The Journal of Physical Chemistry Letters最新文献

Temperature Dependence of Photoinduced Carrier Spin Relaxation Dynamics in CsPbBr3 and MAPbBr3 Perovskite Quantum Dots CsPbBr3和MAPbBr3钙钛矿量子点光诱导载流子自旋弛豫动力学的温度依赖性

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-01 DOI: 10.1021/acs.jpclett.5c01192

Mariam Khvichia, David C. Zeitz, Kai-Chun Chou, Yuan Ping, Jin Z. Zhang

{"title":"Temperature Dependence of Photoinduced Carrier Spin Relaxation Dynamics in CsPbBr3 and MAPbBr3 Perovskite Quantum Dots","authors":"Mariam Khvichia, David C. Zeitz, Kai-Chun Chou, Yuan Ping, Jin Z. Zhang","doi":"10.1021/acs.jpclett.5c01192","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01192","url":null,"abstract":"Temperature dependent carrier spin relaxation dynamics of CH3NH3PbBr3 (MAPbBr3) and CsPbBr3 perovskite quantum dots (PQDs) have been studied at room temperature (RT), 150 K, and 77 K using spin selective femtosecond transient absorption (fs-TA) spectroscopy. Results reveal minimal temperature dependence in the MAPbBr3 PQDs with a lifetime of 2.2 ps. In contrast, the CsPbBr3 PQDs show strong temperature dependence, with the carrier spin lifetime increasing from RT (2.0 ps) to 150 K (11 ps) and to 77 K (57 ps). This behavior suggests the two PQD systems exhibit different carrier spin relaxation mechanisms. The dominant mechanism in CsPbBr3 PQDs is attributed to the Eliot–Yafet (EY) mechanism, modulated primarily by an electron–phonon interaction that is reduced at cryogenic temperatures. In contrast, for the MAPbBr3 PQDs the D’yakonov–Perel (DP) mechanism is dominant, likely due to broken inversion symmetry associated with the presence of MA, which induces a dynamical Rashba effect at finite temperature.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"9 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144188976","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}

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Optical Addressability of the Arylnitrene Spin Triplet 芳基硝基自旋三重态的光学寻址性

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-31 DOI: 10.1021/acs.jpclett.5c01024

Gaetano Ricci, Claire Tonnelé, David Casanova

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Computational Screening of Ligands for Enhanced Interactions between Lead Halide Perovskite Quantum Dots 卤化铅钙钛矿量子点间增强相互作用配体的计算筛选

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-31 DOI: 10.1021/acs.jpclett.5c01307

Elizabeth Stippell, Carlos Mora Perez, Nicholas Favate, Libai Huang, Christina W. Li, Oleg V. Prezhdo

{"title":"Computational Screening of Ligands for Enhanced Interactions between Lead Halide Perovskite Quantum Dots","authors":"Elizabeth Stippell, Carlos Mora Perez, Nicholas Favate, Libai Huang, Christina W. Li, Oleg V. Prezhdo","doi":"10.1021/acs.jpclett.5c01307","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01307","url":null,"abstract":"Ligand choice in nanoparticle systems is vital for developing efficient materials and enhancing electronic and chemical properties. Focusing on CsPbBr3, we demonstrate a strategy for modifying the electronic properties of lead halide perovskites through a systematic computational study on ligands with varying binding motifs, sizes, bridge lengths, π-electron conjugation, and electron withdrawing and donating groups. The calculations are benchmarked against experimental data. Choosing a ligand’s π-electron system and binding group, followed by tuning the ligand’s properties with substituents to the π-system, allows one to introduce ligand electronic states into the perovskite system’s bands, close to band edges, and inside the material’s fundamental band gap. One can also design surface states by inducing local distortions at the binding site, which can be tuned by altering the binding group of the ligand. Extension of a material’s frontier orbitals onto ligands and the creation of surface states make charges available for transport and chemical reactivity, while avoiding charge trapping. In contrast, midgap ligand states trap charges permanently. Large ligands with high coverages interact among themselves, influencing ligand electronic properties and binding. Carboxylate tends to bind more strongly than the ammonium group. Electronegative oxygens in the carboxylate binding group and electron withdrawing substituents bound to the π-system lower ligand orbital energies relative to perovskite states. The reported theoretical analysis guides experimental design of perovskite–ligand systems for optoelectronic, energy, and quantum information applications.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"55 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144183875","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}

