A5008159641- Advanced Chemical Physics Studies
- Spectroscopy and Quantum Chemical Studies
- Machine Learning in Materials Science
- Advanced NMR Techniques and Applications
- Porphyrin and Phthalocyanine Chemistry
- Quantum many-body systems
- Surface Chemistry and Catalysis
- Magnetism in coordination complexes
- Spectroscopy Techniques in Biomedical and Chemical Research
- Molecular Junctions and Nanostructures
- Lipid Membrane Structure and Behavior
- Gold and Silver Nanoparticles Synthesis and Applications
- Parallel Computing and Optimization Techniques
- Chemical and Physical Properties of Materials
- Molecular spectroscopy and chirality
- Advancements in Transdermal Drug Delivery
- Anodic Oxide Films and Nanostructures
- High voltage insulation and dielectric phenomena
- Copper Interconnects and Reliability
- Protein Structure and Dynamics
- Advancements in Semiconductor Devices and Circuit Design
- Perovskite Materials and Applications
- Semiconductor materials and devices
- Metal-Catalyzed Oxygenation Mechanisms
- Random Matrices and Applications
École Polytechnique Fédérale de Lausanne
2024
Czech Academy of Sciences, J. Heyrovský Institute of Physical Chemistry
2016-2023
Charles University
2013-2020
Czech Academy of Sciences, Institute of Physics
2013
In the past decade, quantum chemical version of density matrix renormalization group (DMRG) method has established itself as choice for calculations strongly correlated molecular systems. Despite its favorable scaling, it is in practice not suitable computations dynamic correlation. We present a novel accurate "post-DMRG" treatment correlation based on tailored coupled cluster (CC) theory which DMRG responsible proper description nondynamic correlation, whereas incorporated through framework...
In this article, we investigate the numerical and theoretical aspects of coupled-cluster method tailored by matrix-product states. We formal properties used method, such as energy size consistency equivalence linked unlinked formulation. The existing mathematical analysis is here elaborated in a quantum chemical framework. particular, highlight use what have defined complete active space-external space gap describing basis splitting between external part generalizing concept HOMO-LUMO gap....
MiMiC is a flexible and efficient framework for multiscale simulations in which different subsystems are treated by individual client programs. In this work, we present new interface with OpenMM to be used as an MM program demonstrate its efficiency QM/MM MD simulations. Apart from high performance, especially on GPUs, wide selection of features, highly-flexible easily-extensible program, ideal the development novel methods. Thanks open-ended design MiMiC, OpenMM-MiMiC will automatically...
We have performed a FCI-quality benchmark calculation for the tetramethyleneethane molecule in cc-pVTZ basis set employing subset of CASPT2(6,6) natural orbitals FCIQMC calculation. The results are an excellent agreement with previous large scale diffusion Monte Carlo calculations by Pozun et al. and available experimental results. Our computations verified that there is maximum on PES ground singlet state ($^1\text{A}$) $45^{\circ}$ torsional angle corresponding vertical singlet-triplet...
Active space quantum chemical methods could provide very accurate description of strongly correlated electronic systems, which is tremendous value for natural sciences. The proper choice the active crucial but a nontrivial task. In this article, we present neural network-based approach automatic selection spaces, focused on transition metal systems. training set has been formed from artificial systems composed one and various ligands, have performed density matrix renormalization group...
MiMiC is a framework for performing multiscale simulations in which loosely coupled external programs describe individual subsystems at different resolutions and levels of theory. To make it highly efficient flexible, we adopt an interoperable approach based on multiple-program multiple-data (MPMD) paradigm, serving as intermediary responsible fast data exchange interactions between the subsystems. The main goal to avoid interfering with underlying parallelization programs, including...
We present a new implementation of density matrix renormalization group based tailored coupled clusters method (TCCSD), which employs the domain-based local pair natural orbital approach (DLPNO). Compared to previous (LPNO) version method, is more accurate, offers favorable scaling, and provides consistent behavior across variety systems. On top singles doubles, we include perturbative triples correction (T), able retrieve even dynamic correlation. The methods were tested on three systems:...
Functionalization of surfaces with derivatives Buckminsterfullerene fragment molecules seems to be a promising approach toward bottom-up fabrication carbon nanotube modified electrode surfaces. The modification Cu(100) surface the buckybowl pentaindenocorannulene has been studied by means scanning tunneling microscopy, monoxide-modified noncontact atomic force time-of-flight secondary mass spectrometry, and quantum chemical calculations. Two different adsorbate modes are identified, in which...
Fe(<sc>ii</sc>)-porphyrins play an important role in many reactions, due to their closely lying spin states. We present a thorough study of Fe(<sc>ii</sc>)-porphyrin model system, which we examine how the geometrical parameters influence its state ordering.
Abstract Iron(II) phthalocyanine (FePc) is an important member of the phthalocyanines family with potential applications in fields electrocatalysis, magnetic switching, electrochemical sensing, and phototheranostics. Despite importance electronic properties FePc these applications, a reliable determination its ground‐state still challenging. Here we present combined state art computational methods experimental approaches, that is, Mössbauer spectroscopy Superconducting Quantum Interference...
MiMiC is a framework for performing multiscale simulations in which loosely coupled external programs describe individual subsystems at different resolutions and levels of theory. To make it highly efficient flexible, we adopt an interoperable approach based on multiple-program multiple-data (MPMD) paradigm, serving as intermediary responsible fast data exchange interactions between the subsystems. The main goal to avoid interfering with underlying parallelization programs, including...
We introduce a new implementation of the coupled cluster method tailored by matrix product states wave functions (DMRG-TCCSD), which employs local pair natural orbital approach (LPNO). By exploiting locality in stage calculation, we were able to remove some limitations that hindered application canonical version larger systems and/or with basis sets. assessed accuracy approximation using two systems: tetramethyleneethane (TME) and oxo-Mn(Salen). Using default cut-off parameters, recover over...
The active-space quantum chemical methods could provide very accurate description of strongly correlated electronic systems, which is tremendous value for natural sciences. proper choice the active space crucial, but a non-trivial task. In this article, we present neural network (NN) based approach automatic selection spaces, focused on transition metal systems. training set has been formed from artificial systems composed one and various ligands, have performed DMRG calculated single-site...
In this work, we present the development of a fully-polarizable KS-DFT/AMOEBA embedding scheme for delocalized basis sets such as plane-waves and real-space grids. The augmented problem electron spill-out inherent to polarizable QM/MM implementation with plane-wave is addressed periodicity MM subsystem taken into account, implemented in Tinker-HP software. We discuss software design how computational efficiency enabled through interoperable multiscale simulation framework MiMiC. validated on...
We introduce a new version of the database SC1MC (SC1MC-2022), obtained by extension recent SC1MC-2020, which includes artificial mono transition metal complexes. The involves reference data used as inputs for training machine learning models, one- and two-site entropies, mutual information at DMRG level canonical split-localised orbitals. purpose this is to obtain much possible about electronic correlation structure, could be exploited models estimate these important without significant...
Determination of the electronic ground state isolated iron(II) phthalocyanine (FePc) is still a challenging task. Previous experimental studies performed in gas phase at high temperature or crystalline assigned triplet state. Multireference CASPT2 and DMRG calculations demonstrate greater stability quintet with respect to This finding supported by Mössbauer spectroscopy magnetic measurements FePc frozen nonpolar chlorobenzene solvent, which simulates condition FePc. More information can be...