The Journal of Physical Chemistry Letters最新文献_第7页

Titanium Cluster Nuclearity Controls the Potential of Ti(IV/III) Reduction by Transfer Hydrogenation 钛簇核控制转移加氢还原Ti（IV/III）的电位

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-20 DOI: 10.1021/acs.jpclett.5c0039110.1021/acs.jpclett.5c00391

Brian G. Diamond, Robin E. Bumbaugh and Christopher H. Hendon*,

引用次数: 0

Ground-State Structure and Excited-State Dynamics of a Donor-Acceptor Complex with Two Charge-Transfer Bands. 具有两个电荷转移带的供体-受体配合物的基态结构和激发态动力学。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-20 DOI: 10.1021/acs.jpclett.5c01136

Johannes Wega,Christopher A Rumble,Eric Vauthey

引用次数: 0

Segregation of Chemical Groups at PMMA/H2O Interface Leads to Different Local Hydrophobicity. PMMA/H2O界面化学基团的分离导致了不同的局部疏水性。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-20 DOI: 10.1021/acs.jpclett.5c00569

Mengmeng Wang,Feixiang Chen,Junjun Tan,Shuji Ye

{"title":"Segregation of Chemical Groups at PMMA/H2O Interface Leads to Different Local Hydrophobicity.","authors":"Mengmeng Wang,Feixiang Chen,Junjun Tan,Shuji Ye","doi":"10.1021/acs.jpclett.5c00569","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00569","url":null,"abstract":"The local hydrophilicity of polymer surfaces is essential for many applications, such as coatings and biocompatibility, but revealing its structural origin is challenging. Here, we used poly(methyl methacrylate) (PMMA) film as a model and excavated several SFG spectral features, generated by femtosecond sum-frequency generation vibrational spectroscopy (SFG-VS), to elucidate the nature of microscopic hydrophilicity of a polymer/H2O interface. For the first time, we successfully probed the SFG spectra of the bend-libration combination band of interfacial water, which exhibits high sensitivity to solvent-water interactions. Two local hydrophilic domains are observed at the PMMA/H2O interface. The segregation of -OCH3 and -CH3 groups to the PMMA/H2O interface results in the formation of a local hydrophobic domain, where weak solvent-water interactions, slow vibrational dynamics of OH stretching, and no ice-like interfacial water are detected. In contrast, when both C═O and -OCH3 groups segregate to the PMMA/water interface, a local hydrophilic domain is formed, leading to strong solvent-water interactions, fast vibrational dynamics of OH stretching, and the presence of ice-like interfacial water. The water molecules around the hydrophobic domains of the PMMA surface are mainly liquid-like water rather than ice-like water. This work contributes to a molecular-level understanding of the local hydrophilicity of polymer surfaces.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"97 1","pages":"5334-5340"},"PeriodicalIF":6.475,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144103717","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

Room-Temperature Pulsed Dynamic Nuclear Polarization at 7 T 7 T室温脉冲动态核极化

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-20 DOI: 10.1021/acs.jpclett.5c0073710.1021/acs.jpclett.5c00737

Alexander A. Nevzorov*, Sergey Milikisiyants, Antonin Marek, Ilia Kaminker and Alex I. Smirnov*,