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Tuning the Triplet State of Ligands on FAPbBr3 Quantum Dots toward Low-Threshold Distributed Feedback Lasers FAPbBr3量子点上配体的三重态向低阈值分布反馈激光器调谐

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-31 DOI: 10.1021/acs.jpclett.5c01012

Guitai Fan, Feng Zhang, Zilong Lu, Zihan Ren, Tianrui Zhai

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Unveiling DNA Hybridization Dynamics via High-Sensitivity SERS Detection: Insights into Conformational Changes and Oligonucleotide Length Effects 揭示DNA杂交动力学通过高灵敏度SERS检测：洞察构象变化和寡核苷酸长度效应

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-29 DOI: 10.1021/acs.jpclett.5c00600

Daria Stoia, Dana Maniu, Monica Potara, Ana-Maria Craciun, Mathieu Edely, Serban Grecu, Alida Timar-Gabor, Simion Astilean, Monica Focsan, Marc Lamy de la Chapelle

{"title":"Unveiling DNA Hybridization Dynamics via High-Sensitivity SERS Detection: Insights into Conformational Changes and Oligonucleotide Length Effects","authors":"Daria Stoia, Dana Maniu, Monica Potara, Ana-Maria Craciun, Mathieu Edely, Serban Grecu, Alida Timar-Gabor, Simion Astilean, Monica Focsan, Marc Lamy de la Chapelle","doi":"10.1021/acs.jpclett.5c00600","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00600","url":null,"abstract":"This study demonstrates the highly sensitive detection of DNA hybridization using commercially available Surface-Enhanced Raman Spectroscopy (SERS) substrates. We functionalized the gold nanostructures with thiolated single-stranded adenine (polyA) DNA of various lengths (5–20 bases) and investigated their hybridization with complementary thymine (polyT) strands across different concentrations. DNA hybridization was confirmed by significant spectral changes in the adenine ring breathing mode at 735 cm–1, highlighting its potential as a key marker for hybridization detection. Finite-difference time-domain (FDTD) simulations were used to visualize the distribution of the electromagnetic field at the gold surface. In parallel, principal component analysis (PCA) successfully identified spectral changes resulting from DNA hybridization. By combining experimental SERS measurements with computational modeling, we present a highly sensitive and specific method for monitoring DNA hybridization. These results support the development of advanced nucleic acid detection techniques and offer a reliable platform for investigating biomolecular interactions.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"26 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165718","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}

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Deciphering d–sp Orbital Interaction in MnSe2–CoSe2 with a Built-in Electric Field toward Enhanced Water and Seawater Oxidation Electrocatalysis 基于内建电场的MnSe2-CoSe2中d-sp轨道相互作用对水和海水氧化电催化的影响

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-29 DOI: 10.1021/acs.jpclett.5c01074

Lei Yuan, Xingmei Guo, Yuqi Chen, Qing Wang, Zhongyao Duan, Qianqian Fan, Xiangjun Zheng, Yuanjun Liu, Qinghong Kong, Junhao Zhang

