The browser you are using is not supported by this website. All versions of Internet Explorer are no longer supported, either by us or Microsoft (read more here: https://www.microsoft.com/en-us/microsoft-365/windows/end-of-ie-support).

Please use a modern browser to fully experience our website, such as the newest versions of Edge, Chrome, Firefox or Safari etc.

Default user image.

Erik Donovan Hedegård

Postdoctoral fellow

Default user image.

A method to capture the large relativistic and solvent effects on the UV-vis spectra of photo-activated metal complexes

Author

  • Joel Creutzberg
  • Erik Donovan Hedegård

Summary, in English

We have recently developed a method based on relativistic time-dependent density functional theory (TD-DFT) that allows the calculation of electronic spectra in solution (Creutzberg, Hedegård, J. Chem. Theory Comput.18, 2022, 3671). This method treats the solvent explicitly with a classical, polarizable embedding (PE) description. Furthermore, it employs the complex polarization propagator (CPP) formalism which allows calculations on complexes with a dense population of electronic states (such complexes are known to be problematic for conventional TD-DFT). Here, we employ this method to investigate both the dynamic and electronic effects of the solvent for the excited electronic states of trans-trans-trans-[Pt(N3)2(OH)2(NH3)2] in aqueous solution. This complex decomposes into species harmful to cancer cells under light irradiation. Thus, understanding its photo-physical properties may lead to a more efficient method to battle cancer. We quantify the effect of the underlying structure and dynamics by classical molecular mechanics simulations, refined with a subsequent DFT or semi-empirical optimization on a cluster. Moreover, we quantify the effect of employing different methods to set up the solvated system, e.g., how sensitive the results are to the method used for the refinement, and how large a solvent shell that is required. The electronic solvent effect is always included through a PE potential.

Department/s

  • Computational Chemistry

Publishing year

2023

Language

English

Pages

6153-6163

Publication/Series

Physical Chemistry Chemical Physics

Volume

25

Issue

8

Document type

Journal article

Publisher

Royal Society of Chemistry

Topic

  • Theoretical Chemistry (including Computational Chemistry)
  • Physical Chemistry (including Surface- and Colloid Chemistry)

Status

Published

ISBN/ISSN/Other

  • ISSN: 1463-9076