Understanding X-ray absorption in liquid water using triple excitations in multilevel coupled cluster theory.
Journal
Nature communications
ISSN: 2041-1723
Titre abrégé: Nat Commun
Pays: England
ID NLM: 101528555
Informations de publication
Date de publication:
26 Apr 2024
26 Apr 2024
Historique:
received:
04
08
2023
accepted:
03
04
2024
medline:
27
4
2024
pubmed:
27
4
2024
entrez:
26
4
2024
Statut:
epublish
Résumé
X-ray absorption (XA) spectroscopy is an essential experimental tool to investigate the local structure of liquid water. Interpretation of the experiment poses a significant challenge and requires a quantitative theoretical description. High-quality theoretical XA spectra require reliable molecular dynamics simulations and accurate electronic structure calculations. Here, we present the first successful application of coupled cluster theory to model the XA spectrum of liquid water. We overcome the computational limitations on system size by employing a multilevel coupled cluster framework for large molecular systems. Excellent agreement with the experimental spectrum is achieved by including triple excitations in the wave function and using molecular structures from state-of-the-art path-integral molecular dynamics. We demonstrate that an accurate description of the electronic structure within the first solvation shell is sufficient to successfully model the XA spectrum of liquid water within the multilevel framework. Furthermore, we present a rigorous charge transfer analysis of the XA spectrum, which is reliable due to the accuracy and robustness of the electronic structure methodology. This analysis aligns with previous studies regarding the character of the prominent features of the XA spectrum of liquid water.
Identifiants
pubmed: 38670938
doi: 10.1038/s41467-024-47690-x
pii: 10.1038/s41467-024-47690-x
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
3551Subventions
Organisme : EC | EU Framework Programme for Research and Innovation H2020 | H2020 Priority Excellent Science | H2020 European Research Council (H2020 Excellent Science - European Research Council)
ID : 101020016
Organisme : Norges Forskningsråd (Research Council of Norway)
ID : 275506
Organisme : Vetenskapsrådet (Swedish Research Council)
ID : 2021-04521
Organisme : EC | EU Framework Programme for Research and Innovation H2020 | H2020 Priority Excellent Science | H2020 Marie Skłodowska-Curie Actions (H2020 Excellent Science - Marie Skłodowska-Curie Actions)
ID : 860553
Informations de copyright
© 2024. The Author(s).
Références
Guo, J.-H. et al. X-ray emission spectroscopy of hydrogen bonding and electronic structure of liquid water. Phys. Rev. Lett. 89, 137402 (2002).
pubmed: 12225062
doi: 10.1103/PhysRevLett.89.137402
Wernet, P. et al. The structure of the first coordination shell in liquid water. Science 304, 995–999 (2004).
pubmed: 15060287
doi: 10.1126/science.1096205
Fransson, T. et al. X-ray and electron spectroscopy of water. Chem. Rev. 116, 7551–7569 (2016).
pubmed: 27244473
doi: 10.1021/acs.chemrev.5b00672
Smith, J. W. & Saykally, R. J. Soft x-ray absorption spectroscopy of liquids and solutions. Chem. Rev. 117, 13909–13934 (2017).
pubmed: 29125751
doi: 10.1021/acs.chemrev.7b00213
Jordan, I. et al. Attosecond spectroscopy of liquid water. Science 369, 974–979 (2020).
pubmed: 32820124
doi: 10.1126/science.abb0979
Myneni, S. et al. Spectroscopic probing of local hydrogen-bonding structures in liquid water. J. Phys. Condens. Matter 14, L213 (2002).
doi: 10.1088/0953-8984/14/8/106
Näslund, L.-Å et al. X-ray absorption spectroscopy measurements of liquid water. J. Phys. Chem. B 109, 13835–13839 (2005).
pubmed: 16852732
doi: 10.1021/jp052046q
Gavrila, G. et al. Time-resolved X-ray absorption spectroscopy of infrared-laser-induced temperature jumps in liquid water. Appl. Phys. A 96, 11–18 (2009).