{"title":"Deciphering d–sp Orbital Interaction in MnSe2–CoSe2 with a Built-in Electric Field toward Enhanced Water and Seawater Oxidation Electrocatalysis","authors":"Lei Yuan, Xingmei Guo, Yuqi Chen, Qing Wang, Zhongyao Duan, Qianqian Fan, Xiangjun Zheng, Yuanjun Liu, Qinghong Kong, Junhao Zhang","doi":"10.1021/acs.jpclett.5c01074","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01074","url":null,"abstract":"Constructing efficient hybridized catalysts for water and seawater electrolysis, along with an understanding of their function mechanisms, is essential for advancing green hydrogen production. Herein, a uniform MnSe2–CoSe2 coating is constructed on graphite felt (GF) through a straightforward electrodeposition–selenization approach. The in situ cocrystallization process generates numerous heterointerfaces, which enhance catalytic activity and stability through the establishment of an internal electric field and the modulation of d–sp orbital interactions. Specifically, antibonding regulation facilitates the adsorption and desorption of oxygen-related species, enabling MnSe2–CoSe2/GF to require low overpotentials of 363 and 394 mV to achieve 500 mA cm–2 oxygen evolution in alkaline water and seawater, respectively. Meanwhile, bonding enhancement contributes to improved chemical stability and corrosion resistance, allowing the catalyst to remain stable for more than 200 h with a minimal 9.8% current decay during seawater oxidation. This study provides an innovative method for constructing interface-wealthy heterogeneous structures and reveals the mechanisms behind high-performance seawater electrocatalysis, which is highly valuable for green hydrogen production.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"58 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177307","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}

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Thermal Conductivity and Nonlinear Temperature Dependent Raman Line-Shape Asymmetry in Spinel Co3O4: Inhomogeneous Laser Heating Revisited 尖晶石Co3O4的热导率和非线性温度相关拉曼线形不对称性：非均匀激光加热的再研究

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-29 DOI: 10.1021/acs.jpclett.5c00935

Shivam Kumar, Deb Kumar Rath, Sharmistha Singh, Soumya Tiwari, Subin Kaladi Chondath, Love Bansal, Bhumika Sahu, Nikita Ahlawat, Partha Sarathi Rout, Saumya Srivastava, Anjali Chaudhary, Rajesh Kumar

{"title":"Thermal Conductivity and Nonlinear Temperature Dependent Raman Line-Shape Asymmetry in Spinel Co3O4: Inhomogeneous Laser Heating Revisited","authors":"Shivam Kumar, Deb Kumar Rath, Sharmistha Singh, Soumya Tiwari, Subin Kaladi Chondath, Love Bansal, Bhumika Sahu, Nikita Ahlawat, Partha Sarathi Rout, Saumya Srivastava, Anjali Chaudhary, Rajesh Kumar","doi":"10.1021/acs.jpclett.5c00935","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00935","url":null,"abstract":"Inhomogeneous laser heating has been revisited here in nanocrystalline Co3O4 by means of laser flux dependent Raman scattering experiments. The exploration of microscopic phenomena in nanoscale semiconductors is pivotal for their integration into various industrial applications. Notably, the presence of laser heating effects in such systems serves as a crucial tool for investigating the quantum properties of materials. The evolution of asymmetric Raman line-shapes with increasing laser flux reveals an entirely distinct behavior of the A1g Raman band in Co3O4 nanoparticles compared to their microcrystalline and bulk counterparts. This phenomenon has been further substantiated through the estimation of the local temperature rise and the corresponding thermal conductivity across three different dimensions of Co3O4. These findings offer profound insight into the thermal and quantum dynamics of nanostructured materials.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"19 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165773","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}

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Exciton Dynamic Processes in Colloidal CdS/CdSe/CdS Quantum Well Nanostructures 胶体CdS/CdSe/CdS量子阱纳米结构中的激子动态过程

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-29 DOI: 10.1021/acs.jpclett.5c01150

Ruixiang Xiong, Yibo Li, Chaoyi Yang, Shumin Jiang, Binhao Yang, Yinghui Wang, Jiajia Ning

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Improving Performance and Stability of Solution-Processed Organic Poly-gridofluorene Light-Emitting Diodes via Deuterated Solvents 用氘化溶剂提高溶液法制备有机聚芴发光二极管的性能和稳定性

