%0 Journal Article %K temperature %K oxide %K Perovskite %K oxides %K semiconductor %K chemistry %K semiconductors %K semiconductor quantum dots %K titanium %K Calcium compounds %K Perovskite solar cells %K Stark effect %K Circularly polarized optical pulse %K Dielectric confinement %K Inorganic semiconductors %K Light-matter coupling %K Light-matter interactions %K Perovskite thin films %K Solution processability %K Straightforward strategy %K Semiconductor quantum wells %K calcium derivative %K halogen %K quantum theory %K thermodynamics %K Halogens %A D Giovanni %A W.K Chong %A H.A Dewi %A K Thirumal %A I Neogi %A Ramamoorthy Ramesh %A S Mhaisalkar %A N Mathews %A T.C Sum %B Science Advances %D 2016 %G eng %I American Association for the Advancement of Science %R 10.1126/sciadv.1600477 %T Tunable room-temperature spin-selective optical Stark effect in solution-processed layered halide perovskites %V 2 %X 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.