Towards rovibrationally resolved photochemistry in H2O-CO2
(2026) Belgian Physical Society General Scientific Meeting 2026 — Location: Louvain (27.May.2026)
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- (en) Water and CO2 are the most important greenhouse gases in our atmosphere. The solvation of CO2 is a decisive process in the chemistry of clouds and oceans. A precise characterization of the interaction of these two molecules is thus of prime importance. In the present work, we recorded a rotationally resolved spectrum of the triple excitation of the OH stretch in the H2O-CO2 molecular complex. This represents a further step in our longstanding effort to better characterize the dynamics of CO2-H2O interactions, notably through a systematic increase in vibrational excitation [1–4]. Increasing excitation will ultimately drive the isomerization of the complex into carbonic acid H2CO3. The complexes were formed from an 8 cm-long pulsed slit supersonic jet and probed by the CRDS technique in the spectral range of the second OH overtone of H2O, using the FANTASIO setup [5,6]. A home-built external cavity diode laser (ECDL), stabilized to the frequency comb, was used as the light source. The recorded spectrum was vibrationally assigned to the (v1,v2,v3) ← (v1’,v2’,v3’) = (2,0,1) ← (0,0,0) and (2,0,1) + intermolecular mode ← (0,0,0) where the v1,v2,v3 vibrational quantum numbers of the isolated H2O molecule are used to assign the involved states. In this talk, I will present the experimental spectrum and the improvements to the experimental setup that enabled the recording of this spectral signature. I am going to present our progress in the analysis of this spectrum using group theory and the effective Hamiltonian. Finally, perspectives on going across the isomerization barrier will be presented. [1] C. Lauzin, A.C. Imbreckx, T. Foldes, T. Vanfleteren, N. Moazzen-Ahmadi, and M. Herman, Mol. Phys. 118, e1706776 (2020). [2] A.S. Bogomolov, A. Roucou, R. Bejjani, M. Herman, N. Moazzen-Ahmadi, and C. Lauzin, Chem. Phys. Lett. 774, 138606 (2021). [3] T. Gartner, C. Lauzin, A.R.W. McKellar, and N. Moazzen-Ahmadi, J. Phys. Chem. A 127, 3668 (2023). [4] A.S. Bogomolov, S. Collignon, R. Glorieux, N. Moazzen-Ahmadi, M. Herman, C. Lauzin, Rotationally resolved triple vibrational excitation in D2O-CO2 van der Waals complex, in preparation (2026). [5] M. Herman, K. Didriche, D. Hurtmans, B. Kizil, P. Macko, A. Rizopoulos, and P.V. Poucke, Mol. Phys. 105, 815 (2007). [6] A.S. Bogomolov, R. Glorieux, M. Herman, T. Corbo, S. Collignon, B.M. Hays, D. Lederer, N. Moazzen-Ahmadi, A. Libert, B. Tomasetti, J. Fréreux, and C. Lauzin, Mol.Phys. 123, e2413417 (2025).
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Bogomolov, A., Collignon, S., Moazzen-Ahmadi, N., Herman, M., & Lauzin, C. (2026, May 27). Towards rovibrationally resolved photochemistry in H2O-CO2. Belgian Physical Society General Scientific Meeting 2026, Louvain.