Journal ArticleDOI
Electron excitation energies using a consistent third-order propagator approach: Comparison with full configuration interaction and coupled cluster results
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TLDR
In this article, a consistent third-order propagator method for the treatment of electronic excitation in molecules is tested in first applications and the results reflect a substantial and uniform improvement with respect to the second-order description.Abstract:
A recently developed consistent third-order propagator method for the treatment of electronic excitation in molecules is tested in first applications. The method referred to as third-order algebraic-diagrammatic construction [ADC(3)] extends the existing second-order approximation and aims at a more accurate computation of excitation energies and transition moments than afforded at the second-order level. For a stringent test of the method we compare the ADC(3) energies for over 40 singlet and triplet vertical transitions in H2O, HF, N2, and Ne with the results of recent full configuration interaction (FCI) and coupled cluster (CC) computations. The ADC(3) results reflect a substantial and uniform improvement with respect to the second-order description. The mean absolute deviation of the single excitation energies from the FCI results is below 0.2 eV. Although this does not equal the accuracy of the third-order CC3 model, the ADC(3) method, scaling as N6 with the number of orbitals, may be viewed as a good compromise between accuracy and computational cost.read more
Citations
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Single-reference ab initio methods for the calculation of excited states of large molecules.
Andreas Dreuw,Martin Head-Gordon +1 more
Journal ArticleDOI
Recent advances in wave function-based methods of molecular-property calculations.
TL;DR: Recent Advances in Wave Function-Based Methods of Molecular-Property Calculations Trygve Helgaker, Poul Jørgensen, Kasper Kristensen, Jeppe Olsen, and Kenneth Ruud.
Journal ArticleDOI
The algebraic diagrammatic construction scheme for the polarization propagator for the calculation of excited states
Andreas Dreuw,Michael Wormit +1 more
TL;DR: The algebraic diagrammatic construction (ADC) scheme for the polarization propagator provides a series of ab initio methods for the calculation of excited states based on perturbation theory.
Book ChapterDOI
Structure Optimizations for Excited States with Correlated Second-Order Methods: CC2 and ADC(2)
TL;DR: In this article, the performance of second-order methods for excitation energies CC2 and ADC(2) is investigated and compared with the more approximate CIS and CIS(D) methods as well as with the coupled-cluster models CCSD, CCSDR(3) and CC3.
Journal ArticleDOI
Quantum Mechanical Studies on the Photophysics and the Photochemistry of Nucleic Acids and Nucleobases
TL;DR: This review provides a concise, complete picture of the computational studies carried out, approximately, in the past decade on the photophysics of DNA nucleobases in the gas phase and in solution.
References
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Coupled cluster response functions
Henrik Koch,Poul Jo,rgensen +2 more
TL;DR: The linear and quadratic response functions have been determined for a coupled cluster reference state from the response functions, computationally tractable expressions have been derived for excitation energies, first and second-order matrix transition elements, transition matrix elements between excited states, and second and third-order frequency-dependent molecular properties as discussed by the authors.