TY - JOUR

T1 - Расчет спектров поглощения комплексов серебра с тиолятами

AU - Buglak, A. A.

AU - Pomogaev, V. A.

AU - Kononov, A. I.

N1 - Publisher Copyright: © 2019 Andrey A. Buglak, Vladimir A. Pomogaev, Alexei I. Kononov

PY - 2019

Y1 - 2019

N2 - Ligand protected metal nanoclusters (NCs) have gained much attention due to their unique physico-chemical properties and potential applications in material science. Noble metal NCs protected with thiolate ligands have been of interest because of their long-term stability. The detailed structures of most of the ligand-stabilized metal NCs remain unknown due to the absence of crystal structure data for them. Theoretical calculations using quantum chemistry techniques appear as one of the most promising tools for determining the structure and electronic properties of NCs. That is why finding a cost-effective strategy for calculations is such an important and challenging task. In this work, we compare the performance of different theoretical methods of geometry optimization and absorption spectra calculation for silver-thiolate complexes. We show that second order Moller-Plesset perturbation theory reproduces nicely the geometries obtained at a higher level of theory, in particular, with RI-CC2 method. We compare the absorption spectra of silver-thiolate complexes simulated with different methods: EOM-CCSD, RI-CC2, ADC(2) and TDDFT. We show that the absorption spectra calculated with the ADC(2) method are consistent with the spectra obtained with the EOM-CCSD and RI-CC2 methods. CAM-B3LYP functional fails to reproduce the absorption spectra of the silver-thiolate complexes. However, M062X global hybrid meta-GGA functional seems to be a nice compromise regarding its low computational costs. In our previous study, we have already demonstrated that M062X functional shows good accuracy as compared to ADC(2) ab initio method predicting the excitation spectra of silver nanocluster complexes with nucleobases.

AB - Ligand protected metal nanoclusters (NCs) have gained much attention due to their unique physico-chemical properties and potential applications in material science. Noble metal NCs protected with thiolate ligands have been of interest because of their long-term stability. The detailed structures of most of the ligand-stabilized metal NCs remain unknown due to the absence of crystal structure data for them. Theoretical calculations using quantum chemistry techniques appear as one of the most promising tools for determining the structure and electronic properties of NCs. That is why finding a cost-effective strategy for calculations is such an important and challenging task. In this work, we compare the performance of different theoretical methods of geometry optimization and absorption spectra calculation for silver-thiolate complexes. We show that second order Moller-Plesset perturbation theory reproduces nicely the geometries obtained at a higher level of theory, in particular, with RI-CC2 method. We compare the absorption spectra of silver-thiolate complexes simulated with different methods: EOM-CCSD, RI-CC2, ADC(2) and TDDFT. We show that the absorption spectra calculated with the ADC(2) method are consistent with the spectra obtained with the EOM-CCSD and RI-CC2 methods. CAM-B3LYP functional fails to reproduce the absorption spectra of the silver-thiolate complexes. However, M062X global hybrid meta-GGA functional seems to be a nice compromise regarding its low computational costs. In our previous study, we have already demonstrated that M062X functional shows good accuracy as compared to ADC(2) ab initio method predicting the excitation spectra of silver nanocluster complexes with nucleobases.

KW - CAM-B3LYP

KW - CC2

KW - M062X

KW - MP2

KW - Silver nanoclusters

KW - Silver-thiolate complexes

KW - TDDFT

UR - http://www.scopus.com/inward/record.url?scp=85071521055&partnerID=8YFLogxK

UR - http://www.mendeley.com/research/calculation-absorption-spectra-silverthiolate-complexes

U2 - 10.20537/2076-7633-2019-11-2-275-286

DO - 10.20537/2076-7633-2019-11-2-275-286

M3 - статья

AN - SCOPUS:85071521055

VL - 11

SP - 275

EP - 286

JO - КОМПЬЮТЕРНЫЕ ИССЛЕДОВАНИЯ И МОДЕЛИРОВАНИЕ

JF - КОМПЬЮТЕРНЫЕ ИССЛЕДОВАНИЯ И МОДЕЛИРОВАНИЕ

SN - 2076-7633

IS - 2

ER -