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Understanding the chemistry of 2D rhodium trihalide solid solutions: tuning of optical properties and nanocrystal deposition

  • In the search for novel 2D materials with potentially valuable properties, such as a tunable band gap for optoelectronic or catalytic applications, solid solutions hold the potential to significantly expand the inventory of available 2D nanomaterials. In this study, we present for the first time the synthesis of such 2D rhodium trihalide solid solutions: RhBrxCl3−x and RhBrxI3−x. We use thermodynamic simulations and simultaneous thermal analysis to predict conditions for their rational synthesis and to investigate suitable chemical vapor transport (CVT) parameters for these solid solutions. The evolution of the lattice parameters was investigated by powder x-ray diffraction, showing an isostructural relationship of the synthesized compounds and only minor deviation from Vegard's law. The optical band gap of these materials can be tuned in an energy range from 1.5 eV (RhCl3) to 1.2 eV (RhI3) by choosing the composition of the solid solution, while the samples also exhibit photoluminescence in similar energy ranges. Ultimately, theIn the search for novel 2D materials with potentially valuable properties, such as a tunable band gap for optoelectronic or catalytic applications, solid solutions hold the potential to significantly expand the inventory of available 2D nanomaterials. In this study, we present for the first time the synthesis of such 2D rhodium trihalide solid solutions: RhBrxCl3−x and RhBrxI3−x. We use thermodynamic simulations and simultaneous thermal analysis to predict conditions for their rational synthesis and to investigate suitable chemical vapor transport (CVT) parameters for these solid solutions. The evolution of the lattice parameters was investigated by powder x-ray diffraction, showing an isostructural relationship of the synthesized compounds and only minor deviation from Vegard's law. The optical band gap of these materials can be tuned in an energy range from 1.5 eV (RhCl3) to 1.2 eV (RhI3) by choosing the composition of the solid solution, while the samples also exhibit photoluminescence in similar energy ranges. Ultimately, the successful deposition of bulk as well as ultrathin 2D nanocrystals of RhBrxCl3−x by CVT from 925 °C to 850 °C is shown, where the composition of the deposited crystals is precisely controlled by the choice of the starting composition and the initial amount of material. The high quality of the obtained nanocrystals is confirmed by atomic force microscopy, high resolution transmission electron microscopy and selected area electron diffraction. For RhBrxI3−x, the CVT from 900 °C to 825 °C is more difficult and has only been practically demonstrated for an exemplary case. According to the observed properties, these novel solid solutions and nanocrystals show a great potential for an application in optoelectronic devices.show moreshow less

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Author: Samuel FroeschkeORCiD, Karl-Georg Schroth, Udo SteinerORCiD, Alexey PopovORCiD, Sandra Schiemenz, Daniel WolfORCiD, Lars GiebelerORCiD, Nico GräßlerORCiD, Bernd BüchnerORCiD, Peer SchmidtORCiD, Silke HampelORCiD
URL:https://iopscience.iop.org/article/10.1088/2053-1583/acd012
DOI:https://doi.org/10.1088/2053-1583/acd012
ISSN:2053-1583
Title of the source (English):2D 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:10
Issue number:3
First Page:1
Last Page:12
Article number:035011
Fundername (not EU):DFG
Project number (not EU):665878
Way of publication:Open Access
Faculty/Chair:Fakultät 2 Umwelt und Naturwissenschaften / FG Anorganische Chemie
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