Hot carrier distribution engineering by alloying: picking elements for the desired purposes (2402.12337v1)

Abstract: Metal alloys hold the promise of providing hot carrier generation distributions superior to pure metals in applications such as sensing, catalysis and solar energy harvesting. Guidelines for finding the optimal alloy configuration for a target application require understanding the connection between alloy composition and hot carrier distribution. Here we present a DFT-based computational approach to investigate the photo-generated hot carrier distribution of metal alloys based on the joint density of states and the electronic structure. We classified the metals by their electronic structure into closed d-shell, open d-shell, p-block and s-block elements. It is shown that combining closed d-shell elements enables modulating the distribution of highly energetic holes typical of pure metals but also leads to hot carrier production by IR light excitation and the appearance of highly energetic electrons due to band folding and splitting. This feature arises as an emergent property of alloying and is only unveiled when the hot carrier distribution computation takes momentum conservation into account. The combination of closed d-shell with open d-shell elements allows an abundant production of hot carriers in a broad energy range, while alloying a closed d-shell elements with an s-block element opens the door to hot electron distribution skewed toward high energy electrons. The combination of d-shell with p-block elements results in moderate hot carrier distribution whose asymmetry can be tuned by composition. Overall, the obtained insights that connect alloy composition, band structure and resulting carrier distribution provide a toolkit to match elements in an alloy for the deliberate engineering of hot carrier distribution.