{"title":"Room-Temperature Pulsed Dynamic Nuclear Polarization at 7 T","authors":"Alexander A. Nevzorov*, Sergey Milikisiyants, Antonin Marek, Ilia Kaminker and Alex I. Smirnov*, ","doi":"10.1021/acs.jpclett.5c0073710.1021/acs.jpclett.5c00737","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00737https://doi.org/10.1021/acs.jpclett.5c00737","url":null,"abstract":"Pulsed dynamic nuclear polarization (DNP) can enhance NMR signals by more than 2 orders of magnitude and is applicable to spin systems with short-lived electronic polarization. Recently, several pulsed DNP sequences were demonstrated at low magnetic fields. However, pulsed DNP at magnetic fields of modern NMR spectrometers (7 T and above) necessitates addressing major technical challenges for generating sufficiently high mm-wave B1e amplitudes to match the nuclear Larmor frequencies. Here we describe a first-of-its-kind ESR/NMR spectrometer for pulsed DNP and phase-sensitive electronic detection operating at 7 T magnetic field. Generation of B1e fields with amplitudes of ca. 75 MHz was made possible by employing a pulsed extended interaction klystron and piezo-tunable photonic-band gap resonators with unloaded quality factors Q ≈ 1500. Room-temperature NOVEL DNP yielded natural-abundance 13C NMR signal gains of up to 800 for a 30 μm thick crystal of a synthetic diamond. Simultaneous coherent manipulation of the electronic and nuclear spins was demonstrated by 13C-detected electron Rabi nutations.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 21","pages":"5321–5326 5321–5326"},"PeriodicalIF":4.8,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144166016","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

Correction to “Amorphous Silica Interlayer Unlocks Direct Epitaxial Growth of CsPbBr3 on Silicon via Slip-and-Stick Mechanism” 对“非晶二氧化硅中间层通过滑粘机制解锁CsPbBr3在硅上的直接外延生长”的修正

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-19 DOI: 10.1021/acs.jpclett.5c00586

Christian Tantardini, Simone Argiolas, Paola De Padova, Boris I. Yakobson, Aldo Di Carlo, Alessandro Mattoni

引用次数: 0

Tracking relaxation dynamics of polaritons and reservoir states in organic exciton-polaritons. 跟踪有机激子-极化子的弛豫动力学和储层态。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-19 DOI: 10.1021/acs.jpclett.5c00666

Haolin Chen,Jingxuan Ai,Xiaolu Bai,Shaocong Hou,Stephen R Forrest,Jennifer P Ogilvie,Yin Song

{"title":"Tracking relaxation dynamics of polaritons and reservoir states in organic exciton-polaritons.","authors":"Haolin Chen,Jingxuan Ai,Xiaolu Bai,Shaocong Hou,Stephen R Forrest,Jennifer P Ogilvie,Yin Song","doi":"10.1021/acs.jpclett.5c00666","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00666","url":null,"abstract":"Organic exciton-polaritons have garnered significant attention in optoelectronic devices and photochemistry, primarily due to their micrometer-scale diffusion lengths and tunable energy levels. Recent studies have underscored the critical role of reservoir states in the dynamical processes following polaritonic relaxation. However, questions remain regarding the peak assignments of reservoir states and their specific functions during relaxation. In this study, we employed pump-probe and two-dimensional electronic spectroscopy (2DES) coupled with model simulations to investigate photoexcited dynamics of organic exciton-polaritons. By comparing experimental data with simulations, we identified that reservoir states consist of dark states and excited-state molecules uncoupled to the cavity mode, each exhibiting distinct spectral characteristics. Analyses of the spectral evolution in 2DES reveal that reservoir states are generated through three pathways: direct photoexcitation, rapid relaxation from middle polaritons, and entropy-driven relaxation from lower polaritons. Moreover, we find that equilibrium is established between dark states and uncoupled excited-state molecules following polaritonic relaxation, regardless of the excitation wavelength. This equilibrium facilitates subsequent polaritonic regeneration. Modulating the equilibrium constant can be achieved by engineering the light-matter interaction strength, offering a strategy to control postrelaxation polaritonic dynamics. These insights advance our understanding of relaxation dynamics in organic exciton-polaritons that can benefit the design of next-generation optoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"39 1","pages":"5265-5271"},"PeriodicalIF":6.475,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087709","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

Interface Field Engineering of Weakly Alkaline-Treated PEDOT:PSS for Enhanced Performance and Stability of Tin-Based Perovskite Solar Cells. 弱碱性处理PEDOT:PSS增强锡基钙钛矿太阳能电池性能和稳定性的界面场工程。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-19 DOI: 10.1021/acs.jpclett.5c00830

