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Fluctuating Chromatin Facilitates Enhancer–Promoter Communication by Regulating Transcriptional Clustering Dynamics 波动染色质通过调节转录聚类动态促进增强子-启动子通信
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-07 DOI: 10.1021/acs.jpclett.4c02453
Tao Zhu, Chunhe Li, Xiakun Chu
Enhancers regulate gene expression by forming contacts with distant promoters. Phase-separated condensates or clusters formed by transcription factors (TFs) and cofactors are thought to facilitate these enhancer–promoter (E–P) interactions. Using polymer physics, we developed distinct coarse-grained chromatin models that produce similar ensemble-averaged Hi-C maps but with “stable” and “dynamic” characteristics. Our findings, consistent with recent experiments, reveal a multistep E–P communication process. The dynamic model facilitates E–P proximity by enhancing TF clustering and subsequently promotes direct E–P interactions by destabilizing the TF clusters through chain flexibility. Our study promotes physical understanding of the molecular mechanisms governing E–P communication in transcriptional regulation.
增强子通过与远处的启动子形成接触来调节基因表达。由转录因子(TF)和辅助因子形成的相分离的凝聚体或簇被认为促进了这些增强子-启动子(E-P)的相互作用。利用高分子物理学,我们开发出了不同的粗粒度染色质模型,这些模型能产生类似的集合平均 Hi-C 图谱,但具有 "稳定 "和 "动态 "特征。我们的发现与最近的实验一致,揭示了一个多步骤的 E-P 交流过程。动态模型通过增强 TF 聚类来促进 E-P 接近,随后通过链的灵活性破坏 TF 聚类的稳定性来促进直接的 E-P 相互作用。我们的研究促进了对转录调控中 E-P 通信分子机制的物理理解。
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引用次数: 0
Abnormal Temperature Dependence of Huang-Rhys Factor and Exciton Recombination Kinetics in CsPbBr3 Perovskite Quantum Dots. CsPbBr3 Perovskite 量子点中 Huang-Rhys 因子和激子重组动力学的异常温度依赖性。
IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-07 Epub Date: 2024-10-28 DOI: 10.1021/acs.jpclett.4c02300
Debao Zhang, Xuguang Cao, Canyu Liu, Mingtong Chen, Wanggui Ye, Ji Zhou, Xinye Fan, Guanjun You, Changcheng Zheng, Jiqiang Ning, Shijie Xu

Anomalous thermal behaviors of excitonic luminescence in CsPbBr3 perovskite quantum dots (PQDs) were observed. It is found that the main luminescence peak originated from the excitonic radiative recombination assisted by the longitudinal-optical (LO) phonon, and its integrated intensity first declines as the temperature varies from 10 to 150 K and then turns to increase at ∼160 K, reaching a maximum value at 300 K. A model considering the thermal detrapping and transfer of electrons from a trap level is developed to interpret these abnormal thermal behaviors of the luminescence from the PQDs. On the other hand, the quantum-mechanical multimode Brownian oscillator model was employed to unravel that the Huang-Rhys factor exclusively characterizing the exciton-phonon coupling in the studied CsPbBr3 PQDs decreases from 1.65 at 10 K to 1.31 at 200 K.

在 CsPbBr3 包晶量子点(PQDs)中观察到了激子发光的反常热行为。研究发现,主发光峰源于纵向光(LO)声子辅助的激子辐射重组,其积分强度随着温度在 10 至 150 K 之间的变化先是下降,然后在 ∼ 160 K 时转为上升,并在 300 K 时达到最大值。另一方面,利用量子力学多模布朗振荡器模型揭示了所研究的 CsPbBr3 PQDs 中专门表征激子-声子耦合的 Huang-Rhys 因子从 10 K 时的 1.65 下降到 200 K 时的 1.31。
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引用次数: 0
Ultrafast Time-Domain Spectroscopy Reveals Coherent Vibronic Couplings upon Electronic Excitation in Crystalline Organic Thin Films. 超快时域光谱揭示晶体有机薄膜电子激发时的相干振动耦合。
IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-07 Epub Date: 2024-10-31 DOI: 10.1021/acs.jpclett.4c02711
Somayeh Souri, Daniel Timmer, Daniel C Lünemann, Naby Hadilou, Katrin Winte, Antonietta De Sio, Martin Esmann, Franziska Curdt, Michael Winklhofer, Sebastian Anhäuser, Michele Guerrini, Ana M Valencia, Caterina Cocchi, Gregor Witte, Christoph Lienau

