Visible Light Absorption of N-Doped TiO2 Rutile Using (LR/RT)-TDDFT and Active Space EOMCCSD Calculations
We have performed detailed ground and excited state calculations of pure and N-doped TiO2 rutile to model and analyze the experimentally observed UV/Vis spectrum. Using our embedding model we have performed both linear-response (LR) and real-time (RT) TDDFT calculations of the excited states of the pure and N-doped systems. We have also studied the lowest excitations using high-level active space equation-of-motion coupled cluster (EOMCC) approaches involving all single and inter-band double excitations. We compare and contrast the nature of the excitations in detail for the pure and doped systems and also provide an analysis of the excited-state density using our RT-TDDFT calculations. Our calculations indicate a lowering of the band gap and verify the role of the N3- states on the observed spectrum of N-doped TiO2 rutile as suggested by experimental findings. Both RT-TDDFT and EOMCC calculations show that the excitations in pure TiO2 are more delocalized compared with the N-doped system.
- Research Organization:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 1030451
- Report Number(s):
- PNNL-SA-82229; 42591; KP1704020; TRN: US201124%%212
- Journal Information:
- The Journal of Physical Chemistry Letters, Vol. 2, Issue 21
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
ABSORPTION
EXCITED STATES
RUTILE
calculations
TiO2
TDDFT
equation-of-motion coupled cluster
RT-TDDFT
coupled-cluster method
density-functional theory
excited electronic states
excitation-energies
titanium-dioxide
TIO2(110)
photocatalysis
molecules
surfaces
single
Environmental Molecular Sciences Laboratory