Sugai Yoshiki, Rahane Vijay P, Gale Innes, Verdi Carla, Ireland Alexander R, Canola Sofia, McGregor Sarah K M, Moore Evan G, Jain Nidhi, Namdas Ebinazar B, Lo Shih-Chun
School of Chemistry and Molecular Biosciences, the University of Queensland, Brisbane 4072, Queensland, Australia.
The University of Queensland-Indian Institute of Technology Delhi Academy of Research, Hauz Khas, New Delhi 110016, India.
ACS Appl Mater Interfaces. 2024 Sep 4;16(35):46506-46515. doi: 10.1021/acsami.4c07286. Epub 2024 Aug 19.
Organic lasers have attracted increasing attention owing to their superior characteristics such as lightweight, low-cost manufacturing, high mechanical flexibility, and high emission-wavelength tunability. Recent breakthroughs include electrically pumped organic laser diodes and an electrically driven organic laser, integrated with an organic light-emitting diode pumping. However, the availability of efficient deep blue organic laser chromophores remains limited. In this study, we develop two novel rigid oligophenylenes, end-capped with carbazole and phenylcarbazole groups, to demonstrate exceptional optical and amplified spontaneous emission (ASE) properties. These oligophenylenes are not only solution processable but also exhibit remarkably high solution photoluminescence quantum yields (PLQYs) of 90% and high radiative rates of 1.35 × 10 s in the deep blue range. Our theoretical calculations confirm that the carbazole and phenylcarbazole end groups play a pivotal role in enhancing the optical transitions of the oligophenylene laser chromophores, thereby elevating their emission oscillator strengths. Remarkably, these materials demonstrate low solid-state ASE threshold values of 1.0 and 1.5 μJ/cm (at 431 and 418 nm, respectively). To the best of our knowledge, these ASE thresholds represent the lowest reported at these specific ASE wavelengths in the literature, regardless of whether they are solution-processed or thermally evaporated films. Furthermore, they exhibit excellent thermal and photostability, low triplet quantum yields, as well as negligible overlap of excited-state absorption within the ASE emission region, making them excellent candidates for a new class of deep blue materials for organic lasers. By integrating insights from theoretical calculations and experimental validation, our study provides a comprehensive understanding of the design principles behind these high-performing organic laser chromophores, paving the way for the development of advanced organic lasers with enhanced performance characteristics.
有机激光器因其具有诸如重量轻、制造成本低、高机械柔韧性和高发射波长可调性等优异特性而受到越来越多的关注。最近的突破包括电泵浦有机激光二极管和与有机发光二极管泵浦集成的电驱动有机激光器。然而,高效深蓝色有机激光发色团的可用性仍然有限。在本研究中,我们开发了两种新型的刚性低聚苯撑,其端基为咔唑和苯基咔唑基团,以展示出优异的光学和放大自发辐射(ASE)特性。这些低聚苯撑不仅可溶液加工,而且在深蓝色范围内还表现出高达90%的显著高溶液光致发光量子产率(PLQYs)和1.35×10 s的高辐射率。我们的理论计算证实,咔唑和苯基咔唑端基在增强低聚苯撑激光发色团的光学跃迁中起关键作用,从而提高其发射振子强度。值得注意的是,这些材料在固态下表现出低ASE阈值,分别为1.0和1.5 μJ/cm(分别在431和418 nm处)。据我们所知,无论它们是溶液加工的还是热蒸发薄膜,这些ASE阈值在文献中报道的这些特定ASE波长下都是最低的。此外,它们表现出优异的热稳定性和光稳定性、低三重态量子产率,以及ASE发射区域内激发态吸收的重叠可忽略不计,使其成为一类新型深蓝色有机激光材料的极佳候选者。通过整合理论计算和实验验证的见解,我们的研究提供了对这些高性能有机激光发色团背后设计原理的全面理解,为开发具有增强性能特征的先进有机激光器铺平了道路。