The Journal of Physical Chemistry Letters最新文献_第10页

Structure-Resolved Monitoring of Single-Wall Carbon Nanotube Functionalization from Raman Intermediate Frequency Modes 拉曼中频模式下单壁碳纳米管功能化的结构分辨监测

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-08-30 DOI: 10.1021/acs.jpclett.3c02100

Nima Soltani, Yu Zheng, Sergei M. Bachilo and R. Bruce Weisman*,

引用次数: 0

Elucidating the Self-cleavage Dynamics of Hairpin Ribozyme by Mode-decomposed Infrared Spectroscopy 用模式分解红外光谱研究发夹核酶的自裂解动力学

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-08-30 DOI: 10.1021/acs.jpclett.3c01724

Adnan Gulzar*, Jan Noetzel, Harald Forbert and Dominik Marx,

引用次数: 0

Atomic Positional Embedding-Based Transformer Model for Predicting the Density of States of Crystalline Materials 基于原子位置嵌入的晶体材料态密度预测变压器模型

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-08-30 DOI: 10.1021/acs.jpclett.3c02036

Yaning Cui, Kang Chen, Lingyao Zhang, Haotian Wang, Lei Bai, David Elliston and Wei Ren*,

{"title":"Atomic Positional Embedding-Based Transformer Model for Predicting the Density of States of Crystalline Materials","authors":"Yaning Cui, Kang Chen, Lingyao Zhang, Haotian Wang, Lei Bai, David Elliston and Wei Ren*, ","doi":"10.1021/acs.jpclett.3c02036","DOIUrl":"https://doi.org/10.1021/acs.jpclett.3c02036","url":null,"abstract":"The rapid advancement of machine learning has revolutionized quite a few science fields, leading to a surge in the development of highly efficient and accurate materials discovery methods. Recently, predictions of multiple related properties have received attention, with a particular emphasis on spectral properties, where the electronic density of states (DOS) stands out as the fundamental data with enormous potential to advance our understanding of crystalline materials. Leveraging the power of the Transformer framework, we introduce an Atomic Positional Embedding-Based Transformer (APET), which surpasses existing state-of-the-art models for predicting ab initio DOS. APET utilizes atomic periodical positions as its positional embedding, which incorporates all of the structural information in a crystal, providing a more complete and accurate representation. Furthermore, the interpretability of APET enables us to discover the underlying physical properties of materials with greater precision and accuracy.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 35","pages":"7924–7930"},"PeriodicalIF":5.7,"publicationDate":"2023-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"221370","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

Revealing Charge-Transfer Dynamics at Buried Charge-Selective Heterointerface in Highly Effective Perovskite Solar Cells 揭示高效钙钛矿太阳能电池中埋藏电荷选择异质界面的电荷转移动力学

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-08-30 DOI: 10.1021/acs.jpclett.3c02138

Di Li, Shaobing Xiong, Bo Peng, Weimin Liu*, Bo Li* and Qinye Bao*,

{"title":"Revealing Charge-Transfer Dynamics at Buried Charge-Selective Heterointerface in Highly Effective Perovskite Solar Cells","authors":"Di Li, Shaobing Xiong, Bo Peng, Weimin Liu*, Bo Li* and Qinye Bao*, ","doi":"10.1021/acs.jpclett.3c02138","DOIUrl":"https://doi.org/10.1021/acs.jpclett.3c02138","url":null,"abstract":"The suboptimal carrier dynamics at the heterointerface between the perovskite and charge transport layer severely limit further performance enhancement of the state-of-the-art perovskite solar cells (PSCs). Herein, we completely map charge carrier extraction and recombination kinetics over a broad time range at buried electron-selective heterointerfaces via ultrafast transient technologies. It is revealed that the heterointerfaces carefully contain the electronic processes of free charge generation in perovskite within ∼2.8 ps, relaxation process of trap-state induced electron capturing less than ∼10.0 ps, electron extraction from perovskite to SnO2 within ∼194 ps, trap-assisted recombination within ∼2047 ps, and recombination between back-injected electrons and remaining holes within ∼8.4 ns. Moreover, we further demonstrate that the inserted poly(vinyl alcohol) (PVA) thin layer can effectively enhance the electron extraction from perovskite to SnO2, block the undesired electron back injection, and significantly suppress the nonradiative recombination, contributing to the improved device parameters of photovoltage and fill factor. This work sheds light on charge-transfer limitations at the perovskite buried heterointerface and provides an effective guide of ideal heterointerface design for promoting charge transfer and improving PSC performance.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 35","pages":"7953–7959"},"PeriodicalIF":5.7,"publicationDate":"2023-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"218733","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