Yi Jing,Chensi Gong,Ao Shen,Jiale Yuan,Wenchao Huang,Wenzhen Lv,Runfeng Chen,Ligang Xu

{"title":"Interface Field Engineering of Weakly Alkaline-Treated PEDOT:PSS for Enhanced Performance and Stability of Tin-Based Perovskite Solar Cells.","authors":"Yi Jing,Chensi Gong,Ao Shen,Jiale Yuan,Wenchao Huang,Wenzhen Lv,Runfeng Chen,Ligang Xu","doi":"10.1021/acs.jpclett.5c00830","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00830","url":null,"abstract":"State-of-the-art tin-based perovskite solar cells (TPSCs) commonly use a water-based poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) hole transport layer. However, the strong acidity of PEDOT:PSS, arising from the deprotonation of its -SO3H group in PSS chains due to the low acid dissociation constant (pKa), often degrades tin perovskite films, compromising both the device performance and stability of TPSCs. Here, we present a novel interface engineering strategy using ammonium hydroxide (NH4OH) treated PEDOT:PSS, which effectively neutralizes acidic groups in PSS while simultaneously improving the quality of tin perovskite films due to preferentially oriented crystal growth. Besides, this strategy improves conductivity of the hole transport layer and effectively suppresses charge recombination due to the high-quality perovskite films. As a result, the devices achieve a remarkable power conversion efficiency of 13.3%, alongside significant improvements in stability. Notably, the unencapsulated devices retain 85% of their initial efficiency after approximately 1600 h in N2. Our method marks a significant advancement, integrating enhanced efficiency with improved durability and offering a scalable pathway for the commercialization of tin-based perovskite photovoltaics.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 1","pages":"5258-5264"},"PeriodicalIF":6.475,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087710","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

Intrinsic Electric Fields Promote Delocalized Interlayer Excitons in Janus In2SSe Moiré Bilayers 本征电场促进Janus In2SSe摩尔双分子层间激子的离域

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-19 DOI: 10.1021/acs.jpclett.5c01078

Xinyong Meng, Wei Hu, Jinlong Yang

{"title":"Intrinsic Electric Fields Promote Delocalized Interlayer Excitons in Janus In2SSe Moiré Bilayers","authors":"Xinyong Meng, Wei Hu, Jinlong Yang","doi":"10.1021/acs.jpclett.5c01078","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01078","url":null,"abstract":"The moiré potential in van der Waals (vdW) moiré superlattices is well-established to significantly influence electronic structures and optical excitations. When Janus monolayers are employed to construct twisted bilayers, an additional degree of freedom─the out-of-plane Janus field─is introduced alongside the moiré potential, leading to modifications in both electronic and optical properties. While these two effects have been individually investigated in prior studies on excitons, the behavior of excitons under the simultaneous presence of both effects remained unexplored. In this study, we investigate, for the first time, the interplay between these two effects in twisted Janus In2SSe. Our results demonstrate that the band structures and excitonic properties can be significantly modulated through variations in stacking sequences and intrinsic dipole orientations. This work provides a framework for the precise control of emission energy, exciton characteristics, and the spatial distribution of moiré excitons. We predict the coexistence of intrinsic Janus field-induced interlayer excitons and moiré potential-driven moiré excitons in twisted bilayer Janus In2SSe. These findings not only elucidate the interaction between Janus fields and moiré potentials but also introduce a novel, multifaceted strategy for exciton manipulation.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088245","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

Tracking relaxation dynamics of polaritons and reservoir states in organic exciton-polaritons 跟踪有机激子-极化子的弛豫动力学和储层态

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-19 DOI: 10.1021/acs.jpclett.5c0066610.1021/acs.jpclett.5c00666

Haolin Chen, Jingxuan Ai, Xiaolu Bai, Shaocong Hou*, Stephen R. Forrest, Jennifer P. Ogilvie and Yin Song*,