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-29 DOI: 10.1021/acs.jpclett.5c01157

Hao Li, Mengna Yu, Jiangqiang He, Menghan Wu, Yang Li, Manman Luo, Kuande Wang, Yan Li, Yunfei Zhu, Qianyi Li, Qiuhu Han, Shasha Wang, Zhikuan Chen, Quanyou Feng, Linghai Xie

{"title":"Improving Performance and Stability of Solution-Processed Organic Poly-gridofluorene Light-Emitting Diodes via Deuterated Solvents","authors":"Hao Li, Mengna Yu, Jiangqiang He, Menghan Wu, Yang Li, Manman Luo, Kuande Wang, Yan Li, Yunfei Zhu, Qianyi Li, Qiuhu Han, Shasha Wang, Zhikuan Chen, Quanyou Feng, Linghai Xie","doi":"10.1021/acs.jpclett.5c01157","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01157","url":null,"abstract":"Toluene and chloroform are widely utilized as solvents in optoelectronic device fabrication, but their carcinogenic properties and potential misuse in illicit drug synthesis subject them to strict state regulation. In contrast, their deuterated counterparts (toluene-d8 and chloroform-d) are not recognized as carcinogens by the World Health Organization’s International Agency for Research on Cancer (IARC), presenting a safer alternative. Leveraging seawater-derived deuterium’s natural abundance, we implemented these deuterated solvents for spin-coating superhindered poly-gridofluorene (PODPFG) emissive layers in solution-processed OLEDs. Comparative studies revealed that films fabricated with deuterated solvents demonstrated a nearly 26% enhancement in PLQY and improved luminescence stability. Notably, the devices showed increased external quantum efficiency from 0.72% to 1.12% while preserving deep blue color purity. These improvements are attributed to the formation of larger and ordered aggregates through enhanced intermolecular interactions in deuterated media, which promote optimal interchain aggregation. Our approach establishes a novel paradigm for isotope engineering in green manufacturing of solution-processed OLEDs, simultaneously addressing toxicity concerns and performance optimization through solvent-mediated morphological control for nontoxic, green manufacturing practices and industrial applications.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"9 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177343","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}

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Machine Learning Accelerated Discovery of Antimicrobial Inorganic Nanomaterials 机器学习加速抗菌无机纳米材料的发现

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-29 DOI: 10.1021/acs.jpclett.5c00865

Yonghui Gao, Limin Shang, Jing Liu, Zhiling Zhu

{"title":"Machine Learning Accelerated Discovery of Antimicrobial Inorganic Nanomaterials","authors":"Yonghui Gao, Limin Shang, Jing Liu, Zhiling Zhu","doi":"10.1021/acs.jpclett.5c00865","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00865","url":null,"abstract":"The growing prevalence of infectious diseases and the increasing threat of bacterial resistance have drawn widespread attention to antimicrobial inorganic nanomaterials. However, the diversity, abundance, and complex mechanisms of these materials present significant challenges in identifying new agents that are both efficient and cost-effective with broad-spectrum activity. In response, this study applied machine learning for the first time to discover antimicrobial inorganic nanomaterials. Information on over 2,000 antimicrobial nanomaterials was extracted from more than 8,000 papers. An unsupervised machine learning analysis was conducted to assess data distribution and explore the relationships between material features and antimicrobial activity in high-dimensional space. A series of machine learning models were trained. Through the evaluation of six performance metrics, five key features were identified from 27 dimensions. To further quantify the structure–activity relationships, a genetic programming-symbolic classification model was employed to generate a precise mathematical formula with a prediction accuracy of 0.83. Using this formula, 43 new antimicrobial inorganic nanomaterials were predicted. Of these, four nanomaterials were synthesized and their antibacterial properties were experimentally validated. This work not only provides a next generation approach for designing antimicrobial inorganic nanomaterials but also opens new avenues for applying machine learning in materials science.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"26 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165719","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