Triplet Formation in a 9,10-Bis(phenylethynyl)anthracene Dimer and Trimer Occurs by Charge Recombination Rather than Singlet Fission 9,10-二(苯乙基)蒽二聚体和三聚体中的三重态是通过电荷重组而不是单线态裂变形成的

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-08-29 DOI: 10.1021/acs.jpclett.3c02050

Rasmus Ringström, Zachary W. Schroeder, Letizia Mencaroni, Pavel Chabera, Rik R. Tykwinski and Bo Albinsson*,

{"title":"Triplet Formation in a 9,10-Bis(phenylethynyl)anthracene Dimer and Trimer Occurs by Charge Recombination Rather than Singlet Fission","authors":"Rasmus Ringström, Zachary W. Schroeder, Letizia Mencaroni, Pavel Chabera, Rik R. Tykwinski and Bo Albinsson*, ","doi":"10.1021/acs.jpclett.3c02050","DOIUrl":"https://doi.org/10.1021/acs.jpclett.3c02050","url":null,"abstract":"We present an experimental study investigating the solvent-dependent dynamics of a 9,10-bis(phenylethynyl)anthracene monomer, dimer, and trimer. Using transient absorption spectroscopy, we have discovered that triplet excited state formation in the dimer and trimer molecules in polar solvents is a consequence of charge recombination subsequent to symmetry-breaking charge separation rather than singlet fission. Total internal reflection emission measurements of the monomer demonstrate that excimer formation serves as the primary decay pathway at a high concentration. In the case of highly concentrated solutions of the trimer, we observe evidence of triplet formation without the prior formation of a charge-separated state. We postulate that this is attributed to the formation of small aggregates, suggesting that oligomers mimicking the larger chromophore counts in crystals could potentially facilitate singlet fission. Our experimental study sheds light on the intricate dynamics of the 9,10-bis(phenylethynyl)anthracene system, elucidating the role of solvent- and concentration-dependent factors for triplet formation and charge separation.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 35","pages":"7897–7902"},"PeriodicalIF":5.7,"publicationDate":"2023-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.jpclett.3c02050","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"192381","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ionic Solvent-Assisted MAPbBr3 Perovskite Film for Two-Photon Pumped Single-Mode Laser 离子溶剂辅助双光子泵浦单模激光器用MAPbBr3钙钛矿膜

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-08-29 DOI: 10.1021/acs.jpclett.3c01959

Zijun Zhan, Zhiping Hu, Sihao Huang, Siyu Dong, Qian Li, Zhengzheng Liu*, Juan Du* and Yuxin Leng*,

{"title":"Ionic Solvent-Assisted MAPbBr3 Perovskite Film for Two-Photon Pumped Single-Mode Laser","authors":"Zijun Zhan, Zhiping Hu, Sihao Huang, Siyu Dong, Qian Li, Zhengzheng Liu*, Juan Du* and Yuxin Leng*, ","doi":"10.1021/acs.jpclett.3c01959","DOIUrl":"https://doi.org/10.1021/acs.jpclett.3c01959","url":null,"abstract":"Miniaturized coherent light sources on the nanoscale are highly desired for on-chip photonics integration. However, when approaching the diffraction limit, the sub-wavelength-scale all-dielectric lasers are difficult to realize due to the trade-off between lasing performance and physical size. Especially for a thin-film laser, usually an externally complex cavity is required to provide the necessary optical feedback. Herein, we successfully shrink the MAPbBr3 perovskite thin-film laser to sub-wavelength scale (300 nm) with simplified cavity design using only an ultraviolet glue layer and a quartz glass. The morphology quality and the gain properties of the film are enhanced by introducing ionic liquid. Consequently, the stable and low-threshold single-mode laser with a highly linear polarization degree of 78.6% and a narrow line width of 0.35 nm is achieved under two-photon excitation. The excellent single-mode laser with sub-wavelength scale and ultrasimplified structure could provide a facile and versatile platform for future integrated optoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 35","pages":"7903–7909"},"PeriodicalIF":5.7,"publicationDate":"2023-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"192384","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

