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Controlled Nanoplatelet Deposition of 2D Chromium Trihalide Solid Solutions

  • The two-dimensional (2D) chromium trihalides CrCl3, CrBr3, and CrI3 are most famous for their exotic magnetic properties when their crystals get downscaled to nanometer dimensions. One way to tune the properties of such materials and to further increase their potential utility, e.g., in spintronics, is the formation of solid solutions. Here, we present a detailed theoretical and experimental study on the synthesis and nanoplatelet growth of CrBrxCl3–x and CrBrxI3–x solid solutions. Phase pure powder was obtained by tempering the respective parent compounds at 600 and 550 °C, using additional iodine in the case of CrBrxI3–x. The dominant stacking order changes at x = 1.8 for CrBrxCl3–x while remaining similar to CrI3 for the whole CrBrxI3–x series. A consecutive chemical vapor transport from 575 → 525 °C for 2 h (CrBrxCl3–x) or 600 → 550 °C for 3 h with 0.1 mmol additional iodine (CrBrxI3–x) resulted in the deposition of high-quality nanoplatelets on a substrate with only several nanometers in height. The composition can be controlledThe two-dimensional (2D) chromium trihalides CrCl3, CrBr3, and CrI3 are most famous for their exotic magnetic properties when their crystals get downscaled to nanometer dimensions. One way to tune the properties of such materials and to further increase their potential utility, e.g., in spintronics, is the formation of solid solutions. Here, we present a detailed theoretical and experimental study on the synthesis and nanoplatelet growth of CrBrxCl3–x and CrBrxI3–x solid solutions. Phase pure powder was obtained by tempering the respective parent compounds at 600 and 550 °C, using additional iodine in the case of CrBrxI3–x. The dominant stacking order changes at x = 1.8 for CrBrxCl3–x while remaining similar to CrI3 for the whole CrBrxI3–x series. A consecutive chemical vapor transport from 575 → 525 °C for 2 h (CrBrxCl3–x) or 600 → 550 °C for 3 h with 0.1 mmol additional iodine (CrBrxI3–x) resulted in the deposition of high-quality nanoplatelets on a substrate with only several nanometers in height. The composition can be controlled by the choice of the starting material, since only small shifts in the anion ratio occur during the transport. The deposited CrBrxCl3–x nanoplatelets can then be easily delaminated by ultrasonication in ethanol to reduce the height even further to few-layer dimensions. These nanoplatelets could potentially be used to investigate the property changes (e.g., in terms of magnetic response) for the downscaling of these solid solutions. We further demonstrate the quality of the deposited material by transmission electron microscopy, selected area electron diffraction, and X-ray photoelectron spectroscopy. Raman spectroscopy of the solid solution series reveals a complex evolution of vibrational modes. Photoluminescence measurements on solid solution samples show emission peaks in the near-infrared energy range with the specific energy and intensity being composition and temperature dependent.show moreshow less

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Metadaten
Author: Samuel FroeschkeORCiD, Nadia Yasmen, Alexey PopovORCiD, Sandra Schiemenz, Daniel WolfORCiD, Lars GiebelerORCiD, Martin HantuschORCiD, Nico GräßlerORCiD, Bernd BüchnerORCiD, Peer SchmidtORCiD, Silke HampelORCiD
URL:https://pubs.acs.org/doi/full/10.1021/acs.chemmater.2c03785
DOI:https://doi.org/10.1021/acs.chemmater.2c03785
ISSN:1520-5002
ISSN:0897-4756
Title of the source (English):Chemistry of Materials
Document Type:Scientific journal article peer-reviewed
Language:English
Year of publication:2023
Tag:2D layered compounds; Chemical vapor transport; Crystal growth; Crystal structure; Halides; Thermodynamic modeling
Volume/Year:35
Issue number:11
First Page:4136
Last Page:4148
Fundername (not EU):DFG
Project number (not EU):665878
Faculty/Chair:Fakultät 2 Umwelt und Naturwissenschaften / FG Anorganische Chemie
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