Tunable room-temperature spin-selective optical Stark effect in solution-processed layered halide perovskites

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Science Advances  17 Jun 2016:
Vol. 2, no. 6, e1600477
DOI: 10.1126/sciadv.1600477

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Ultrafast spin manipulation for opto–spin logic applications requires material systems that have strong spin-selective 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.

  • Non-linear
  • light-matter interactions
  • Ultrafast
  • Spin-selective
  • Optical Stark Effect
  • Solution Processed
  • Layered Halide Perovskites
  • room temperature
  • opto-spin-logic
  • Rabi-splitting

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