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.
| Originalsprog | Engelsk |
|---|---|
| Tidsskrift | Journal of Chemical Theory and Computation |
| Vol/bind | 14 |
| Udgave nummer | 12 |
| Sider (fra-til) | 6391-6404 |
| ISSN | 1549-9618 |
| DOI | |
| Status | Udgivet - 2018 |
Fingeraftryk
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Modeling of Magnetic Circular Dichroism and UV/Vis Absorption Spectra Using Fluctuating Charges or Polarizable Embedding within a Resonant-Convergent Response Theory Formalism. / Reinholdt, Peter; Nørby, Morten S.; Kongsted, Jacob.
I: Journal of Chemical Theory and Computation, Bind 14, Nr. 12, 2018, s. 6391-6404.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › peer review
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
IS - 12
ER -