增强供体-色团-受体系统中的光生自由基对特性,促进量子信息应用。

IF 2.7 2区 化学 Q3 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry A Pub Date : 2024-10-31 Epub Date: 2024-10-16 DOI:10.1021/acs.jpca.4c05015
Paige J Brown, Yunfan Qiu, Elisabeth I Latawiec, Brian T Phelan, Nikolai A Tcyrulnikov, Jonathan R Palmer, Matthew D Krzyaniak, Sebastian M Kopp, Yuheng Huang, Ryan M Young, Michael R Wasielewski
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引用次数: 0

摘要

我们报告了新的供体-发色团-受体三元组 BDX-ANI-NDI 和 BDX-ANI-xy-NDI,其中 BDX 供体是 2,2,6,6-四甲基苯并[1,2-d;4,5-d]双[1,3]二恶茂,ANI 发色团是 4-(N-哌啶基)萘-1,8-二甲酰亚胺,NDI 受体是萘-1,8:4,5-双(二甲酰亚胺),xy 是 2,5-xylyl 间隔物。这些化合物的研究结果与以对甲氧基苯胺(MeOAn)为供体的类似衍生物进行了比较。与 MeOAn-+ 相比,BDX-+ 没有氮原子,只有一个氢原子与其非配对电子自旋耦合,因此超频相互作用显著减少。我们使用飞秒瞬态吸收(fsTA)和纳秒 TA(nsTA)光谱(后者在施加静态磁场的情况下)研究电荷转移动力学,并确定 BDX-+-ANI-NDI-- 和 BDX-+-ANI-xy-NDI-- 在环境温度和低温下的自旋-自旋交换相互作用 (J)。对这些自旋相关自由基对(SCRPs)的时间分辨电子顺磁共振(EPR)和脉冲电子顺磁共振测量被用来探测它们的自旋动力学。我们证明,BDX-+-ANI-xy-NDI--在 85 K 的玻璃丁腈(PrCN)中具有 ∼550 μs 的超长寿命,这使得它可以用于针对量子信息科学(QIS)应用的脉冲-EPR 研究。我们还表明,BDX 基团围绕连接它与邻近苯基的单键的旋转对自旋动力学,特别是 J 的大小有重大影响。通过将这些化合物的研究结果与类似的 MeOAn 系列进行比较,我们深入了解了为量子信息科学研究创建更好的自旋相关自由基对系统的设计原则。
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Enhancing Photogenerated Radical Pair Properties in Donor-Chromophore-Acceptor Systems for Quantum Information Applications.

We report on new donor-chromophore-acceptor triads BDX-ANI-NDI and BDX-ANI-xy-NDI where the BDX donor is 2,2,6,6-tetramethylbenzo[1,2-d;4,5-d]bis[1,3]dioxole, the ANI chromophore is 4-(N-piperidinyl)naphthalene-1,8-dicarboximide, the NDI acceptor is naphthalene-1,8:4,5-bis(dicarboximide), and xy is a 2,5-xylyl spacer. The results on these compounds are compared to the analogous derivatives having a p-methoxyaniline (MeOAn) as the donor. BDX+ has no nitrogen atoms and only a single hydrogen atom coupled to its unpaired electron spin, and therefore has significantly decreased hyperfine interactions compared to MeOAn•+. We use femtosecond transient absorption (fsTA) and nanosecond TA (nsTA) spectroscopies, the latter with an applied static magnetic field, to study the charge transfer dynamics and determine the spin-spin exchange interaction (J) for BDX•+-ANI-NDI•- and BDX•+-ANI-xy-NDI•- at both ambient and cryogenic temperatures. Time-resolved electron paramagnetic resonance (EPR) and pulse-EPR measurements on these spin-correlated radical pairs (SCRPs) were used to probe their spin dynamics. We demonstrate that BDX•+-ANI-xy-NDI•- has an unusually long lifetime of ∼550 μs in glassy butyronitrile (PrCN) at 85 K, which makes it useful for pulse-EPR studies that target quantum information science (QIS) applications. We also show that rotation of the BDX group about the single bond linking it to the neighboring phenyl group has a significant impact on the spin dynamics, and in particular the magnitude of J. By comparing the results on these compounds to the analogous MeOAn series, insights into design principles for creating improved spin-correlated radical pair systems for QIS studies are obtained.

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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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