The coherent coupling between electronic excitations and vibrational modes of molecules largely affects the optical and charge transport properties of organic semiconductors and molecular solids. To analyze these couplings by means of ultrafast spectroscopy, highly ordered crystalline films with large domains are particularly suitable because the domains can be addressed individually, hence allowing azimuthal polarization-resolved measurements. Impressive examples of this are highly ordered crystalline thin films of perfluoropentacene (PFP) molecules, which adopt different molecular orientations on different alkali halide substrates. Here, we report polarization-resolved time-domain vibrational spectroscopy with 10 fs time resolution and Raman spectroscopy of crystalline PFP thin films grown on NaF(100) and KCl(100) substrates. Coherent oscillations in the time-resolved spectra reveal vibronic coupling to a high-frequency, 25 fs, in-plane deformation mode that is insensitive to the optical polarization, while the coupling to a lower-frequency, 85 fs, out-of-plane ring bending mode depends significantly on the crystalline and molecular orientation. Comparison with calculated Raman spectra of isolated PFP molecules in vacuo supports this interpretation and indicates a dominant role of solid-state effects in the vibronic properties of these materials. Our results represent a first step toward uncovering the role of anisotropic vibronic couplings for singlet fission processes in crystalline molecular thin films.

电子激发和分子振动模式之间的相干耦合在很大程度上影响着有机半导体和分子固体的光学和电荷传输特性。要通过超快光谱分析这些耦合,具有大晶域的高度有序结晶薄膜尤为合适,因为晶域可以单独处理,从而实现方位偏振分辨测量。这方面令人印象深刻的例子是全氟并五苯(PFP)分子的高度有序结晶薄膜,它们在不同的卤化碱基底上具有不同的分子取向。在此,我们报告了在 NaF(100) 和 KCl(100) 基质上生长的全氟并五苯结晶薄膜的 10 fs 时间分辨率偏振分辨时域振动光谱和拉曼光谱。时间分辨光谱中的相干振荡揭示了与高频(25 fs)面内形变模式的振子耦合,这种耦合对光学偏振不敏感,而与低频(85 fs)面外环形弯曲模式的耦合则在很大程度上取决于晶体和分子取向。与真空中分离的全氟辛烷磺酸分子的拉曼光谱的计算结果进行比较,支持这一解释,并表明固态效应在这些材料的振动特性中起着主导作用。我们的研究结果为揭示晶体分子薄膜中单子裂变过程中各向异性振子耦合的作用迈出了第一步。
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引用次数: 0
Warm-White Light Emission of Lead-free CsAg2I3 Single Crystal Scintillator with a One-Dimensional Electronic Structure. 具有一维电子结构的无铅 CsAg2I3 单晶闪烁体的暖白光发射。
IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-07 Epub Date: 2024-10-29 DOI: 10.1021/acs.jpclett.4c02725
Lu Cheng, Wanying Zou, Lei Cao, Danwen Zhang, Xilei Sun, Yang Liu, Haiying He, Yongsheng Huang, Wei Zheng

Presently, the exploration of novel inorganic lead-free perovskite scintillators has emerged as a prominent topic in the field of perovskite materials. Extensive attention has been garnered by materials such as Cs3Cu2I5 due to their notable advantage in scintillation intensity, but the response time constants in the microsecond or even millisecond range severely constrain their potential applications in scintillators. In this study, large-sized (5-6 mm) CsAg2I3 single crystals with an ultrafast warm-white light emission on a nanosecond time scale are presented. Specifically, upon X-ray excitation, the single crystal demonstrates a broad-spectrum white light emission with a color temperature as high as 5129 K, attributed to its self-trapped exciton emission. The 137Cs energy spectrum reveals that CsAg2I3 possesses an ultrafast response for γ rays with a time constant of 15 ns, which is significantly faster than that of Cs3Cu2I5. Furthermore, time-resolved photoluminescence unveils a subnanosecond component with a response time of 0.9 ns. The characteristics of ultrafast warm-white light emission exhibit the significant potential of CsAg2I3 in radiation scintillation detection and its probability of playing a pivotal role in future radiation detection technology.

