The Journal of Physical Chemistry Letters最新文献_第5页

Boosting Excitonic Emission in 2D Multiple Quantum Well Superlattices by Plasma-Assisted Electrochemical Intercalation 等离子体辅助电化学插层增强二维多量子阱超晶格中的激子发射

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-22 DOI: 10.1021/acs.jpclett.5c0082610.1021/acs.jpclett.5c00826

Shixuan Wang, Jian Li, Peiyu Zeng, Xu Han, Jinshu Zhang, Xiaoya Liu, Weiqiao Xia, Zhexing Duan, Wei Liu, Shaoqing Xiao, Qiang Fu*, Qi Zhang*, Junpeng Lu and Zhenhua Ni,

{"title":"Boosting Excitonic Emission in 2D Multiple Quantum Well Superlattices by Plasma-Assisted Electrochemical Intercalation","authors":"Shixuan Wang, Jian Li, Peiyu Zeng, Xu Han, Jinshu Zhang, Xiaoya Liu, Weiqiao Xia, Zhexing Duan, Wei Liu, Shaoqing Xiao, Qiang Fu*, Qi Zhang*, Junpeng Lu and Zhenhua Ni, ","doi":"10.1021/acs.jpclett.5c0082610.1021/acs.jpclett.5c00826","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00826https://doi.org/10.1021/acs.jpclett.5c00826","url":null,"abstract":"Scalable fabrication of multiple quantum-well (MQW) superlattices via layer-by-layer stacking of two-dimensional (2D) materials remains challenging. Here, we propose a plasma-assisted electrochemical intercalation strategy to overcome this limitation. By intercalating 1-ethyl-3-methylimidazolium (EMIM+) cations into multilayer molybdenum disulfide (MoS2), followed by oxygen plasma intercalation, we achieve large-area (∼100 μm) MQW superlattices with hundreds of active layers. This approach enhances MoS2 photoluminescence (PL) by 2 orders of magnitude, with the PL quantum yield (PLQY) increasing with both excitation power and thickness. The enhancement arises from interlayer-decoupling-induced bandgap directness and electron extraction induced by oxygen plasma, effectively suppressing charge transfer between heterointerfaces. Our findings provide a scalable route for fabricating quasi-MQW superlattices, opening new avenues for photophysics research and next-generation optoelectronics.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 21","pages":"5405–5411 5405–5411"},"PeriodicalIF":4.8,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165886","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

Theoretical Insights into Ultrafast-Decaying and Long-Lived States of ortho-Nitrophenol upon Photoexcitation in the Gas Phase 气相光激发下邻硝基苯酚超快衰变和长寿命态的理论见解

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-21 DOI: 10.1021/acs.jpclett.5c0078510.1021/acs.jpclett.5c00785

Satoi Wada, Takuro Tsutsumi, Kenichiro Saita, Taro Sekikawa and Tetsuya Taketsugu*,

{"title":"Theoretical Insights into Ultrafast-Decaying and Long-Lived States of ortho-Nitrophenol upon Photoexcitation in the Gas Phase","authors":"Satoi Wada, Takuro Tsutsumi, Kenichiro Saita, Taro Sekikawa and Tetsuya Taketsugu*, ","doi":"10.1021/acs.jpclett.5c0078510.1021/acs.jpclett.5c00785","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00785https://doi.org/10.1021/acs.jpclett.5c00785","url":null,"abstract":"Nitrophenols in the atmosphere are chromophore pollutants that absorb sunlight. Among them, ortho-nitrophenol (o-NP) stands out due to its strong intramolecular hydrogen bond which facilitates excited-state intramolecular proton transfer (ESIPT) and influences its photoisomerization and dissociation. Time-resolved experiments have captured both ultrafast-decaying and long-lived signals. Here, we employ non-adiabatic molecular dynamics simulations and the reaction space projector method to elucidate the photoinduced reactions of o-NP. Our simulations show that photoexcited o-NP in the S1(ππ*) state undergoes ultrafast ESIPT followed by rapid decay through one of two non-adiabatic pathways: ultrafast internal conversion to the S0 state and intersystem crossing (ISC) to the triplet states. Furthermore, trajectories undergoing ISC remain trapped in triplet states, with reverse ISC to the singlet states rarely observed. These trajectories are clearly linked to the long-lived excited-state signal, providing more conclusive computational evidence of the origin.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 21","pages":"5373–5380 5373–5380"},"PeriodicalIF":4.8,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165883","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

Density Matrix Embedding Pair-Density Functional Theory for Molecules 分子密度矩阵嵌入对-密度泛函理论

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-21 DOI: 10.1021/acs.jpclett.5c00829

Shreya Verma, Matthew R. Hermes, Laura Gagliardi

引用次数: 0

Chirality-Induced Spin Selectivity at the Molecular Level: A Different Perspective to Understand and Exploit the Phenomenon 分子水平上手性诱导的自旋选择性：从不同角度理解和利用这一现象

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-21 DOI: 10.1021/acs.jpclett.5c0075510.1021/acs.jpclett.5c00755

