Optimized long-range corrected density functionals for electronic and optical properties of bare and ligated CdSe quantum dots

O. S. Bokareva, M. F. Shibl, Jaber Al Marri, T. Pullerits, O. Kühn

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

The reliable prediction of optical and fundamental gaps of finite size systems using density functional theory requires to account for the potential self-interaction error, which is notorious for degrading the description of charge transfer transitions. One solution is provided by parametrized long-range corrected functionals such as LC-BLYP, which can be tuned such as to describe certain properties of the particular system at hand. Here, bare and 3-mercaptoprotionic acid covered Cd33Se33 quantum dots are investigated using the optimally tuned LC-BLYP functional. The range separation parameter, which determines the switching on of the exact exchange contribution, is found to be 0.12 bohr-1 and 0.09 bohr-1 for the bare and covered quantum dot, respectively. It is shown that density functional optimization indeed yields optical and fundamental gaps and thus exciton binding energies, considerably different compared with standard functionals such as the popular PBE and B3LYP ones. This holds true, despite the well established fact that the leading transitions are localized on the quantum dot and do not show pronounced long-range charge transfer character.

Original languageEnglish
Pages (from-to)110-116
Number of pages7
JournalJournal of Chemical Theory and Computation
Volume13
Issue number1
DOIs
Publication statusPublished - 1 Jan 2017
Externally publishedYes

Fingerprint

functionals
Electronic properties
Semiconductor quantum dots
Optical properties
quantum dots
optical properties
Charge transfer
charge transfer
electronics
Binding energy
Excitons
Density functional theory
binding energy
excitons
density functional theory
acids
optimization
Acids
predictions
interactions

ASJC Scopus subject areas

  • Computer Science Applications
  • Physical and Theoretical Chemistry

Cite this

Optimized long-range corrected density functionals for electronic and optical properties of bare and ligated CdSe quantum dots. / Bokareva, O. S.; Shibl, M. F.; Al Marri, Jaber; Pullerits, T.; Kühn, O.

In: Journal of Chemical Theory and Computation, Vol. 13, No. 1, 01.01.2017, p. 110-116.

Research output: Contribution to journalArticle

@article{a57e6f709d8f4be4bb6e70b6924a4c02,
title = "Optimized long-range corrected density functionals for electronic and optical properties of bare and ligated CdSe quantum dots",
abstract = "The reliable prediction of optical and fundamental gaps of finite size systems using density functional theory requires to account for the potential self-interaction error, which is notorious for degrading the description of charge transfer transitions. One solution is provided by parametrized long-range corrected functionals such as LC-BLYP, which can be tuned such as to describe certain properties of the particular system at hand. Here, bare and 3-mercaptoprotionic acid covered Cd33Se33 quantum dots are investigated using the optimally tuned LC-BLYP functional. The range separation parameter, which determines the switching on of the exact exchange contribution, is found to be 0.12 bohr-1 and 0.09 bohr-1 for the bare and covered quantum dot, respectively. It is shown that density functional optimization indeed yields optical and fundamental gaps and thus exciton binding energies, considerably different compared with standard functionals such as the popular PBE and B3LYP ones. This holds true, despite the well established fact that the leading transitions are localized on the quantum dot and do not show pronounced long-range charge transfer character.",
author = "Bokareva, {O. S.} and Shibl, {M. F.} and {Al Marri}, Jaber and T. Pullerits and O. K{\"u}hn",
year = "2017",
month = "1",
day = "1",
doi = "10.1021/acs.jctc.6b01039",
language = "English",
volume = "13",
pages = "110--116",
journal = "Journal of Chemical Theory and Computation",
issn = "1549-9618",
publisher = "American Chemical Society",
number = "1",

}

TY - JOUR

T1 - Optimized long-range corrected density functionals for electronic and optical properties of bare and ligated CdSe quantum dots

AU - Bokareva, O. S.

AU - Shibl, M. F.

AU - Al Marri, Jaber

AU - Pullerits, T.

AU - Kühn, O.

PY - 2017/1/1

Y1 - 2017/1/1

N2 - The reliable prediction of optical and fundamental gaps of finite size systems using density functional theory requires to account for the potential self-interaction error, which is notorious for degrading the description of charge transfer transitions. One solution is provided by parametrized long-range corrected functionals such as LC-BLYP, which can be tuned such as to describe certain properties of the particular system at hand. Here, bare and 3-mercaptoprotionic acid covered Cd33Se33 quantum dots are investigated using the optimally tuned LC-BLYP functional. The range separation parameter, which determines the switching on of the exact exchange contribution, is found to be 0.12 bohr-1 and 0.09 bohr-1 for the bare and covered quantum dot, respectively. It is shown that density functional optimization indeed yields optical and fundamental gaps and thus exciton binding energies, considerably different compared with standard functionals such as the popular PBE and B3LYP ones. This holds true, despite the well established fact that the leading transitions are localized on the quantum dot and do not show pronounced long-range charge transfer character.

AB - The reliable prediction of optical and fundamental gaps of finite size systems using density functional theory requires to account for the potential self-interaction error, which is notorious for degrading the description of charge transfer transitions. One solution is provided by parametrized long-range corrected functionals such as LC-BLYP, which can be tuned such as to describe certain properties of the particular system at hand. Here, bare and 3-mercaptoprotionic acid covered Cd33Se33 quantum dots are investigated using the optimally tuned LC-BLYP functional. The range separation parameter, which determines the switching on of the exact exchange contribution, is found to be 0.12 bohr-1 and 0.09 bohr-1 for the bare and covered quantum dot, respectively. It is shown that density functional optimization indeed yields optical and fundamental gaps and thus exciton binding energies, considerably different compared with standard functionals such as the popular PBE and B3LYP ones. This holds true, despite the well established fact that the leading transitions are localized on the quantum dot and do not show pronounced long-range charge transfer character.

UR - http://www.scopus.com/inward/record.url?scp=85016325821&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85016325821&partnerID=8YFLogxK

U2 - 10.1021/acs.jctc.6b01039

DO - 10.1021/acs.jctc.6b01039

M3 - Article

VL - 13

SP - 110

EP - 116

JO - Journal of Chemical Theory and Computation

JF - Journal of Chemical Theory and Computation

SN - 1549-9618

IS - 1

ER -