Full minimal coupling Maxwell-TDDFT: An ab initio framework for light-matter interaction beyond the dipole approximation

作     者：Franco P. Bonafé Esra Ilke Albar Sebastian T. Ohlmann Valeriia P. Kosheleva Carlos M. Bustamante Francesco Troisi Angel Rubio Heiko Appel 

作者机构：Max Planck Institute for the Structure and Dynamics of Matter Center for Free Electron Laser Science Luruper Chaussee 149 22761 Hamburg Germany Max Planck Computing and Data Facility Gießenbachstrasse 2 85748 Garching Germany Center for Computational Quantum Physics (CCQ) The Flatiron Institute 162 Fifth Avenue New York New York 10010 USA 

出 版 物：《Physical Review B》 (Phys. Rev. B)

年 卷 期：2025年第111卷第8期

页      面：085114-085114页

核心收录：

基　　金：Max Planck-New York City Center for Non-Equilibrium Quantum Phenomena International Max Planck Research School for Environmental, Cellular and Molecular Microbiology, IMPRS-Mic European Research Council, ERC, (IT1453-22, ERC-2015-AdG694097) Horizon 2020, (895747) Deutsche Forschungsgemeinschaft, DFG, (170620586, SFB-925) 

主　　题：Light scattering 

摘      要：We report an ab initio, nonrelativistic QED method that couples light and matter self-consistently beyond the electric dipole approximation and without multipolar truncations. This method is based on an extension of the Maxwell-Pauli-Kohn-Sham approach to a full minimal coupling Hamiltonian, where the space- and time-dependent vector potential is coupled to the matter system, and its back reaction to the radiated fields is generated by the full current density. The implementation in the open-source code octopus is designed for massively parallel multiscale simulations considering different grid spacings for the Maxwell and matter subsystems. Here, we show applications of this framework to simulate renormalized Cherenkov radiation of an electronic wave packet, magneto-optical effects with nonchiral light in nonchiral molecular systems, and renormalized plasmonic modes in a nanoplasmonic dimer. We show that in some cases, the beyond-dipole effects cannot be captured by a multipolar expansion Hamiltonian in the length gauge. Finally, we discuss further opportunities enabled by the framework in the field of twisted light and orbital angular momentum, inelastic light scattering, and strong-field physics.