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Two-dimensional (2D) elemental semiconductors have great potential for deviceapplications, but their performance is limited by the lack of efficient dopingmethods. Here, combining molecular beam epitaxy, scanning tunnelingmicroscopy/spectroscopy, X-ray photoelectron spectroscopy, and densityfunctional theory calculations, we investigate the evolution of the structuraland electronic properties of 2D selenium/tellurium films with increased Sedosages on graphene/6H-SiC(0001) substrates. We found that Se atoms formisovalent dopants by replacing surface Te atoms, which introduces efficientelectron doping and lowers the work function of Te films. With the Se dosageincreasing, two types of elemental 2D crystalline Se structures, trigonal Seand Se8 molecular assembly films, are obtained on ultrathin Te films, which aredistinct from the amorphous Se acquired by depositing Se directly ongraphene/6H-SiC(0001). Our results shed light on tuning the electronicproperties of 2D elemental semiconductors by isovalent doping and constructingheterostructures of isovalent 2D elemental materials.

Selenium / Tellurium Two-Dimensional Structures: from Isovalent Se Dopants in Te to Atomically Thin Se Films