Modern quantum chemistry with [Open]Molcas

Aquilante, Francesco; Autschbach, Jochen; Baiardi, Alberto; Battaglia, Stefano; Borin, Veniamin; Chibotaru, Liviu F.; Conti, Irene; Vico, Luca De; Delcey, Mickaël G.; Galván, Ignacio Fernández; Ferré, Nicolas; Freitag, Leon; Garavelli, Marco; Gong, Xuejun; Knecht, Stefan; Larsson, Ernst D.; Lindh, Roland; Lundberg, Marcus; Malmqvist, Per‐Åke; Nenov, Artur; Norell, Jesper; Odelius, Michael; Olivucci, Massimo; Pedersen, Thomas Bondo; Pedraza-González, Laura; Phung, Quan Manh; Pierloot, Kristine; Reiher, Markus; Schapiro, Igor; Segarra‐Martí, Javier; Segatta, Francesco; Seijo, Luis; Sen, Saumik; Sergentu, Dumitru‐Claudiu; Stein, Christopher J.; Ungur, Liviu; Vacher, Morgane; Valentini, Alessio; Veryazov, Valera

doi:10.1063/5.0004835

Cited by 378 publications

(330 citation statements)

References 195 publications

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“…Here, our focus is on multiconfigurational WF techniques labeled as multi-configurational selfconsistent field (MCSCF) methods, and the techniques emerging through the linear-response TD extension of DFT categorized as TDDFT methods. As part of this work, we demonstrate the iSPECTRON interface with the widely used OpenMolcas 13,14 and NWChem 15,16 computational chemistry programs, respectively.…”

Section: Electronic Structure Methodsmentioning

confidence: 99%

“…Here, our focus is on multi‐configurational WF techniques labeled as multi‐configurational self‐consistent field (MCSCF) methods, and the techniques emerging through the linear‐response TD extension of DFT categorized as TDDFT methods. As part of this work, we demonstrate the iSPECTRON interface with the widely used OpenMolcas 13,14 and NWChem 15,16 computational chemistry programs, respectively. MCSCF techniques, such as the complete active space self consistent field (CASSCF, and its variants, as, e.g., the restricted active space (RAS) SCF), 22–25 employed in tandem with second order perturbative corrections (CASPT2, or RASPT2), 26 represent the state‐of‐the‐art method for the computation of excited state properties in generic molecular systems. The CASSCF/CASPT2 protocol has been extensively used over the past 30 years and is widely considered the gold standard for a number of applications in photochemistry 27 .…”

Section: Methodsmentioning

confidence: 99%

“…This is particularly valuable for resolving states intermediately populated during the non‐adiabatic decay which are dark with respect to the ground state (i.e., dark or phantom states). Thus, states from the f manifold could be considered “spectator states” in the terminology of transient IR spectroscopy 14,39 …”

Section: Methodsmentioning

confidence: 99%

“…Thus, states from the f manifold could be considered "spectator states" in the terminology of transient IR spectroscopy. 14,39 Three non vanishing (under the RWA) independent third-order signals can be obtained for the three-level scheme ( Figure 2d In the SOS framework the first-and third-order response functions (Equations (3) and (5)) are expanded in terms of the system eigenstates. R (1) (t 1 ) thus becomes:…”

Section: The Linear and Nonlinear Response Functionsmentioning

confidence: 99%

“…Over the years, specialized programs that address steps (i) and (ii) have been developed by different groups and made available to the user community. For the former, various proprietary and open source packages for quantum mechanics (QM) calculations exist-Gaussian, 12 Molcas, 13,14 NWChem, 15,16 GAMESS 17 to name a fewbut none of them encompass the entire array of existing and emerging electronic structure methods. General purpose codes for simulating spectroscopy are less common, reflecting the complexity associated with system specific input parameters required to simulate the nonlinear response.…”

