TY - JOUR KW - Temperature KW - Oxide KW - Perovskite KW - Oxides KW - Semiconductor KW - Chemistry KW - Semiconductors KW - Semiconductor quantum dots KW - Titanium KW - Calcium compounds KW - Perovskite solar cells KW - Stark effect KW - Circularly polarized optical pulse KW - Dielectric confinement KW - Inorganic semiconductors KW - Light-matter coupling KW - Light-matter interactions KW - Perovskite thin films KW - Solution processability KW - Straightforward strategy KW - Semiconductor quantum wells KW - Calcium derivative KW - Halogen KW - Quantum Theory KW - Thermodynamics KW - Halogens AU - D Giovanni AU - W.K Chong AU - H.A Dewi AU - K Thirumal AU - I Neogi AU - Ramamoorthy Ramesh AU - S Mhaisalkar AU - N Mathews AU - T.C Sum AB - Ultrafast spin manipulation for opto-spin logic applications requires material systems that have strong spinselective light-matter interaction. Conventional inorganic semiconductor nanostructures [for example, epitaxial II to VI quantum dots and III to V multiple quantum wells (MQWs)] are considered forerunners but encounter challenges such as lattice matching and cryogenic cooling requirements. Two-dimensional halide perovskite semiconductors, combining intrinsic tunable MQW structures and large oscillator strengths with facile solution processability, can offer breakthroughs in this area. We demonstrate novel room-temperature, strong ultrafast spin-selective optical Stark effect in solution-processed (C6H4FC2H4NH3)2PbI4 perovskite thin films. Exciton spin states are selectively tuned by ∼6.3 meV using circularly polarized optical pulses without any external photonic cavity (that is, corresponding to a Rabi energy of ∼55 meV and equivalent to applying a 70 T magnetic field), which is much larger than any conventional system. The facile halide and organic replacement in these perovskites affords control of the dielectric confinement and thus presents a straightforward strategy for tuning light-matter coupling strength. © 2016 The Authors. BT - Science Advances DO - 10.1126/sciadv.1600477 LA - eng M1 - 6 N1 - cited By 33 N2 - Ultrafast spin manipulation for opto-spin logic applications requires material systems that have strong spinselective light-matter interaction. Conventional inorganic semiconductor nanostructures [for example, epitaxial II to VI quantum dots and III to V multiple quantum wells (MQWs)] are considered forerunners but encounter challenges such as lattice matching and cryogenic cooling requirements. Two-dimensional halide perovskite semiconductors, combining intrinsic tunable MQW structures and large oscillator strengths with facile solution processability, can offer breakthroughs in this area. We demonstrate novel room-temperature, strong ultrafast spin-selective optical Stark effect in solution-processed (C6H4FC2H4NH3)2PbI4 perovskite thin films. Exciton spin states are selectively tuned by ∼6.3 meV using circularly polarized optical pulses without any external photonic cavity (that is, corresponding to a Rabi energy of ∼55 meV and equivalent to applying a 70 T magnetic field), which is much larger than any conventional system. The facile halide and organic replacement in these perovskites affords control of the dielectric confinement and thus presents a straightforward strategy for tuning light-matter coupling strength. © 2016 The Authors. PB - American Association for the Advancement of Science PY - 2016 T2 - Science Advances TI - Tunable room-temperature spin-selective optical Stark effect in solution-processed layered halide perovskites VL - 2 SN - 23752548 ER -