Spin-Flip Unitary Coupled Cluster Method: Toward Accurate Description of Strong Electron Correlation on Quantum Computers 量子计算机上强电子相关的精确描述

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-08-28 DOI: 10.1021/acs.jpclett.3c01935

Fabijan Pavošević*, Ivano Tavernelli and Angel Rubio,

{"title":"Spin-Flip Unitary Coupled Cluster Method: Toward Accurate Description of Strong Electron Correlation on Quantum Computers","authors":"Fabijan Pavošević*, Ivano Tavernelli and Angel Rubio, ","doi":"10.1021/acs.jpclett.3c01935","DOIUrl":"https://doi.org/10.1021/acs.jpclett.3c01935","url":null,"abstract":"Quantum computers have emerged as a promising platform to simulate strong electron correlation that is crucial to catalysis and photochemistry. However, owing to the choice of a trial wave function employed in the variational quantum eigensolver (VQE) algorithm, accurate simulation is restricted to certain classes of correlated phenomena. Herein, we combine the spin-flip (SF) formalism with the unitary coupled cluster with singles and doubles (UCCSD) method via the quantum equation-of-motion (qEOM) approach to allow for an efficient simulation of a large family of strongly correlated problems. We show that the developed qEOM-SF-UCCSD/VQE method outperforms its UCCSD/VQE counterpart for simulation of the cis–trans isomerization of ethylene, and the automerization of cyclobutadiene and the predicted qEOM-SF-UCCSD/VQE barrier heights are in a good agreement with the experimentally determined values. The developments presented herein will further stimulate the investigation of this approach for simulations of other types of correlated/entangled phenomena on quantum computers.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 35","pages":"7876–7882"},"PeriodicalIF":5.7,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"211188","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: 4

Slip-Enhanced Transport by Graphene in the Microporous Layer for High Power Density Proton-Exchange Membrane Fuel Cells 高功率密度质子交换膜燃料电池微孔层中石墨烯的滑移增强输运

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-08-28 DOI: 10.1021/acs.jpclett.3c01661

Ye Liu, Ningran Wu, Haiou Zeng, Dandan Hou, Shengping Zhang, Yue Qi, Ruizhi Yang and Luda Wang*,

引用次数: 1

Application of a Fluctuating Charge Polarization Model to Large Polyaromatic Hydrocarbons and Graphene Nanoflakes 波动电荷极化模型在大型多芳烃和石墨烯纳米片上的应用

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-08-28 DOI: 10.1021/acs.jpclett.3c02013

Devin M. Mulvey, and , Kenneth D. Jordan*,

{"title":"Application of a Fluctuating Charge Polarization Model to Large Polyaromatic Hydrocarbons and Graphene Nanoflakes","authors":"Devin M. Mulvey,  and , Kenneth D. Jordan*, ","doi":"10.1021/acs.jpclett.3c02013","DOIUrl":"https://doi.org/10.1021/acs.jpclett.3c02013","url":null,"abstract":"We present a polarization model incorporating coupled fluctuating charges and point inducible dipoles that is able to accurately describe the dipole polarizabilities of small hydrocarbons and, for sufficiently large graphene nanoflakes, reproduce the classical image potential of an infinite conducting sheet. When our fluctuating charge model is applied to the hexagonal carbon nanoflake C60000 we attain excellent agreement with the image potential and induced charge distribution of a conducting sheet. With the inclusion of inducible dipole terms, the model predicts an image plane of zim = 1.3334 a0, which falls in line with prior estimates for graphene. We consider the case of two charges placed on opposite sides of C60000 and find that the fluctuating charge model reproduces classical electrostatics once again. By testing opposing and similar signs of the external charges, we conclude that an atomically thin molecule or extended system does not fully screen their interaction.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 35","pages":"7869–7875"},"PeriodicalIF":5.7,"publicationDate":"2023-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.jpclett.3c02013","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"211068","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Disorder and Photogeneration Efficiency in Organic Semiconductors 有机半导体的无序和光发生效率

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-08-28 DOI: 10.1021/acs.jpclett.3c02120

Artem V. Toropin, Vladimir R. Nikitenko*, Nikolai A. Korolev and Oleg V. Prezhdo*,

引用次数: 0