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A study of the valence photoelectron spectrum of uracil and mixed water-uracil clusters

التفاصيل البيبلوغرافية
العنوان: A study of the valence photoelectron spectrum of uracil and mixed water-uracil clusters
المؤلفون: Giuseppe Mattioli, Lorenzo Avaldi, Paola Bolognesi, Annarita Casavola, Filippo Morini, Thomas Van Caekenberghe, John D. Bozek, Mattea C. Castrovilli, Jacopo Chiarinelli, Alicja Domaracka, Suvasthika Indrajith, Sylvain Maclot, Aleksandar R. Milosavljević, Chiara Nicolafrancesco, Christophe Nicolas, Patrick Rousseau
المساهمون: Morini, Filippo/0000-0001-9293-5791, Mattioli, Giuseppe, Avaldi, Lorenzo, Bolognesi, Paola, Casavola, Annarita, MORINI, Filippo, Van Caekenberghe, Thomas, Bozek, John D., Castrovilli, Mattea C., Chiarinelli, Jacopo, Domaracka, Alicja, Indrajith, Suvasthika, Maclot, Sylvain, Milosavljevic, Aleksandar R., Nicolafrancesco, Chiara, Nicolas, Christophe, Rousseau, Patrick, Istituto di Struttura della Materia (CNR-ISM), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), Hasselt University (UHasselt), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Atomes, Molécules et Agrégats (AMA), Centre de recherche sur les Ions, les MAtériaux et la Photonique (CIMAP - UMR 6252), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Matériaux, Défauts et IRradiations (MADIR), Institut Lumière Matière [Villeurbanne] (ILM), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)
المصدر: Journal of Chemical Physics
Journal of Chemical Physics, 2023, 158 (11), pp.114301. ⟨10.1063/5.0135574⟩
بيانات النشر: AIP Publishing, 2023.
سنة النشر: 2023
مصطلحات موضوعية: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, General Physics and Astronomy, Physical and Theoretical Chemistry
الوصف: The valence ionization of uracil and mixed water-uracil clusters has been studied experimentally and by ab initio calculations. In both measurements, the spectrum onset shows a red shift with respect to the uracil molecule, with the mixed cluster characterized by peculiar features unexplained by the sum of independent contributions of the water or uracil aggregation. To interpret and assign all the contributions, we performed a series of multi-level calculations, starting from an exploration of several cluster structures using automated conformer-search algorithms based on a tight-binding approach. Ionization energies have been assessed on smaller clusters via a comparison between accurate wavefunction-based approaches and cost-effective DFT-based simulations, the latter of which were applied to clusters up to 12 uracil and 36 water molecules. The results confirm that (i) the bottom-up approach based on a multilevel method [Mattioli et al. Phys. Chem. Chem. Phys. 23, 1859 (2021)] to the structure of neutral clusters of unknown experimental composition converges to precise structure-property relationships and (ii) the coexistence of pure and mixed clusters in the water-uracil samples. A natural bond orbital (NBO) analysis performed on a subset of clusters highlighted the special role of H-bonds in the formation of the aggregates. The NBO analysis yields second-order perturbative energy between the H-bond donor and acceptor orbitals correlated with the calculated ionization energies. This sheds light on the role of the oxygen lone-pairs of the uracil CO group in the formation of strong H-bonds, with a stronger directionality in mixed clusters, giving a quantitative explanation for the formation of core-shell structures. This article is based upon work from COST Action CA18212—Molecular Dynamics in the GAS phase (MD-GAS) supported by COST (European Cooperation in Science and Technology), and it was partially supported by the CNRS PICS Project BIFACE, the International Associated Laboratory “DYNAMO,” and the PRIN 20173B72NB “Predicting and controlling the fate of bio-molecules driven by extreme-ultraviolet radiation”. C.N. is co-funded by Région Normandie and Synchrotron SOLEIL. SOLEIL support is acknowledged under Project No. 20171346. A.C. acknowledges the access to the CINECA supercomputer facility via the ISCRA C HP10C652JX Grant. F.M. and T.V.C. acknowledge the VSC (Flemish Supercomputer Center), funded by the Research Foundation-Flanders (FWO) and the Flemish Government.
وصف الملف: application/pdf
اللغة: English
تدمد: 0021-9606
1089-7690
URL الوصول: https://explore.openaire.eu/search/publication?articleId=doi_dedup___::d5fb1d1907d45ae8e09d533da5a3fd07
http://hdl.handle.net/1942/39986
حقوق: OPEN
رقم الأكسشن: edsair.doi.dedup.....d5fb1d1907d45ae8e09d533da5a3fd07
قاعدة البيانات: OpenAIRE
الوصف
تدمد:00219606
10897690