Vibrational Spectroscopy of Bisulfate/Sulfuric Acid/Water Clusters: Structure, Stability, and Infrared Multiple-Photon Dissociation Intensities

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• 作者：Tara I. Yacovitch ; Nadja Heine ; Claudia Brieger ; Torsten Wende ; Christian Hock ; Daniel M. Neumark ; Knut R. Asmis
• 刊名：The Journal of Physical Chemistry A
• 出版年：2013
• 出版时间：August 15, 2013
• 年：2013
• 卷：117
• 期：32
• 页码：7081-7090
• 全文大小：536K
• 年卷期：v.117,no.32(August 15, 2013)
• ISSN：1520-5215

文摘

The structure and stability of mass-selected bisulfate, sulfuric acid, and water cluster anions, HSO₄^{鈥?/sup>(H₂SO₄)_m(H₂O)_n, are studied by infrared photodissociation spectroscopy aided by electronic structure calculations. The triply hydrogen-bound HSO₄鈥?/sup>(H₂SO₄) configuration appears as a recurring motif in the bare clusters, while incorporation of water disrupts this stable motif for clusters with m > 1. Infrared-active vibrations predominantly involving distortions of the hydrogen-bound network are notably missing from the infrared multiple-photon dissociation (IRMPD) spectra of these ions but are fully recovered by messenger-tagging the clusters with H₂. A simple model is used to explain the observed 鈥淚RMPD transparency鈥?}