsorption of poly(ethylene oxide)-b-poly(epsilon-caprolactone) copolymers at the silica-water interface
Vangeyte, Patrick; Leyh, Bernard ULg; Rojas, O. J. et al

in Langmuir (2005), 21(7), 2930-2940

The adsorption of amphiphilic poly(ethylene oxide)-b-poly(epsilon-caprolactone) and poly(ethylene oxide)-b-poly(gamma-methyl-epsilon-caprolactone) copolymers in aqueous solution on silica and glass ... [more ▼]

The adsorption of amphiphilic poly(ethylene oxide)-b-poly(epsilon-caprolactone) and poly(ethylene oxide)-b-poly(gamma-methyl-epsilon-caprolactone) copolymers in aqueous solution on silica and glass surfaces has been investigated by flow microcalorimetry, small-angle neutron scattering (SANS), surface forces, and complementary techniques. The studied copolymers consist of a poly(ethylene oxide) (PEO) block of M(n) = 5000 and a hydrophobic polyester block of poly(epsilon-caprolactone) (PCL) or poly(gamma-methyl-epsilon-caprolactone) (PMCL) of M(n) in the 950-2200 range. Compared to homoPEO, the adsorption of the copolymers is significantly increased by the connection of PEO to an aliphatic polyester block. According to calorimetric experiments, the copolymers interact with the surface mainly through the hydrophilic block. At low surface coverage, the PEO block interacts with the surface such that both PEO and PCL chains are exposed to the aqueous solution. At high surface coverage, a dense copolymer layer is observed with the PEO blocks oriented toward the solution. The structure of the copolymer layer has been analyzed by neutron scattering using the contrast matching technique and by tapping mode atomic force microscopy. The experimental observations agree with the coadsorption of micelles and free copolymer chains at the interface. [less ▲]

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See detailRole of angular momentum conservation in unimolecular translational energy release: Validity of the orbiting transition state theory
Gridelet, Evelyne; Lorquet, Jean-Claude ULg; Leyh, Bernard ULg

in Journal of Chemical Physics (2005), 122(9), 94106

The translational kinetic energy release distribution (KERD) for the halogen loss reaction of the bromobenzene and iodobenzene cations has been reinvestigated on the microsecond time scale. Two necessary ... [more ▼]

The translational kinetic energy release distribution (KERD) for the halogen loss reaction of the bromobenzene and iodobenzene cations has been reinvestigated on the microsecond time scale. Two necessary conditions of validity of the orbiting transition state theory (OTST) for the calculation of kinetic energy release distributions (KERDs) have been formulated. One of them examines the central ion-induced dipole potential approximation. As a second criterion, an adiabatic parameter is derived. The lower the released translational energy and the total angular momentum, the larger the reduced mass, the rotational constant of the molecular fragment, and the polarizability of the released atom, the more valid is the OTST. Only the low-energy dissociation of the iodobenzene ion (E approximately 0.45 eV, where E is the internal energy above the reaction threshold) is found to fulfill the criteria of validity of the OTST. The constraints that act on the dissociation dynamics have been studied by the maximum entropy method. Calculations of entropy deficiencies (which measure the deviation from a microcanonical distribution) show that the pair of fragments does not sample the whole of the phase space that is compatible with the mere specification of the internal energy. The major constraint that results from conservation of angular momentum is related to a reduction of the dimensionality of the dynamics of the translational motion to a two-dimensional space. A second and minor constraint that affects the KERD leads to a suppression of small translational releases, i.e., accounts for threshold behavior. At high internal energies, the effects of curvature of the reaction path and of angular momentum conservation are intricately intermeddled and it is not possible to specify the share of each effect. [less ▲]

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See detailThe Photoabsorption and Photoionization of Halogenated Ethylenes: brominated Derivatives.
Locht, Robert ULg; Leyh, Bernard ULg; Jochims, H.-W. et al

Book published by Berliner Elektronen Speicherring für Synchrotron Strahlung m.b.H - on CD-ROM (2005)

The V-UV photoabsorption spectrum of C2HBrF2, C2BrF3 and C2ClF3 have been measured using synchrotron radiation. The mass spectrometric photoionization of C2HBrF2 is also reported.

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See detailThe vacuum UV photoabsorption spectrum of methyl bromide (CH3Br) and its perdeuterated isotopomer CD3Br: a vibrational analysis
Locht, Robert ULg; Leyh, Bernard ULg; Dehareng, Dominique ULg et al

in Chemical Physics (2005), 317(1), 87-102

The fine structure of the vacuum UV photoabsorption spectrum of CH3Br and CD3Br has been analyzed in the 6.9-10.2 eV photon energy range. A large number of lines have been observed, classified and ... [more ▼]

