TY - JOUR
T1 - High-level Ab Initio Absorption Spectra Simulations of Neutral, Anionic and Neutral+ Chromophore of Green Fluorescence Protein Chromophore Models in Gas Phase and Solution
AU - Georgieva, Ivelina
AU - Aquino, Adelia J.A.
AU - Trendafilova, Natasha
AU - Lischka, Hans
N1 - Funding Information:
Acknowledgements—Computer time at the Vienna Scientific Cluster (VSC), project 70376, is gratefully acknowledged. I.G. and N.T. thank the National Science Fund of the Bulgarian Ministry of Education and Science for the financial support under Grant No DH09/9.
Publisher Copyright:
© 2017 The American Society of Photobiology
PY - 2017/11/1
Y1 - 2017/11/1
N2 - Semiclassical ab initio simulations of the absorption spectra of neutral and anionic p-hydroxybenzylidene-2,3-dimethylimidazolinone (p-HBDI), a model chromophore of green fluorescent protein (GFP) and of a positively charged neutral (N+)-HBDI chromophore model, were performed in gas phase with the resolution-of-identity algebraic diagrammatic construction through second-order (RI-ADC(2)) method. The calculated absorption spectra in gas phase are composed of one band centered at 3.51 eV (HBDI), 2.50 eV (HBDI−) and 3.02 eV ((N+)-HBDI) owing to the absorption of the first 1ππ* transition. Band maxima are redshifted by ~0.1 eV with respect to the corresponding vertical energies. The COSMO-RI-ADC(2) calculations of the first vertical excitation energy of HBDI, HBDI− and (N+)-HBDI forms in polar solution including microsolvation simulate the observed solvent redshift for neutral HBDI and the solvent blueshift of the HBDI− and (N+)-HBDI forms. The state-specific solvation approach applied to TDDFT calculations reproduced the experimental solvent shifts for the three HBDI forms, demonstrating a more accurate theoretical description as compared to the linear-response TDDFT approach.
AB - Semiclassical ab initio simulations of the absorption spectra of neutral and anionic p-hydroxybenzylidene-2,3-dimethylimidazolinone (p-HBDI), a model chromophore of green fluorescent protein (GFP) and of a positively charged neutral (N+)-HBDI chromophore model, were performed in gas phase with the resolution-of-identity algebraic diagrammatic construction through second-order (RI-ADC(2)) method. The calculated absorption spectra in gas phase are composed of one band centered at 3.51 eV (HBDI), 2.50 eV (HBDI−) and 3.02 eV ((N+)-HBDI) owing to the absorption of the first 1ππ* transition. Band maxima are redshifted by ~0.1 eV with respect to the corresponding vertical energies. The COSMO-RI-ADC(2) calculations of the first vertical excitation energy of HBDI, HBDI− and (N+)-HBDI forms in polar solution including microsolvation simulate the observed solvent redshift for neutral HBDI and the solvent blueshift of the HBDI− and (N+)-HBDI forms. The state-specific solvation approach applied to TDDFT calculations reproduced the experimental solvent shifts for the three HBDI forms, demonstrating a more accurate theoretical description as compared to the linear-response TDDFT approach.
UR - http://www.scopus.com/inward/record.url?scp=85021326927&partnerID=8YFLogxK
U2 - 10.1111/php.12778
DO - 10.1111/php.12778
M3 - Article
C2 - 28436037
AN - SCOPUS:85021326927
VL - 93
SP - 1356
EP - 1367
JO - Photochemistry and Photobiology
JF - Photochemistry and Photobiology
SN - 0031-8655
IS - 6
ER -