Large polarization-dependent exciton optical Stark effect in lead iodide perovskites

Ye Yang (), Mengjin Yang, Kai Zhu, Justin C. Johnson, Joseph J. Berry, Jao van de Lagemaat and Matthew C. Beard ()
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Ye Yang: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Mengjin Yang: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Kai Zhu: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Justin C. Johnson: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Joseph J. Berry: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Jao van de Lagemaat: Chemistry and Nanoscience Center, National Renewable Energy Laboratory
Matthew C. Beard: Chemistry and Nanoscience Center, National Renewable Energy Laboratory

Nature Communications, 2016, vol. 7, issue 1, 1-5

Abstract: Abstract A strong interaction of a semiconductor with a below-bandgap laser pulse causes a blue-shift of the bandgap transition energy, known as the optical Stark effect. The energy shift persists only during the pulse duration with an instantaneous response time. The optical Stark effect has practical relevance for applications, including quantum information processing and communication, and passively mode-locked femtosecond lasers. Here we demonstrate that solution-processable lead-halide perovskites exhibit a large optical Stark effect that is easily resolved at room temperature resulting from the sharp excitonic feature near the bandedge. We also demonstrate that a polarized pump pulse selectively shifts one spin state producing a spin splitting of the degenerate excitonic states. Such selective spin manipulation is an important prerequisite for spintronic applications. Our result implies that such hybrid semiconductors may have great potential for optoelectronic applications beyond photovoltaics.

Date: 2016
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DOI: 10.1038/ncomms12613

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