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  1. AU="Aquilante, Francesco"
  2. AU="Dillon, Robert C"
  3. AU="Yuan Qu"
  4. AU="Dufour, A"
  5. AU="Hannus, Jill"
  6. AU="Rieber, Julia"
  7. AU="Gulmuradov, Tashpulat"
  8. AU="Romeu Fontanillas, Teresa"
  9. AU="Fleming, Renée"
  10. AU="Cao, Fang"
  11. AU="Sally J L Moore"
  12. AU="Moreno, Yolanda"
  13. AU="Vasiliy Ya. Kolyuchkin"

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  1. Artikel ; Online: A Multiconfigurational Wave Function Implementation of the Frenkel Exciton Model for Molecular Aggregates.

    Kaiser, Andy / Daoud, Razan E / Aquilante, Francesco / Kühn, Oliver / De Vico, Luca / Bokarev, Sergey I

    Journal of chemical theory and computation

    2023  Band 19, Heft 10, Seite(n) 2918–2928

    Abstract: We present an implementation of the Frenkel exciton model into the OpenMolcas program package enabling calculations of collective electronic excited states of molecular aggregates based on a multiconfigurational wave function description of the ... ...

    Abstract We present an implementation of the Frenkel exciton model into the OpenMolcas program package enabling calculations of collective electronic excited states of molecular aggregates based on a multiconfigurational wave function description of the individual monomers. The computational protocol avoids using diabatization schemes and, thus, supermolecule calculations. Additionally, the use of the Cholesky decomposition of the two-electron integrals entering pair interactions enhances the efficiency of the computational scheme. The application of the method is exemplified for two test systems, that is, a formaldehyde oxime and a bacteriochlorophyll-like dimer. For the sake of comparison with the dipole approximation, we restrict our considerations to situations where intermonomer exchange can be neglected. The protocol is expected to be beneficial for aggregates composed of molecules with extended π systems, unpaired electrons such as radicals or transition metal centers, where it should outperform widely used methods based on time-dependent density functional theory.
    Sprache Englisch
    Erscheinungsdatum 2023-04-28
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ISSN 1549-9626
    ISSN (online) 1549-9626
    DOI 10.1021/acs.jctc.3c00185
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  2. Buch ; Online: Accurate electronic properties and intercalation voltages of olivine-type Li-ion cathode materials from extended Hubbard functionals

    Timrov, Iurii / Aquilante, Francesco / Cococcioni, Matteo / Marzari, Nicola

    2022  

    Abstract: The design of novel cathode materials for Li-ion batteries would greatly benefit from accurate first-principles predictions of structural, electronic, and magnetic properties as well as intercalation voltages in compounds containing transition-metal ... ...

    Abstract The design of novel cathode materials for Li-ion batteries would greatly benefit from accurate first-principles predictions of structural, electronic, and magnetic properties as well as intercalation voltages in compounds containing transition-metal elements. For such systems, density-functional theory (DFT) with standard (semi-)local exchange-correlation functionals is of limited use as it often fails due to strong self-interaction errors that are especially relevant in the partially filled $d$ shells. Here, we perform a detailed comparative study of the phospho-olivine cathode materials Li$_x$MnPO$_4$, Li$_x$FePO$_4$, and the mixed transition metal Li$_x$Mn$_{1/2}$Fe$_{1/2}$PO$_4$ ($x=0, 1/4, 1/2, 3/4, 1$) using four electronic-structure methods: DFT, DFT+$U$, DFT+$U$+$V$, and HSE06. We show that DFT+$U$+$V$, with onsite $U$ and intersite $V$ Hubbard parameters determined from first principles and self-consistently with respect to the structural parameters by means of density-functional perturbation theory (linear response), provides the most accurate description of the electronic structure of these challenging compounds. In particular, we demonstrate that DFT+$U$+$V$ displays very clearly "digital" changes in oxidation states of the transition-metal ions in all compounds, including the mixed-valence phases occurring at intermediate Li concentrations, leading to voltages in remarkable agreement with experiments. We show that the inclusion of intersite Hubbard interactions is essential for the accurate prediction of thermodynamic quantities, balancing the drive for localization induced by the onsite $U$ with intersite $V$ orbital hybridizations.
    Schlagwörter Condensed Matter - Materials Science
    Thema/Rubrik (Code) 540
    Erscheinungsdatum 2022-03-29
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    Dokumenttyp Buch ; Online
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  3. Artikel ; Online: Characterizing Conical Intersections in DNA/RNA Nucleobases with Multiconfigurational Wave Functions of Varying Active Space Size.

