Acid solvation versus dissociation at 'stardust conditions': Reaction sequence matters
| Autor: | Devendra Mani, Britta Redlich, Nitish Pal, Saskia Körning, Ricardo Pérez de Tudela, Raffael Schwan, Martina Havenith, A. F. G. van der Meer, Dominik Marx, Gerhard Schwaab, Harald Forbert |
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| Rok vydání: | 2019 |
| Předmět: |
Hydronium
Interstellar cloud Ab initio 02 engineering and technology 010402 general chemistry 01 natural sciences 7. Clean energy Chemical reaction Acid dissociation constant Dissociation (chemistry) chemistry.chemical_compound Physics::Chemical Physics Research Articles Astrophysics::Galaxy Astrophysics Multidisciplinary Chemistry fungi Solvation food and beverages SciAdv r-articles FELIX Infrared and Terahertz Spectroscopy 021001 nanoscience & nanotechnology 0104 chemical sciences 13. Climate action Chemical physics Astrophysics::Earth and Planetary Astrophysics 0210 nano-technology FELIX Fel Technology Stoichiometry Research Article |
| Zdroj: | Science Advances Science Advances, 5, 1-8 Science Advances, 5, 6, pp. 1-8 |
| ISSN: | 2375-2548 |
| Popis: | Chemistry, such as dissociation of acids, can even be triggered at ultracold “stardust conditions” in the absence of radiation. Chemical reactions at ultralow temperatures are of fundamental importance to primordial molecular evolution as it occurs on icy mantles of dust nanoparticles or on ultracold water clusters in dense interstellar clouds. As we show, studying reactions in a stepwise manner in ultracold helium nanodroplets by mass-selective infrared (IR) spectroscopy provides an avenue to mimic these “stardust conditions” in the laboratory. In our joint experimental/theoretical study, in which we successively add H2O molecules to HCl, we disclose a unique IR fingerprint at 1337 cm−1 that heralds hydronium (H3O+) formation and, thus, acid dissociation generating solvated protons. In stark contrast, no reaction is observed when reversing the sequence by allowing HCl to interact with preformed small embryonic ice-like clusters. Our ab initio simulations demonstrate that not only reaction stoichiometry but also the reaction sequence needs to be explicitly considered to rationalize ultracold chemistry. |
| Databáze: | OpenAIRE |
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