Intrinsic Self-Trapped Excitons in Graphitic Carbon Nitride. 2024

Junhong Yu, and Yunhu Wang, and Yubu Zhou, and Wenhui Fang, and Baiquan Liu, and Jun Xing
LUMINOUS! Centre of Excellence for Semiconductor Lighting and Displays, School of Electrical and Electronic Engineering, Nanyang Technological University, 50 Nanyang Avenue 639798, Singapore.

Graphitic carbon nitrides (g-C3N4) as low-cost, chemically stable, and ecofriendly layered semiconductors have attracted rapidly growing interest in optoelectronics and photocatalysis. However, the nature of photoexcited carriers in g-C3N4 is still controversial, and an independent charge-carrier picture based on the band theory is commonly adopted. Here, by performing transient spectroscopy studies, we show characteristics of self-trapped excitons (STEs) in g-C3N4 nanosheets including broad trapped exciton-induced absorption, picosecond exciton trapping without saturation at high photoexcitation density, and transient STE-induced stimulated emissions. These features, together with the ultrafast exciton trapping polarization memory, strongly suggest that STEs intrinsically define the nature of the photoexcited states in g-C3N4. These observations provide new insights into the fundamental photophysics of carbon nitrides, which may enlighten novel designs to boost energy conversion efficiency.

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