It provides a straightforward guidance to the design and optimization of OIHP‐based solar cells. The results provide the spectroscopic perception on how doping concentration affects trap density, carrier dynamics, transport behavior, and ultimately the parameters of devices. The optimization of solar cell performance requires the tradeoff of competitive relation between the passivation and introduction of trapping centers. This directly manipulates the transient transport of the photocarriers and finally influences the output of devices. The results indicate that doping would reduce the trap density by passivating defects and induce extra trapping centers. Systematic spectroscopic characterizations indicate that doping significantly influences the photocarrier dynamics via directly regulating the trap states. Herein, typical OIHPs (CH3NH3PbI3 and Cs0.05FA0.85MA0.10Pb(I0.97Br0.03)3) doped with RbI are employed to expound the doping mechanism in affecting the efficiency of devices. Nevertheless, the perception of trap states regulated by doping and their effects on the performance of solar cells is not in‐depth. To enhance the efficiency and stability of the organic–inorganic hybrid perovskite (OIHP) solar cells, doping has been demonstrated as a straightforward method. This work has implications in offering guidance for broadening the photovoltaic applications of CH3NH3PbI3. The detailed analyses on the thermodynamic stabilities of doped structures have been made through examining their phonon dispersions and decomposition energies. The effects of band-gap reduction and electron-mobility enhancement jointly contribute to the promotion in optoelectronics of CH3NH3PbI3. Furthermore, the electron mobility is found to be enhanced by 28%, which is beneficial for separating and collecting the photo-excited carriers. First, we examine the dependence of band gap on the Cd doping concentration, and find that the increased Cd content narrows the band gap up to 1.41 eV, extending the photoabsorption wavelength of CH3NH3PbI3 into the range of near-infrared spectrum. The electronic properties and optoelectronic functionalities of tetragonal CH3NH3PbI3 doped with different concentrations (6.25%, 12.5% and 25%) of Cd have been investigated using the the generalized gradient approximation with the correction of van der Waals interactions (GGA+vdW).

Strontium charge