Title: Strategies to Achieve High Circularly Polarized Luminescence from Colloidal Organic–Inorganic Hybrid Perovskite Nanocrystals

Abstract

Colloidal metal halide perovskite nanocrystals (NCs) with chiral ligands are outstanding candidates as a circularly polarized luminescence (CPL) light source due to many advantages such as high photoluminescence quantum efficiency, large spin–orbit coupling, and extensive tunability via composition and choice of organic ligands. However, achieving pronounced and controllable polarized light emission remains challenging. In this study, we develop strategies to achieve high CPL responses from colloidal formamidinium lead bromide (FAPbBr₃) NCs at room temperature using chiral surface ligands. First, we show that replacing a portion of typical ligands (oleylamine) with short chiral ligands ((R)-2-octylamine) during FAPbBr₃ NC synthesis results in small and monodisperse NCs that yield high CPL with average luminescence dissymmetry g-factor, g_lum = 6.8 × 10^–2. To the best of our knowledge, this is the highest among reported perovskite materials at room temperature to date and represents around 10-fold improvement over the previously reported colloidal CsPbCl_xBr_yI_3-x-y NCs. In order to incorporate NCs into any optoelectronic or spintronic application, the NCs necessitate purification, which removes a substantial amount of the chiral ligands and extinguishes the CPL signals. To circumvent this issue, we also developed a postsynthetic ligand treatment using a different chiral ligand, (R-/S-)methylbenzylammonium bromide, which also induces amore » CPL with an average g_lum = ±1.18 × 10^–2. This postsynthetic method is also amenable for long-range charge transport since methylbenzylammonium is quite compact in relation to other surface ligands. Our demonstrations of high CPL and g_lum from both as-synthesized and purified perovskite NCs at room temperature suggest a route to demonstrate colloidal NC-based spintronics.« less

Authors:

Kim, Young-Hoon ^[1]; Zhai, Yaxin  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-5862-1764"

Gaulding, E. Ashley ^[1]; Habisreutinger, Severin N.  ^[1];

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Moot, Taylor ^[1]; Rosales, Bryan A.  ^[1];

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Lu, Haipeng  ^[1];

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Hazarika, Abhijit  ^[1];

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Brunecky, Roman ^[1]; Wheeler, Lance M.  ^[1];

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Berry, Joseph J.  ^[1];

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Beard, Matthew C.  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-2711-1355"

Luther, Joseph M.  ^[1]

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• Search DOE PAGES for ORCID "0000-0002-4054-8244"

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+ Show Author Affiliations

1. National Renewable Energy Laboratory, Golden, Colorado 80401, United States

Publication Date:

Thu Jul 09 00:00:00 EDT 2020

Research Org.:

National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

2316078

Alternate Identifier(s):

OSTI ID: 1660163

Report Number(s):

NREL/JA-5900-76365
Journal ID: ISSN 1936-0851

Grant/Contract Number:  

AC36-08GO28308

Resource Type:

Published Article

Journal Name:

ACS Nano

Additional Journal Information:

Journal Name: ACS Nano Journal Volume: 14 Journal Issue: 7; Journal ID: ISSN 1936-0851

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; circularly polarized luminescence (CPL); nanocrystals; perovskites