Time-domain quantum dynamics: Optical properties from time-dependent electronic-structure theory
Abstract
Within the field of nonlinear optics, nonlinear optical properties are defined as frequency-dependent responses. This definition emerged in the frequency domain, as lasers used in these early experiments emitted monochromatic continuous waves. This led to the development of time-dependent electronic-structure theory predominantly in the frequency domain, using perturbation-theory based response theory. However, in recent years, advances in computing power and the advent of ultrashort laser pulses have sparked interest in the time-domain for both electronic-structure theory and nonlinear optics. Time-domain electronic-structure theory provides a time-resolved description of light-matter interaction, closely mimicking experiment. Additionally, they offer the advantage of highly nonlinear responses being straightforward to implement. This thesis contributes to the field of time-domain time-dependent electronic-structure theory for the description of nonlinear optical properties by: Investigating the potential of dynamic (time-dependent) orbitals for improving the description of nonlinear optical properties, extending a hierarchy of time-domain time-dependent coupled-cluster methods to accommodate strong magnetic fields, and by developing an efficient approach for extracting higher-order response properties.List of papers
Paper I. Kristiansen, H. E., Ofstad, B. S. , Hauge, E., Aurbakken, E., Schøyen, Ø. S., Kvaal, S., & Pedersen, T. B. (2022). Linear and Nonlinear Optical Properties from TDOMP2 Theory. Journal of Chemical Theory and Computation, 18 (6), 3687–3702. DOI: 10.1021/acs.jctc.1c01309. The article is included in the thesis. Also available at: https://doi.org/10.1021/acs.jctc.1c01309 |
Paper II. Ofstad, B. S., Kristiansen, H. E., Aurbakken, E., Schøyen, Ø. S., Kvaal, S., & Pedersen, T. B. (2023). Adiabatic extraction of nonlinear optical properties from real-time time-dependent electronic-structure theory. The Journal of Chemical Physics, 158 (15), 154102. DOI: 10.1063/5.0145521. The article is included in the thesis. Also available at: https://doi.org/10.1063/5.0145521 |
Paper III. Ofstad, B. S., Wibowo-Teale, M., Kristiansen, H. E., Aurbakken, E., Kitsaras, P., Schøyen, Ø. S., Irons, T., Kvaal, S., Stopkowicz, S., Wibowo-Teale, A., & Pedersen, T. B. (2023). Magnetic Optical Activity from Real-Time Simulations. The Journal of Chemical Physics, 159, 204109 (2023). DOI: 10.1063/5.0171927. The article is included in the thesis. Also available at: https://doi.org/10.1063/5.0171927 |
Paper IV. Aurbakken, E., Ofstad, B. S., Kristiansen, H. E., Schøyen, Ø. S., Kvaal, S., Sørensen, L. K., Lindh, R., & Pedersen, T. B. (2023). Transient spectroscopy from time-dependent electronic-structure theory without multipole expansions [Manuscript submitted for publication]. To be published. The paper is not available in DUO awaiting publishing. Preprint available at arXiv: https://doi.org/10.48550/arXiv.2307.02519 |
Paper V. Ofstad, B. S., Aurbakken, E., Sigmundson, Ø. S., Kristiansen, H. E., Kvaal, S., & Pedersen, T. B. (2023). Time-dependent coupled-cluster theory. WIREs Computational Molecular Science, 13 (5) e1666. DOI: 10.1002/wcms.1666. The article is included in the thesis. Also available at: https://doi.org/10.1002/wcms.1666 |