目前,探索新型无机无铅闪烁体已成为闪烁体材料领域的一个重要课题。Cs3Cu2I5 等材料因其在闪烁强度方面的显著优势而受到广泛关注,但其微秒甚至毫秒级的响应时间常数严重制约了其在闪烁体中的潜在应用。本研究展示了具有纳秒级超快暖白光发射的大尺寸(5-6 毫米)CsAg2I3 单晶。具体来说,在 X 射线激发下,该单晶体会发出色温高达 5129 K 的宽光谱白光,这归因于其自俘获激子发射。137Cs 能谱显示,CsAg2I3 对 γ 射线具有超快响应,时间常数为 15 ns,明显快于 Cs3Cu2I5。此外,时间分辨光致发光揭示了一个响应时间为 0.9 ns 的亚纳秒成分。超快暖白光发射的特性显示了 CsAg2I3 在辐射闪烁探测方面的巨大潜力,并有可能在未来的辐射探测技术中发挥关键作用。
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引用次数: 0
Oxygen Concentration Effect in Photosensitized Generation of 1O2 from Normoxia to Hypoxia. 从正常缺氧到缺氧过程中光敏生成 1O2 的氧气浓度效应
IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-07 Epub Date: 2024-10-31 DOI: 10.1021/acs.jpclett.4c02547
Zong Chang, Like Guo, Jianglan Cai, Yang Shu, Jie Ding, Qinchao Sun

Photodynamic therapy (PDT) has gained widespread acceptance as a clinical cancer treatment modality and has been attracting intensive attention on developing novel PDT strategies. However, the hypoxic environment in tumors is considered as a significant challenge for efficient type II PDT, based on the inference of the highly oxygen-concentration-related 1O2 generation. Contrary to this conventional understanding, our research demonstrates oxygen concentration independence in the photosensitized generation of 1O2, as evidenced through steady-state and transient spectroscopy for chlorin e6 and methylene blue from normoxic to hypoxic conditions. We propose an oxygen-concentration-independent kinetic model, suggesting that efficient 1O2 generation can take place as long as the triplet-state lifetime ratio of the photosensitizer (τhn) is in a similar range to pO2n/pO2h. Our findings provide insights into PDT mechanisms and indicate that the oxygen concentration reduction concerns may not be critical for effective PDT in hypoxic tumor environments.

作为一种临床癌症治疗方法,光动力疗法(PDT)已被广泛接受,开发新型光动力疗法策略也一直备受关注。然而,根据与氧浓度高度相关的 1O2 生成推论,肿瘤中的低氧环境被认为是高效 II 型光动力疗法面临的重大挑战。与这一传统认识相反,我们的研究证明了 1O2 的光敏生成与氧浓度无关,这一点通过氯素 e6 和亚甲蓝从常氧到缺氧条件下的稳态和瞬态光谱分析得到了证明。我们提出了一个与氧浓度无关的动力学模型,认为只要光敏剂的三重态寿命比(τh/τn)与 pO2n/pO2h 的范围相似,就能高效生成 1O2。我们的研究结果提供了对光导放疗机制的深入了解,并表明氧浓度降低问题可能不是缺氧肿瘤环境中有效光导放疗的关键。
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引用次数: 0
Spectroscopic Differentiation of Structural Transitions from Carbon Nanobelts to Carbon Nanotubes. 从碳纳米管到碳纳米管的结构转变的光谱差异。
IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-07 Epub Date: 2024-10-31 DOI: 10.1021/acs.jpclett.4c02555
Jungpil Kim

