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We apply the density-functional theory to study various phases (including non-magnetic (NM), anti-ferromagnetic (AFM), and ferromagnetic (FM)) in monolayer magnetic chromium triiodide (CrI 3 ), a recently fabricated 2D magnetic material. It is found that: (1) the introduction of magnetism in monolayer CrI 3 gives rise to metal-to-semiconductor transition; (2) the electronic band topologies as well as the nature of direct and indirect band gaps in either AFM or FM phases exhibit delicate dependence on the magnetic ordering and spin–orbit coupling; and (3) the phonon modes involving Cr atoms are particularly sensitive to the magnetic ordering, highlighting distinct spin–lattice and spin–phonon coupling in this magnet. First-principles simulations of the Raman spectra demonstrate that both frequencies and intensities of the Raman peaks strongly depend on the magnetic ordering. The polarization dependent A 1g modes at 77 cm −1 and 130 cm −1 along with the E g mode at about 50 cm −1 in the FM phase may offer a useful fingerprint to characterize this material. Our results not only provide a detailed guiding map for experimental characterization of CrI 3 , but also reveal how the evolution of magnetism can be tracked by its lattice dynamics and Raman response.
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Raman scattering spectra of boron imidazolate frameworks containing different magnetic ions
We present a Raman scattering spectroscopic study of boron imidazolate metal-organic frameworks (BIFs) with three different magnetic metal ions and one non-magnetic in a wide frequency range from 25 to 1700 cm−1, which covers local vibrations of the imidazolate linkers as well as collective lattice vibrations. We show that the spectral region above 800 cm−1 belongs to the local vibrations of the linkers, which have the same frequencies for the studied BIFs without any dependence on the structure of the BIFs and are easily interpreted based on the spectra of imidazolate linkers. In contrast, collective lattice vibrations, observed below 100 cm−1, show a distinction between cage and two-dimensional BIFs structures, with a weak dependence on the metal node. We identify the range of vibrations around 200 cm−1, which are distinct for each metal-organic framework, depending on a metal node. Our work demonstrates the energy hierarchy in the vibrational response of BIFs.
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- Award ID(s):
- 2004074
- PAR ID:
- 10443077
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 158
- Issue:
- 21
- ISSN:
- 0021-9606
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1063/5.0152070