doi: 10.1007/s00339-009-5190-6
Fuchs, O. et al. Isotope and temperature effects in liquid water probed by X-ray absorption and resonant X-ray emission spectroscopy. Phys. Rev. Lett. 100, 027801 (2008).
pubmed: 18232928
doi: 10.1103/PhysRevLett.100.027801
Nilsson, A. et al. X-ray absorption spectroscopy and X-ray Raman scattering of water and ice; an experimental view. J. Electron Spectros. Relat. Phenom. 177, 99–129 (2010).
doi: 10.1016/j.elspec.2010.02.005
Cisneros, G. A. et al. Modeling molecular interactions in water: From pairwise to many-body potential energy functions. Chem. Rev. 116, 7501–7528 (2016).
pubmed: 27186804
doi: 10.1021/acs.chemrev.5b00644
Prendergast, D. & Galli, G. X-ray absorption spectra of water from first principles calculations. Phys. Rev. Lett. 96, 215502 (2006).
pubmed: 16803246
doi: 10.1103/PhysRevLett.96.215502
Iannuzzi, M. X-ray absorption spectra of hexagonal ice and liquid water by all-electron Gaussian and augmented plane wave calculations. J. Chem. Phys. 128, 204506 (2008).
pubmed: 18513031
doi: 10.1063/1.2928842
Chen, W., Wu, X. & Car, R. X-ray absorption signatures of the molecular environment in water and ice. Phys. Rev. Lett. 105, 017802 (2010).
pubmed: 20867480
doi: 10.1103/PhysRevLett.105.017802
Triguero, L., Pettersson, L. & Ågren, H. Calculations of near-edge x-ray-absorption spectra of gas-phase and chemisorbed molecules by means of density-functional and transition-potential theory. Phys. Rev. B 58, 8097 (1998).
doi: 10.1103/PhysRevB.58.8097
Leetmaa, M., Ljungberg, M. P., Lyubartsev, A., Nilsson, A. & Pettersson, L. G. M. Theoretical approximations to X-ray absorption spectroscopy of liquid water and ice. J. Electron Spectros. Relat. Phenom. 177, 135–157 (2010).
doi: 10.1016/j.elspec.2010.02.004
Fransson, T. et al. Requirements of first-principles calculations of X-ray absorption spectra of liquid water. Phys. Chem. Chem. Phys. 18, 566–583 (2016).
pubmed: 26619162
doi: 10.1039/C5CP03919C
Hetényi, B., De Angelis, F., Giannozzi, P. & Car, R. Calculation of near-edge x-ray-absorption fine structure at finite temperatures: Spectral signatures of hydrogen bond breaking in liquid water. J. Chem. Phys. 120, 8632–8637 (2004).
pubmed: 15267791
doi: 10.1063/1.1703526
Martelli, F. Properties of Water from Numerical and Experimental Perspectives (CRC Press, Taylor & Francis Group, Boca Raton, 2022).
Brancato, G., Rega, N. & Barone, V. Accurate density functional calculations of near-edge X-ray and optical absorption spectra of liquid water using nonperiodic boundary conditions: the role of self-interaction and long-range effects. Phys. Rev. Lett. 100, 107401 (2008).
pubmed: 18352228
doi: 10.1103/PhysRevLett.100.107401
Besley, N. A. & Asmuruf, F. A. Time-dependent density functional theory calculations of the spectroscopy of core electrons. Phys. Chem. Chem. Phys. 12, 12024–12039 (2010).
pubmed: 20714478
doi: 10.1039/c002207a
Besley, N. A. Density functional theory based methods for the calculation of X-ray spectroscopy. Acc. Chem. Res. 53, 1306–1315 (2020).
pubmed: 32613827
doi: 10.1021/acs.accounts.0c00171
Norman, P. & Dreuw, A. Simulating X-ray spectroscopies and calculating core-excited states of molecules. Chem. Rev. 118, 7208–7248 (2018).
pubmed: 29894157
doi: 10.1021/acs.chemrev.8b00156
Rankine, C. D. & Penfold, T. J. Progress in the theory of x-ray spectroscopy: From quantum chemistry to machine learning and ultrafast dynamics. J. Phys. Chem. A 125, 4276–4293 (2021).
