Dynamic Exciton Polarons Enabling Dual-Mode White-Light Emission with Tunable Color Temperatures in 2D Hybrid Lead Bromides

White-light emission (WLE) with tunable chromaticity and correlated color temperature (CCT) is critical for lighting, display, and sensing applications. While recent two-dimensional (2D) lead halide perovskites have emerged as promising single-component WLE materials, their application is hindered by constrained and low CCT due to dominant localized exciton (LE) emission. Here, we report a dynamic exciton polaron mechanism in ⟨100⟩-oriented 2D lead bromides, (C<sub><i>n</i></sub>H<sub>2<i>n</i>+4</sub>N<sub>2</sub>)PbBr<sub>4</sub> (<i>n</i> = 5, 7, 9, 11), enabling intrinsic dual-mode WLE with widely tunable CCT. By combining ultrafast transient absorption spectroscopy and thermodynamic analyses, we reveal a double-well potential energy landscape driving the dynamic equilibrium between band-edge exciton (BE) and self-trapped LE states, and thus the formation of a dynamic exciton polaron. By elongating the ligand from <i>n</i> = 5 to 11, the self-trapping barrier decreases from 23.3 ± 1.3 to 10.1 ± 0.8 meV, and the trapping depth increases from 3.8 ± 0.4 to 14.7 ± 1.8 meV due to enhanced exciton-phonon coupling, which shifts the BE/LE emission ratio and tunes CCT from 21 000 K (bluish cold white) to 5100 K (reddish warm white). The dynamic exciton polaron with correlated BE and LE exhibits matched radiative lifetimes, ensuring stable dual-mode WLE without spectral distortion. Our work establishes that the dynamic exciton polaron, combined with ligand engineering, acts as a general principle for designing single-component multimode WLE materials with tailored chromatic properties, advancing their potential in efficient lighting and multifunctional optoelectronics.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2025-05-07
DOI
https://doi.org/10.1021/jacs.5c02446
Citations
3
Primary Topic
Perovskite Materials and Applications
Type
article
Field-Weighted Citation Impact
2.19
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article

Dynamic Exciton Polarons Enabling Dual-Mode White-Light Emission with Tunable Color Temperatures in 2D Hybrid Lead Bromides

Caiwei Zhang, Yuhang Feng, Guohua He, Haiming Zhu et al.
3 citations
Journal of the American Chemical Society
Perovskite Materials and Applications
2.19
article

Dynamic Exciton Polarons Enabling Dual-Mode White-Light Emission with Tunable Color Temperatures in 2D Hybrid Lead Bromides

Caiwei Zhang, Yuhang Feng, Guohua He, Haiming Zhu, Yao Zhang, Jinyang Yu
article en
3 citations

Abstract

White-light emission (WLE) with tunable chromaticity and correlated color temperature (CCT) is critical for lighting, display, and sensing applications. While recent two-dimensional (2D) lead halide perovskites have emerged as promising single-component WLE materials, their application is hindered by constrained and low CCT due to dominant localized exciton (LE) emission. Here, we report a dynamic exciton polaron mechanism in ⟨100⟩-oriented 2D lead bromides, (C<sub><i>n</i></sub>H<sub>2<i>n</i>+4</sub>N<sub>2</sub>)PbBr<sub>4</sub> (<i>n</i> = 5, 7, 9, 11), enabling intrinsic dual-mode WLE with widely tunable CCT. By combining ultrafast transient absorption spectroscopy and thermodynamic analyses, we reveal a double-well potential energy landscape driving the dynamic equilibrium between band-edge exciton (BE) and self-trapped LE states, and thus the formation of a dynamic exciton polaron. By elongating the ligand from <i>n</i> = 5 to 11, the self-trapping barrier decreases from 23.3 ± 1.3 to 10.1 ± 0.8 meV, and the trapping depth increases from 3.8 ± 0.4 to 14.7 ± 1.8 meV due to enhanced exciton-phonon coupling, which shifts the BE/LE emission ratio and tunes CCT from 21 000 K (bluish cold white) to 5100 K (reddish warm white). The dynamic exciton polaron with correlated BE and LE exhibits matched radiative lifetimes, ensuring stable dual-mode WLE without spectral distortion. Our work establishes that the dynamic exciton polaron, combined with ligand engineering, acts as a general principle for designing single-component multimode WLE materials with tailored chromatic properties, advancing their potential in efficient lighting and multifunctional optoelectronics.

Journal of the American Chemical SocietyVol. 147(20)
Zhejiang University of Science and Technology (CN), ASM International (Finland) (FI), Zhejiang University (CN)
Affordable and clean energy
Openalex Percentile: Top 12%
Perovskite Materials and Applications
2.19
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