Project B5: Multi-resolution methods including quantum chemistry, force fields, and hybrid particle-field schemes
Multiscaling techniques that involve a quantum-chemical treatment of the electronic structure for the part with the highest resolution are promising computational tools. They are particularly useful for dealing with problems involving large systems like enzymes, membranes, polymers, etc., where, for example, chemical reactions take place. Having completed in the previous funding period of the TRR (i.e., the first funding period of this project) a corresponding QM/MM implementation that allows to include high-accuracy quantum-chemical methods from either coupled-cluster (CC) theory (i.e., CCSD, CCSD(T), etc.) or of multiconfigurational nature (i.e., CASSCF), we intend to complete the envisioned QM/MM/CG/hPF implementation that extends the QM/MM approach to coarse-grained (CG) treatments. In particular, we plan on using hybrid particle-field (hPF) theory based on its Hamiltonian reformulation, where the latter has been accomplished in the first funding period of this project. This reformulation facilitates the coupling of the regimes of different resolution as well as the use of the intended QM/MM/CG/hPF scheme in molecular dynamics (MD) simulations. In order to reduce the computational cost for the QM part which is the time-determining step of QM/MM and QM/MM/CG/hPF treatments and limits their applicability when using high-accuracy quantum-chemical methods, we propose to
use Cholesky decomposition (CD) of the two-electron integrals to speed up the treatment of the QM region. We intend to implement CD based QM/MM and QM/MM/CG/hPF schemes using CD based nuclear forces to perform corresponding MD simulations. We also propose to implement CD based QM/MM and QM/MM/CG/hPF schemes for the computation of spectroscopic properties (NMR, EPR, vibrational) such that an accurate joint experimental and theoretical spectroscopic characterization of soft-matter systems (e.g., biological systems, molecules in solution or non-crystalline solids) becomes possible. In addition, we intend to extend the CD based schemes to include also those from CC and equation-of-motion CC (for the treatment of excited states) theory, and plan to develop schemes, again using CD techniques in a QM/MM or QM/MM/CG/hPF framework that allow the investigation of large systems under the influence of magnetic fields in a non-perturbative manner. Finally, the project intends to use the developed schemes in applications, in close collaboration with projects B1, B3, and B4 to simulate force-probe experiments and to investigate force fields for hydrated ions.
Self-Assembly of Unconventional Triphenylene-Based Frustrated Amphiphile in Solution
H.M. Cezar, G. Berton, T. Lorenzetto, S. Zorzi, C.J.D. Foumthuim, S.M. Szostak, P. Ballester, C. Mondelli, R. Schweins, V. Cristiglio, F. Fabris, R. Lund, A. Scarso, A. Giacometti, M. Cascella
Langmuir 42, 4507-4517 (2026)
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A Novel Implementation of CCSD Analytic Gradients Using Cholesky Decomposition of the Two-Electron Integrals and Abelian Point-Group Symmetry
Luca Melega, Tommaso Nottoli, Jürgen Gauss, Filippo Lipparini
J. Phys. Chem. A 130, 2097-2111 (2026)
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Beyond Core-Shell Micellar Structures: Complex Structures in Simple Surfactant
Henrique Musseli Cezar, Victoria Ariel Bjørnestad, Sylvain Prevost, Reidar Lund, Michele Cascella
Small structures 6, 2400553 (2025)
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Structural pores not required: Antimicrobial peptides induce ion permeabilization of lipid membranes through transient water channels
Rosenov Koynarev, V., Nader, M. L., Cezar, H. M., Narayanan, T., Porcar, L., Cascella, M., Lund, R.