Section: Introductionmentioning

confidence: 99%

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iSPECTRON: A simulation interface for linear and nonlinear spectra with ab‐initio quantum chemistry software

et al. 2021

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We introduce iSPECTRON, a program that parses data from common quantum chemistry software (NWChem, OpenMolcas, Gaussian, Cobramm, etc.), produces the input files for the simulation of linear and nonlinear spectroscopy of molecules with the Spectron code, and analyzes the spectra with a broad range of tools. Vibronic spectra are expressed in term of the electronic eigenstates, obtained from quantum chemistry computations, and vibrational/bath effects are incorporated in the framework of the displaced harmonic oscillator model, where all required quantities are computed at the Franck-Condon point. The program capabilities are illustrated by simulating linear absorption, transient absorption and two dimensional electronic spectra of the pyrene molecule. Calculations at two levels of electronic structure theory, time-dependent density functional theory (with NWChem) and RASSCF/ RASPT2 (with OpenMolcas) are presented and compared where possible. The iSPECTRON program is available online at https://github.com/ispectrongit/ iSPECTRON/ and distributed open source under the terms of the Educational Community License version 2.0 (ECL 2.0).

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Section: Electronic Structure Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: The Linear and Nonlinear Response Functionsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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iSPECTRON: A simulation interface for linear and nonlinear spectra with ab‐initio quantum chemistry software

et al. 2021

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Spinristor: A Spin‐Filtering Memristor

Jaroš

Sasar

Tučková

et al. 2023

Adv Elect Materials

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In this paper, an in silico proof of concept of a spinristor is proposed and provided; a new electronic component that combines a spin-filter and a memristor in a single molecule, useful for in-memory processing. It builds on the idea of an open-shell transition metal ion enclosed within an elliptical fullerene connected to a pair of electrodes. The spin-and electronic-polarization induced by the enclosed open-shell metallic ion leads to differential rectification of the electrons at low voltages applied between the source-drain electrodes, V SD . The position of the encapsulated ion can be switched by a high V SD which leads to a change in the direction of the rectification and the spin-filtering ratio. The system can thus be used as a switching rectifier, that is, a memristor and a spin-filter; therefore, a spinristor. The effect of different linkers on the function of the proposed device is further analyzed to show that linkers reduce the overall conductivity by an order of magnitude, but improve the spin-filtering ratio. The computations suggest that nitrile and isocyanide linkers enhance the rectification, too. To the best of the authors' knowledge, spinristor has no macroscopic counterpart in electronics, so far.

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Spin‐State Control in Dysprosium(III) Metallacrown Magnets via Thioacetal Modification

Deng,

Wu,

Ruan

et al. 2024

Angewandte Chemie

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Integrating controllable spin states into single‐molecule magnets (SMMs) enables precise manipulation of magnetic interactions at a molecular level, but remains a synthetic challenge. Herein, we developed a 3d‐4f metallacrown (MC) magnet [DyNi5(quinha)5(Clsal)2(py)8](ClO4)∙4H2O (H2quinha = quinaldichydroxamic acid, HClsal = 5‐chlorosalicylaldehyde) wherein a square planar NiII is stabilized by chemical stacking. Thioacetal modification was employed via post‐synthetic ligand substitutions and yielded [DyNi5(quinha)5(Clsaldt)2(py)8](ClO4)·3H2O (HClsaldt = 4‐chloro‐2‐(1,3‐dithiolan‐2‐yl)phenol). Thanks to the additional ligations of thioacetal onto the NiII site, coordination‐induced spin state switching (CISSS) took place with spin state altering from low‐spin S = 0 to high‐spin S = 1. The synergy of CISSS effect and magnetic interactions results in distinct energy splitting and magnetic dynamics. Magnetic studies indicate prominent enhancement of reversal barrier from 57 cm−1 to 423 cm−1, along with hysteresis opening and an over 200‐fold increment in coercive field at 2 K. Ab initio calculations provide deeper insights into the exchange models and rationalize the relaxation/tunnelling pathways. These results demonstrate here provide a fire‐new perspective in modulating the magnetization relaxation via the incorporation of controllable spin states and magnetic interactions facilitated by the CISSS approach.

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Modern quantum chemistry with [Open]Molcas

Cited by 378 publications

References 195 publications

iSPECTRON: A simulation interface for linear and nonlinear spectra with ab‐initio quantum chemistry software

iSPECTRON: A simulation interface for linear and nonlinear spectra with ab‐initio quantum chemistry software

Spinristor: A Spin‐Filtering Memristor

Spin‐State Control in Dysprosium(III) Metallacrown Magnets via Thioacetal Modification

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