溴查尔酮衍生物的双光子吸收和激发态动力学。

IF 2.8 2区 化学 Q3 CHEMISTRY, PHYSICAL
Nathan B Marucci, João V P Valverde, Gabriel de O Campos, Eli S A Ducas, Pablo J Gonçalves, Leonardo De Boni, Cleber R Mendonça
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引用次数: 0

摘要

有机化合物中的双光子吸收(2PA)由于其在非线性光学中的应用而引起了极大的兴趣,包括双光子荧光显微镜、光动力治疗和激光微加工。本文采用实验和计算相结合的方法研究了4′-溴查尔酮衍生物的双光子吸收截面(2PACS)和激发态动力学。利用密度泛函理论(DFT)和时变DFT (TD-DFT)进行量子化学计算,分析了分子的电子性质。实验表征包括线性光学测量(紫外-可见吸收和荧光光谱)、飞秒瞬态吸收光谱(TAS)和开孔(AO) z扫描测量,以确定简并2PACS (D-2PACS)。我们的研究结果表明共振供体取代基,如二甲胺基,增强了非线性吸收,特别是在低能带。此外,TAS还揭示了与扭曲分子内电荷转移(TICT)态形成相关的有趣动力学,这一点得到了各向异性和溶剂变色测量以及计算模拟的证实。这些发现为分子结构与非线性光学性质之间的关系提供了见解,有助于开发用于光子应用的优化材料。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Two-Photon Absorption and Dynamics of Excited States in Bromochalcone Derivatives.

Two-photon absorption (2PA) in organic compounds has gained significant interest due to its applications in nonlinear optics, including two-photon fluorescence microscopy, photodynamic therapy, and laser microfabrication. This study investigates the two-photon absorption cross section (2PACS) and the excited-state dynamics of 4'-bromochalcone derivatives using a combination of experimental and computational approaches. Quantum chemical calculations employing density functional theory (DFT) and time-dependent DFT (TD-DFT) were performed to analyze the electronic properties of the molecules. Experimental characterization involved linear optical measurements (UV-vis absorption and fluorescence spectroscopy), femtosecond transient absorption spectroscopy (TAS), and open-aperture (AO) Z-scan measurements to determine the degenerate 2PACS (D-2PACS). Our results reveal that resonant donor substituents, such as the dimethylamino group, enhance nonlinear absorption, especially in the lower-energy band. Furthermore, TAS revealed an intriguing dynamic associated with the formation of a twisted intramolecular charge transfer (TICT) state, which was corroborated by anisotropy and solvatochromism measurements as well as by computational simulations. These findings provide insights into the relationship between the molecular structure and nonlinear optical properties, contributing to the development of optimized materials for photonic applications.

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来源期刊
The Journal of Physical Chemistry A
The Journal of Physical Chemistry A 化学-物理:原子、分子和化学物理
CiteScore
5.20
自引率
10.30%
发文量
922
审稿时长
1.3 months
期刊介绍: The Journal of Physical Chemistry A is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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