    Cuéllar-Zuquin, Juliana / Pepino, Ana Julieta / Fdez Galván, Ignacio / Rivalta, Ivan / Aquilante, Francesco / Garavelli, Marco / Lindh, Roland / Segarra-Martí, Javier

    Journal of chemical theory and computation

    2023  Band 19, Heft 22, Seite(n) 8258–8272

    Abstract: We characterize the photochemically relevant conical intersections between the lowest-lying accessible electronic excited states of the different DNA/RNA nucleobases using Cholesky decomposition-based complete active space self-consistent field (CASSCF) ... ...

    Abstract We characterize the photochemically relevant conical intersections between the lowest-lying accessible electronic excited states of the different DNA/RNA nucleobases using Cholesky decomposition-based complete active space self-consistent field (CASSCF) algorithms. We benchmark two different basis set contractions and several active spaces for each nucleobase and conical intersection type, measuring for the first time how active space size affects conical intersection topographies in these systems and the potential implications these may have toward their description of photoinduced phenomena. Our results show that conical intersection topographies are highly sensitive to the electron correlation included in the model: by changing the amount (and type) of correlated orbitals, conical intersection topographies vastly change, and the changes observed do not follow any converging pattern toward the topographies obtained with the largest and most correlated active spaces. Comparison across systems shows analogous topographies for almost all intersections mediating population transfer to the dark
    Mesh-Begriff(e) DNA ; Photochemistry ; Electrons
    Chemische Substanzen DNA (9007-49-2)
    Sprache Englisch
    Erscheinungsdatum 2023-10-26
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ISSN 1549-9626
    ISSN (online) 1549-9626
    DOI 10.1021/acs.jctc.3c00577
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  4. Buch ; Online: Pulay forces in density-functional theory with extended Hubbard functionals

    Timrov, Iurii / Aquilante, Francesco / Binci, Luca / Cococcioni, Matteo / Marzari, Nicola

    From nonorthogonalized to orthogonalized manifolds

    2020  

    Abstract: We present a derivation of the exact expression for Pulay forces in density-functional theory calculations augmented with extended Hubbard functionals, and arising from the use of orthogonalized atomic orbitals as projectors for the Hubbard manifold. The ...

    Abstract We present a derivation of the exact expression for Pulay forces in density-functional theory calculations augmented with extended Hubbard functionals, and arising from the use of orthogonalized atomic orbitals as projectors for the Hubbard manifold. The derivative of the inverse square root of the orbital overlap matrix is obtained as a closed-form solution of the associated Lyapunov (Sylvester) equation. The expression for the resulting contribution to the forces is presented in the framework of ultrasoft pseudopotentials and the projector-augmented-wave method, and using a plane wave basis set. We have benchmarked the present implementation with respect to finite differences of total energies for the case of NiO, finding excellent agreement. Owing to the accuracy of Hubbard-corrected density-functional theory calculations - provided the Hubbard parameters are computed for the manifold under consideration - the present work paves the way for systematic studies of solid-state and molecular transition-metal and rare-earth compounds.

    Comment: 16 pages, 1 figure
    Schlagwörter Condensed Matter - Materials Science ; Condensed Matter - Strongly Correlated Electrons
    Thema/Rubrik (Code) 530 ; 541
    Erscheinungsdatum 2020-10-26
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    Dokumenttyp Buch ; Online
    Datenquelle BASE - Bielefeld Academic Search Engine (Lebenswissenschaftliche Auswahl)

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  5. Artikel ; Online: Multiconfigurational Second-Order Perturbation Theory with Frozen Natural Orbitals Extended to the Treatment of Photochemical Problems.

    Segarra-Martí, Javier / Garavelli, Marco / Aquilante, Francesco

    Journal of chemical theory and computation

    2015  Band 11, Heft 8, Seite(n) 3772–3784

    Abstract: A new flavor of the frozen natural orbital complete active space second-order perturbation theory method (FNO-CASPT2, Aquilante et al., J. Chem. Phys. 131, 034113) is proposed herein. In this new implementation, the virtual space in Cholesky ... ...

    Abstract A new flavor of the frozen natural orbital complete active space second-order perturbation theory method (FNO-CASPT2, Aquilante et al., J. Chem. Phys. 131, 034113) is proposed herein. In this new implementation, the virtual space in Cholesky decomposition-based CASPT2 computations (CD-CASPT2) is truncated by excluding those orbitals that contribute the least toward preserving a predefined value of the trace of an approximate density matrix, as that represents a measure of the amount of dynamic correlation retained in the model. In this way, the amount of correlation included is practically constant at all nuclear arrangements, thus allowing for the computation of smooth electronic states surfaces and energy gradients-essential requirements for theoretical studies in photochemistry. The method has been benchmarked for a series of relevant biochromophores for which large speed-ups have been recorded while retaining the accuracy achieved in the corresponding CD-CASPT2 calculations. Both vertical excitation energies and gradient calculations have been carried out to establish general guidelines as to how much correlation needs to be retained in the calculation for the results to be consistent with the CD-CASPT2 findings. Our results feature errors within a tenth of an eV for the most difficult cases and have been validated to be used for gradient computations where an up to 3-fold speed-up is observed depending on the size of the system and the basis set employed.
    Sprache Englisch
    Erscheinungsdatum 2015-08-11
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ISSN 1549-9626
    ISSN (online) 1549-9626
    DOI 10.1021/acs.jctc.5b00479
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  6. Artikel ; Online: Orthogonality of embedded wave functions for different states in frozen-density embedding theory.

