Aligned molecular collisions and a stereodynamical mechanism for selective chirality

Aquilanti, Vincenz̊o; Grossi, Gaia; Lombardi, Andrea; Maciel, Glauciete S.; Palazzetti, Federico

doi:10.1007/s12210-011-0123-7

Cited by 44 publications

(10 citation statements)

References 62 publications

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“…Specifically, previous studies [9][10][11] indicate that molecular directionality and alignment should strongly amplify dichroism and provide stereodynamical mechanisms for discrimination of enantiomers other than via circularly polarized light. In the present work, we take initial steps in both these directions: Propylene oxide 12,13 is a prototypically experimentally available chiral molecule and unique in having been characterized in previous experiments for directional and aligning properties by electrostatic hexapole techniques. 14,15 Such a study is being extended in our laboratory, coupling the mechanical molecular velocity selector method (permitting the control of the velocity dependence of molecular alignment) [5][6][7][8] with electronion imaging detection using tunable synchrotron radiation with high intensity.…”

Section: Introductionmentioning

confidence: 99%

Double photoionization of propylene oxide: A coincidence study of the ejection of a pair of valence-shell electrons

Falcinelli

Vecchiocattivi

Alagia

et al. 2018

The Journal of Chemical Physics

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Propylene oxide, a favorite target of experimental and theoretical studies of circular dichroism, was recently discovered in interstellar space, further amplifying the attention to its role in the current debate on protobiological homochirality. In the present work, a photoelectron-photoion-photoion coincidence technique, using an ion-imaging detector and tunable synchrotron radiation in the 18.0-37.0 eV energy range, permits us (i) to observe six double ionization fragmentation channels, their relative yields being accounted for about two-thirds by the couple (CH, CHO) and one-fifth by (CH, CHO); (ii) to measure thresholds for their openings as a function of photon energy; and (iii) to unravel a pronounced bimodality for a kinetic-energy-released distribution, fingerprint of competitive non-adiabatic mechanisms.

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Section: Introductionmentioning

confidence: 99%

Double photoionization of propylene oxide: A coincidence study of the ejection of a pair of valence-shell electrons

Falcinelli

Vecchiocattivi

Alagia

et al. 2018

The Journal of Chemical Physics

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“…Although work is constantly being done to achieve the feasibility of exact quantum calculations (e.g., through new coordinates and basis sets Aquilanti et al, 2000, 2002, 2004a,b, 2006; Sevyuk et al, 2005; Castro Palacio et al, 2007; Barreto et al, 2011, 2012; Palazzetti et al, 2011), these remain mainly limited to three-atom systems. For energy transfer, reactive and photodissociating systems involving triatomic and larger molecules, or for the simulation of more complex environments such as gaseous mixtures and flows, classical trajectories are widely employed to interpret experimental results, saving computing time (see e.g., Lombardi et al, 2010; Aquilanti et al, 2011; Palazzetti et al, 2013; Nakamura et al, 2015).…”

Section: Quantum Classical Calculations For Vibrational Energy Tramentioning

confidence: 99%

Full Dimensional Potential Energy Function and Calculation of State-Specific Properties of the CO+N2 Inelastic Processes Within an Open Molecular Science Cloud Perspective

et al. 2019

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A full dimensional Potential Energy Surface (PES) of the CO + N 2 system has been generated by extending an approach already reported in the literature and applied to N 2 -N 2 (Cappelletti et al., 2008 ), CO 2 -CO 2 (Bartolomei et al., 2012 ), and CO 2 -N 2 (Lombardi et al., 2016b ) systems. The generation procedure leverages at the same time experimental measurements and high-level ab initio electronic structure calculations. The procedure adopts an analytic formulation of the PES accounting for the dependence of the electrostatic and non-electrostatic components of the intermolecular interaction on the deformation of the monomers. In particular, the CO and N 2 molecular multipole moments and electronic polarizabilities, the basic physical properties controlling the behavior at intermediate and long-range distances of the interaction components, were made to depend on relevant internal coordinates. The formulated PES exhibits substantial advantages when used for structural and dynamical calculations. This makes it also well suited for reuse in Open Molecular Science Cloud services.

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“…Many alternative choices are available for adopting a specific set of angular coordinates Ω, some of them lead to a compact analytic expression of the PES and an intuitive connection with the geometric properties of the system. [30][31][32][33][34][35][36] Compact expansions can be obtained in terms of special angular functions (i.e., hyperspherical harmonics [37][38][39][40][41][42][43][44][45][46][47] ).…”

Section: A Potential Energy Surfacementioning

confidence: 99%

Energy transfer upon collision of selectively excited CO2 molecules: State-to-state cross sections and probabilities for modeling of atmospheres and gaseous flows

Lombardi

Faginas-Lago

Pacifici

et al. 2015

The Journal of Chemical Physics

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Carbon dioxide molecules can store and release tens of kcal/mol upon collisions, and such an energy transfer strongly influences the energy disposal and the chemical processes in gases under the extreme conditions typical of plasmas and hypersonic flows. Moreover, the energy transfer involving CO2 characterizes the global dynamics of the Earth-atmosphere system and the energy balance of other planetary atmospheres. Contemporary developments in kinetic modeling of gaseous mixtures are connected to progress in the description of the energy transfer, and, in particular, the attempts to include non-equilibrium effects require to consider state-specific energy exchanges. A systematic study of the state-to-state vibrational energy transfer in CO2 + CO2 collisions is the focus of the present work, aided by a theoretical and computational tool based on quasiclassical trajectory simulations and an accurate full-dimension model of the intermolecular interactions. In this model, the accuracy of the description of the intermolecular forces (that determine the probability of energy transfer in molecular collisions) is enhanced by explicit account of the specific effects of the distortion of the CO2 structure due to vibrations. Results show that these effects are important for the energy transfer probabilities. Moreover, the role of rotational and vibrational degrees of freedom is found to be dominant in the energy exchange, while the average contribution of translations, under the temperature and energy conditions considered, is negligible. Remarkable is the fact that the intramolecular energy transfer only involves stretching and bending, unless one of the colliding molecules has an initial symmetric stretching quantum number greater than a threshold value estimated to be equal to 7.

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Aligned molecular collisions and a stereodynamical mechanism for selective chirality

Cited by 44 publications

References 62 publications

Double photoionization of propylene oxide: A coincidence study of the ejection of a pair of valence-shell electrons

Double photoionization of propylene oxide: A coincidence study of the ejection of a pair of valence-shell electrons

Full Dimensional Potential Energy Function and Calculation of State-Specific Properties of the CO+N2 Inelastic Processes Within an Open Molecular Science Cloud Perspective

Energy transfer upon collision of selectively excited CO2 molecules: State-to-state cross sections and probabilities for modeling of atmospheres and gaseous flows

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