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An electric field suffers a discontinuity at a surface charge. Similarly, a magnetic field is discontinuous at a surface current. The perpendicular component of a magnetic field is continuous across the interface of two magnetic mediums. In contrast, its parallel component, perpendicular to the current, is discontinuous by the amount equal to the product of the vacuum permeability and the surface current. Like the scalar potential in electrostatics, the vector potential is also continuous...
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Real-time time-dependent self-consistent field methods with dynamic magnetic fields.

Meilani Wibowo-Teale1, Benjamin J Ennifer1, Andrew M Wibowo-Teale1,2

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This study introduces a new computational method for studying electron behavior in dynamic magnetic fields. The approach accurately models molecular responses, proving effective even with modest basis sets.

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Area of Science:

  • Computational Chemistry
  • Quantum Dynamics
  • Theoretical Physics

Background:

  • Accurate simulation of molecular systems in time-dependent magnetic fields is crucial for understanding electron dynamics.
  • Existing methods often face challenges with basis set convergence and computational cost.

Purpose of the Study:

  • To present the first finite basis set implementation of the real-time time-dependent self-consistent field (RT-TDSCF) method using London atomic orbitals (LAOs) in dynamic magnetic fields.
  • To benchmark the accuracy of this new implementation against literature data for model systems.
  • To assess the suitability of compact LAO basis sets for such calculations.

Main Methods:

  • Real-time time-dependent self-consistent field (RT-TDSCF) method.
  • Implementation using London atomic orbitals (LAOs) in a finite basis set.
  • Benchmarking against literature results for hydrogen atom and H2 molecule in oscillating magnetic fields.

Main Results:

  • The LAO-based RT-TDSCF method accurately reproduces electron dynamics and spectral properties for hydrogen atom and H2.
  • Modest, compact LAO basis sets are sufficient for accurate calculations in strong, dynamic magnetic fields.
  • The method correctly captures time evolution of orbital occupations and coherent emission spectra.
  • The implementation demonstrates flexibility in handling varying molecular orientations relative to the magnetic field.

Conclusions:

  • The developed LAO-based RT-TDSCF method is a robust and accurate tool for studying systems in extreme dynamic magnetic fields.
  • This approach provides a reliable method for selecting appropriate basis sets for future theoretical investigations.
  • The study highlights the utility of LAO-based calculations for a range of dynamic magnetic field scenarios.