    Zech, Alexander / Aquilante, Francesco / Wesolowski, Tomasz A

    The Journal of chemical physics

    2015  Band 143, Heft 16, Seite(n) 164106

    Abstract: Other than lowest-energy stationary embedded wave functions obtained in Frozen-Density Embedding Theory (FDET) [T. A. Wesolowski, Phys. Rev. A 77, 012504 (2008)] can be associated with electronic excited states but they can be mutually non-orthogonal. ... ...

    Abstract Other than lowest-energy stationary embedded wave functions obtained in Frozen-Density Embedding Theory (FDET) [T. A. Wesolowski, Phys. Rev. A 77, 012504 (2008)] can be associated with electronic excited states but they can be mutually non-orthogonal. Although this does not violate any physical principles--embedded wave functions are only auxiliary objects used to obtain stationary densities--working with orthogonal functions has many practical advantages. In the present work, we show numerically that excitation energies obtained using conventional FDET calculations (allowing for non-orthogonality) can be obtained using embedded wave functions which are strictly orthogonal. The used method preserves the mathematical structure of FDET and self-consistency between energy, embedded wave function, and the embedding potential (they are connected through the Euler-Lagrange equations). The orthogonality is built-in through the linearization in the embedded density of the relevant components of the total energy functional. Moreover, we show formally that the differences between the expectation values of the embedded Hamiltonian are equal to the excitation energies, which is the exact result within linearized FDET. Linearized FDET is shown to be a robust approximation for a large class of reference densities.
    Sprache Englisch
    Erscheinungsdatum 2015-10-28
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ZDB-ID 3113-6
    ISSN 1089-7690 ; 0021-9606
    ISSN (online) 1089-7690
    ISSN 0021-9606
    DOI 10.1063/1.4933372
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  7. Artikel ; Online: Self-consistency in frozen-density embedding theory based calculations.

    Aquilante, Francesco / Wesołowski, Tomasz A

    The Journal of chemical physics

    2011  Band 135, Heft 8, Seite(n) 84120

    Abstract: The bi-functional for the non-electrostatic part of the exact embedding potential of frozen-density embedding theory (FDET) depends on whether the embedded part is described by means of a real interacting many-electron system or the reference system of ... ...

    Abstract The bi-functional for the non-electrostatic part of the exact embedding potential of frozen-density embedding theory (FDET) depends on whether the embedded part is described by means of a real interacting many-electron system or the reference system of non-interacting electrons (see [Wesolowski, Phys. Rev. A. 77, 11444 (2008)]). The difference δΔF(MD)[ρ(A)]/δρ(A)(r<combining arrow>), where ΔF(MD)[ρ(A)] is the functional bound from below by the correlation functional E(c)[ρ(A)] and from above by zero. Taking into account ΔF(MD)[ρ(A)] in both the embedding potential and in energy is indispensable for assuring that all calculated quantities are self-consistent and that FDET leads to the exact energy and density in the limit of exact functionals. Since not much is known about good approximations for ΔF(MD)[ρ(A)], we examine numerically the adequacy of neglecting ΔF(MD)[ρ(A)] entirely. To this end, we analyze the significance of δΔF(MD)[ρ(A)]/δρ(A)(r<combining arrow>) in the case where the magnitude of ΔF(MD)[ρ(A)] is the largest, i.e., for Hartree-Fock wavefunction. In hydrogen bonded model systems, neglecting δΔF(MD)[ρ(A)]/δρ(A)(r<combining arrow>) in the embedding potential marginally affects the total energy (less than 5% change in the interaction energy) but results in qualitative changes in the calculated hydrogen-bonding induced shifts of the orbital energies. Based on this estimation, we conclude that neglecting δΔF(MD)[ρ(A)]/δρ(A)(r<combining arrow>) may represent a good approximation for multi-reference variational methods using adequate choice for the active space. Doing the same for single-reference perturbative methods is not recommended. Not only it leads to violation of self-consistency but might result in large effect on orbital energies. It is shown also that the errors in total energy due to neglecting δΔF(MD)[ρ(A)]/δρ(A)(r<combining arrow>) do not cancel but rather add up to the errors due to approximation for the bi-functional of the non-additive kinetic potential.
    Sprache Englisch
    Erscheinungsdatum 2011-08-28
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ZDB-ID 3113-6
    ISSN 1089-7690 ; 0021-9606
    ISSN (online) 1089-7690
    ISSN 0021-9606
    DOI 10.1063/1.3624888
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  8. Artikel ; Online: A two-scale approach to electron correlation in multiconfigurational perturbation theory.

