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To further increase the open‐circuit voltage (Voc) of perovskite solar cells (PSCs), many efforts have been devoted to doping the TiO2 electron transport/selective layers by using metal dopants with higher electronegativity than Ti. However, those dopants can introduce undesired charge traps that hinder charge transport through TiO2, so the improvement in the Voc is often accompanied by an undesired photocurrent density–voltage (J–V) hysteresis problem. Herein, it is demonstrated that the use of a rapid flame doping process (40 s) to introduce cobalt dopant into TiO2 not only solves the J–V hysteresis problem but also increases the Voc and power conversion efficiency of both mesoscopic and planar PSCs. The reasons for the simultaneous improvements are two fold. First, the flame‐doped Co‐TiO2 film forms Co‐Ov (cobalt dopant‐oxygen vacancy) pairs and hence reduces the number density of Ti3+ trap states. Second, Co doping upshifts the band structure of TiO2, facilitating efficient charge extraction. As a result, for planar PSCs, the flame doping of Co increases the efficiency from 17.1% to 18.0% while reducing the hysteresis from 16.0% to 1.7%. Similarly, for mesoscopic PSCs, the flame doping of Co increases the efficiency from 18.5% to 20.0% while reducing the hysteresis from 7.0% to 0.1%. A rapid flame‐processed cobalt‐doped TiO2 for highly efficient perovskite solar cells with resolved hysteresis is described. The flame doping of Co2+ forms cobalt‐oxygen vacancy pairs in the TiO2 lattice that reduces the intrinsic defective Ti3+ and upshifts the band structure of TiO2, solving the current density‐voltage (J–V) hysteresis and enhancing the efficiency of both mesoscopic and planar perovskite solar cells. [ABSTRACT FROM AUTHOR]

To further increase the open‐circuit voltage (Voc) of perovskite solar cells (PSCs), many efforts have been devoted to doping the TiO2 electron transport/selective layers by using metal dopants with higher electronegativity than Ti. However, those dopants can introduce undesired charge traps that hinder charge transport through TiO2, so the improvement in the Voc is often accompanied by an undesired photocurrent density–voltage (J–V) hysteresis problem. Herein, it is demonstrated that the use of a rapid flame doping process (40 s) to introduce cobalt dopant into TiO2 not only solves the J–V hysteresis problem but also increases the Voc and power conversion efficiency of both mesoscopic and planar PSCs. The reasons for the simultaneous improvements are two fold. First, the flame‐doped Co‐TiO2 film forms Co‐Ov (cobalt dopant‐oxygen vacancy) pairs and hence reduces the number density of Ti3+ trap states. Second, Co doping upshifts the band structure of TiO2, facilitating efficient charge extraction. As a result, for planar PSCs, the flame doping of Co increases the efficiency from 17.1% to 18.0% while reducing the hysteresis from 16.0% to 1.7%. Similarly, for mesoscopic PSCs, the flame doping of Co increases the efficiency from 18.5% to 20.0% while reducing the hysteresis from 7.0% to 0.1%. A rapid flame‐processed cobalt‐doped TiO2 for highly efficient perovskite solar cells with resolved hysteresis is described. The flame doping of Co2+ forms cobalt‐oxygen vacancy pairs in the TiO2 lattice that reduces the intrinsic defective Ti3+ and upshifts the band structure of TiO2, solving the current density‐voltage (J–V) hysteresis and enhancing the efficiency of both mesoscopic and planar perovskite solar cells. [ABSTRACT FROM AUTHOR]