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

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms12613· OSTI ID:1320387

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.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office
Grant/Contract Number:
AC36-08GO28308
OSTI ID:
1320387
Report Number(s):
NREL/JA-5900-66100
Journal Information:
Nature Communications, Vol. 7; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 96 works
Citation information provided by
Web of Science

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Cited By (16)

Perovskites for Light Emission journal August 2018
Spin‐Polarized Electronic Transport through Ferromagnet/Organic–Inorganic Hybrid Perovskite Spinterfaces at Room Temperature journal August 2019
Investigation on Charge Carrier Recombination of Hybrid Organic-Inorganic Perovskites Doped with Aggregation-Induced Emission Luminogen under High Photon Flux Excitation journal May 2018
Photoinduced Lattice Symmetry Enhancement in Mixed Hybrid Perovskites and Its Beneficial Effect on the Recombination Behavior journal February 2019
Spintronics of Hybrid Organic–Inorganic Perovskites: Miraculous Basis of Integrated Optoelectronic Devices journal June 2019
Understanding the physical properties of hybrid perovskites for photovoltaic applications journal July 2017
Spatially segregated free-carrier and exciton populations in individual lead halide perovskite grains journal March 2017
Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices journal January 2019
Resonant optical Stark effect in monolayer WS2 journal December 2019
Structural fluctuations cause spin-split states in tetragonal (CH 3 NH 3 )PbI 3 as evidenced by the circular photogalvanic effect journal September 2018
Anisotropic Stark effect of carbon monoxide: emergent orbital cooperativity journal March 2019
Nontrivial strength of van der Waals epitaxial interaction in soft perovskites journal July 2018
Lead halide perovskites: Crystal-liquid duality, phonon glass electron crystals, and large polaron formation journal October 2017
Exciton control in a room temperature bulk semiconductor with coherent strain pulses journal November 2019
Lead halide perovskites: Crystal-liquid duality, phonon glass electron crystals, and large polaron formation text January 2017
Understanding the physical properties of hybrid perovskites for photovoltaic applications text January 2017

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