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

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. Lastly, our result implies that such hybrid semiconductors may have great potential for optoelectronic applications beyond photovoltaics.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Solar Energy Technologies Office (EE-4S)
OSTI Identifier:
1320387
Report Number(s):
NREL/JA-5900-66100
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; perovskite; optical Stark effect; ultrafast spectroscopy

Citation Formats

Yang, Ye, Yang, Mengjin, Zhu, Kai, Johnson, Justin C., Berry, Joseph J., van de Lagemaat, Jao, and Beard, Matthew C.. Large polarization-dependent exciton optical Stark effect in lead iodide perovskites. United States: N. p., 2016. Web. doi:10.1038/ncomms12613.
Yang, Ye, Yang, Mengjin, Zhu, Kai, Johnson, Justin C., Berry, Joseph J., van de Lagemaat, Jao, & Beard, Matthew C.. Large polarization-dependent exciton optical Stark effect in lead iodide perovskites. United States. doi:10.1038/ncomms12613.
Yang, Ye, Yang, Mengjin, Zhu, Kai, Johnson, Justin C., Berry, Joseph J., van de Lagemaat, Jao, and Beard, Matthew C.. 2016. "Large polarization-dependent exciton optical Stark effect in lead iodide perovskites". United States. doi:10.1038/ncomms12613. https://www.osti.gov/servlets/purl/1320387.
@article{osti_1320387,
title = {Large polarization-dependent exciton optical Stark effect in lead iodide perovskites},
author = {Yang, Ye and Yang, Mengjin and Zhu, Kai and Johnson, Justin C. and Berry, Joseph J. and van de Lagemaat, Jao and Beard, Matthew C.},
abstractNote = {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. Lastly, our result implies that such hybrid semiconductors may have great potential for optoelectronic applications beyond photovoltaics.},
doi = {10.1038/ncomms12613},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = 2016,
month = 8
}

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