Alessandro Chiesa, Alberto Privitera, Elena Garlatti, Giuseppe Allodi, Robert Bittl*, Michael R. Wasielewski*, Roberta Sessoli* and Stefano Carretta*,

引用次数: 0

Density Matrix Embedding Pair-Density Functional Theory for Molecules 分子密度矩阵嵌入对-密度泛函理论

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-21 DOI: 10.1021/acs.jpclett.5c0082910.1021/acs.jpclett.5c00829

Shreya Verma, Matthew R. Hermes and Laura Gagliardi*,

{"title":"Density Matrix Embedding Pair-Density Functional Theory for Molecules","authors":"Shreya Verma, Matthew R. Hermes and Laura Gagliardi*, ","doi":"10.1021/acs.jpclett.5c0082910.1021/acs.jpclett.5c00829","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00829https://doi.org/10.1021/acs.jpclett.5c00829","url":null,"abstract":"We combine density matrix embedding theory (DMET) with multiconfiguration pair-density functional theory (MC-PDFT) to explore finite systems exhibiting localized strong electron correlation effects. This methodology, termed density matrix embedded pair-density functional theory (DME-PDFT), provides a substantial cost reduction compared to traditional nonembedded MC-PDFT. Additionally, we compare it with second order n-electron valence state perturbation theory within DMET (NEVPT2-DMET). We have validated these methods by computing the bond dissociation in methyl diazine and spin-splitting energy gap in the [Fe(H2O)6]2+ complex, showing that DME-PDFT splitting energies converge faster compared to NEVPT2-DMET to the corresponding nonembedding limits. We finally compare embedding schemes with truncation schemes for two extended transition metal complexes, Fe[N(H)Ar*]2 and [NiC90N20H120]2+, and show that embedding schemes are more accurate than truncations when the transition metal is not fully coordinated.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 21","pages":"5348–5357 5348–5357"},"PeriodicalIF":4.8,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165882","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

Theoretical Insights into Ultrafast-Decaying and Long-Lived States of ortho-Nitrophenol upon Photoexcitation in the Gas Phase 气相光激发下邻硝基苯酚超快衰变和长寿命态的理论见解

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-21 DOI: 10.1021/acs.jpclett.5c00785

Satoi Wada, Takuro Tsutsumi, Kenichiro Saita, Taro Sekikawa, Tetsuya Taketsugu

{"title":"Theoretical Insights into Ultrafast-Decaying and Long-Lived States of ortho-Nitrophenol upon Photoexcitation in the Gas Phase","authors":"Satoi Wada, Takuro Tsutsumi, Kenichiro Saita, Taro Sekikawa, Tetsuya Taketsugu","doi":"10.1021/acs.jpclett.5c00785","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00785","url":null,"abstract":"Nitrophenols in the atmosphere are chromophore pollutants that absorb sunlight. Among them, ortho-nitrophenol (o-NP) stands out due to its strong intramolecular hydrogen bond which facilitates excited-state intramolecular proton transfer (ESIPT) and influences its photoisomerization and dissociation. Time-resolved experiments have captured both ultrafast-decaying and long-lived signals. Here, we employ non-adiabatic molecular dynamics simulations and the reaction space projector method to elucidate the photoinduced reactions of o-NP. Our simulations show that photoexcited o-NP in the S1(ππ*) state undergoes ultrafast ESIPT followed by rapid decay through one of two non-adiabatic pathways: ultrafast internal conversion to the S0 state and intersystem crossing (ISC) to the triplet states. Furthermore, trajectories undergoing ISC remain trapped in triplet states, with reverse ISC to the singlet states rarely observed. These trajectories are clearly linked to the long-lived excited-state signal, providing more conclusive computational evidence of the origin.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 1","pages":"5373-5380"},"PeriodicalIF":6.475,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114377","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

First-Principles Insights into the Effect of Spin-Insulating Substrates on Molecular Kondo States 自旋绝缘衬底对分子近藤态影响的第一性原理研究

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-21 DOI: 10.1021/acs.jpclett.5c0123710.1021/acs.jpclett.5c01237

Dawei He, Daochi Zhang, Wenwen Shi, Lyuzhou Ye, Rui-Xue Xu, Sai Duan* and Xiao Zheng*,

{"title":"First-Principles Insights into the Effect of Spin-Insulating Substrates on Molecular Kondo States","authors":"Dawei He, Daochi Zhang, Wenwen Shi, Lyuzhou Ye, Rui-Xue Xu, Sai Duan* and Xiao Zheng*, ","doi":"10.1021/acs.jpclett.5c0123710.1021/acs.jpclett.5c01237","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01237https://doi.org/10.1021/acs.jpclett.5c01237","url":null,"abstract":"Surface magnetic molecular systems have attracted increasing attention because of their potential applications in spintronic devices. Recent experiments have shown that bis(phthalocyaninato)terbium(III) molecules adsorbed on a bare Cu substrate exhibit a Kondo state, whereas introducing an insulating NaCl layer on the Cu surface significantly suppresses this spin response around the zero bias voltage. The microscopic mechanism underlying this transition remains unclear. To address this issue, we employed a combined approach of the density functional theory and hierarchical equations of motion method (DFT + HEOM) to examine how spin-insulating layers affect the molecular Kondo state. We first developed a novel algorithm to evaluate the hybridization functions that allows quantitative assessments of the molecule–substrate interactions in different configurations at the DFT level. Subsequently, we combined the HEOM method to simulate the differential conductance (dI/dV) spectra of the molecule adsorbed on different substrates. The obtained dI/dV spectra via the present combined approach agree well with the experimental observations. Our results indicate that the strength of the molecule–substrate hybridization critically determines the magnetic properties of the adsorbed molecule. Our work elucidates the important role of spin-insulating layers in tuning the Kondo effect and provides valuable insights for the rational design of surface magnetic molecular systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 21","pages":"5381–5389 5381–5389"},"PeriodicalIF":4.8,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165884","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