In this study, simulated X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy were utilized to differentiate the early stage structures as carbon nanobelts (CNBs) evolved into carbon nanotubes (CNTs). The effects of edge type, length, and diameter on the spectroscopic characteristics of armchair and zigzag CNTs were examined. Variations in XPS spectra were found to correspond to changes in the bandgap, while Raman spectra provided distinct bands associated with specific structural features. Notably, in armchair CNTs, the C 1s XPS peak positions exhibited clear differences depending on the structure. Additionally, the Kekulé vibration band and other characteristic bands in Raman spectra varied with length and diameter, enabling differentiation of armchair CNT structures. Although the structural analysis of zigzag CNTs was challenging using XPS, Raman spectroscopy proved to be effective in distinguishing structural differences. This study lays the groundwork for future spectroscopic analyses, contributing to the broader understanding of nanocarbon materials such as CNBs and CNTs and their potential applications in advanced electronic materials.

本研究利用模拟 X 射线光电子能谱 (XPS) 和拉曼光谱来区分碳纳米管 (CNT) 演化成碳纳米管 (CNB) 的早期结构。研究了边缘类型、长度和直径对扶手形和人字形碳纳米管光谱特性的影响。研究发现,XPS 光谱的变化与带隙的变化相对应,而拉曼光谱则提供了与特定结构特征相关的独特波段。值得注意的是,在扶手形 CNT 中,C 1s XPS 峰位置因结构不同而有明显差异。此外,拉曼光谱中的 Kekulé 振动带和其他特征带也随长度和直径的变化而变化,从而实现了对 armchair CNT 结构的区分。尽管使用 XPS 分析人字形 CNT 的结构具有挑战性,但拉曼光谱在区分结构差异方面证明是有效的。这项研究为未来的光谱分析奠定了基础,有助于更广泛地了解 CNB 和 CNT 等纳米碳材料及其在先进电子材料中的潜在应用。
{"title":"Spectroscopic Differentiation of Structural Transitions from Carbon Nanobelts to Carbon Nanotubes.","authors":"Jungpil Kim","doi":"10.1021/acs.jpclett.4c02555","DOIUrl":"10.1021/acs.jpclett.4c02555","url":null,"abstract":"<p><p>In this study, simulated X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy were utilized to differentiate the early stage structures as carbon nanobelts (CNBs) evolved into carbon nanotubes (CNTs). The effects of edge type, length, and diameter on the spectroscopic characteristics of armchair and zigzag CNTs were examined. Variations in XPS spectra were found to correspond to changes in the bandgap, while Raman spectra provided distinct bands associated with specific structural features. Notably, in armchair CNTs, the C 1s XPS peak positions exhibited clear differences depending on the structure. Additionally, the Kekulé vibration band and other characteristic bands in Raman spectra varied with length and diameter, enabling differentiation of armchair CNT structures. Although the structural analysis of zigzag CNTs was challenging using XPS, Raman spectroscopy proved to be effective in distinguishing structural differences. This study lays the groundwork for future spectroscopic analyses, contributing to the broader understanding of nanocarbon materials such as CNBs and CNTs and their potential applications in advanced electronic materials.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":4.8,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142542932","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Nonlinear Optical Properties of the Topological Material Bi2Se3 Family for the Application of an Ultrafast Pulse Laser Based on the Occupied and Unoccupied Band Structures 基于占带和非占带结构的拓扑材料 Bi2Se3 家族的非线性光学特性--用于超快脉冲激光器的应用
