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Two-dimensional (2D) materials are easily fabricated when their bulk form has a layered structure. The monolayer form in layered transition-metal dichalcogenides is typically the same as a single layer of the bulk material. However, PdSe_{2} presents a puzzle. Its monolayer form has been theoretically shown to be stable, but there have been no reports that monolayer PdSe_{2} has been fabricated. Here, combining atomic-scale imaging in a scanning transmission electron microscope and density functional theory, we demonstrate that the preferred monolayer form of this material amounts to a melding of two bulk monolayers accompanied by the emission of Se atoms so that the resulting stoichiometry is Pd_{2}Se_{3}. We further verify the interlayer melding mechanism by creating Se vacancies in situ in the layered PdSe_{2} matrix using electron irradiation. The discovery that strong interlayer interactions can be induced by defects and lead to the formation of new 2D materials opens a new venue for the exploration of defect engineering and novel 2D structures.

physical review letters

Novel <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi>Pd</mml:mi></mml:mrow><mml:mrow><mml:mn>2</mml:mn></mml:mrow></mml:msub><mml:msub><mml:mrow><mml:mi>Se</mml:mi></mml:mrow><mml:mrow><mml:mn>3</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math> Two-Dimensional Phase Driven by Interlayer Fusion in Layered <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi>PdSe</mml:mi…

Novel Pd2Se3 Two-Dimensional Phase Driven by Interlayer Fusion in Layered PdSe