Unravelling molecular interactions in uracil clusters by XPS measurements assisted by ab initio and tight-binding simulations

被引:11
作者
Mattioli, Giuseppe [1 ]
Avaldi, Lorenzo [1 ]
Bolognesi, Paola [1 ]
Bozek, John D. [2 ]
Castrovilli, Mattea C. [1 ]
Chiarinelli, Jacopo [1 ]
Domaracka, Alicja [3 ]
Indrajith, Suvasthika [3 ]
Maclot, Sylvain [4 ,5 ]
Milosavljevic, Aleksandar R. [2 ]
Nicolafrancesco, Chiara [2 ,3 ]
Nicolas, Christophe [2 ]
Rousseau, Patrick [3 ]
机构
[1] CNR, Ist Struttura Mat, Area Ric Roma 1,CP 10, Monterotondo, Italy
[2] Synchrotron SOLEIL, LOrme Merisiers, BP48, F-91192 Gif Sur Yvette, France
[3] Normandie Univ, ENSICAEN, UNICAEN, CEA,CNRS,CIMAP, F-14000 Caen, France
[4] AlbaNova Univ Ctr, Dept Appl Phys, Biomed & Xray Phys, KTH Royal Inst Technol, S-10691 Stockholm, Sweden
[5] Lund Univ, Dept Phys, POB 118, S-22100 Lund, Sweden
关键词
PHOTOELECTRON-SPECTROSCOPY; METHANOL;
D O I
10.1038/s41598-020-69947-3
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The C, N and O 1s XPS spectra of uracil clusters in the gas phase have been measured. A new bottom-up approach, which relies on computational simulations starting from the crystallographic structure of uracil, has been adopted to interpret the measured spectra. This approach sheds light on the different molecular interactions (H-bond, pi -stacking, dispersion interactions) at work in the cluster and provides a good understanding of the observed XPS chemical shifts with respect to the isolated molecule in terms of intramolecular and intermolecular screening occurring after the core-hole ionization. The proposed bottom-up approach, reasonably expensive in terms of computational resources, has been validated by finite-temperature molecular dynamics simulations of clusters composed of up to fifty molecules.
引用
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页数:6
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