The Journal of Physical Chemistry Letters最新文献_第3页

Machine Learning Prediction of the Corrosion Rate of Zinc-Based Alloys Containing Copper, Lithium, Magnesium, and Silver

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-20 DOI: 10.1021/acs.jpclett.4c03357

Artur Davletshin, Elena A. Korznikova, Andrey A. Kistanov

引用次数: 0

Stabilizing Diketopyrrolopyrrole Radical Cations Through Carbazoles: Substitution Pattern vs Spin Delocalization

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-20 DOI: 10.1021/acs.jpclett.4c03335

Sanchari Debnath, Jungjin Park, Vithobha Hugar, Ram Kumar Canjeevaram Balasubramanyam, Juwon Oh, Woojae Kim, Satish Patil

{"title":"Stabilizing Diketopyrrolopyrrole Radical Cations Through Carbazoles: Substitution Pattern vs Spin Delocalization","authors":"Sanchari Debnath, Jungjin Park, Vithobha Hugar, Ram Kumar Canjeevaram Balasubramanyam, Juwon Oh, Woojae Kim, Satish Patil","doi":"10.1021/acs.jpclett.4c03335","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03335","url":null,"abstract":"The synthesis of organic radicals continues to garner significant interest due to their fascinating optical, electronic, and magnetic properties. Moreover, the growing demand for chemically stable organic radicals is driven by the rapid expansion of the market for electronic devices utilizing organic semiconductors. In this context, the development of multifaceted approaches for the design of stable organic radicals is of great importance. In this work, we introduce a strategy for generating stable radical cations of diketopyrrolopyrroles (DPP) by modulating the substitution pattern of the electron-donating carbazole substituent. Using electronic, spin resonance, and vibrational spectroscopies, supported by density functional theory, we carefully investigated the electronic structures and chemical stability of the DPP radical cations. Our findings demonstrate that the position of electron-rich heteroatoms and the presence of Clar’s aromatic sextets in donor moieties play a pivotal role in enhancing the chemical stability of DPP radical cations.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"496 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858021","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

Quantum Tunneling: History and Mystery of Large Amplitude Motions over a Century

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-20 DOI: 10.1021/acs.jpclett.4c02914

Ha Vinh Lam Nguyen

{"title":"Quantum Tunneling: History and Mystery of Large Amplitude Motions over a Century","authors":"Ha Vinh Lam Nguyen","doi":"10.1021/acs.jpclett.4c02914","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02914","url":null,"abstract":"Large amplitude motions (LAMs), most notably represented by proton tunneling, mark a significant departure from small amplitude vibrations where protons merely oscillate around their equilibrium positions. These substantial displacements require tunneling through potential energy barriers, leading to splittings in, e.g., rotational spectra. Since Hund’s pioneering work in 1927, proton tunneling has offered a unique glimpse into the internal dynamics of gas-phase molecules, with microwave spectroscopy being the key technique for such investigations. The ubiquous LAM type is methyl internal rotation, characterized by 3-fold potentials arising from the interaction between methyl rotors and their molecular frame, with the barrier hindering methyl torsion and the orientation of the torsional axis being defining features. Investigating methyl internal rotations plays a key role in fields ranging from molecular physics, where the methyl rotor serves as a sensitive probe for molecular structures, to atmospheric chemistry and astrophysics, where methyl-containing species have been detected in the Earth’s atmosphere and interstellar environments and even discussed as potential probes for effects beyond the standard model of physics. Despite nearly a century of study, modeling methyl internal rotations with appropriate model Hamiltonians and fully understanding the origins of these motions, particularly the factors that influence torsional barriers, remain partially unresolved, reflecting the enduring mystery of quantum tunneling. This Perspective reviews the history of LAMs, highlights advances in decoding their complex spectra, and explores future research directions aimed at uncovering the remaining mysteries of these fascinating motions.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"13 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858020","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

Multiconfigurational Electronic Structure of Nickel Cross-Coupling Catalysts Revealed by X-ray Absorption Spectroscopy

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-19 DOI: 10.1021/acs.jpclett.4c02917