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-07 DOI: 10.1021/acs.jpclett.4c02600
Yujiu Jiang, Xiaowei Xing, Peng Zhu, Kejian Wang, Zhiyang Zhang, Qi Liu, Zhiwei Wang, Wenjun Liu, Jinjian Zhou, Junfeng Han
The Bi2Se3 family can exhibit many intriguing topological insulator properties, including a narrow bandgap and strong surface states, which show excellent nonlinear optical properties. Thinning bulk Bi2Se3 family materials to create a low-cost photoelectric modulation device and explaining the mechanisms of nonlinear optical differences in different types of materials remain challenges. Based on liquid-phase exfoliation technology and tapered fiber, this work prepared optoelectronic modulation devices for various samples within the Bi2Se3 family, quantitatively compared their nonlinear optical properties, and analyzed the sources of differentiation using the occupied and unoccupied multiband structure theory. The results correspond well to the phenomena observed in the ultrafast laser, which will provide strong support for the design of higher performance photoelectric devices based on topological insulators.
Bi2Se3 族材料可表现出许多引人入胜的拓扑绝缘体特性,包括窄带隙和强表面态,从而显示出卓越的非线性光学特性。稀释块状 Bi2Se3 家族材料以制造低成本光电调制器件,以及解释不同类型材料的非线性光学差异机制,仍然是一项挑战。本研究基于液相剥离技术和锥形光纤,制备了Bi2Se3家族中不同样品的光电调制器件,定量比较了它们的非线性光学特性,并利用占位和非占位多带结构理论分析了差异的来源。研究结果与在超快激光器中观察到的现象十分吻合,这将为设计基于拓扑绝缘体的更高性能光电器件提供有力支持。
{"title":"Nonlinear Optical Properties of the Topological Material Bi2Se3 Family for the Application of an Ultrafast Pulse Laser Based on the Occupied and Unoccupied Band Structures","authors":"Yujiu Jiang, Xiaowei Xing, Peng Zhu, Kejian Wang, Zhiyang Zhang, Qi Liu, Zhiwei Wang, Wenjun Liu, Jinjian Zhou, Junfeng Han","doi":"10.1021/acs.jpclett.4c02600","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02600","url":null,"abstract":"The Bi<sub>2</sub>Se<sub>3</sub> family can exhibit many intriguing topological insulator properties, including a narrow bandgap and strong surface states, which show excellent nonlinear optical properties. Thinning bulk Bi<sub>2</sub>Se<sub>3</sub> family materials to create a low-cost photoelectric modulation device and explaining the mechanisms of nonlinear optical differences in different types of materials remain challenges. Based on liquid-phase exfoliation technology and tapered fiber, this work prepared optoelectronic modulation devices for various samples within the Bi<sub>2</sub>Se<sub>3</sub> family, quantitatively compared their nonlinear optical properties, and analyzed the sources of differentiation using the occupied and unoccupied multiband structure theory. The results correspond well to the phenomena observed in the ultrafast laser, which will provide strong support for the design of higher performance photoelectric devices based on topological insulators.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594505","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Resistance of a PdAu12(8e) Core to Growth in Collision-Induced Sequential Reductive Elimination of (C≡CR)2 from [PdAu24(C≡CR)18]2. PdAu12(8e) 内核在[PdAu24(C≡CR)18]2 碰撞诱导 (C≡CR)2 顺序还原消解过程中的生长阻力。
IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-07 Epub Date: 2024-10-29 DOI: 10.1021/acs.jpclett.4c02798
Shun Ito, Koto Hirano, Kiichirou Koyasu, Xian-Kai Wan, Quan-Ming Wang, Tatsuya Tsukuda

