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Response to "Comment on 'Sum-frequency vibrational spectroscopy of centrosymmetric molecule at interfaces'" [J. Chem. Phys. 160, 107101 (2024)].

J Chem Phys

March 2024

Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Zhongguancun, Beijing 100190, People's Republic of China.

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In our recent paper titled "Bi-layering at ionic liquid surfaces: a sum-frequency generation vibrational spectroscopy- and molecular dynamics simulation-based study" co-authored by T. Iwahashi, T. Ishiyama, Y.

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This Comment raises several questions concerning the surface structure concluded in the paper referenced in the title. Specifically, that paper ignores previous experiments and simulations which demonstrate for the same ionic liquids depth-decaying, multilayered surface-normal density profiles rather than the claimed molecular mono- or bi-layers. We demonstrate that the claimed structure does not reproduce the measured X-ray reflectivity, which probes directly the surface-normal density profile.

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