{"title":"Tracking relaxation dynamics of polaritons and reservoir states in organic exciton-polaritons","authors":"Haolin Chen, Jingxuan Ai, Xiaolu Bai, Shaocong Hou*, Stephen R. Forrest, Jennifer P. Ogilvie and Yin Song*, ","doi":"10.1021/acs.jpclett.5c0066610.1021/acs.jpclett.5c00666","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00666https://doi.org/10.1021/acs.jpclett.5c00666","url":null,"abstract":"Organic exciton-polaritons have garnered significant attention in optoelectronic devices and photochemistry, primarily due to their micrometer-scale diffusion lengths and tunable energy levels. Recent studies have underscored the critical role of reservoir states in the dynamical processes following polaritonic relaxation. However, questions remain regarding the peak assignments of reservoir states and their specific functions during relaxation. In this study, we employed pump–probe and two-dimensional electronic spectroscopy (2DES) coupled with model simulations to investigate photoexcited dynamics of organic exciton-polaritons. By comparing experimental data with simulations, we identified that reservoir states consist of dark states and excited-state molecules uncoupled to the cavity mode, each exhibiting distinct spectral characteristics. Analyses of the spectral evolution in 2DES reveal that reservoir states are generated through three pathways: direct photoexcitation, rapid relaxation from middle polaritons, and entropy-driven relaxation from lower polaritons. Moreover, we find that equilibrium is established between dark states and uncoupled excited-state molecules following polaritonic relaxation, regardless of the excitation wavelength. This equilibrium facilitates subsequent polaritonic regeneration. Modulating the equilibrium constant can be achieved by engineering the light-matter interaction strength, offering a strategy to control postrelaxation polaritonic dynamics. These insights advance our understanding of relaxation dynamics in organic exciton-polaritons that can benefit the design of next-generation optoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 21","pages":"5265–5271 5265–5271"},"PeriodicalIF":4.8,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144166022","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

Intrinsic Electric Fields Promote Delocalized Interlayer Excitons in Janus In2SSe Moiré Bilayers 本征电场促进Janus In2SSe摩尔双分子层间激子的离域

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-19 DOI: 10.1021/acs.jpclett.5c0107810.1021/acs.jpclett.5c01078

Xinyong Meng, Wei Hu* and Jinlong Yang,

{"title":"Intrinsic Electric Fields Promote Delocalized Interlayer Excitons in Janus In2SSe Moiré Bilayers","authors":"Xinyong Meng, Wei Hu* and Jinlong Yang, ","doi":"10.1021/acs.jpclett.5c0107810.1021/acs.jpclett.5c01078","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01078https://doi.org/10.1021/acs.jpclett.5c01078","url":null,"abstract":"The moiré potential in van der Waals (vdW) moiré superlattices is well-established to significantly influence electronic structures and optical excitations. When Janus monolayers are employed to construct twisted bilayers, an additional degree of freedom─the out-of-plane Janus field─is introduced alongside the moiré potential, leading to modifications in both electronic and optical properties. While these two effects have been individually investigated in prior studies on excitons, the behavior of excitons under the simultaneous presence of both effects remained unexplored. In this study, we investigate, for the first time, the interplay between these two effects in twisted Janus In2SSe. Our results demonstrate that the band structures and excitonic properties can be significantly modulated through variations in stacking sequences and intrinsic dipole orientations. This work provides a framework for the precise control of emission energy, exciton characteristics, and the spatial distribution of moiré excitons. We predict the coexistence of intrinsic Janus field-induced interlayer excitons and moiré potential-driven moiré excitons in twisted bilayer Janus In2SSe. These findings not only elucidate the interaction between Janus fields and moiré potentials but also introduce a novel, multifaceted strategy for exciton manipulation.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 21","pages":"5272–5280 5272–5280"},"PeriodicalIF":4.8,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165856","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