High-level theoretical benchmark investigations of the UV-vis absorption spectra of paradigmatic polycyclic aromatic hydrocarbons as models for graphene quantum dots

Result code in IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388963%3A_____%2F19%3A00504187" target="_blank" >RIV/61388963:_____/19:00504187 - isvavai.cz</a>

Alternative codes found

RIV/61989592:15310/19:73597972

Result on the web

<a href="https://aip.scitation.org/doi/10.1063/1.5086760" target="_blank" >https://aip.scitation.org/doi/10.1063/1.5086760</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1063/1.5086760" target="_blank" >10.1063/1.5086760</a>

Result language

angličtina

Original language name

High-level theoretical benchmark investigations of the UV-vis absorption spectra of paradigmatic polycyclic aromatic hydrocarbons as models for graphene quantum dots

Original language description

Five paradigmatic polycyclic aromatic hydrocarbons (PAHs) (pyrene, circum-1-pyrene, coronene, circum-1-coronene, and circum-2coronene) are used for studying the performance of three single-reference methods {scaled opposite-spin-algebraic diagrammatic construction to second-order [SOS-ADC(2)], time-dependent (TD)-B3LYP, and TD-Coulomb-attenuating method (CAM)-B3LYP} and three multireference (MR) methods [density functional theory/multireference configuration interaction (DFT/MRCI), strongly contracted-nelectron valence state perturbation theory to second order (NEVPT2), and spectroscopy oriented configuration interaction (SORCI)]. The performance of these methods was evaluated by comparison of the calculated vertical excitation energies with experiments, where available. DFT/MRCI performs best and thus was used as a benchmark for other approaches where experimental values were not available. Both TD-B3LYP and NEVPT2 agree well with the benchmark data. SORCI performs better for coronene than for pyrene. SOS-ADC(2) does reasonably well in terms of excitation energies for smaller systems, but the error increases somewhat as the size of the system gets bigger. The natural transition orbital analysis for SOS-ADC(2) results indicated that at least two configurations were essential to characterize most of the lower-case electronic states. TD-CAM-B3LYP gives the largest errors for excitation energies and also gives an incorrect order of the lowest two states in circum-1-pyrene. A strong density increase of dark states was observed in the UV spectra with increasing size except for the lowest few states which remained well separated. An extrapolation of the UV spectra to infinite PAH size for S-1, S-2, and the first bright state based on the coronene series was made. The extrapolated excitation energies closest to experimental measurements on graphene quantum dots were obtained by TD-CAM-B3LYP.

Czech name

—

Czech description

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Type

J_imp - Article in a specialist periodical, which is included in the Web of Science database

CEP classification

—

OECD FORD branch

10403 - Physical chemistry

Project

<a href="/en/project/GA16-16959S" target="_blank" >GA16-16959S: Theoretical Description of the Excited states of Covalently and Non-covalently Functionalized Graphenes</a><br>

Continuities

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Publication year

2019

Confidentiality

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Name of the periodical

Journal of Chemical Physics

ISSN

0021-9606

e-ISSN

—

Volume of the periodical

150

Issue of the periodical within the volume

12

Country of publishing house

US - UNITED STATES

Number of pages

13

Pages from-to

124302

UT code for WoS article

000462914300017

EID of the result in the Scopus database

2-s2.0-85063431257