pubmed: 33729774
doi: 10.1021/acs.jpca.0c11267
Bussy, A. & Hutter, J. First-principles correction scheme for linear-response time-dependent density functional theory calculations of core electronic states. J. Chem. Phys. 155, 034108 (2021).
pubmed: 34293885
doi: 10.1063/5.0058124
Besley, N. A. Equation of motion coupled cluster theory calculations of the X-ray emission spectroscopy of water. Chem. Phys. Lett. 542, 42–46 (2012).
doi: 10.1016/j.cplett.2012.05.059
Carter-Fenk, K., Cunha, L. A., Arias-Martinez, J. E. & Head-Gordon, M. Electron-affinity time-dependent density functional theory: Formalism and applications to core-excited states. J. Phys. Chem. Lett. 13, 9664–9672 (2022).
pubmed: 36215404
doi: 10.1021/acs.jpclett.2c02564
Carter-Fenk, K. & Head-Gordon, M. On the choice of reference orbitals for linear-response calculations of solution-phase K-edge X-ray absorption spectra. Phys. Chem. Chem. Phys. 24, 26170–26179 (2022).
pubmed: 36278791
doi: 10.1039/D2CP04077H
Vinson, J., Kas, J. J., Vila, F. D., Rehr, J. J. & Shirley, E. L. Theoretical optical and x-ray spectra of liquid and solid H
doi: 10.1103/PhysRevB.85.045101
Tang, F. et al. Many-body effects in the X-ray absorption spectra of liquid water. Proc. Natl Acad. Sci. 119, e2201258119 (2022).
pubmed: 35561212
doi: 10.1073/pnas.2201258119
Nakanishi, N. A general survey of the theory of the Bethe-Salpeter equation. Prog. Theor. Phys. Suppl. 43, 1–81 (1969).
doi: 10.1143/PTPS.43.1
Hedin, L. New method for calculating the one-particle Green’s function with application to the electron-gas problem. Phys. Rev. 139, A796 (1965).
doi: 10.1103/PhysRev.139.A796
Hedin, L. On correlation effects in electron spectroscopies and the GW approximation. J. Phys. Condens. Matter 11, R489 (1999).
doi: 10.1088/0953-8984/11/42/201
Reining, L. The GW approximation: content, successes and limitations. Wiley Interdiscip. Rev. Comput. Mol. Sci. 8, e1344 (2018).
doi: 10.1002/wcms.1344
Onida, G., Reining, L. & Rubio, A. Electronic excitations: density-functional versus many-body Green’s-function approaches. Rev. Mod. Phys. 74, 601 (2002).
doi: 10.1103/RevModPhys.74.601
Leng, X., Jin, F., Wei, M. & Ma, Y. GW method and Bethe–Salpeter equation for calculating electronic excitations. Wiley Interdiscip. Rev. Comput. Mol. Sci. 6, 532–550 (2016).
doi: 10.1002/wcms.1265
Vinson, J., Rehr, J., Kas, J. & Shirley, E. Bethe-Salpeter equation calculations of core excitation spectra. Phys. Rev. B 83, 115106 (2011).
doi: 10.1103/PhysRevB.83.115106
Blase, X., Duchemin, I. & Jacquemin, D. The Bethe–Salpeter equation in chemistry: relations with TD-DFT, applications and challenges. Chem. Soc. Rev. 47, 1022–1043 (2018).
pubmed: 29250615
doi: 10.1039/C7CS00049A
Helgaker, T., Jørgensen, P. & Olsen, J. Molecular electronic-structure theory (John Wiley & Sons, Chichester, 2013).
Coriani, S., Christiansen, O., Fransson, T. & Norman, P. Coupled-cluster response theory for near-edge x-ray-absorption fine structure of atoms and molecules. Phys. Rev. A 85, 022507 (2012).
doi: 10.1103/PhysRevA.85.022507
Carbone, J. P. et al. Chapter Eleven - An analysis of the performance of coupled cluster methods for K-edge core excitations and ionizations using standard basis sets. In State of The Art of Molecular Electronic Structure Computations: Correlation Methods, Basis Sets and More, Vol. 79 of Advances in Quantum Chemistry (eds Ancarani, L. U. & Hoggan, P. E.) 241–261 (Academic Press, London, 2019).
