Multilevel coupled cluster theory: Development, implementation and application of multilevel coupled cluster theory for core and valence excited states
Doctoral thesis
Permanent lenke
http://hdl.handle.net/11250/2416154Utgivelsesdato
2016Metadata
Vis full innførselSamlinger
- Institutt for kjemi [1353]
Sammendrag
This thesis consist of seven papers and an introduction describing the ongoing
development and applications of multilevel coupled cluster theory. Coupled cluster
theory is one of the most accurate, but also one of the most computationally
demanding methods currently available in electronic structure theory. Multilevel
coupled cluster theory can greatly reduce the cost by treating only a part of the
molecule with a high level theory and the rest more approximately.
X-ray spectroscopy involving core excitations is becoming increasingly important
in chemical investigations. Modelling core excitations is challenging and require
high level methods. This thesis demonstrates how coupled cluster models can be
combined with novel experimental techniques to follow the evolution of excited
states in thymine.
Core excitations are highly local, being dominated by a single core electron. This
makes them well suited for the multilevel coupled cluster approach. The method
can be combined with a new type of orbitals, generated specifically for the excitation
being investigated. We achieved almost two orders of magnitude reductions in
computational cost with this approach.
Består av
Paper A: Myhre, Rolf Heilemann; de Merás, Alfredo Sánchez; Koch, Henrik. The extended CC2 model ECC2. Molecular Physics 2013 ;Volum 111.(9-11) s. 1109-1118Paper B: Myhre, Rolf Heilemann; Sanchez De Meras, Alfredo M J; Koch, Henrik. Multi-level coupled cluster theory. Journal of Chemical Physics 2014 ;Volum 141.(22)
Paper C: Paper C: Myhre,Rolf Heilemann; Koch, Henrik. The multilevel CC3 coupled cluster model The Journal of Chemical Physics 145, 044111 (2016); http://dx.doi.org/10.1063/1.4959373
Paper D: Myhre, Rolf Heilemann;Coriani, Sonia;Koch, Henrik. Near-Edge X-ray Absorption Fine Structure within Multilevel Coupled Cluster Theory. Journal of Chemical Theory and Computation 2016 12 (6), 2633-2643 DOI: 10.1021/acs.jctc.6b00216
Paper E: Myhre,Rolf Heilemann; Coriani,Sonia; Koch, Henrik. Core-level and UV spectra of glycine within Coupled Cluster Linear Response theory
Paper F: Myhre,Rolf Heilemann;Wolf,Thomas J. A.; Coriani, Sonia;Gühr,Markus; Koch,Henrik. A theoretical and experimental benchmark study of core excited states in N2
Paper G: Thomas J. A.;Myhre,Rolf Heilemann; Cryan,James P.; Coriani, Sonia; Squibb,Richard; The Thymine Collaboration; Koch,Henrik; Gühr,Markus. Probing ultrafast ππ∗/nπ∗ internal conversion in organic chromophores via K-edge resonant absorption - Final published version in Nature Communications 8, Article number: 29 (2017) http://dx.doi.org/10.1038/s41467-017-00069-7 This article is licensed under a Creative Commons Attribution 4.0