Engineering Multifunctionality in MoSe₂ Nanostructures Via Strategic Mn Doping for Electrochemical Energy Storage and Photosensing

To achieve advanced functionalities in nanostructured MoSe2 for enhanced electrochemical charge storage and improved photosensing, here we propose an effective strategy, i.e., the substitutional doping of the heteroatom Mn. We achieve a 313% increase in specific capacitance for 6.2% of Mn doping compared to pristine MoSe2 at the scan rate of 5 mV/s in a three-electrode configuration. For a two-electrode arrangement, also superior charge-storage performance is noted. The enhanced electrode performance can be attributed to the increase of electrical conductivity arising due to an increase of electron density for the n-type nature of Mn doping realized via an X-ray photoelectron spectroscopy study and density functional theory calculation. The latter one also unveils that Mn doping introduces catalytically active sites by disrupting homogeneous charge distribution over the topology of the MoSe2 basal plane contributing to better charge-storage performance. Mn doping-induced shift in the Fermi level of MoSe2 toward the conduction band also minimizes the contact barrier height signifying its improved capabilities for a photosensor device. Additionally, Mn doping causes alleviation of the charge-recombination process resulting in increase of photocarrier separation. As a result, we observe a 187% enhancement in the photocurrent and significantly higher responsivity and detectivity for 6.2% Mn-doped MoSe2 than its pristine counterpart. Our proposed doping strategy to modulate charge storage as well as photoresponse properties demonstrates high potential for MoSe2 along with other two-dimensional transition-metal dichalcogenides in developing next-generation energy-storage and optoelectronic devices