SEQUENTIAL CLUSTERING OF HCl IN ARGON: NEAR INFRARED SPECTRA OF $Ar_{2}HCl$ AND $Ar_{3}HCl$

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1997

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Ohio State University

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High resolution near infrared spectra of the $v_{HCL} =1\leftarrow 0$ fundamental stretch in and $Ar_{2}HCl$ and $Ar_{3}HCl$ have been characterized using a slit-jet infrared spectrometer. Analysis of the jet cooled, rotationally resolved spectra i) permit unambigous identification of the cluster size, ii) provide vibrationally averaged geometries in the $v_{HCL} =1$ excited, state, and iii) allow the vibrational shift of the HCl chromophore to be measured as a function of the number of Aar atoms in the complex. The equilibrium structures of the $Ar_{n}HCl (n=1-3)$ clusters calculated using accurate Ar-Ar and Ar-HCl pair potentials are consistent with the vibrationally averaged structures inferred spectroscopically. The vibrational redshifts for the $Ar_{n} HCl (n=l-3)$ reflect a near-linear dependence on the number of Ar atoms, which is qualitatively reproduced by simple classical calculations of the $v_{HCL}=0$ and 1 pairwise additive potential surfaces. Finally, predictions of the HCl matrix shifts in a relaxed fee lattice of Ar atoms significantly overshoot the matrix value and indicate an appreciable sensitivity to non-nearest neighbors in $2^{nd}, 3^{rd}$ and higher order solvation shells.

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Author Institution: JILA, National institute of Standards and Technology and Department of Chemistry and Biochemistry, University of Colorado

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