Real-time time-dependent electronic structure theory

5 years ago

Real-time time-dependent electronic structure theory

Joshua J. Goings, Xiaosong Li, Patrick J. Lestrange

Real-time time-dependent electronic structure theory is one of the most promising methods for investigating time-dependent molecular responses and electronic dynamics. Since its first modern use in the 1990s, it has been used to study a wide variety of spectroscopic properties and electronic responses to intense external electromagnetic fields, complex environments, and open quantum systems. It has also been used to study molecular conductance, excited state dynamics, ionization, and nonlinear optical effects. Real-time techniques describe non-perturbative responses of molecules, allowing for studies that go above and beyond the more traditional energy- or frequency-domain-based response theories. Recent progress in signal analysis, accurate treatment of environmental responses, relativistic Hamiltonians, and even quantized electromagnetic fields have opened up new avenues of research in time-dependent molecular response. After discussing the history of real-time methods, we explore some of the necessary mathematical theory behind the methods, and then survey a wide (yet incomplete) variety of applications for real-time methods. We then present some brief remarks on the future of real-time time-dependent electronic structure theory. For further resources related to this article, please visit the WIREs website. “Real-time electronic structure theory consists of computational methods that simulate the interaction of molecules with various perturbations explicitly in time. Here, the simulated interaction with a pulsed electromagnetic field can be used to study nonlinear response properties, charge and spin dynamics, as well as simulate experimental spectroscopies, such as electronic absorption spectra.”.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/wcms.1341