    Farahani, Pooria / Roca-Sanjuán, Daniel / Aquilante, Francesco

    Journal of computational chemistry

    2014  Band 35, Heft 22, Seite(n) 1609–1617

    Abstract: We present a new approach for the calculation of dynamic electron correlation effects in large molecular systems using multiconfigurational second-order perturbation theory (CASPT2). The method is restricted to cases where partitioning of the molecular ... ...

    Abstract We present a new approach for the calculation of dynamic electron correlation effects in large molecular systems using multiconfigurational second-order perturbation theory (CASPT2). The method is restricted to cases where partitioning of the molecular system into an active site and an environment is meaningful. Only dynamic correlation effects derived from orbitals extending over the active site are included at the CASPT2 level of theory, whereas the correlation effects of the environment are retrieved at lower computational costs. For sufficiently large systems, the small errors introduced by this approximation are contrasted by the substantial savings in both storage and computational demands compared to the full CASPT2 calculation. Provided that static correlation effects are correctly taken into account for the whole system, the proposed scheme represent a hierarchical approach to the electron correlation problem, where two molecular scales are treated each by means of the most suitable level of theory.
    Sprache Englisch
    Erscheinungsdatum 2014-08-15
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ZDB-ID 1479181-x
    ISSN 1096-987X ; 0192-8651
    ISSN (online) 1096-987X
    ISSN 0192-8651
    DOI 10.1002/jcc.23666
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  9. Artikel ; Online: Analytical gradients of the state-average complete active space self-consistent field method with density fitting.

    Delcey, Mickaël G / Pedersen, Thomas Bondo / Aquilante, Francesco / Lindh, Roland

    The Journal of chemical physics

    2015  Band 143, Heft 4, Seite(n) 44110

    Abstract: An efficient implementation of the state-averaged complete active space self-consistent field (SA-CASSCF) gradients employing density fitting (DF) is presented. The DF allows a reduction both in scaling and prefactors of the different steps involved. The ...

    Abstract An efficient implementation of the state-averaged complete active space self-consistent field (SA-CASSCF) gradients employing density fitting (DF) is presented. The DF allows a reduction both in scaling and prefactors of the different steps involved. The performance of the algorithm is demonstrated on a set of molecules ranging up to an iron-Heme b complex which with its 79 atoms and 811 basis functions is to our knowledge the largest SA-CASSCF gradient computed. For smaller systems where the conventional code could still be used as a reference, both the linear response calculation and the gradient formation showed a clear timing reduction and the overall cost of a geometry optimization is typically reduced by more than one order of magnitude while the accuracy loss is negligible.
    Sprache Englisch
    Erscheinungsdatum 2015-07-28
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ZDB-ID 3113-6
    ISSN 1089-7690 ; 0021-9606
    ISSN (online) 1089-7690
    ISSN 0021-9606
    DOI 10.1063/1.4927228
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  10. Artikel ; Online: First time combination of frozen density embedding theory with the algebraic diagrammatic construction scheme for the polarization propagator of second order.

    Prager, Stefan / Zech, Alexander / Aquilante, Francesco / Dreuw, Andreas / Wesolowski, Tomasz A

    The Journal of chemical physics

    2016  Band 144, Heft 20, Seite(n) 204103

    Abstract: The combination of Frozen Density Embedding Theory (FDET) and the Algebraic Diagrammatic Construction (ADC) scheme for the polarization propagator for describing environmental effects on electronically excited states is presented. Two different ways of ... ...

    Abstract The combination of Frozen Density Embedding Theory (FDET) and the Algebraic Diagrammatic Construction (ADC) scheme for the polarization propagator for describing environmental effects on electronically excited states is presented. Two different ways of interfacing and expressing the so-called embedding operator are introduced. The resulting excited states are compared with supermolecular calculations of the total system at the ADC(2) level of theory. Molecular test systems were chosen to investigate molecule-environment interactions of varying strength from dispersion interaction up to multiple hydrogen bonds. The overall difference between the supermolecular and the FDE-ADC calculations in excitation energies is lower than 0.09 eV (max) and 0.032 eV in average, which is well below the intrinsic error of the ADC(2) method itself.
    Mesh-Begriff(e) Electrons ; Environment ; Hydrogen Bonding ; Models, Chemical ; Quantum Theory
    Sprache Englisch
    Erscheinungsdatum 2016-05-28
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ZDB-ID 3113-6
    ISSN 1089-7690 ; 0021-9606
    ISSN (online) 1089-7690
    ISSN 0021-9606
    DOI 10.1063/1.4948741
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