Proceedings of the National Academy of Sciences of the United States of America, 122(44), e2517944122 (2025)
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Cholesky Decomposition in Spin-Free Dirac-Coulomb Coupled-Cluster Calculation
Tereza Uhlirova, Davide Cianchino, Tommaso Nottoli, Filippo Lipparini, Jürgen Gauss
J. Phys. Chem. A 128, 8292-8303 (2024)
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Cholesky Decomposition-Based Implementation of Relativistic Two-Component Coupled-Cluster Methods for Medium-Sized Molecules
Chaoqun Zhang, Filippo Lipparini, Stella Stopkowicz, Jürgen Gauss, Lan Cheng
J. Chem. Theory Comp. 20, 787-798 (2024)
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Phase coexistence in Hamiltonian hybrid particle-field theory using a multi-Gaussian approach
Samirah Sen, Henrique Musseli Cezar, Morgen Ledum, Xinmeng Li, Michele Cascella
J. Phys. Chem. B 128, 11739-11747 (2024)
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Finite-field Cholesky decomposed coupled-cluster techniques (ff-CD-CC): theory and application to pressure broadening of Mg by a He atmosphere and a strong magnetic field
Simon Blaschke, Marios-Petros Kitsaras, Stella Stopkowicz
Phys. Chem. Chem. Phys. 26, 28828-28848 (2024)
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Efficient approximate screening techniques for integrals over London atomic orbital
Simon Blaschke, Stella Stopkowicz, Ansgar Pausch
J. Chem. Phys. 161, 024117 (2024)
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Learning Force Field Parameters from Differentiable Particle-Field Molecular Dynamics
Manuel Carrer, Henrique Musseli Cezar, Sigbjørn Løland Bore, Morten Ledum, Michele Cascela
J. Chem. Inform. Modelling 64, 5510-5520 (2024)
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A DZ white dwarf with a 30 MG magnetic field}
M.A. Hollands, S. Stopkowicz, M.-P. Kitsaras, F. Hampe, S. Blaschke, J.J. Hermes
Monthly Notices of the Royal Astonomical Society 520, 3560-3575 (2023)
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Another Torture Track for Quantum Chemistry: Reinvestigation of the Benzaldehyde Amidation by Nitrogen-Atom Transfer from Platinum(II) and Palladium(II) Metallonitrenes
H. Verplancke, M. Diefenbach, J.N. Lienert, M. Ugandi, M.-P. Kitsaras, M. Röhmelt, S. Stopkowicz, M.C. Holthausen
Israel J. Chemistry 63, e292399960 (2023)
see publication
Micelle kinetics of photoswitchable surfactants: Self-assembly pathways and relaxation mechanisms
V.A. Bjørnestad, X. Li, C. Tribet, R. Lund, M. Cascella
J. Coll. Interf. Sci. 646, 883-899 (2023)
see publication
Cholesky decomposition of two-electron integrals in quantum-chemical calculations with perturbative or finite magnetic fields using gauge-including atomic orbitals
Jürgen Gauss, Simon Blaschke, Sophia Burger, Tommaso Nottoli, Filippo Lipparini, Stella Stopkowicz
Molecular Physics 121, 11-12 (2023)
see publication
HylleraasMD: A Domain Decomposition-Based Hybrid Particle-Field Software for Multiscale Simulations of Soft Matter
Morten Ledum, Samirah Sen, Xinmeng Li, Manuel Carrer, Yu Feng, Michele Cascella, Sibjørn Løland Bore
J. Chem. Theory Comp. 19, 2939-2952 (2023)
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SANS Spectra with PLUMED: Implementation and Application to Metainference
Henrique M. Cezar, Michele Cascella
J. Chem. Information Modelling 63, 4979-4985 (2023)
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Soft Matter under Pressure: Pushing Particle-Field Molecular Dynamics to the Isobaric Ensemble
Samirah Sen, Morten Ledum, Sigbjørn Løland Bore, Michele Cascella
Journal of Chemical Information and Modeling 63, 2207-2217 (2023)
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On the equivalence of the hybrid particle-field and Gaussian core models
Morten Ledum, Samirah Sen, Sigbjørn Løland Bore, Michele Cascella
J. Chem. Phys. 158, 1194902 (2023)
see publication
A novel coupled-cluster singles and doubles implementation that combines the exploitation of point-group symmetry and Cholesky decomposition of the two-electron integrals
Tommaso Nottoli, Jürgen Gauss, Filippo Lipparini
J. Chem. Phys. 159, 231101 (2023)
see publication
Computation of NMR shieldings at the CASSCF level using gauge-including atomic orbitals and Cholesky decomposition
T. Nottoli, S. Burger, S. Stopkowicz, J. Gauss, F. Lipparini
J. Chem. Phys. 157, 084122 (2022)
see publication
Wavefunction-Based Electrostatic-Embedding QM/MM Using CFOUR through MiMiC
Till Kirsch, Jógvan Magnus Haugaard Olsen, Viacheslav Bolnykh, Simone Meloni, Emiliano Ippoliti, Ursula Rothlisberger, Michele Cascella, Jürgen Gauss
Journal of Chemical Theory and Computation 18 (1),13-24 (2022)
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Hamiltonian and alias-free hybrid particle-field molecular dynamic
Sigbjørb Løland Bore, Michele Cascella
J. Chem. Phys. 152, 094106 (2020)
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Automated determination of hybrid particle-field parameters by machine learning
Morten Ledum, Sigbjørn Løland Bore, Michele Cascella
Molecular Physics 118 (19-20), e1785571 (2020)
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Hybrid particle-field molecular dynamics under constant pressure
Sigbjørn Løland Bore, Hima Bindu Kolli, Antonio De Nicola, Maksym Byshkin, Toshihiro Kawakatsu, Giuseppe Milano, Michele Cascella
J. Chem. Phys. 152, 184908 (2020)
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The Grignard Reaction – Unraveling a Chemical Puzzle
Raphael Mathias Peltzer, Jürgen Gauss, Odile Eisenstein, Michele Cascella
Journal of the American Chemical Society 142 (6), 2984-2994 (2020)
see publication
A fundamental catalytic difference between zinc and manganese dependent enzymes revealed in a bacterial isatin hydrolase
Theis Sommer, Kaare Bjerregaard-Andersen, Lalita Uribe, Michael Etzerodt, Gregor Diezemann, Jürgen Gauss, Michele Cascella, J. Preben Morth
Scientific Reports 8 (1), 13104 (2018)
see publication