Kacie J. Nelson, Nathanael P. Kazmierczak, David A. Cagan, Alec H. Follmer, Thais R. Scott, Sumana L. Raj, Douglas Garratt, Natalia Powers-Riggs, Kelly J. Gaffney, Ryan G. Hadt, Amy A. Cordones

{"title":"Multiconfigurational Electronic Structure of Nickel Cross-Coupling Catalysts Revealed by X-ray Absorption Spectroscopy","authors":"Kacie J. Nelson, Nathanael P. Kazmierczak, David A. Cagan, Alec H. Follmer, Thais R. Scott, Sumana L. Raj, Douglas Garratt, Natalia Powers-Riggs, Kelly J. Gaffney, Ryan G. Hadt, Amy A. Cordones","doi":"10.1021/acs.jpclett.4c02917","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02917","url":null,"abstract":"NiII 2,2′-bipyridine complexes are commonly invoked intermediates in metallaphotoredox cross-coupling reactions. Despite their ubiquity, design principles targeting improved catalytic performance remain underdetermined. A series of Ni(Rbpy)(R′Ar)Cl (R = MeOOC, t-Bu, R′ = CH3, CF3) complexes were proposed to have multiconfigurational electronic structures on the basis of multiconfigurational/multireference calculations, with significant mixing of Ni → bpy metal-to-ligand charge transfer (MLCT) configurations into the ground-state wave function. Here, Ni K-edge and L2,3-edge X-ray absorption spectroscopies provide experimental support for the highly covalent and multiconfigurational electronic structures of these complexes. The pre-edge intensity in the K-edge spectrum reflects highly covalent Ni–aryl bonding. The L3-edge spectral shape is dependent on ligand functionalization, and a feature reflecting the MLCT character is assigned using prior ab initio and new semiempirical calculations. The results suggest the push/pull effects of the aryl/bpy ligands moderate the changes in electron density on Ni during the multiredox cross-coupling reaction cycle.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"96 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849769","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

Kinetics of Volatile and Nonvolatile Halide Perovskite Devices: The Conductance-Activated Quasi-Linear Memristor (CALM) Model

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-19 DOI: 10.1021/acs.jpclett.4c03132

Agustín Bou, Cedric Gonzales, Pablo P. Boix, Yana Vaynzof, Antonio Guerrero, Juan Bisquert

{"title":"Kinetics of Volatile and Nonvolatile Halide Perovskite Devices: The Conductance-Activated Quasi-Linear Memristor (CALM) Model","authors":"Agustín Bou, Cedric Gonzales, Pablo P. Boix, Yana Vaynzof, Antonio Guerrero, Juan Bisquert","doi":"10.1021/acs.jpclett.4c03132","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03132","url":null,"abstract":"Memristors stand out as promising components in the landscape of memory and computing. Memristors are generally defined by a conductance mechanism containing a state variable that imparts a memory effect. The current–voltage cycling causes transitions of conductance, which are determined by different physical mechanisms, such as the formation of conducting filaments in an insulating surrounding. Here, we provide a unified description of the set and reset processes using a conductance-activated quasi-linear memristor (CALM) model with a unique voltage-dependent relaxation time of the memory variable. We focus on halide perovskite memristors and their intersection with neuroscience-inspired computing. We show that the modeling approach adeptly replicates the experimental traits of both volatile and nonvolatile memristors. Its versatility extends across various device materials and configurations, as W/SiGe/a-Si/Ag, Si/SiO2/Ag, and SrRuO3/Cr-SrZrO3/Au memristors, capturing nuanced behaviors such as scan rate and upper vertex dependence. The model also describes the response to sequences of voltage pulses that cause synaptic potentiation effects. This model is a potent tool for comprehending and probing the dynamical response of memristors by indicating the relaxation properties that control observable responses.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"53 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849763","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

Single-Atom Catalysts: Are You Really Single? 单原子催化剂：你真的是单身吗？

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-19 DOI: 10.1021/acs.jpclett.4c02844

Ana S. Dobrota, Igor A. Pašti

引用次数: 0

Correction to “Spectral Map: Embedding Slow Kinetics in Collective Variables”

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-19 DOI: 10.1021/acs.jpclett.4c03457

