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In-plane and out-of-plane excitonic coupling in 2D molecular crystals

Author

Listed:
  • Dogyeong Kim

    (Pohang University of Science and Technology (POSTECH))

  • Sol Lee

    (Yonsei University
    Center for Nanomedicine, Institute for Basic Science (IBS))

  • Jiwon Park

    (Pohang University of Science and Technology (POSTECH))

  • Jinho Lee

    (Pohang University of Science and Technology (POSTECH))

  • Hee Cheul Choi

    (Pohang University of Science and Technology (POSTECH))

  • Kwanpyo Kim

    (Yonsei University
    Center for Nanomedicine, Institute for Basic Science (IBS))

  • Sunmin Ryu

    (Pohang University of Science and Technology (POSTECH))

Abstract

Understanding the nature of molecular excitons in low-dimensional molecular solids is of paramount importance in fundamental photophysics and various applications such as energy harvesting, switching electronics and display devices. Despite this, the spatial evolution of molecular excitons and their transition dipoles have not been captured in the precision of molecular length scales. Here we show in-plane and out-of-plane excitonic evolution in quasilayered two-dimensional (2D) perylene-3, 4, 9, 10-tetracarboxylic dianhydride (PTCDA) crystals assembly-grown on hexagonal boron nitride (hBN) crystals. Complete lattice constants with orientations of two herringbone-configured basis molecules are determined with polarization-resolved spectroscopy and electron diffraction methods. In the truly 2D limit of single layers, two Frenkel emissions Davydov-split by Kasha-type intralayer coupling exhibit energy inversion with decreasing temperature, which enhances excitonic coherence. As the thickness increases, the transition dipole moments of newly emerging charge transfer excitons are reoriented because of mixing with the Frenkel states. The current spatial anatomy of 2D molecular excitons will inspire a deeper understanding and groundbreaking applications of low-dimensional molecular systems.

Suggested Citation

  • Dogyeong Kim & Sol Lee & Jiwon Park & Jinho Lee & Hee Cheul Choi & Kwanpyo Kim & Sunmin Ryu, 2023. "In-plane and out-of-plane excitonic coupling in 2D molecular crystals," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-38438-0
    DOI: 10.1038/s41467-023-38438-0
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    References listed on IDEAS

    as
    1. Kwanghee Park & Haneul Kang & Seonghyun Koo & DaeEung Lee & Sunmin Ryu, 2019. "Redox-governed charge doping dictated by interfacial diffusion in two-dimensional materials," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    2. Huijuan Zhao & Yingbo Zhao & Yinxuan Song & Ming Zhou & Wei Lv & Liu Tao & Yuzhang Feng & Biying Song & Yue Ma & Junqing Zhang & Jun Xiao & Ying Wang & Der-Hsien Lien & Matin Amani & Hyungjin Kim & Xi, 2019. "Strong optical response and light emission from a monolayer molecular crystal," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    3. Archana Raja & Andrey Chaves & Jaeeun Yu & Ghidewon Arefe & Heather M. Hill & Albert F. Rigosi & Timothy C. Berkelbach & Philipp Nagler & Christian Schüller & Tobias Korn & Colin Nuckolls & James Hone, 2017. "Coulomb engineering of the bandgap and excitons in two-dimensional materials," Nature Communications, Nature, vol. 8(1), pages 1-7, August.
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