Matthews, D. A. EOM-CC methods with approximate triple excitations applied to core excitation and ionisation energies. Mol. Phys. 118, e1771448 (2020).
doi: 10.1080/00268976.2020.1771448
Coriani, S., Fransson, T., Christiansen, O. & Norman, P. Asymmetric-lanczos-chain-driven implementation of electronic resonance convergent coupled-cluster linear response theory. J. Chem. Theory Comput. 8, 1616–1628 (2012).
pubmed: 26593655
doi: 10.1021/ct200919e
Christiansen, O., Koch, H. & Jørgensen, P. The second-order approximate coupled cluster singles and doubles model CC2. Chem. Phys. Lett. 243, 409–418 (1995).
doi: 10.1016/0009-2614(95)00841-Q
List, N. H., Coriani, S., Kongsted, J. & Christiansen, O. Lanczos-driven coupled–cluster damped linear response theory for molecules in polarizable environments. J. Chem. Phys. 141, 244107 (2014).
pubmed: 25554133
doi: 10.1063/1.4903981
Sneskov, K., Schwabe, T., Kongsted, J. & Christiansen, O. The polarizable embedding coupled cluster method. J. Chem. Phys. 134, 104108 (2011).
pubmed: 21405157
doi: 10.1063/1.3560034
Coriani, S. & Koch, H. Communication: X-ray absorption spectra and core-ionization potentials within a core-valence separated coupled cluster framework. J. Chem. Phys. 143, 181103 (2015).
pubmed: 26567637
doi: 10.1063/1.4935712
Coriani, S. & Koch, H. Erratum: “Communication: X-ray absorption spectra and core-ionization potentials within a core-valence separated coupled cluster framework” [J. Chem. Phys. 143, 181103 (2015)]. J. Chem. Phys. 145, 149901 (2016).
pubmed: 27782510
doi: 10.1063/1.4964714
Cederbaum, L. S. Many-body theory of multiple core holes. Phys. Rev. A 35, 622–631 (1987).
doi: 10.1103/PhysRevA.35.622
Vaz da Cruz, V. et al. Probing Hydrogen Bond Strength in Liquid Water by Resonant Inelastic X-ray Scattering. Nat. Commun. 10, 1013 (2019).
pubmed: 30833573
doi: 10.1038/s41467-019-08979-4
Myhre, R. H., Sánches de Merás, A. M. J. & Koch, H. The extended CC2 model ECC2. Mol. Phys. 111, 1109–1118 (2013).
doi: 10.1080/00268976.2013.798435
Myhre, R. H., Sánches de Merás, A. M. J. & Koch, H. Multi-level coupled cluster theory. J. Chem. Phys. 141, 224105 (2014).
pubmed: 25494730
doi: 10.1063/1.4903195
Myhre, R. H. & Koch, H. The multilevel CC3 coupled cluster model. J. Chem. Phys. 145, 044111 (2016).
pubmed: 27475352
doi: 10.1063/1.4959373
Myhre, R. H., Coriani, S. & Koch, H. Near-Edge X-ray Absorption Fine Structure within Multilevel Coupled Cluster Theory. J. Chem. Theory Comput. 12, 2633–2643 (2016).
pubmed: 27182829
doi: 10.1021/acs.jctc.6b00216
Folkestad, S. D. & Koch, H. Multilevel CC2 and CCSD methods with correlated natural transition orbitals. J. Chem. Theory Comput. 16, 179–189 (2019).
pubmed: 31743013
doi: 10.1021/acs.jctc.9b00701
Folkestad, S. D. & Koch, H. Equation-of-motion MLCCSD and CCSD-in-HF oscillator strengths and their application to core excitations. J. Chem. Theory Comput. 16, 6869–6879 (2020).
pubmed: 32955866
doi: 10.1021/acs.jctc.0c00707
Folkestad, S. D., Kjønstad, E. F., Goletto, L. & Koch, H. Multilevel CC2 and CCSD in reduced orbital spaces: electronic excitations in large molecular systems. J. Chem. Theory Comput. 17, 714–726 (2021).