Chirality-Induced Spin Selectivity at the Molecular Level: A Different Perspective to Understand and Exploit the Phenomenon. 分子水平上手性诱导的自旋选择性：从不同角度理解和利用这一现象。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-21 DOI: 10.1021/acs.jpclett.5c00755

Alessandro Chiesa,Alberto Privitera,Elena Garlatti,Giuseppe Allodi,Robert Bittl,Michael R Wasielewski,Roberta Sessoli,Stefano Carretta

引用次数: 0

First-Principles Insights into the Effect of Spin-Insulating Substrates on Molecular Kondo States 自旋绝缘衬底对分子近藤态影响的第一性原理研究

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-21 DOI: 10.1021/acs.jpclett.5c01237

Dawei He, Daochi Zhang, Wenwen Shi, Lyuzhou Ye, Rui-Xue Xu, Sai Duan, Xiao Zheng

{"title":"First-Principles Insights into the Effect of Spin-Insulating Substrates on Molecular Kondo States","authors":"Dawei He, Daochi Zhang, Wenwen Shi, Lyuzhou Ye, Rui-Xue Xu, Sai Duan, Xiao Zheng","doi":"10.1021/acs.jpclett.5c01237","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01237","url":null,"abstract":"Surface magnetic molecular systems have attracted increasing attention because of their potential applications in spintronic devices. Recent experiments have shown that bis(phthalocyaninato)terbium(III) molecules adsorbed on a bare Cu substrate exhibit a Kondo state, whereas introducing an insulating NaCl layer on the Cu surface significantly suppresses this spin response around the zero bias voltage. The microscopic mechanism underlying this transition remains unclear. To address this issue, we employed a combined approach of the density functional theory and hierarchical equations of motion method (DFT + HEOM) to examine how spin-insulating layers affect the molecular Kondo state. We first developed a novel algorithm to evaluate the hybridization functions that allows quantitative assessments of the molecule–substrate interactions in different configurations at the DFT level. Subsequently, we combined the HEOM method to simulate the differential conductance (dI/dV) spectra of the molecule adsorbed on different substrates. The obtained dI/dV spectra via the present combined approach agree well with the experimental observations. Our results indicate that the strength of the molecule–substrate hybridization critically determines the magnetic properties of the adsorbed molecule. Our work elucidates the important role of spin-insulating layers in tuning the Kondo effect and provides valuable insights for the rational design of surface magnetic molecular systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"56 1","pages":"5381-5389"},"PeriodicalIF":6.475,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114378","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

A Monolithic Neuromorphic Device for In-Sensor Tactile Computing 传感器触觉计算的单片神经形态装置

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-20 DOI: 10.1021/acs.jpclett.5c0058310.1021/acs.jpclett.5c00583

Yi Du, Lu Yang, Jiangdong Gong, Jiahe Hu, Jiaqi Liu, Song Zhang, Shangda Qu, Jiaxin Chen, Hwa Sung Lee and Wentao Xu*,

{"title":"A Monolithic Neuromorphic Device for In-Sensor Tactile Computing","authors":"Yi Du, Lu Yang, Jiangdong Gong, Jiahe Hu, Jiaqi Liu, Song Zhang, Shangda Qu, Jiaxin Chen, Hwa Sung Lee and Wentao Xu*, ","doi":"10.1021/acs.jpclett.5c0058310.1021/acs.jpclett.5c00583","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00583https://doi.org/10.1021/acs.jpclett.5c00583","url":null,"abstract":"To emulate the tactile perception of human skin, the integration of tactile sensors with neuromorphic devices has emerged as a promising approach to achieve near-sensor information processing. Here, we present a monolithic electronic device that seamlessly integrates tactile perception and neuromorphic computing functionalities within a single architecture, with synaptic plasticity directly tunable by tactile inputs. This unique capability stems from our engineered device structure employing SnO2 nanowires as the conductive channel coupled with a pressure-sensitive chitosan layer ionic gating layer. The device demonstrates pressure-dependent memory retention and learning behaviors, effectively mimicking the enhanced cognitive functions observed in humans under stressful conditions. Furthermore, the integrated design exhibits potential for implementing bioinspired electronic systems requiring adaptive tactile information processing.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 21","pages":"5312–5320 5312–5320"},"PeriodicalIF":4.8,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144166018","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