Chinese Optics Letters, Volume. 20, Issue 7, 073602(2022)

Probing fluorescence quantum efficiency of single molecules in an organic matrix by monitoring lifetime change during sublimation

Penglong Ren1,2, Shangming Wei1,2, Pu Zhang1,2, and Xue-Wen Chen1,2,*
Author Affiliations
  • 1School of Physics and Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, China
  • 2Institute for Quantum Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
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    Quantum efficiency is a critical piece of information of a quantum emitter and regulates the emitter’s fluorescence decay dynamics in an optical environment through the Purcell effect. Here, we present a simple way to experimentally probe fluorescence quantum efficiency of single dibenzoterrylene molecules embedded in a thin anthracene microcrystal obtained through a co-sublimation process. In particular, we correlate the fluorescence lifetime change of single dibenzoterrylene molecules with the variation of the matrix thickness due to natural sublimation. With the identification of the molecule emission dipole orientation, we could deduce the near-unity intrinsic quantum efficiency of dibenzoterrylene molecules in the anthracene matrix.

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    1. Introduction

    Organic molecules are attractive to both physicists and chemists because molecules could have high quantum efficiencies in light emission and be chemically synthesized to have transitions at desired wavelengths. In the past several decades, single molecules embedded in solids, as isolated individual quantum systems, have become an attractive class of sources of single photons since a single two-level system cannot emit two photons simultaneously, as each excitation and emission cycle requires a finite time[1,2]. Single photons are one of the key building blocks for photonic quantum technologies, such as quantum computation, quantum key distribution, and metrology[26]. Compared to various other solid-state single-photon emitters such as self-assembled quantum dots[79], color centers in diamond[1012], and defects in two-dimensional materials[13], single molecules possess several unique properties including small size of about one nanometer (suitable for high-density doping), flexibility in the synthesis, and strong and stable Fourier-transform-limited zero-phonon lines at low temperature. In particular, 7,8:15,16-dibenzoterrylene (DBT) molecules embedded in anthracene (AC) have been actively studied as definitely stable single-photon emitters with nonblinking emission[1316] and lifetime-limited linewidth[1719]. Recent reports have explored the integration of single DBT molecules with planar photonic circuits[15,2023]. However, despite enormous studies, the quantum efficiency of single DBT molecules in the AC matrix, as a critical piece of information, has not been experimentally measured.

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    Penglong Ren, Shangming Wei, Pu Zhang, Xue-Wen Chen. Probing fluorescence quantum efficiency of single molecules in an organic matrix by monitoring lifetime change during sublimation[J]. Chinese Optics Letters, 2022, 20(7): 073602

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    Paper Information

    Category: Nanophotonics, Metamaterials, and Plasmonics

    Received: Jan. 17, 2022

    Accepted: Apr. 14, 2022

    Published Online: May. 6, 2022

    The Author Email: Xue-Wen Chen (xuewen_chen@hust.edu.cn)

    DOI:10.3788/COL202220.073602

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