Unraveling the Role of Interfacial Charge Transfer on Photoactivity and Anomalous Luminescence Quenching of V<sub>4</sub>C<sub>3</sub>T<i><sub><i>x</i></sub></i>/Protonated g-C<sub>3</sub>N<sub>4</sub> Heterostructures
Muhammad Abiyyu Kenichi Purbayanto, Madhurya Chandel, Michał Makowski, Muhammad Danang Birowosuto, Verónica Montes‐García, Kaitlyn Prenger, Artur Ciesielski, Michael Naguib, Agnieszka Jastrzębska
Abstract
High Resolution Image Download MS PowerPoint Slide Two-dimensional van der Waals heterostructures with exotic quantum phenomena have garnered a huge surge in the field of optoelectronic devices. Herein, we report spectroscopic evidence of efficient interfacial charge transfers at the interface of a novel 2D/2D V 4 C 3 T x MXene/protonated g-C 3 N 4 (PCN) heterostructured thin film, demonstrating robust photosensitivity and a large exciton activation energy of 139.5 meV. Through temperature-dependent photoluminescence (PL) and time-resolved PL spectroscopy, we unravel the photophysical mechanism driving efficient charge transfer and photosensitivity in V 4 C 3 T x /PCN heterostructures. These heterostructures exhibit superior photosensitivity to white and UV light compared with either PCN or V 4 C 3 T x pristine materials. Additionally, we observed significant PL quenching with unusual negative thermal quenching and extended charge carrier lifetime in the V 4 C 3 T x /PCN heterostructures across a broad temperature range of 70–370 K. Notably, at the elevated temperature of 370 K, the carrier lifetime was enhanced by more than 2-fold, making the heterostructures promising for optoelectronic applications. This work provides critical insight into the charge transfer mechanism between V 4 C 3 T x MXene and PCN, opening a new avenue for rationally designing g-C 3 N 4 -based heterostructures for highly photosensitive optoelectronic devices.