Spectroscopic Determination of Key Energy Scales for the Base Hamiltonian of Chromium Trihalides

Y C Shao; B Karki; W Huang; X Feng; G Sumanasekera; J-H Guo; Y-D Chuang; B Freelon

doi:10.1021/acs.jpclett.0c03476

Spectroscopic Determination of Key Energy Scales for the Base Hamiltonian of Chromium Trihalides

J Phys Chem Lett. 2021 Jan 14;12(1):724-731. doi: 10.1021/acs.jpclett.0c03476. Epub 2021 Jan 5.

Authors

Y C Shao^{1

2}, B Karki³, W Huang^{1

4}, X Feng¹, G Sumanasekera³, J-H Guo¹, Y-D Chuang¹, B Freelon^{2

5}

Affiliations

¹ Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
² Department of Physics, University of Houston, Houston, Texas 77204, United States.
³ Department of Physics and Astronomy, University of Louisville, Louisville, Kentucky 40292, United States.
⁴ State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and InformationTechnology, Chinese Academy of Sciences, Shanghai 200050, China.
⁵ Texas Center for Superconductivity, University of Houston, Houston Texas 77204, United States.

PMID: 33400873
DOI: 10.1021/acs.jpclett.0c03476

Abstract

The van der Waals (vdW) chromium trihalides (CrX₃) exhibit field-tunable, two-dimensional magnetic orders that vary with the halogen species and the number of layers. Their magnetic ground states with proximity in energies are sensitive to the degree of ligand-metal (p-d) hybridization and relevant modulations in the Cr d-orbital interactions. We use soft X-ray absorption (XAS) and resonant inelastic X-ray scattering (RIXS) spectroscopy at Cr L-edge along with the atomic multiplet simulations to determine the key energy scales such as the crystal field 10 Dq and interorbital Coulomb interactions under different ligand metal charge transfer (LMCT) in CrX₃ (X= Cl, Br, and I). Through this systematic study, we show that our approach compared to the literature has yielded a set of more reliably determined parameters for establishing a base Hamiltonian for CrX₃.