Light-matter interactions within the Ehrenfest–Maxwell–Pauli–Kohn–Sham framework: fundamentals, implementation, and nano-optical applications
Advances In Physics 68. issue 4, 225 - 333 (2020)
Light-matter interactions within the Ehrenfest–Maxwell–Pauli–Kohn–Sham framework: fundamentals, implementation, and nano-optical applications
In recent years significant experimental advances in nano-scale fabrication techniques and in available light sources have opened the possibility to study a vast set of novel light-matter interaction scenarios, including strong coupling cases. In many situations nowadays,classical electromagnetic modeling is insufficient as quantum effects, both in matter and light,start to play an important role. Instead, a fully self-consistent and microscopic coupling of light and matter becomes necessary. We provide here a critical review of current approaches for electromagnetic modeling, highlighting their limitations. We show how to overcome these limitations by introducing the theoretical foundations and the implementation details of a density-functional approach for coupled photons, electrons, and effective nuclei in nonrelativistic quantum electrodynamics. Starting point of the formalism is a generalization of the Pauli–Fierz field theory for which we establish a one-to-one correspondence between external fields and internal variables. Based on this correspondence, we introduce a Kohn-Sham construction which provides a computationally feasible approach for ab-initio light-matter interactions. In the mean-field limit, the formalism reduces to coupled Ehrenfest–Maxwell–Pauli–Kohn–Sham equations. We present an implementation of the approach in the real-space real-time code Octopus using the Riemann–Silberstein formulation of classical electrodynamics to rewrite Maxwell’s equations in Schrödinger form. This allows us to use existing very efficient time-evolution algorithms developed for quantum-mechanical systems also for Maxwell’s equations. We show how to couple the time-evolution of the electromagnetic fields self-consistently with the quantum time-evolution of the electrons and nuclei. This approach is ideally suited for applications in nano-optics, nano-plasmonics, (photo) electrocatalysis, lightmatter coupling in 2D materials, cases where laser pulses carry orbital angular momentum, or light-tailored chemical reactions in optical cavities just to name but a few.
Additional Information
- Download
- Preprint - 5.78 MB
- Doi
- http://dx.doi.org/https://doi.org/10.1080/00018732.2019.1695875
- Notes
- This work was supported by the European Research Council [grant number ERC-2015- AdG694097], the Cluster of Excellence – Advanced Imaging of Matter’ (AIM), Grupos Consolidados [grant number IT1249-19], SFB925 Light induced dynamics and control of correlated quantum systems’ and partially by Federal Ministry of Education and Research Grant RouTe-13N14839. The Flatiron Institute is a division of the Simons Foundation.
Related Projects
- Center for Computational Quantum Physics (CCQ), The Flatiron Institute, New York
- Cluster of Excellence
- MPSD-Max-Planck Hamburg