The fine structure of the vacuum UV photoabsorption spectrum of CH3Br and CD3Br has been analyzed in the 6.9-10.2 eV photon energy range. A large number of lines have been observed, classified and assigned to the vibrational excitation accompanying a series of Rydberg transitions. The effects of the Jahn-Teller distortion and of the spin-orbit splitting of the ground electronic state of the ion have been considered. The former effect has been evaluated by ab initio calculations, showing that the E-2 state (in the C-3v symmetry group) splits into (2)A' and (2)A" states in the C-s symmetry group. Even though the energy difference of about 1 meV is extremely small, the (2)A' state is energetically the lowest component whereas the (2)A" is found to be a transition state. The Jahn-Teller stabilization energy and the wavenumbers associated with all vibrational modes have been calculated. Experimentally, the entire fine structure could be described in terms of three vibrational modes, i.e., hc omega(4) = 146 +/- 6 meV (1178 +/- 48 cm(-1)), hc omega(5) = 107 +/- 6 meV (863 +/- 48 cm(-1)) and hc omega(6) = 71 +/- 4 meV (572 +/- 32 cm(-1)), respectively, as resulting from an average over all analyzed Rydberg states. In CD3Br the corresponding energies are hc omega(4) = 104 +/- 3 meV (839 +/- 24 cm(-1)), hc omega(5)=82 +/- 4 meV (661 +/- 32 cm(-1)) and hc omega(6) = 62 +/- 4 meV (500 +/- 32 cm(-1)). These values are in fairly good agreement with those predicted by the present ab initio calculations for the ionic ground state. The experimental isotopic ratio rho(i) = [omega/omega(isot)](i) is 1.15 +/- 0.14, 1.31 +/- 0.14 and 1.39 +/- 1.0 and is predicted to be 1.04, 1.34 and 1.36, respectively, for omega(6), omega(5) and omega(4). On the basis of the present study an alternative assignment of the CH3Br+((X) over tilde E-2) photoelectron band structure is proposed. (C) 2005 Elsevier B.V. All rights reserved. [less ▲]

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See detailGround and Excited State Dissociation Dynamics of Ionized 1,1-Difluoroethene
Gridelet, Evelyne; Dehareng, Dominique ULg; Locht, Robert ULg et al

in Journal of Physical Chemistry A (2005), 109(37), 8225-8235

The kinetic energy release distributions (KERDs) for the fluorine atom loss from the 1,1-difluoroethene cation have been recorded with two spectrometers in two different energy ranges. A first experiment ... [more ▼]

The kinetic energy release distributions (KERDs) for the fluorine atom loss from the 1,1-difluoroethene cation have been recorded with two spectrometers in two different energy ranges. A first experiment uses dissociative photoionization with the He(I) and Ne(I) resonance lines, providing the ions with a broad internal energy range, up to 7 eV above the dissociation threshold. The second experiment samples the metastable range, and the average ion internal energy is limited to about 0.2 eV above the threshold. In both energy domains, KERDs are found to be bimodal. Each component has been analyzed by the maximum entropy method. The narrow, low kinetic energy components display for both experiments the characteristics of a statistical, simple bond cleavage reaction: constraint equal to the square root of the fragment kinetic energy and ergodicity index higher than 90%. Furthermore, this component is satisfactorily accounted for in the metastable time scale by the orbiting transition state theory. Potential energy surfaces corresponding to the five lowest electronic states of the dissociating 1,1-C2H2F2+ ion have been investigated by ab initio calculations at various levels. The equilibrium geometry of these states, their dissociation energies, and their vibrational wavenumbers have been calculated, and a few conical intersections between these surfaces have been identified. It comes out that the ionic ground state (X) over tilde B-2(1) is adiabatically correlated with the lowest dissociation asymptote. Its potential energy curve increases in a monotonic way along the reaction coordinate, giving rise to the narrow KERD component. Two states embedded in the third photoelectron band ( (B) over tilde (2)A(1), at 15.95 eV and (C) over tilde B-2(2) at 16.17 eV) also correlate with the lowest asymptote at 14.24 eV. We suggest that their repulsive behavior along the reaction coordinate be responsible for the KERD high kinetic energy contribution. [less ▲]

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See detailMixed self-assembly of poly(ethylene oxide)-b-poly(epsilon-caprolactone) copolymers and sodium dodecyl sulfate in aqueous solution
Vangeyte, Patrick; Leyh, Bernard ULg; Auvray, L. et al

in Langmuir (2004), 20(21), 9019-9028

Interaction of amphiphilic poly(ethylene oxide)-b-poly(epsilon-caprolactone) copolymers with anionic sodium dodecyl sulfate (SDS) has been investigated in aqueous solution. Formation of mixed micelles has ... [more ▼]

Interaction of amphiphilic poly(ethylene oxide)-b-poly(epsilon-caprolactone) copolymers with anionic sodium dodecyl sulfate (SDS) has been investigated in aqueous solution. Formation of mixed micelles has been confirmed by surface tension measurements, whereas the influence of the surfactant on the copolymer self-assembling has been studied by measurement of the 1H NMR self-diffusion coefficients and by small-angle neutron scattering. As a rule, the surfactant decreases the heterogeneity of the micellar structures formed by the copolymer in water. Moreover, increasing the content of SDS results in the increasingly more important extension of the poly(ethylene oxide) (PEO) corona chains and the copolymer micelle deaggregation. The stability of the micelles against SDS increases with the length of the hydrophobic block. Preliminary two-dimensional NMR measurements with nuclear Overhauser enhancement have confirmed the spatial vicinity between SDS and the constitutive blocks of the copolymer. [less ▲]

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