Previous studies have reported that [PdAu24(PAF)18]2- (PAF = 3,5-(CF3)2C6H3C≡C) with an icosahedral superatomic PdAu12(8e) core underwent collision-induced sequential reductive elimination (CISRE) of 1,3-diyne (PAF)2 ( J. Phys. Chem. C 2020, 124, 19119). The most likely scenario after the CISRE of (PAF)2 is the growth of the PdAu12(8e) core via the fusion of the Au(0) atoms produced from the Au2(PAF)3 units on the core surface. Contrary to expectation, anion photoelectron spectroscopy and theoretical calculations regarding the CISRE products [PdAu24(PAF)18-2n]2- (n = 1-6) revealed that the electronically closed PdAu12(8e) core does not grow to a single superatom with (8 + 2n)e but assembles with Au2(2e) units. Characterization of the CISRE products of other alkynyl-protected Au clusters suggested that even the non-superatomic Au17(8e) core was resistant to growth due probably to rigidification by PA ligands. We propose that there is a kinetic bottleneck in the growth process of protected Au clusters at the stage where they are electronically closed and/or lose their structural fluxionality by ligation.

先前的研究报告称,具有二十面体超原子 PdAu12(8e) 内核的 [PdAu24(PAF)18]2- (PAF = 3,5-(CF3)2C6H3C≡C) 经历了 1,3 二炔 (PAF)2 的碰撞诱导顺序还原消除 (CISRE) ( J. Phys. Chem. C 2020, 124, 19119)。(PAF)2发生CISRE后最可能的情况是,通过核表面Au2(PAF)3单元产生的Au(0)原子的融合,PdAu12(8e)核增长。与预期相反,阴离子光电子能谱和有关 CISRE 产物 [PdAu24(PAF)18-2n]2- (n = 1-6)的理论计算显示,电子封闭的 PdAu12(8e) 内核并没有成长为具有 (8 + 2n)e 的单个超原子,而是与 Au2(2e) 单元组装在一起。对其他炔基保护金簇的 CISRE 产物进行的表征表明,即使是非超原子的 Au17(8e) 内核也可能由于 PA 配体的刚性化而无法生长。我们认为,在受保护金簇的生长过程中,在其电子封闭和/或因连接而失去结构通性的阶段存在一个动力学瓶颈。
{"title":"Resistance of a PdAu<sub>12</sub>(8e) Core to Growth in Collision-Induced Sequential Reductive Elimination of (C≡CR)<sub>2</sub> from [PdAu<sub>24</sub>(C≡CR)<sub>18</sub>]<sup>2</sup>.","authors":"Shun Ito, Koto Hirano, Kiichirou Koyasu, Xian-Kai Wan, Quan-Ming Wang, Tatsuya Tsukuda","doi":"10.1021/acs.jpclett.4c02798","DOIUrl":"10.1021/acs.jpclett.4c02798","url":null,"abstract":"<p><p>Previous studies have reported that [PdAu<sub>24</sub>(PA<sup>F</sup>)<sub>18</sub>]<sup>2-</sup> (PA<sup>F</sup> = 3,5-(CF<sub>3</sub>)<sub>2</sub>C<sub>6</sub>H<sub>3</sub>C≡C) with an icosahedral superatomic PdAu<sub>12</sub>(8e) core underwent collision-induced sequential reductive elimination (CISRE) of 1,3-diyne (PA<sup>F</sup>)<sub>2</sub> ( <i>J. Phys. Chem. C</i> 2020, 124, 19119). The most likely scenario after the CISRE of (PA<sup>F</sup>)<sub>2</sub> is the growth of the PdAu<sub>12</sub>(8e) core via the fusion of the Au(0) atoms produced from the Au<sub>2</sub>(PA<sup>F</sup>)<sub>3</sub> units on the core surface. Contrary to expectation, anion photoelectron spectroscopy and theoretical calculations regarding the CISRE products [PdAu<sub>24</sub>(PA<sup>F</sup>)<sub>18-2<i>n</i></sub>]<sup>2-</sup> (<i>n</i> = 1-6) revealed that the electronically closed PdAu<sub>12</sub>(8e) core does not grow to a single superatom with (8 + 2<i>n</i>)e but assembles with Au<sub>2</sub>(2e) units. Characterization of the CISRE products of other alkynyl-protected Au clusters suggested that even the non-superatomic Au<sub>17</sub>(8e) core was resistant to growth due probably to rigidification by PA ligands. We propose that there is a kinetic bottleneck in the growth process of protected Au clusters at the stage where they are electronically closed and/or lose their structural fluxionality by ligation.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":4.8,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142520272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Toward Efficient Modeling of Nonradiative Decay in Extended INVEST: Overcoming Computational Challenges in Quantum Dynamics Simulations. 在扩展 INVEST 中实现非辐射衰变的高效建模:克服量子动力学模拟中的计算挑战。
IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-07 Epub Date: 2024-10-29 DOI: 10.1021/acs.jpclett.4c02713
Alessandro Landi, Gaetano Ricci, Yoann Olivier, Amedeo Capobianco, Andrea Peluso

