Abstract SERENITY [J Comput Chem . 2018;39:788–798] is an open‐source quantum chemistry software that provides extensive development platform focused on quantum‐mechanical multilevel and embedding approaches. In this study, we give overview over the developments done in Serenity since its original publication 2018. This includes efficient electronic‐structure methods for ground states such as domain‐based local pair natural orbital coupled cluster Møller–Plesset perturbation theory well...

We present a computational analysis of the spin-density asymmetry in cation radical states reaction center models from photosystem I, II, and bacteria Synechococcus elongatus, Thermococcus vulcanus, Rhodobacter sphaeroides, respectively. The recently developed frozen-density embedding (FDE)-diab methodology [J. Chem. Phys., 2018, 148, 214104] allowed us to effectively avoid overdelocalization error characteristic for standard Kohn–Sham density functional theory reliably calculate...

Subsystem density-functional theory compiles a set of features that allow for efficiently calculating properties very large open-shell radical systems such as organic crystals, proteins, or deoxyribonucleic acid stacks. It is computationally less costly than correlated ab initio wave function approaches and can pragmatically avoid the overdelocalization problem Kohn-Sham without employing hard constraints on electron-density. Additionally, subsystem calculations commonly start from isolated...

Abstract Polycyclic aromatic hydrocarbons (PAHs) are widely established as ubiquitous in the interstellar medium (ISM), but considering their prevalence harsh vacuum environments, role of ionisation formation PAH clusters is poorly understood, particularly if a chirality-dependent aggregation route considered. Here we report on photoelectron spectroscopy experiments [4]helicene performed with ultraviolet synchrotron beamline. Aggregates (up to heptamer) [4]helicene, smallest helical...

Hinge-type molecular models for electron donors in reaction centers of Photosystems I and II purple bacteria were investigated using a two-state computational approach based on frozen-density embedding (FDE). This methodology, dubbed FDE-diab, is known to avoid consequences the self-interaction error as far intermolecular phenomena are concerned, which allows prediction qualitatively correct spin densities large biomolecular systems. The calculated density distributions good agreement with...

Abstract. The electron donor in photosystem I (PSI), the chlorophyll dimer P700, is studied by photochemically induced dynamic nuclear polarization (photo-CIDNP) magic angle spinning (MAS) magnetic resonance (NMR) on selectively 13C and uniformly 15N labeled PSI core preparations (PSI-100) obtained from aquatic plant duckweed (Spirodela oligorrhiza). Light-induced signals originate isotope-labeled nuclei of cofactors involved spin-correlated radical pair forming upon light excitation....

We present a systematic benchmark of isotropic electron-paramagnetic-resonance hyperfine coupling constants calculated for radical cation and anion complexes molecules contained in the S22 test set using frozen-density embedding quasi-diabatization (FDE-diab) approach. The results are compared to those from Kohn-Sham density-functional theory embedding, employing domain-based local pair natural orbital coupled cluster singles doubles method as reference. demonstrate that our new approach...

We present a multi-state implementation of the recently developed frozen-density embedding diabatization (FDE-diab) methodology [D. G. Artiukhin and J. Neugebauer, Chem. Phys. 148, 214104 (2018)] in Serenity program. The new framework extends original approach such that any number charge-localized quasi-diabatic states can be coupled, giving an access to calculations ground excited state spin-density distributions as well excitation energies. show it is possible obtain results similar those...

We present the Serestipy software as an add-on to quantum-chemistry program Serenity. is a representational-state transfer-oriented application programming interface written in Python language enabling parallel subsystem density-functional theory calculations. introduce approximate strategies context of frozen-density embedding time-dependent make large-scale excited-state calculations feasible. Their accuracy carefully benchmarked with for model system consisting porphine rings. apply this...

We present a computational analysis of the spin-density asymmetry in cation radical states reaction center models from photosystem I, II, and bacteria Synechococcus elongatus, Thermococcus vulcanus, Rhodobacter sphaeroides, respectively. The recently developed FDE-diab methodology [J. Chem. Phys., 148 (2018), 214104] allowed us to effectively avoid overdelocalization error characteristic for standard Kohn–Sham Density Functional Theory reliably calculate distributions electronic couplings...

Hinge-type molecular models for electron donors in reaction centers of Photosystem I, II, and purple bacteria were investigated using a two-state computational approach based on Frozen-Density Embedding. This methodology, dubbed FDE-diab, is known to avoid consequences the self-interaction error as far intermolecular phenomena are concerned, which allows predict qualitatively correct spin densities large bio-molecular systems. The calculated density distributions good agreement with...

We describe the Serestipy software, which is an add-on to quantum-chemistry program Serenity. a representational-state transfer-oriented application programming interface written in Python language enabling parallel subsystem density-functional theory calculations. introduce approximate strategies context of frozen-density embedding time-dependent make large-scale excited-state calculations feasible. Their accuracy carefully benchmarked with for large assemblies porphine molecules. apply...

We present a multi-state implementation of the recently developed FDE-diab methodology [J. Chem. Phys., 148 (2018), 214104] in Serenity program. The new framework extends original approach such that any number charge-localized quasi-diabatic states can be coupled, giving an access to calculations ground and excited state spin-density distributions as well excitation energies. show it is possible obtain results similar those from correlated wave function approaches complete active space...

We present a computational analysis of the spin-density asymmetry in cation radical states reaction center models from photosystem I, II, and bacteria Synechococcus elongatus, Thermococcus vulcanus, Rhodobacter sphaeroides, respectively. The recently developed FDE-diab methodology [J. Chem. Phys., 148 (2018), 214104] allowed us to effectively avoid overdelocalization error characteristic for standard Kohn–Sham Density Functional Theory reliably calculate distributions electronic couplings...

Hinge-type molecular models for electron donors in reaction centers of Photosystem I, II, and purple bacteria were investigated using a two-state computational approach based on Frozen-Density Embedding. This methodology, dubbed FDE-diab, is known to avoid consequences the self-interaction error as far intermolecular phenomena are concerned, which allows predict qualitatively correct spin densities large bio-molecular systems. The calculated density distributions good agreement with...

Abstract. The electron donor in photosystem I, the chlorophyll dimer P700, is studied by photo-CIDNP (photochemically induced dynamic nuclear polarization) MAS (magic-angle spinning) NMR on selectively 13C and uniformly 15N labeled PSI core preparations (PSI-100) obtained from aquatic plant duckweed (Spirodela oligorrhiza). Light-induced signals originate isotope labelled nuclei of cofactors involved spin-correlated radical pair forming upon light excitation. Signals are assigned to two (Chl...

We present a computational analysis of the asymmetry in reaction center models photosystem I, II, and bacteria from Synechococcus elongatus , Thermococcus vulcanus Rhodobacter sphaeroides respectively. The recently developed FDE-diab methodology [J. Chem. Phys., 148 (2018), 214104] allowed us to effectively avoid spin-density overdelocalization error characteristic for standard Kohn–Sham Density Functional Theory reliably calculate distributions electronic couplings number molecular systems...