Two-dimensional-lattice-confined single-molecule-like aggregates

Kang Wang, Zih-Yu Lin, Angana De, Conrad A. Kocoj, Wenhao Shao, Hanjun Yang, Zehua He, Aidan H. Coffey, Colton B. Fruhling, Yuanhao Tang, Dharini Varadharajan, Chenhui Zhu, Yong Sheng Zhao, Alexandra Boltasseva, Vladimir M. Shalaev, Peijun Guo, Brett M. Savoie () and Letian Dou ()
Additional contact information
Kang Wang: Purdue University
Zih-Yu Lin: Purdue University
Angana De: Purdue University
Conrad A. Kocoj: Yale University
Wenhao Shao: Purdue University
Hanjun Yang: Purdue University
Zehua He: Institute of Chemistry, Chinese Academy of Sciences
Aidan H. Coffey: Lawrence Berkeley National Laboratory
Colton B. Fruhling: Purdue University
Yuanhao Tang: Purdue University
Dharini Varadharajan: Purdue University
Chenhui Zhu: Lawrence Berkeley National Laboratory
Yong Sheng Zhao: Institute of Chemistry, Chinese Academy of Sciences
Alexandra Boltasseva: Purdue University
Vladimir M. Shalaev: Purdue University
Peijun Guo: Yale University
Brett M. Savoie: Purdue University
Letian Dou: Purdue University

Nature, 2024, vol. 633, issue 8030, 567-574

Abstract: Abstract Intermolecular distance largely determines the optoelectronic properties of organic matter. Conventional organic luminescent molecules are commonly used either as aggregates or as single molecules that are diluted in a foreigner matrix. They have garnered great research interest in recent decades for a variety of applications, including light-emitting diodes1,2, lasers3–5 and quantum technologies6,7, among others8–10. However, there is still a knowledge gap on how these molecules behave between the aggregation and dilution states. Here we report an unprecedented phase of molecular aggregate that forms in a two-dimensional hybrid perovskite superlattice with a near-equilibrium distance, which we refer to as a single-molecule-like aggregate (SMA). By implementing two-dimensional superlattices, the organic emitters are held in proximity, but, surprisingly, remain electronically isolated, thereby resulting in a near-unity photoluminescence quantum yield, akin to that of single molecules. Moreover, the emitters within the perovskite superlattices demonstrate strong alignment and dense packing resembling aggregates, allowing for the observation of robust directional emission, substantially enhanced radiative recombination and efficient lasing. Molecular dynamics simulations together with single-crystal structure analysis emphasize the critical role of the internal rotational and vibrational degrees of freedom of the molecules in the two-dimensional lattice for creating the exclusive SMA phase. This two-dimensional superlattice unifies the paradoxical properties of single molecules and aggregates, thus offering exciting possibilities for advanced spectroscopic and photonic applications.

Date: 2024
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DOI: 10.1038/s41586-024-07925-9

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