Resonant Spin Amplification and Accumulation in MAPbI₃ Single Crystals

Quantum technologic and spintronic applications require reliable semiconducting materials that enable a significant, long-living spin polarization of electronic excitations and offer the ability to manipulate it optically in an external field. Due to the specifics of band structure and remarkable spin-dependent properties, the lead halide perovskite semiconductors are suitable candidates for that. Here, the carrier spin dynamics in a MAPbI₃ (MA = methylammonium) perovskite single crystal with thickness of 20 µm are studied by the time-resolved Kerr ellipticity technique at cryogenic temperatures. Long times of longitudinal electron spin relaxation T₁ = 30 ns and transverse electron spin dephasing <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:semantics> <mml:mrow><mml:msubsup><mml:mi>T</mml:mi> <mml:mrow><mml:mn>2</mml:mn> <mml:mo>,</mml:mo> <mml:mi>e</mml:mi></mml:mrow> <mml:mo>∗</mml:mo></mml:msubsup> <mml:mo>=</mml:mo> <mml:mn>21</mml:mn></mml:mrow> <mml:annotation>$T_{2,e}^*=21$</mml:annotation></mml:semantics> </mml:math> ns are found. The spin dynamics lasting longer than the applied laser pulse repetition period give rise to spin accumulation effects. They are exploited through the resonant spin amplification, polarization recovery, and spin inertia techniques to study the electron and hole spin systems coupled with the nuclear spins. These results establish the lead halide perovskite semiconductors as suitable platform for quantum technologies relying on spin-dependent phenomena.