Vibrational spectra of water complexes with H2, N2, and CO

Sadlej, Joanna; Rowland, Brad; Devlin, J. Paul; Buch, V.

doi:10.1063/1.469528

Cited by 99 publications

(95 citation statements)

References 91 publications

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“…For the 1:1 water-carbon monoxide system, the two possible structures were experimentally identified (Lundell & Rasanen 1995), with the conclusion that the two complexes coexist. Results based on highly-correlated quantum chemical calculations agree with experiments (Reed et al 1986;Parish et al 1992;Lundell 1995;Sadlej et al 1995;Lundell et al 1997). We here predict that the C-attached complex is the most stable one from the computed potential interaction energies for the W3-carbon monoxide complex at L1.…”

Section: Results Of Quantum Chemical Calculationssupporting

confidence: 75%

Combined quantum chemical and modeling study of CO hydrogenation on water ice

Rimola

Taquet

Ugliengo

et al. 2014

A&A

105

108

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Context. Successive hydrogenation reactions of CO on interstellar icy grain surfaces are considered one of the most efficient mechanisms in interstellar environments for the formation of H 2 CO and CH 3 OH, two of the simplest organic molecules detected in space. In the past years, several experimental and theoretical works have been focused on these reactions, providing relevant information both at the macroscopic and atomic scale. However, several questions still remain open, such as the exact role played by water in these processes, a crucial aspect because water is the dominant constituent of the ice mantles around dust grain cores. Aims. We here present a quantum chemical description of the successive H additions to CO both in the gas phase and on the surfaces of several water clusters. Methods. The hydrogenation steps were calculated by means of accurate quantum chemical methods and structural cluster models consisting of 3, 18, and 32 water molecules. Results. Our main result is that the interaction of CO and H 2 CO with the water cluster surfaces through H-bonds with the O atoms increases the C−O polarization, thus weakening the C−O bond. Consequently, the C atoms are more prone to receiving H atoms, which in turn lowers the energy barriers for the H additions compared to the gas-phase processes. The calculated energy barriers and transition frequencies associated with the reaction coordinate were adopted as input parameters in our numerical model of the surface chemistry (GRAINOBLE) to simulate the distribution of the H 2 CO and CH 3 OH ice abundances (with respect to water). Our GRAINOBLE results based on the energy barriers and transition frequencies for the reactions on the 32 water molecule cluster compare well with the observed abundances in low-mass protostars and dark cores.

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Section: Results Of Quantum Chemical Calculationssupporting

confidence: 75%

Combined quantum chemical and modeling study of CO hydrogenation on water ice

Rimola

Taquet

Ugliengo

et al. 2014

A&A

105

108

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“…Direct information coming from gas phase molecular beam scattering experiments, to our knowledge, is not available. Scattering data could be crucial also to test the validity of numerous theoretical calculations available on the intermolecular interactions [10,[17][18][19][20][21][22][23].…”

Section: Introductionmentioning

confidence: 99%

“…Experimental information on the present case studies is limited to a microwave spectroscopic characterization of gas phase H 2 O-N 2 [9] and low temperature investigations on solid matrix of H 2 O-N 2 [10,11] and H 2 O-O 2 [12,13].…”

Section: Introductionmentioning

confidence: 99%

A molecular beam scattering study of the weakly bound complexes of water and hydrogen sulphide with the main components of air

Cappelletti¹,

Candori²,

Roncaratti³

et al. 2010

Molecular Physics

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“…The current work focuses on spectroscopy, dynamics, and interaction potentials for H 2 + H 2 O, 1,13,[15][16][17][18][19][20][21] which proves to be relevant in a wide range of terrestrial and extraterrestrial venues. 2,[22][23][24][25][26] In high temperature H 2 /O 2 combustion, for example, collisions of the highly energized product H 2 O molecules with H 2 reactant provide an important mechanism for heat flow as well as establishing local thermodynamic equilibrium in the flames.…”

Section: Introductionmentioning

confidence: 99%

Overtone vibrational spectroscopy in H2-H2O complexes: A combined high level theoretical ab initio, dynamical and experimental study

Ziemkiewicz

Pluetzer

Nesbitt

et al. 2012

The Journal of Chemical Physics

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First results are reported on overtone (v OH = 2 ← 0) spectroscopy of weakly bound H 2 -H 2 O complexes in a slit supersonic jet, based on a novel combination of (i) vibrationally mediated predissociation of H 2 -H 2 O, followed by (ii) UV photodissociation of the resulting H 2 O, and (iii) UV laser induced fluorescence on the nascent OH radical. In addition, intermolecular dynamical calculations are performed in full 5D on the recent ab initio intermolecular potential of Valiron et al. [J. Chem. Phys. 129, 134306 (2008)] in order to further elucidate the identity of the infrared transitions detected. Excellent agreement is achieved between experimental and theoretical spectral predictions for the most strongly bound van der Waals complex consisting of ortho (I = 1) H 2 and ortho (I = 1) H 2 O (oH 2 -oH 2 O). Specifically, two distinct bands are seen in the oH 2 -oH 2 O spectrum, corresponding to internal rotor states in the upper vibrational manifold of and rotational character. However, none of the three other possible nuclear spin modifications (pH 2 -oH 2 O, pH 2 -pH 2 O, or oH 2 -pH 2 O) are observed above current signal to noise level, which for the pH 2 complexes is argued to arise from displacement by oH 2 in the expansion mixture to preferentially form the more strongly bound species. Direct measurement of oH 2 -oH 2 O vibrational predissociation in the time domain reveals lifetimes of 15(2) ns and <5(2) ns for the and states, respectively. Theoretical calculations permit the results to be interpreted in terms of near resonant energy levels and intermolecular alignment of the H 2 and H 2 O wavefunctions, providing insight into predissociation dynamical pathways from these metastable levels.

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Vibrational spectra of water complexes with H2, N2, and CO

Cited by 99 publications

References 91 publications

Combined quantum chemical and modeling study of CO hydrogenation on water ice

Combined quantum chemical and modeling study of CO hydrogenation on water ice

A molecular beam scattering study of the weakly bound complexes of water and hydrogen sulphide with the main components of air

Overtone vibrational spectroscopy in H2-H2O complexes: A combined high level theoretical ab initio, dynamical and experimental study

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