Influence of Orbital Character on the Ground State Electronic Properties in the van Der Waals Transition Metal Iodides VI₃ and CrI₃

Abstract

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Large Orbital Magnetic Moment in VI3

“…Figure a shows the V L 3,2 (2p 3/2,1/2 → 3d, between 505 and 530 eV) helicity-summed XAS of VI 3 and XMCD spectra derived as σ + (ω) – σ – (ω) measured at 2 K and 5 T applied parallel to the c R -axis. The XAS spectrum agrees well with the V 3+ valence state published for V 2 O 3 and the previous XAS published for VI 3 . , For the 2 K spectrum besides the V L 3,2 absorption edges, we detected another two resonances above 530 eV which were identified as the O K absorption edge; see Figure b. The 90 K XAS measurement (see Supporting Information, Figure S2) shows an oxygen-free spectrum (Figure b shows XAS spectrum taken at 300 K as reference) measured after the low-temperature data, clearly showing that the O 2 is not intrinsic to the sample surface.…”

“…Recently an ARPES investigation has revealed a significant occupation of a 1g orbitals, in addition to e g orbitals. 34 In their work, the authors attribute that to V 2+ at the surface, although their XAS agrees with V 3+ . The argument for this proposition is based on a prediction that e g should be fully occupied at the ground state and only the existence of V 2+ could then explain the observed a 1g occupation.…”

“…Recently an ARPES investigation has revealed a significant occupation of orbitals, in addition to orbitals . In their work, the authors attribute that to V 2+ at the surface, although their XAS agrees with V 3+ .…”

Epitaxial Growth and Electronic Properties of Single- and Few-Layer FeBr2 on Bi(111)

“…Indeed, the band structures calculated for the FM or AFM states agree much better with the experimental ones than those calculated for the nonmagnetic states. Such agreement between band structures calculated for FM states and experimental ones above magnetic transition temperatures is also reported for bulk vdW ferromagnets such as VI 3 , CrI 3 , and Cr 2 Ge 2 Te 6 . − …”

Atomic structure and large magnetic anisotropy in air-sensitive layered ferromagnetic VI3

“…Furthermore, this calculated value and other reported theoretical data are larger than the reported optical measurement of the direct band gap (0.67 eV), 11,12 which may be affected by orbital characteristics and actual defects. 21,49 Moreover, a very recent theoretical work has reported that the electronic band gap of monolayer VI 3 can be tuned over a wide range of 0.34–1.98 eV via V doping, 22 rendering a future experimental study of the relationships between defects and the electronic structure imperative.…”