pubmed: 33417769
doi: 10.1021/acs.jctc.0c00590
Paul, A. C., Folkestad, S. D., Myhre, R. H. & Koch, H. Oscillator strengths in the framework of equation of motion multilevel CC3. J. Chem. Theory Comput. 18, 5246–5258 (2022).
pubmed: 35921447
doi: 10.1021/acs.jctc.2c00164
Folkestad, S. D. et al. eT 1.0: An open source electronic structure program with emphasis on coupled cluster and multilevel methods. J. Chem. Phys. 152, 184103 (2020).
pubmed: 32414265
doi: 10.1063/5.0004713
Høyvik, I.-M., Myhre, R. H. & Koch, H. Correlated natural transition orbitals for core excitation energies in multilevel coupled cluster models. J. Chem. Phys. 146, 144109 (2017).
pubmed: 28411605
doi: 10.1063/1.4979908
Kühne, T. D. et al. CP2K: An electronic structure and molecular dynamics software package - Quickstep: Efficient and accurate electronic structure calculations. J. Chem. Phys.152 194103 (2020).
Ceriotti, M. et al. Nuclear quantum effects in water and aqueous systems: Experiment, theory, and current challenges. Chem. Rev. 116, 7529–7550 (2016).
pubmed: 27049513
doi: 10.1021/acs.chemrev.5b00674
Thomsen, B. & Shiga, M. Nuclear quantum effects on autoionization of water isotopologs studied by ab initio path integral molecular dynamics. J. Chem. Phys. 154, 084117 (2021).
pubmed: 33639728
doi: 10.1063/5.0040791
Sun, J., Ruzsinszky, A. & Perdew, J. P. Strongly Constrained and Appropriately Normed Semilocal Density Functional. Phys. Rev. Lett. 115, 036402 (2015).
pubmed: 26230809
doi: 10.1103/PhysRevLett.115.036402
Sellberg, J. A. et al. Comparison of x-ray absorption spectra between water and ice: New ice data with low pre-edge absorption cross-section. J. Chem. Phys. 141, 034507 (2014).
pubmed: 25053326
doi: 10.1063/1.4890035
Tokushima, T. et al. High resolution X-ray emission spectroscopy of liquid water: The observation of two structural motifs. Chem. Phys. Lett. 460, 387–400 (2008).
doi: 10.1016/j.cplett.2008.04.077
Cavalleri, M., Ogasawara, H., Pettersson, L. & Nilsson, A. The interpretation of X-ray absorption spectra of water and ice. Chem. Phys. Lett. 364, 363–370 (2002).
doi: 10.1016/S0009-2614(02)00890-4
Sun, Z. et al. Electron-hole theory of the effect of quantum nuclei on the X-ray absorption spectra of liquid water. Phys. Rev. Lett. 121, 137401 (2018).
pubmed: 30312094
doi: 10.1103/PhysRevLett.121.137401
Richard, R. M. & Herbert, J. M. Time-Dependent Density-Functional Description of the 1La State in Polycyclic Aromatic Hydrocarbons: Charge-Transfer Character in Disguise? J. Chem. Theory Comput. 7, 1296–1306 (2011).
pubmed: 26610124
doi: 10.1021/ct100607w
Luzanov, A. V. & Zhikol, O. A. Electron invariants and excited state structural analysis for electronic transitions within CIS, RPA, and TDDFT models. Int. J. Quantum Chem. 110, 902–924 (2010).
doi: 10.1002/qua.22041
Plasser, F. & Lischka, H. Analysis of Excitonic and Charge Transfer Interactions from Quantum Chemical Calculations. J. Chem. Theory Comput. 8, 2777–2789 (2012).
pubmed: 26592119
doi: 10.1021/ct300307c
Plasser, F., Wormit, M. & Dreuw, A. New tools for the systematic analysis and visualization of electronic excitations. I. Formalism. J. Chem. Phys.141, 024106 (2014).
