Analytic Gradients for Complete Active Space Pair-Density Functional Theory

Sand, Andrew M.; Hoyer, Chad E.; Sharkas, Kamal; Kidder, Katherine M.; Lindh, Roland; Truhlar, Donald G.; Gagliardi, Laura

doi:10.1021/acs.jctc.7b00967

Cited by 50 publications

(76 citation statements)

References 71 publications

(180 reference statements)

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“…The second new aspectc ould offer am ulticonfigurationalg eometry optimizer that is competitive with the standard DFT schemes, both in accuracy and speed. This can possibly be advantageousi ns ituations for which the assumption of as ingle Kohn-Sham determinant becomes arguable as in systemsw ith strongb iradicalar character.M C-pDFT analytical gradients can be used for single-state calculations [154] and when the state averaged variant is available, the methodc an in principle be tested for excited-state geometry optimizations.…”

Section: Discussionmentioning

confidence: 99%

“…This can possibly be advantageous in situations for which the assumption of a single Kohn–Sham determinant becomes arguable as in systems with strong biradicalar character. MC‐pDFT analytical gradients can be used for single‐state calculations and when the state averaged variant is available, the method can in principle be tested for excited‐state geometry optimizations.…”

Section: Discussionmentioning

confidence: 99%

See 1 more Smart Citation

Deactivation of Excited States in Transition‐Metal Complexes: Insight from Computational Chemistry

Sousa

Alías-Rodríguez

Domingo

et al. 2018

Chemistry A European J

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Investigation of the excited-state decay dynamics of transition-metal systems is a crucial step for the development of photoswitchable molecular based materials with applications in growing fields as energy conversion, data storage, or molecular devices. The photophysics of these systems is an entangled problem arising from the interplay of electronic and geometrical rearrangements that take place on a short time scale. Several factors play a role in the process: various electronic states of different spin and chemical character are involved, the system undergoes important structural variations and several nonradiative processes can occur. Computational chemistry is a useful tool to get insight into the microscopic description of the photophysics of these materials, since it provides unique information about the character of the electronic spin states involved, the energetics and time evolution of the system. In this review article, we present an overview of the state of the art methodologies available to address the several aspects that have to be incorporated to properly describe the deactivation of excited states in transition-metal complexes. The most recent developments in theoretical methods are discussed and illustrated with examples.

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Section: Discussionmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

Deactivation of Excited States in Transition‐Metal Complexes: Insight from Computational Chemistry

Sousa

Alías-Rodríguez

Domingo

et al. 2018

Chemistry A European J

View full text Add to dashboard Cite

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“…OpenMolcas includes analytical gradients for MC-PDFT when a state-specific CASSCF (SS-CASSCF) wave function is used as a reference (SS-CAS-PDFT), and these gradients enable the fast and efficient determination of equilibrium and transition state structures. 205 Because MC-PDFT is a nonvariational method, the computation of the gradient requires the construction of a Lagrangian. In general, the computation of analytical gradients can be performed at least an order of magnitude faster than the corresponding gradient calculation using a numerical finite-difference method.…”

Section: Analytical Gradients For Ss-cas-pdftmentioning

confidence: 99%

OpenMolcas: From Source Code to Insight

Galván

Vacher

Alavi

et al. 2019

J. Chem. Theory Comput.

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743

408

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In this article we describe the OpenMolcas environment and invite the computational chemistry community to collaborate. The open-source project already includes a large number of new developments realized during the transition from the commercial MOLCAS product to the open-source platform. The paper initially describes the technical details of the new software development platform. This is followed by brief presentations of many new methods, implementations, and features of the OpenMolcas program suite. These developments include novel wave function methods such as stochastic complete active space self-consistent field, density matrix renormalization group (DMRG) methods, and hybrid multiconfigurational

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“…392,409 State-specific ground-state analytical gradients for MC-PDFT have recently been reported in Ref. 410…”

Section: Multiconfigurational Dftmentioning

confidence: 99%

Multireference Approaches for Excited States of Molecules

et al. 2018

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Understanding the properties of electronically excited states is a challenging task that becomes increasingly important for numerous applications in chemistry, molecular physics, molecular biology, and materials science. A substantial impact is exerted by the fascinating progress in time-resolved spectroscopy, which leads to a strongly growing demand for theoretical methods to describe the characteristic features of excited states accurately. Whereas for electronic ground state problems of stable molecules the quantum chemical methodology is now so well developed that informed nonexperts can use it efficiently, the situation is entirely different concerning the investigation of excited states. This review is devoted to a specific class of approaches, usually denoted as multireference (MR) methods, the generality of which is needed for solving many spectroscopic or photodynamical problems. However, the understanding and proper application of these MR methods is often found to be difficult due to their complexity and their computational cost. The purpose of this review is to provide an overview of the most important facts about the different theoretical approaches available and to present by means of a collection of characteristic examples useful information, which can guide the reader in performing their own applications.

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Analytic Gradients for Complete Active Space Pair-Density Functional Theory

Cited by 50 publications

References 71 publications

Deactivation of Excited States in Transition‐Metal Complexes: Insight from Computational Chemistry

Deactivation of Excited States in Transition‐Metal Complexes: Insight from Computational Chemistry

OpenMolcas: From Source Code to Insight

Multireference Approaches for Excited States of Molecules

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