Origins of Narrowband Emission in Nitrogen/Carbonyl Multiresonance Thermally Activated Delayed Fluorescence Emitters: Steric Locks and Vibrational Coupling Effects

IF 5.4 3区材料科学 Q2 CHEMISTRY, PHYSICAL

ACS Applied Energy Materials Pub Date : 2024-11-14 DOI:10.1021/acs.jpclett.4c02423

Zhipeng Guo, Yanan Zhu, Aowei Zhou, Yang Zhao, Wanli Nie, Valentina Utochnikova, Hong Meng

{"title":"Origins of Narrowband Emission in Nitrogen/Carbonyl Multiresonance Thermally Activated Delayed Fluorescence Emitters: Steric Locks and Vibrational Coupling Effects","authors":"Zhipeng Guo, Yanan Zhu, Aowei Zhou, Yang Zhao, Wanli Nie, Valentina Utochnikova, Hong Meng","doi":"10.1021/acs.jpclett.4c02423","DOIUrl":null,"url":null,"abstract":"The incorporation of tert-butyl groups and spiro-functionalization into C═O/N-embedded multiresonance thermally activated delayed fluorescence (MR-TADF) systems has yielded materials with superior narrowband emission and excellent color purity. To elucidate the mechanisms underlying the enhanced properties, we present a theoretical study of a series of fused nitrogen/carbonyl derivatives with narrower emission profiles. The key steric factors that contribute to narrowband emission were identified through energy decomposition analysis, induced by structural relaxation in states S0 and S1. Additionally, we achieved potential narrower-band and deep-blue emission by targeting the suppression of vibrational coupling effects. This work provides compelling evidence that a 1-tert-butyl substitution, acting as an end lock, offers minimal reorganization energy and optimal structural stability when combined with a fused lock. Furthermore, new compounds such as 1tBuCZQ and 1tBuDQAO have been identified as promising MR-TADF emitters, delivering ultranarrowband emission as high-quality organic light-emitting diodes.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4000,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Energy Materials","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpclett.4c02423","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}

引用次数: 0

Abstract

The incorporation of tert-butyl groups and spiro-functionalization into C═O/N-embedded multiresonance thermally activated delayed fluorescence (MR-TADF) systems has yielded materials with superior narrowband emission and excellent color purity. To elucidate the mechanisms underlying the enhanced properties, we present a theoretical study of a series of fused nitrogen/carbonyl derivatives with narrower emission profiles. The key steric factors that contribute to narrowband emission were identified through energy decomposition analysis, induced by structural relaxation in states S₀ and S₁. Additionally, we achieved potential narrower-band and deep-blue emission by targeting the suppression of vibrational coupling effects. This work provides compelling evidence that a 1-tert-butyl substitution, acting as an end lock, offers minimal reorganization energy and optimal structural stability when combined with a fused lock. Furthermore, new compounds such as 1tBuCZQ and 1tBuDQAO have been identified as promising MR-TADF emitters, delivering ultranarrowband emission as high-quality organic light-emitting diodes.

Abstract Image

查看原文本刊更多论文

氮/羰基多共振热激活延迟荧光发射器窄带发射的起源：立体锁和振动耦合效应

通过在 C═O/N 嵌入式多共振热激活延迟荧光（MR-TADF）系统中加入叔丁基和螺官能团，产生了具有卓越窄带发射和出色色纯度的材料。为了阐明增强特性的内在机制，我们对一系列具有更窄发射曲线的融合氮/羰基衍生物进行了理论研究。通过能量分解分析（由 S0 和 S1 状态的结构弛豫引起），我们确定了导致窄带发射的关键立体因素。此外，我们还通过抑制振动耦合效应实现了潜在的窄带和深蓝色发射。这项工作提供了令人信服的证据，证明 1-叔丁基取代作为端锁，与融合锁结合后可提供最小的重组能和最佳的结构稳定性。此外，1tBuCZQ 和 1tBuDQAO 等新化合物已被确定为有前途的 MR-TADF 发射器，可作为高质量的有机发光二极管实现超宽带发射。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

ACS Applied Energy Materials Materials Science-Materials Chemistry

CiteScore

10.30

自引率

6.20%

发文量

1368

期刊介绍： ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.