In recent years, an increasing number of fully organic molecules capable of thermally activated delayed fluorescence (TADF) have been reported, often with very small or even inverted singlet-triplet (INVEST) energy gaps. These molecules typically exhibit complex photophysics due to the close energy levels of multiple singlet and triplet states, which create various transition pathways toward emission. A predictive model for the rates of these transitions is thus essential for assessing the suitability of new materials for light-emitting devices. Quantum Dynamics (QD) calculations are ideal for this purpose, as they include quantum effects, without the limitations of first-order perturbative approaches, also allowing taking into account more than two electronic states at once. However, the huge computational demands of QD methodologies, especially for large molecules, currently limit their use as a standard tool. To address this problem, we here employ a strategy that allows us to include almost the whole set of the vibrational coordinates by selecting the key elements of the Hilbert space that significantly impact dynamics, thereby hugely reducing the computational burden. Application of this protocol to two relatively large INVEST molecules reveals that internal conversion in these systems is very fast, making indirect emissive pathways a possible channel for the population of the S1 state. More importantly, this study demonstrates that the dynamics can be accurately described even with a significantly reduced vibrational space, thus allowing quantum dynamics calculations that yield accurate transition rates in a few minutes of computational time.

近年来,越来越多能够产生热激活延迟荧光(TADF)的全有机分子被报道出来,它们通常具有非常小甚至倒置的单线态-三线态(INVEST)能隙。由于多个单线态和三线态的能级接近,这些分子通常会表现出复杂的光物理特性,从而产生各种发射过渡途径。因此,这些转变速率的预测模型对于评估新材料是否适合用于发光器件至关重要。量子动力学(QD)计算是实现这一目的的理想方法,因为它包含量子效应,不受一阶微扰方法的限制,还能同时考虑两个以上的电子状态。然而,QD 方法的计算量巨大,尤其是对于大分子,目前限制了其作为标准工具的使用。为了解决这个问题,我们在这里采用了一种策略,通过选择希尔伯特空间中对动力学有重大影响的关键元素,我们几乎可以包含整套振动坐标,从而大大减轻了计算负担。将这一方案应用于两个相对较大的 INVEST 分子后发现,这些系统中的内部转换非常快,从而使间接发射途径成为 S1 态群体的可能通道。更重要的是,这项研究表明,即使振动空间大幅缩小,也能准确描述动力学,因此量子动力学计算只需几分钟的计算时间就能获得准确的转换率。
{"title":"Toward Efficient Modeling of Nonradiative Decay in Extended INVEST: Overcoming Computational Challenges in Quantum Dynamics Simulations.","authors":"Alessandro Landi, Gaetano Ricci, Yoann Olivier, Amedeo Capobianco, Andrea Peluso","doi":"10.1021/acs.jpclett.4c02713","DOIUrl":"10.1021/acs.jpclett.4c02713","url":null,"abstract":"<p><p>In recent years, an increasing number of fully organic molecules capable of thermally activated delayed fluorescence (TADF) have been reported, often with very small or even inverted singlet-triplet (INVEST) energy gaps. These molecules typically exhibit complex photophysics due to the close energy levels of multiple singlet and triplet states, which create various transition pathways toward emission. A predictive model for the rates of these transitions is thus essential for assessing the suitability of new materials for light-emitting devices. Quantum Dynamics (QD) calculations are ideal for this purpose, as they include quantum effects, without the limitations of first-order perturbative approaches, also allowing taking into account more than two electronic states at once. However, the huge computational demands of QD methodologies, especially for large molecules, currently limit their use as a standard tool. To address this problem, we here employ a strategy that allows us to include almost the whole set of the vibrational coordinates by selecting the key elements of the Hilbert space that significantly impact dynamics, thereby hugely reducing the computational burden. Application of this protocol to two relatively large INVEST molecules reveals that internal conversion in these systems is very fast, making indirect emissive pathways a possible channel for the population of the S<sub>1</sub> state. More importantly, this study demonstrates that the dynamics can be accurately described even with a significantly reduced vibrational space, thus allowing quantum dynamics calculations that yield accurate transition rates in a few minutes of computational time.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":4.8,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142520283","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Regulation of Sensitized Phosphorescence in Two-Dimensional Lead Bromine Perovskites by Tuning Excited-State Interactions. 通过调谐激发态相互作用调节二维溴化铅过氧化物中的敏化磷光。
IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-07 Epub Date: 2024-10-31 DOI: 10.1021/acs.jpclett.4c02570
Yuming Deng, Xinyue Liu, Lan Jiang, Yongfeng Zhang, Yingchu Dong, Qianyu Liu, Xinyu Liu, Guoquan Gao, Yuanyuan Guo, Gang Tang, Cheng Zhu, Qi Chen, Tong Zhu

