TY - JOUR KW - Temperature KW - Faraday effect KW - Perovskite KW - Probes KW - Polarization KW - Nanotechnology KW - Magnetic moments KW - Spin polarization KW - Rotation KW - Magnetoelectronics KW - Semiconductor quantum wells KW - Electrospinning KW - Light emission KW - Pinch effect KW - Carrier diffusion length KW - Electron spin polarization KW - Electron-spin relaxation KW - Low temperature solutions KW - Photoinduced magnetization KW - Polycrystalline perovskite KW - Pump probe KW - Time-resolved Faraday rotation KW - Spin dynamics AU - D Giovanni AU - H Ma AU - J Chua AU - M Grätzel AU - Ramamoorthy Ramesh AU - S Mhaisalkar AU - N Mathews AU - T.C Sum AB - 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. BT - Nano Letters DO - 10.1021/nl5039314 LA - eng M1 - 3 N1 - cited By 75 N2 - 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. PB - American Chemical Society PY - 2015 SP - 1553 EP - 1558 T2 - Nano Letters TI - Highly spin-polarized carrier dynamics and ultralarge photoinduced magnetization in CH3NH3PbI3 perovskite thin films VL - 15 SN - 15306984 ER -