Direct FTIR high resolution probe of small and medium size Arn(CO2)m van der Waals complexes formed in a slit supersonic expansion

Thiévin, Jonathan; Cadudal, Y.; Georges, Robert; Vigasin, A. A.

doi:10.1016/j.jms.2006.09.010

Cited by 20 publications

(10 citation statements)

References 36 publications

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“…Calculated frequencies reported in Table III also shows a saturation in frequency shift in CO 2 ͑Ar͒ m clusters with m ജ 5. This direction of shifts are in agreement with the earlier dynamics studies of Severson 38 and Böyukata et al 39 and direct supersonic fourier transform infrared spectroscopy ͑FTIR͒ experimental studies of Thiévin et al 40 The present ab initio studies show a good agreement in geometry and frequency shifts with the most stable higher CO 2 ͑Ar͒ m clusters with m =6-8, obtained via molecular dynamics simulation. Table III reports the frequencies of the CO 2 ͑Ar͒ m clusters through m =1-8 and the values show an increasing red frequency shifts from 0.7 through 5.6 cm −1 with number of argon atoms.…”

Section: B Effect Of Argon Matrix On the Asymmetric Stretching Frequsupporting

confidence: 92%

An ab initio investigation on (CO2)n and CO2(Ar)m clusters: Geometries and IR spectra

Jose

Gadre

2008

The Journal of Chemical Physics

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An ab initio investigation on CO(2) homoclusters is done at MPWB1K6-31++G(2d) level of theory. Electrostatic guidelines are found to be useful for generating initial structures of (CO(2))(n) clusters. The ab initio minimum energy geometries of (CO(2))(n) with n=2-8 are T shaped, cyclic, trigonal pyramidal, tetragonal pyramidal, tetragonal bipyramidal, pentagonal bipyramidal, and pentagonal bipyramid with one CO(2) molecule attached to it. A test calculation on (CO(2))(20) cluster is also reported. The geometric parameters of the energetically most favored (CO(2))(n) clusters match quite well their experimental counterparts (wherever available) as well as those derived from molecular dynamics studies. The effect of clustering is quantified through the asymmetric C-O stretching frequency shift relative to the single CO(2) molecule. (CO(2))(n) clusters show an increasing blueshift from 1.8 to 9.6 cm(-1) on increasing number of CO(2) molecules from n=2 to 8. The energetics and geometries of CO(2)(Ar)(m) clusters have also been explored at the same level of theory. The geometries for m=1-6 show a predominant T type of the argon-CO(2) molecule interaction. Higher clusters with m=7-12 show that the argon atoms cluster around the oxygen atom after the saturation of the central carbon atom. The CO(2)(Ar)(m) clusters exhibit an increasing redshift in the C-O asymmetric stretch relative to CO(2) molecule of 0.7-5.6 cm(-1) with increasing number of argon atoms through m=1-8.

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Section: B Effect Of Argon Matrix On the Asymmetric Stretching Frequsupporting

confidence: 92%

An ab initio investigation on (CO2)n and CO2(Ar)m clusters: Geometries and IR spectra

Jose

Gadre

2008

The Journal of Chemical Physics

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“…Although they have been observed with C 2 H 2 seeded in either argon or neon, it cannot be excluded that the carrier species also contains some of the RG used in the expansion. Similar broad features have been reported for CO 2 clusters [127].…”

Section: Molecular Physics 2789supporting

confidence: 87%

Experimental 2CH excitation in acetylene-containing van der Waals complexes

et al. 2012

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“…In Table 1, we present an updated review, which we have restricted to high-resolution investigations. We mention the following research groups active in this field with particular topics: the Université Libre de Bruxelles (hydrocarbons (Lee et al 2007, Hurtmans et al 2001, Lafferty et al 2006, Flaud et al 2001)); Université de Rennes (small clusters (Thiévin et al 2006)), Monash University (fluorohydrocarbons (Thompson et al 2003)); Université Pierre et Marie Curie, Paris (XY 4 and XY 6 spherical tops (Asselin et al 2008, Rey et al 2001, clusters (Asselin et al 2006(Asselin et al , 2007); and our group at ETH Zürich (simple molecules and spherical tops, methane (Dübal et al 1984, Amrein et al 1988a, ammonia (Snels et al 2006a), substituted methanes , XY 6 spherical tops and Jahn-Teller molecules (Boudon et al 2002), fluoro(hydro, chloro)carbons, hydrogenfluoride clusters, and other applications (Snels et al 1995, Luckhaus et al 1995, He et al 2007, Hippler et al 2007)) and chiral molecules (Beil et al 1994, Bauder et al 1997) see also , Quack (2011).…”

Section: An Overview Of Ftir Spectroscopic Supersonic-jet Investigationsmentioning

confidence: 99%

High‐ResolutionFTIRand Diode Laser Spectroscopy of Supersonic Jets

Snels

Horká‐Zelenková

Hollenstein

et al. 2011

Handbook of High‐resolution Spectroscopy

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Fourier transform infrared (FTIR) spectrometers and tunable diode lasers in combination with a supersonic molecular beam expansion are a perfect tool for the investigation of molecules, ions, and radicals at low temperatures. The internal degrees of freedom of the molecules are adiabatically cooled to very low temperatures and thus only low-lying energy levels are populated. The reduction of the number of populated levels at low temperatures makes the assignment of the spectra much easier as compared to the congested room-temperature spectra. Under certain conditions, the Doppler linewidths are greatly reduced, corresponding to very low effective translational temperatures. Supersonic expansion also provides a suitable method for producing and investigating van der Waals clusters and hydrogen-bonded complexes. Unstable species such as radicals and ions can be efficiently produced and studied in a molecular beam. The low rotational temperature allows for the study of nuclear spin symmetry conservation or conversion between nuclear spin isomers. A molecular beam expansion can be obtained by expanding gas through a slit or a circular nozzle. Both expansion geometries can be used in combination with a multipass optical setup and with cavity ring down spectroscopy, which enhances the effective absorption path length. Cooling of the molecules can be promoted by seeding in noble gases. This article summarizes the general aspects of the experimental technique as well as current developments. To demonstrate how powerful the combination of a molecular beam expansion with tunable diode laser and FTIR spectroscopy can be, we report results on some important current examples.

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Direct FTIR high resolution probe of small and medium size Arn(CO2)m van der Waals complexes formed in a slit supersonic expansion

Cited by 20 publications

References 36 publications

An ab initio investigation on (CO2)n and CO2(Ar)m clusters: Geometries and IR spectra

An ab initio investigation on (CO2)n and CO2(Ar)m clusters: Geometries and IR spectra

Experimental 2CH excitation in acetylene-containing van der Waals complexes

High‐ResolutionFTIRand Diode Laser Spectroscopy of Supersonic Jets

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