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Low Amplified Spontaneous Emission Threshold from Solution Processable Excited-State Intramolecular Proton Transfer Chromophores
Advanced Optical Materials ( IF 8.0 ) Pub Date : 2024-06-17 , DOI: 10.1002/adom.202400840
Vijay P. Rahane 1, 2, 3, 4 , Atul Shukla 4, 5 , Ras Baizureen Roseli 3 , Alexander R. Ireland 3 , Innes Gale 3, 4 , Elizabeth H. Krenske 3 , Evan G. Moore 3 , Ebinazar B. Namdas 4, 5 , Nidhi Jain 2 , Shih‐Chun Lo 3, 4
Advanced Optical Materials ( IF 8.0 ) Pub Date : 2024-06-17 , DOI: 10.1002/adom.202400840
Vijay P. Rahane 1, 2, 3, 4 , Atul Shukla 4, 5 , Ras Baizureen Roseli 3 , Alexander R. Ireland 3 , Innes Gale 3, 4 , Elizabeth H. Krenske 3 , Evan G. Moore 3 , Ebinazar B. Namdas 4, 5 , Nidhi Jain 2 , Shih‐Chun Lo 3, 4
Affiliation
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Chromophores undergoing excited-state intramolecular proton transfer (ESIPT) feature a distinct four-level photocycle and significant Stokes shift, which make them ideal for achieving population inversion upon photoexcitation, a fundamental prerequisite for lasing, by mitigating the concerns of self-absorption owing to spectral overlap. This study focuses on functionalizing the hydroxyphenyl-benzothiazole (HBT) ESIPT laser dye through the introduction of fluorene and phenyl-carbazole moieties at the para-position to the hydroxyl group, to demonstrate amplified spontaneous emission (ASE) activities. The synthesized HBT derivatives not only exhibit high thermal and photostability, but also high photoluminescence quantum yields, exceeding 40%, which is noteworthy for ESIPT materials emitting in the yellow–orange to red color ranges. Computational analyses show that these new HBT materials possess substantially lower ESIPT energy barriers, compared to their parent HBT, facilitating their efficient ESIPT processes. Moreover, these derivatives demonstrate a high radiative rate of 1.47 × 108 s−1. Thin films of a fluorene-substituted HBT (HBT-pFl) show a low solid-state amplified spontaneous emission threshold value of 3.8 µJ cm−2 at 582 nm, representing the lowest reported solid-state ASE threshold for laser dyes in the orange emission region (575–600 nm) to date.
中文翻译：
可溶液处理的激发态分子内质子转移发色团的低放大自发发射阈值
经历激发态分子内质子转移（ESIPT）的发色团具有独特的四级光循环和显着的斯托克斯位移，这使得它们非常适合在光激发时实现粒子数反转，这是激光发射的基本先决条件，通过减轻由于自吸收引起的问题光谱重叠。本研究重点是通过在羟基的对位引入芴和苯基咔唑部分来功能化羟基苯基苯并噻唑 ( HBT ) ESIPT 激光染料，以证明放大的自发发射 (ASE) 活性。合成的HBT衍生物不仅表现出较高的热稳定性和光稳定性，而且具有超过40%的高光致发光量子产率，这对于在黄橙色到红色范围内发光的ESIPT材料来说是值得注意的。计算分析表明，与母体 HBT 相比，这些新型 HBT 材料的 ESIPT 能垒要低得多，从而促进了高效的 ESIPT 过程。此外，这些衍生物表现出1.47×10 8 s -1的高辐射率。芴取代的 HBT ( HBT - pFl ) 薄膜在 582 nm 处表现出 3.8 µJ cm -2的低固态放大自发发射阈值，代表了橙色发射中激光染料的最低固态 ASE 阈值迄今为止的区域（575-600 nm）。
更新日期：2024-06-17
中文翻译：
可溶液处理的激发态分子内质子转移发色团的低放大自发发射阈值
经历激发态分子内质子转移（ESIPT）的发色团具有独特的四级光循环和显着的斯托克斯位移，这使得它们非常适合在光激发时实现粒子数反转，这是激光发射的基本先决条件，通过减轻由于自吸收引起的问题光谱重叠。本研究重点是通过在羟基的对位引入芴和苯基咔唑部分来功能化羟基苯基苯并噻唑 ( HBT ) ESIPT 激光染料，以证明放大的自发发射 (ASE) 活性。合成的HBT衍生物不仅表现出较高的热稳定性和光稳定性，而且具有超过40%的高光致发光量子产率，这对于在黄橙色到红色范围内发光的ESIPT材料来说是值得注意的。计算分析表明，与母体 HBT 相比，这些新型 HBT 材料的 ESIPT 能垒要低得多，从而促进了高效的 ESIPT 过程。此外，这些衍生物表现出1.47×10 8 s -1的高辐射率。芴取代的 HBT ( HBT - pFl ) 薄膜在 582 nm 处表现出 3.8 µJ cm -2的低固态放大自发发射阈值，代表了橙色发射中激光染料的最低固态 ASE 阈值迄今为止的区域（575-600 nm）。
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