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Two-dimensional (2D) layered materials are very important and versatileplatform for exploring novel electronic properties in different phases. Thechemical doping in two-dimensional (2D) layered materials can engineer theelectronic structure with useful physical properties which are distinct incomparison with the pristine one. Herein, we employed angle-resolvedphotoemission spectroscopy (ARPES) combined with first-principles densityfunctional theory (DFT) calculations, to show the possible phase engineering ofZrSe2 via Hafnium (Hf) atoms substitution, which manifests asemiconducting-to-metallic transition. The emergence of conduction band at highsymmetry M point around the Brillouin zone boundary due to extra charge doping,clearly demonstrates the conceivable evidence of semiconductor to metaltransition in ZrSe2, through Hf substitution (about 12.5 percent) at roomtemperature. Similarly, the electrical resistance measurements further revealedthe decrease of resistance with increasing temperature for ZrSe2 that confirmsthe semiconducting behavior, while the resistance increases with increasingtemperature for Hf doped ZrSe2 that in an indication of the metallic behavior.This study further demonstrates the possibility of the band gap engineeringthrough heavily doped metal in 2D materials thereby modulating the electronicproperties of layered materials for next-generation electronic applications.

Emergence of conduction band-induced semiconductor-to-metal transition in ZrSe2 through Hf substitution