Modeling of Magnetic Circular Dichroism and UV/Vis Absorption Spectra Using Fluctuating Charges or Polarizable Embedding within a Resonant-Convergent Response Theory Formalism

Peter Reinholdt*, Morten S. Nørby, Jacob Kongsted

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Resumé

In recent years computational methods based on embedding have become of increasing popularity when the aim is to introduce environmental effects into quantum chemistry calculations of molecular properties. This is due in particular to the efficiency of such methods while still retaining a high degree of accuracy compared to full quantum chemistry treatments. In the present paper we compare two popular embedding methods - fluctuating charges (FQ) and polarizable embedding (PE) - highlighting their similar mathematical structure. Furthermore, based on a unified formulation of the two embedding methods, we present theory and implementation of these embedding methods within resonant-convergent response theory up to the level of quadratic response. A numerical comparison between FQ and PE is presented for a set of solute-solvent systems based on calculations of UV/vis and magnetic circular dichroism spectra. Overall, we find in the cases considered the FQ and PE models to perform rather similarly, especially upon introducing effects of explicit conformational sampling into the theoretical predictions.

OriginalsprogEngelsk
TidsskriftJournal of Chemical Theory and Computation
Vol/bind14
Udgave nummer12
Sider (fra-til)6391-6404
ISSN1549-9618
DOI
StatusUdgivet - 2018

Fingeraftryk

Quantum chemistry
embedding
dichroism
Absorption spectra
formalism
absorption spectra
Dichroism
Computational methods
Environmental impact
Sampling
quantum chemistry
molecular properties
retaining
Circular Dichroism
solutes
sampling
formulations
predictions

Citer dette

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title = "Modeling of Magnetic Circular Dichroism and UV/Vis Absorption Spectra Using Fluctuating Charges or Polarizable Embedding within a Resonant-Convergent Response Theory Formalism",
abstract = "In recent years computational methods based on embedding have become of increasing popularity when the aim is to introduce environmental effects into quantum chemistry calculations of molecular properties. This is due in particular to the efficiency of such methods while still retaining a high degree of accuracy compared to full quantum chemistry treatments. In the present paper we compare two popular embedding methods - fluctuating charges (FQ) and polarizable embedding (PE) - highlighting their similar mathematical structure. Furthermore, based on a unified formulation of the two embedding methods, we present theory and implementation of these embedding methods within resonant-convergent response theory up to the level of quadratic response. A numerical comparison between FQ and PE is presented for a set of solute-solvent systems based on calculations of UV/vis and magnetic circular dichroism spectra. Overall, we find in the cases considered the FQ and PE models to perform rather similarly, especially upon introducing effects of explicit conformational sampling into the theoretical predictions.",
author = "Peter Reinholdt and N{\o}rby, {Morten S.} and Jacob Kongsted",
year = "2018",
doi = "10.1021/acs.jctc.8b00660",
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pages = "6391--6404",
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TY - JOUR

T1 - Modeling of Magnetic Circular Dichroism and UV/Vis Absorption Spectra Using Fluctuating Charges or Polarizable Embedding within a Resonant-Convergent Response Theory Formalism

AU - Reinholdt, Peter

AU - Nørby, Morten S.

AU - Kongsted, Jacob

PY - 2018

Y1 - 2018

N2 - In recent years computational methods based on embedding have become of increasing popularity when the aim is to introduce environmental effects into quantum chemistry calculations of molecular properties. This is due in particular to the efficiency of such methods while still retaining a high degree of accuracy compared to full quantum chemistry treatments. In the present paper we compare two popular embedding methods - fluctuating charges (FQ) and polarizable embedding (PE) - highlighting their similar mathematical structure. Furthermore, based on a unified formulation of the two embedding methods, we present theory and implementation of these embedding methods within resonant-convergent response theory up to the level of quadratic response. A numerical comparison between FQ and PE is presented for a set of solute-solvent systems based on calculations of UV/vis and magnetic circular dichroism spectra. Overall, we find in the cases considered the FQ and PE models to perform rather similarly, especially upon introducing effects of explicit conformational sampling into the theoretical predictions.

AB - In recent years computational methods based on embedding have become of increasing popularity when the aim is to introduce environmental effects into quantum chemistry calculations of molecular properties. This is due in particular to the efficiency of such methods while still retaining a high degree of accuracy compared to full quantum chemistry treatments. In the present paper we compare two popular embedding methods - fluctuating charges (FQ) and polarizable embedding (PE) - highlighting their similar mathematical structure. Furthermore, based on a unified formulation of the two embedding methods, we present theory and implementation of these embedding methods within resonant-convergent response theory up to the level of quadratic response. A numerical comparison between FQ and PE is presented for a set of solute-solvent systems based on calculations of UV/vis and magnetic circular dichroism spectra. Overall, we find in the cases considered the FQ and PE models to perform rather similarly, especially upon introducing effects of explicit conformational sampling into the theoretical predictions.

U2 - 10.1021/acs.jctc.8b00660

DO - 10.1021/acs.jctc.8b00660

M3 - Journal article

VL - 14

SP - 6391

EP - 6404

JO - Journal of Chemical Theory and Computation

JF - Journal of Chemical Theory and Computation

SN - 1549-9618

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