cm2c03785_si_001.pdf (9.88 MB)
Controlled Nanoplatelet Deposition of 2D Chromium Trihalide Solid Solutions
journal contribution
posted on 2023-05-22, 12:35 authored by Samuel Froeschke, Nadia Yasmen, Alexey A. Popov, Sandra Schiemenz, Daniel Wolf, Lars Giebeler, Martin Hantusch, Nico Gräßler, Bernd Büchner, Peer Schmidt, Silke HampelThe 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.
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using additional iodinetransmission electron microscopyrespective parent compoundsphase pure powdercrystals get downscaledchromium trihalides crclanion ratio occur550 ° cray photoelectron spectroscopyinfrared energy rangenanoplatelets could potentially> sub >.> sub >)exotic magnetic properties3 subcontrolled nanoplatelet deposition> subspecific energyraman spectroscopynanoplatelet growthmagnetic responsesub ><3 –<3 hx vibrational modestemperature dependentstarting materialsolid solutionssmall shiftsseveral nanometersremaining similarproperty changespotential utilityphotoluminescence measurementsone waynanometer dimensionslayer dimensionsg .,experimental studyeasily delaminateddetailed theoreticaldeposited materialcomplex evolution2 h
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