Jakub Rydzewski

引用次数: 0

The Synergy Effect of Al/Ti Electrodes on Effective Electron Injection for n-Channel Transistors and Ambipolar Complementary Circuits

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-19 DOI: 10.1021/acs.jpclett.4c03140

Quanhua Chen, Lijian Chen, Hong Zhu, Walid Boukhili, Guangan Yang, Xiang Wan, Zhihao Yu, Chee Leong Tan, Huabin Sun, Dongyoon Khim, Yong Xu

{"title":"The Synergy Effect of Al/Ti Electrodes on Effective Electron Injection for n-Channel Transistors and Ambipolar Complementary Circuits","authors":"Quanhua Chen, Lijian Chen, Hong Zhu, Walid Boukhili, Guangan Yang, Xiang Wan, Zhihao Yu, Chee Leong Tan, Huabin Sun, Dongyoon Khim, Yong Xu","doi":"10.1021/acs.jpclett.4c03140","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03140","url":null,"abstract":"This paper reports the utilization of cost-effective bottom-contact electrodes composed of aluminum (Al) and titanium (Ti) to facilitate efficient electron injection in n-channel organic transistors. The optimized Al/Ti electrode has a low work function of around 4.03 eV, combining the high conductivity of Al with the stable interface of Ti, making it highly suitable for the electrodes of n-channel transistors. Diketopyrrolopyrrole (DPP)-based polymeric semiconductor transistors with Al/Ti electrodes result in a notable enhancement of the n-channel performance while also leading to a significant decrease in the p-channel properties. The transmission-line method (TLM) and low-frequency noise (LFN) techniques are employed to quantitatively evaluate the effects of Al/Ti electrodes on the charge injection of n-channel OFETs. Finally, complementary inverters composed of different electrodes (Au as a p-channel and Al/Ti as an n-channel electrode) are demonstrated. The inverters showed high static and dynamic characteristics such as ideal voltage transfer curves (VTCs) with minimal hysteresis, high gain (∼25), high noise margins (68%), and low static power consumption (19.9 μW).","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"38 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849767","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

Light Harvesting Complex II Resists Non-bilayer Lipid-Induced Polymorphism in Plant Thylakoid Membranes via Lipid Redistribution

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-19 DOI: 10.1021/acs.jpclett.4c03300

Avinash Garg, Ananya Debnath

引用次数: 0

Unravelling the Effect of Oxygen on the Sintering Mechanism of Pt/CeO2 in the CO Oxidation Reaction 揭示 CO 氧化反应中氧气对 Pt/CeO2 烧结机理的影响

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-18 DOI: 10.1021/acs.jpclett.4c02935

Lei Zhang, Yiming Niu, Yinghui Pu, Yongzhao Wang, Shaoming Dong, Zhong-Wen Liu, Bingsen Zhang

{"title":"Unravelling the Effect of Oxygen on the Sintering Mechanism of Pt/CeO2 in the CO Oxidation Reaction","authors":"Lei Zhang, Yiming Niu, Yinghui Pu, Yongzhao Wang, Shaoming Dong, Zhong-Wen Liu, Bingsen Zhang","doi":"10.1021/acs.jpclett.4c02935","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02935","url":null,"abstract":"Sintering significantly contributes to the deactivation of supported metal catalysts under reaction conditions, influenced by various factors, including temperature, atmosphere, and metal–support interactions. The sintering mechanism under the reaction conditions remains complex and ambiguous. This study delves into the sintering behavior of platinum on CeO2 under CO oxidation conditions, mainly employing transmission electron microscopy to elucidate the effects of different gas components on the sintering mechanism at elevated temperatures. An atmosphere rich in oxygen promotes the sintering of Pt via the Ostwald ripening mechanism, characterized by the growth of larger nanoparticles at the expense of smaller ones. Conversely, sintering proceeds through particle migration and coalescence in the absence of oxygen, leading to the aggregation of nanoparticles. The obtained Pt/CeO2 catalysts exhibit enhanced catalytic performance after treatment with argon and stoichiometric reaction gases, contrasting with the deactivation observed under oxygen-rich conditions, which is attributed to varied Pt valence states. These findings provide insights into understanding the sintering mechanisms and inform the design of heterogeneous catalysts.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"115 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841876","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