Paul, A. C., Myhre, R. H. & Koch, H. New and efficient implementation of CC3. J. Chem. Theory Comput. 17, 117–126 (2020).
pubmed: 33263255
doi: 10.1021/acs.jctc.0c00686
Kadaoluwa Pathirannahalage, S. P. et al. Systematic Comparison of the Structural and Dynamic Properties of Commonly Used Water Models for Molecular Dynamics Simulations. J. Chem. Inf. Model. 61, 4521–4536 (2021).
pubmed: 34406000
doi: 10.1021/acs.jcim.1c00794
Head-Gordon, T. & Johnson, M. E. Tetrahedral structure or chains for liquid water. Proc. Natl Acad. Sci. 103, 7973–7977 (2006).
pubmed: 16698934
doi: 10.1073/pnas.0510593103
Head-Gordon, T. & Johnson, M. E. Erratum: Tetrahedral structure or chains for liquid water. Proc. Natl Acad. Sci. 103, 16615 (2006).
doi: 10.1073/pnas.0510593103
Markland, T. E. & Ceriotti, M. Nuclear quantum effects enter the mainstream. Nat. Rev. Chem. 2, 0109 (2018).
doi: 10.1038/s41570-017-0109
Chen, W., Ambrosio, F., Miceli, G. & Pasquarello, A. Ab initio electronic structure of liquid water. Phys. Rev. Lett. 117, 186401 (2016).
pubmed: 27835004
doi: 10.1103/PhysRevLett.117.186401
Kapil, V. et al. i-PI 2.0: A universal force engine for advanced molecular simulations. Comput. Phys. Commun. 236, 214–223 (2019).
doi: 10.1016/j.cpc.2018.09.020
Habershon, S., Manolopoulos, D. E., Markland, T. E. & Miller III, T. F. Ring-Polymer Molecular Dynamics: Quantum Effects in Chemical Dynamics from Classical Trajectories in an Extended Phase Space. Annu. Rev. Phys. Chem. 64, 387 (2012).
doi: 10.1146/annurev-physchem-040412-110122
Herrero, C., Pauletti, M., Tocci, G., Iannuzzi, M. & Joly, L. Connection between water’s dynamical and structural properties: Insights from ab initio simulations. Proc. Natl Acad. Sci. 119, e2121641119 (2022).
pubmed: 35588447
doi: 10.1073/pnas.2121641119
Bussy, A. & Hutter, J. Efficient and low-scaling linear-response time-dependent density functional theory implementation for core-level spectroscopy of large and periodic systems. Phys. Chem. Chem. Phys. 23, 4736–4746 (2021).
pubmed: 33598668
doi: 10.1039/D0CP06164F
Koch, H., Christiansen, O., Jørgensen, P., Sanchez de Merás, A. M. & Helgaker, T. The CC3 model: An iterative coupled cluster approach including connected triples. J. Chem. Phys. 106, 1808–1818 (1997).
doi: 10.1063/1.473322
Dunning, J. & Thom, H. Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen. J. Chem. Phys. 90, 1007–1023 (1989).
doi: 10.1063/1.456153
Kendall, R. A., Dunning, J., Thom, H. & Harrison, R. J. Electron affinities of the first-row atoms revisited. Systematic basis sets and wave functions. J. Chem. Phys. 96, 6796–6806 (1992).
doi: 10.1063/1.462569
Paul, A. C., Folkestad, S. D. & Paul, R. eT code for MLCC3 and charge transfer number calculations used in “Understanding X-ray absorption in liquid water using triple excitations in multilevel coupled cluster theory". Zenodo, https://doi.org/10.5281/zenodo.10837580 (2024).
Rohatgi, A. Webplotdigitizer: Version 4.6. https://automeris.io/WebPlotDigitizer (2022). Accessed May 30, 2022.
Pulay, P. Localizability of dynamic electron correlation. Chem. Phys. Lett. 100, 151–154 (1983).
doi: 10.1016/0009-2614(83)80703-9
Sæbø, S. & Pulay, P. Local treatment of electron correlation. Annu. Rev. Phys. Chem. 44, 213–236 (1993).
doi: 10.1146/annurev.pc.44.100193.001241