2D Perovskites with Giant Excitonic Optical Nonlinearities for High-Performance Sub-Bandgap Photodetection

Feng Zhou; Ibrahim Abdelwahab; Kai Leng; Kian Ping Loh; Wei Ji

doi:10.1002/adma.201904155

2D Perovskites with Giant Excitonic Optical Nonlinearities for High-Performance Sub-Bandgap Photodetection

Feng Zhou, Ibrahim Abdelwahab, Kai Leng, Kian Ping Loh, Wei Ji

Research output: Journal article publication › Journal article › Academic research › peer-review

82 Citations (Scopus)

Abstract

Two-dimensional (2D) perovskites have proved to be promising semiconductors for photovoltaics, photonics, and optoelectronics. Here, a strategy is presented toward the realization of highly efficient, sub-bandgap photodetection by employing excitonic effects in 2D Ruddlesden–Popper-type halide perovskites (RPPs). On near resonance with 2D excitons, layered RPPs exhibit degenerate two-photon absorption (D-2PA) coefficients as giant as 0.2–0.64 cm MW⁻ ¹. 2D RPP-based sub-bandgap photodetectors show excellent detection performance in the near-infrared (NIR): a two-photon-generated current responsivity up to 1.2 × 10⁴ cm² W⁻² s⁻¹, two orders of magnitude greater than InAsSbP-pin photodiodes; and a dark current as low as 2 pA at room temperature. More intriguingly, layered-RPP detectors are highly sensitive to the light polarization of incoming photons, showing a considerable anisotropy in their D-2PA coefficients (β_[001]/β_[011] = 2.4, 70% larger than the ratios reported for zinc-blende semiconductors). By controlling the thickness of the inorganic quantum well, it is found that layered RPPs of (C₄H₉NH₃)₂(CH₃NH₃)Pb₂I₇ can be utilized for three-photon photodetection in the NIR region.

Original language	English
Article number	1904155
Journal	Advanced Materials
Volume	31
Issue number	48
DOIs	https://doi.org/10.1002/adma.201904155
Publication status	Published - 28 Nov 2019
Externally published	Yes

Keywords

2D Ruddlesden–Popper perovskites
excitonic effects
nonlinear optics
sub-bandgap photodetection
two-photon absorption

ASJC Scopus subject areas

General Materials Science
Mechanics of Materials
Mechanical Engineering

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10.1002/adma.201904155

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title = "2D Perovskites with Giant Excitonic Optical Nonlinearities for High-Performance Sub-Bandgap Photodetection",

abstract = "Two-dimensional (2D) perovskites have proved to be promising semiconductors for photovoltaics, photonics, and optoelectronics. Here, a strategy is presented toward the realization of highly efficient, sub-bandgap photodetection by employing excitonic effects in 2D Ruddlesden–Popper-type halide perovskites (RPPs). On near resonance with 2D excitons, layered RPPs exhibit degenerate two-photon absorption (D-2PA) coefficients as giant as 0.2–0.64 cm MW− 1. 2D RPP-based sub-bandgap photodetectors show excellent detection performance in the near-infrared (NIR): a two-photon-generated current responsivity up to 1.2 × 104 cm2 W−2 s−1, two orders of magnitude greater than InAsSbP-pin photodiodes; and a dark current as low as 2 pA at room temperature. More intriguingly, layered-RPP detectors are highly sensitive to the light polarization of incoming photons, showing a considerable anisotropy in their D-2PA coefficients (β[001]/β[011] = 2.4, 70% larger than the ratios reported for zinc-blende semiconductors). By controlling the thickness of the inorganic quantum well, it is found that layered RPPs of (C4H9NH3)2(CH3NH3)Pb2I7 can be utilized for three-photon photodetection in the NIR region.",

keywords = "2D Ruddlesden–Popper perovskites, excitonic effects, nonlinear optics, sub-bandgap photodetection, two-photon absorption",

author = "Feng Zhou and Ibrahim Abdelwahab and Kai Leng and Loh, {Kian Ping} and Wei Ji",