Excited-state interactions within the organic layer play a critical role in sensitized phosphorescence of two-dimensional (2D) perovskites. Herein, we regulate excited-state interactions utilizing isomeric organic ligands 1-naphthylmethylamine (1-NMA) and 1-(2-naphthyl)-methanamine (2-NMA). Transient absorption and first-principles calculations are employed to elucidate the mechanisms of triplet energy transfer (TET) and triplet excimer formation. The results indicate that wave function hybridization and tunneling effect at the inorganic/organic interface contribute to rapid (∼20 ps) and highly efficient (>98%) TET, with the triplet excimer being generated in (1-NMA)2PbBr4 at picosecond time-scale. However, triplet excimer is barely observed in (2-NMA)2PbBr4 due to varying ligand stacking modes. Despite rapid TET, the efficiency of sensitized phosphorescence is low (<0.5%), which is ascribed to pronounced nonradiative decay. By mixing isomeric ligands and optimizing respective ratio, a maximum phosphorescence enhancement of 7.6 folds is achieved. This work provides a detailed mechanistic understanding of triplet excimer sensitization and regulation of sensitized phosphorescence.

有机层内的激发态相互作用在二维(2D)包晶石的敏化磷光中起着至关重要的作用。在此,我们利用异构有机配体 1-萘基甲胺(1-NMA)和 1-(2-萘基)-甲胺(2-NMA)来调节激发态相互作用。瞬态吸收和第一原理计算被用来阐明三重能转移(TET)和三重准分子形成的机制。结果表明,无机/有机界面上的波函数杂化和隧道效应促成了快速(∼20 ps)和高效(>98%)的三重能转移(TET),三重准分子在 (1-NMA)2PbBr4 中产生的时间为皮秒级。然而,由于配体堆叠模式的不同,在 (2-NMA)2PbBr4 中几乎观察不到三重准分子。尽管 TET 速度很快,但敏化磷光的效率却很低 (
{"title":"Regulation of Sensitized Phosphorescence in Two-Dimensional Lead Bromine Perovskites by Tuning Excited-State Interactions.","authors":"Yuming Deng, Xinyue Liu, Lan Jiang, Yongfeng Zhang, Yingchu Dong, Qianyu Liu, Xinyu Liu, Guoquan Gao, Yuanyuan Guo, Gang Tang, Cheng Zhu, Qi Chen, Tong Zhu","doi":"10.1021/acs.jpclett.4c02570","DOIUrl":"10.1021/acs.jpclett.4c02570","url":null,"abstract":"<p><p>Excited-state interactions within the organic layer play a critical role in sensitized phosphorescence of two-dimensional (2D) perovskites. Herein, we regulate excited-state interactions utilizing isomeric organic ligands 1-naphthylmethylamine (1-NMA) and 1-(2-naphthyl)-methanamine (2-NMA). Transient absorption and first-principles calculations are employed to elucidate the mechanisms of triplet energy transfer (TET) and triplet excimer formation. The results indicate that wave function hybridization and tunneling effect at the inorganic/organic interface contribute to rapid (∼20 ps) and highly efficient (>98%) TET, with the triplet excimer being generated in (1-NMA)<sub>2</sub>PbBr<sub>4</sub> at picosecond time-scale. However, triplet excimer is barely observed in (2-NMA)<sub>2</sub>PbBr<sub>4</sub> due to varying ligand stacking modes. Despite rapid TET, the efficiency of sensitized phosphorescence is low (<0.5%), which is ascribed to pronounced nonradiative decay. By mixing isomeric ligands and optimizing respective ratio, a maximum phosphorescence enhancement of 7.6 folds is achieved. This work provides a detailed mechanistic understanding of triplet excimer sensitization and regulation of sensitized phosphorescence.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":4.8,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142542931","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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The Journal of Physical Chemistry Letters
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