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Updated: Jan 28, 2026

Experimental Methods for Spin- and Angle-Resolved Photoemission Spectroscopy Combined with Polarization-Variable Laser
Published on: June 28, 2018
A Combined Spin-Flip and IP/EA Approach for Handling Spin and Spatial Degeneracies: Application to Double Exchange
Shannon E Houck1, Nicholas J Mayhall1
1Department of Chemistry , Virginia Tech , Blacksburg , Virginia 24060 , United States.
Abstract:
Many multiconfigurational systems, such as single-molecule magnets, are difficult to study using traditional computational methods due to the simultaneous existence of both spin and spatial degeneracies. In this work, a new approach termed n-spin-flip ionization potential/electron affinity ( nSF-IP or nSF-EA) is introduced which combines the spin-flip method of Anna Krylov with particle-number changing IP/EA methods. We demonstrate the efficacy of the approach by applying it to the strongly correlated N2+, as well as several double exchange systems. We also demonstrate that when these systems are well-described by a double exchange model Hamiltonian, only 1SF-IP/EA is required to extract the double exchange parameters and accurately predict energies for the low-spin states. This significantly reduces the computational effort for studying such systems. The effects of including additional excitations (using a RAS- nSF-IP/EA scheme) are also examined, with particular emphasis on hole and particle excitations.
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