note = "Funding Information: F.Z., I.A., and L.K. contributed equally to this work. F.Z. carried out the theoretical calculations, conducted optical characterization and data analysis. I.A. fabricated all 2D-RPPs based phototransistors, prepared all the samples for 2PPL, and performed 1PPL and AFM measurements. K.L. synthesized all single crystals of 2D-RPPs. All authors contributed to the overall scientific interpretation. Financial supports from Ministry of Education/National University of Singapore (MOE/NUS) grant R144-000-401-114 are acknowledged. K.P.L. acknowledges support from the National Research Foundation, Prime Minister's Office, Midsized Centre program (CA2DM), Singapore. Publisher Copyright: {\textcopyright} 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim",

year = "2019",

month = nov,

day = "28",

doi = "10.1002/adma.201904155",

language = "English",

volume = "31",

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AU - Zhou, Feng

AU - Abdelwahab, Ibrahim

AU - Leng, Kai

AU - Loh, Kian Ping

AU - Ji, Wei

N1 - Funding Information: F.Z., I.A., and L.K. contributed equally to this work. F.Z. carried out the theoretical calculations, conducted optical characterization and data analysis. I.A. fabricated all 2D-RPPs based phototransistors, prepared all the samples for 2PPL, and performed 1PPL and AFM measurements. K.L. synthesized all single crystals of 2D-RPPs. All authors contributed to the overall scientific interpretation. Financial supports from Ministry of Education/National University of Singapore (MOE/NUS) grant R144-000-401-114 are acknowledged. K.P.L. acknowledges support from the National Research Foundation, Prime Minister's Office, Midsized Centre program (CA2DM), Singapore. Publisher Copyright: © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

PY - 2019/11/28

Y1 - 2019/11/28

N2 - Two-dimensional (2D) perovskites have proved to be promising semiconductors for photovoltaics, photonics, and optoelectronics. Here, a strategy is presented toward the realization of highly efficient, sub-bandgap photodetection by employing excitonic effects in 2D Ruddlesden–Popper-type halide perovskites (RPPs). On near resonance with 2D excitons, layered RPPs exhibit degenerate two-photon absorption (D-2PA) coefficients as giant as 0.2–0.64 cm MW− 1. 2D RPP-based sub-bandgap photodetectors show excellent detection performance in the near-infrared (NIR): a two-photon-generated current responsivity up to 1.2 × 104 cm2 W−2 s−1, two orders of magnitude greater than InAsSbP-pin photodiodes; and a dark current as low as 2 pA at room temperature. More intriguingly, layered-RPP detectors are highly sensitive to the light polarization of incoming photons, showing a considerable anisotropy in their D-2PA coefficients (β[001]/β[011] = 2.4, 70% larger than the ratios reported for zinc-blende semiconductors). By controlling the thickness of the inorganic quantum well, it is found that layered RPPs of (C4H9NH3)2(CH3NH3)Pb2I7 can be utilized for three-photon photodetection in the NIR region.

AB - Two-dimensional (2D) perovskites have proved to be promising semiconductors for photovoltaics, photonics, and optoelectronics. Here, a strategy is presented toward the realization of highly efficient, sub-bandgap photodetection by employing excitonic effects in 2D Ruddlesden–Popper-type halide perovskites (RPPs). On near resonance with 2D excitons, layered RPPs exhibit degenerate two-photon absorption (D-2PA) coefficients as giant as 0.2–0.64 cm MW− 1. 2D RPP-based sub-bandgap photodetectors show excellent detection performance in the near-infrared (NIR): a two-photon-generated current responsivity up to 1.2 × 104 cm2 W−2 s−1, two orders of magnitude greater than InAsSbP-pin photodiodes; and a dark current as low as 2 pA at room temperature. More intriguingly, layered-RPP detectors are highly sensitive to the light polarization of incoming photons, showing a considerable anisotropy in their D-2PA coefficients (β[001]/β[011] = 2.4, 70% larger than the ratios reported for zinc-blende semiconductors). By controlling the thickness of the inorganic quantum well, it is found that layered RPPs of (C4H9NH3)2(CH3NH3)Pb2I7 can be utilized for three-photon photodetection in the NIR region.

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KW - excitonic effects

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DO - 10.1002/adma.201904155

M3 - Journal article

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SN - 0935-9648

VL - 31

JO - Advanced Materials

JF - Advanced Materials

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M1 - 1904155

ER -

2D Perovskites with Giant Excitonic Optical Nonlinearities for High-Performance Sub-Bandgap Photodetection

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