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• W1676149739 abstract "Experiments explore the influence of different C–H stretching eigenstates of CH3D on the reaction of CH3D with Cl(P3∕22). We prepare the ∣110⟩∣0⟩(A1,E), ∣200⟩∣0⟩(E), and ∣100⟩∣0⟩+ν3+ν5 eigenstates by direct midinfrared absorption near 6000cm−1. The vibrationally excited molecules react with photolytic Cl atoms, and we monitor the vibrational states of the CH2D or CH3 radical products by 2+1 resonance enhanced multiphoton ionization. Initial excitation of the ∣200⟩∣0⟩(E) state leads to a twofold increase in CH2D products in the vibrational ground state compared to ∣100⟩∣0⟩+ν3+ν5 excitation, indicating mode-selective chemistry in which the C–H stretch motion couples more effectively to the H-atom abstraction coordinate than bend motion. For two eigenstates that differ only in the symmetry of the vibrational wave function, ∣110⟩∣0⟩(A1) and ∣110⟩∣0⟩(E), the ratio of reaction cross sections is 1.00±0.05, showing that there is no difference in enhancement of the H-atom abstraction reaction. Molecules with excited local modes corresponding to one quantum of C–H stretch in each of two distinct oscillators react exclusively to form C–H stretch excited CH2D products. Conversely, eigenstates containing stretch excitation in a single C–H oscillator form predominantly ground vibrational state CH2D products. Analyzing the product state yields for reaction of the ∣110⟩∣0⟩(A1) state of CH3D yields an enhancement of 20±4 over the thermal reaction. A local mode description of the vibrational motion along with a spectator model for the reactivity accounts for all of the observed dynamics." @default.
• W1676149739 created "2016-06-24" @default.
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• W1676149739 date "2006-10-02" @default.
• W1676149739 modified "2023-10-17" @default.
• W1676149739 title "Mode- and bond-selective reaction of Cl(P3∕22) with CH3D: C–H stretch overtone excitation near 6000cm−1" @default.
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• W1676149739 doi "https://doi.org/10.1063/1.2352742" @default.
• W1676149739 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/17029427" @default.
• W1676149739 hasPublicationYear "2006" @default.
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