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Bi2O2Se has attracted intensive attention due to its potential inelectronics, optoelectronics, as well as ferroelectric applications. Despitethat, there have only been a handful of experimental studies based on ultrafastspectroscopy to elucidate the carrier dynamics in Bi2O2Se thin films, Differentgroups have reported various ultrafast timescales and associated mechanismsacross films of different thicknesses. A comprehensive understanding inrelation to thickness and fluence is still lacking. In this work, we havesystematically explored the thickness-dependent Raman spectroscopy andultrafast carrier dynamics in chemical vapor deposition (CVD)-grown Bi2O2Sethin films on mica substrate with thicknesses varying from 22.44 nm down to4.62 nm at both low and high pump fluence regions. Combining the thicknessdependence and fluence dependence of the slow decay time, we demonstrate aferroelectric transition in the thinner (< 8 nm) Bi2O2Se films, influenced bysubstrate-induced compressive strain and non-equilibrium states. Moreover, thistransition can be manifested under highly non-equilibrium states. Our resultsdeepen the understanding of the interplay between the ferroelectric phase andsemiconducting characteristics of Bi2O2Se thin films, providing a new route tomanipulate the ferroelectric transition.

Hidden phase uncovered by ultrafast carrier dynamics in thin Bi2O2Se