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.
Authors
- Caiwei Zhang
- Yuhang Feng (ORCID: https://orcid.org/0000-0002-3321-0827)
- Guohua He (ORCID: https://orcid.org/0009-0006-3874-0575)
- Haiming Zhu (ORCID: https://orcid.org/0000-0001-7747-9054)
- Yao Zhang (ORCID: https://orcid.org/0000-0002-8305-4359)
- Jinyang Yu (ORCID: https://orcid.org/0009-0004-3031-1114)
Institutions
- Zhejiang University of Science and Technology (CN)
- ASM International (Finland) (FI)
- Zhejiang University (CN)
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