%0 Journal Article %K temperature %K faraday effect %K Perovskite %K probes %K Polarization %K Nanotechnology %K Magnetic moments %K Spin polarization %K rotation %K Magnetoelectronics %K Semiconductor quantum wells %K Electrospinning %K Light emission %K Pinch effect %K Carrier diffusion length %K Electron spin polarization %K Electron-spin relaxation %K Low temperature solutions %K Photoinduced magnetization %K Polycrystalline perovskite %K Pump probe %K Time-resolved Faraday rotation %K Spin dynamics %A D Giovanni %A H Ma %A J Chua %A M Grätzel %A Ramamoorthy Ramesh %A S Mhaisalkar %A N Mathews %A T.C Sum %B Nano Letters %D 2015 %G eng %I American Chemical Society %P 1553-1558 %R 10.1021/nl5039314 %T Highly spin-polarized carrier dynamics and ultralarge photoinduced magnetization in CH3NH3PbI3 perovskite thin films %V 15 %X Low-temperature solution-processed organic-inorganic halide perovskite CH3NH3PbI3 has demonstrated great potential for photovoltaics and light-emitting devices. Recent discoveries of long ambipolar carrier diffusion lengths and the prediction of the Rashba effect in CH3NH3PbI3, that possesses large spin-orbit coupling, also point to a novel semiconductor system with highly promising properties for spin-based applications. Through circular pump-probe measurements, we demonstrate that highly polarized electrons of total angular momentum (J) with an initial degree of polarization Pini ∼ 90% (i.e., -30% degree of electron spin polarization) can be photogenerated in perovskites. Time-resolved Faraday rotation measurements reveal photoinduced Faraday rotation as large as 10°/m at 200 K (at wavelength γ = 750 nm) from an ultrathin 70 nm film. These spin polarized carrier populations generated within the polycrystalline perovskite films, relax via intraband carrier spin-flip through the Elliot-Yafet mechanism. Through a simple two-level model, we elucidate the electron spin relaxation lifetime to be ∼7 ps and that of the hole is ∼1 ps. Our work highlights the potential of CH3NH3PbI3 as a new candidate for ultrafast spin switches in spintronics applications. © 2015 American Chemical Society.