The Journal of Physical Chemistry Letters最新文献_第2页

Direct Two-Dimensional Infrared Protein Spectroscopy of Beer Foam in H2O 啤酒泡沫在水中的直接二维红外蛋白质光谱研究

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-19 DOI: 10.1021/acs.jpclett.6c02299

Asger Berg Thomassen,Pelle Roos Hansen,Khezar Hayat Saeed,Tobias Weidner

{"title":"Direct Two-Dimensional Infrared Protein Spectroscopy of Beer Foam in H2O","authors":"Asger Berg Thomassen,Pelle Roos Hansen,Khezar Hayat Saeed,Tobias Weidner","doi":"10.1021/acs.jpclett.6c02299","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02299","url":null,"abstract":"Two-dimensional infrared (2D IR) spectroscopy is uniquely sensitive to protein secondary structure and dynamics, but the technique has historically been restricted to D2O solutions because the bending vibration of liquid H2O overlaps with the amide I band. The Hunt group has shown that 2D IR can be performed on protein solutions in H2O when the protein signal dominates over the residual water response, but these demonstrations have generally relied on purified or laboratory-prepared protein samples. Here we go one step further and acquire complete 2D IR spectra and related spectral dynamics directly on a natural, off-the-shelf, protein-rich aqueous sample, beer foam, with no isotopic exchange, purification, or chemical modification. Beer foam has a high surface-to-volume ratio and is naturally concentrating interfacial proteins. Using Grøn Tuborg as the reference system, we resolve α-helix, β-sheet, and β-sheet cross peaks, side-chain modes, and the amide I/II cross peak. Center line slope (CLS) analysis reveals an essentially static low-frequency β-sheet component coexisting with normally relaxing backbone modes, consistent with a solvent-shielded aggregate buried in the foam film. A survey of four additional beers (Guld Tuborg, Westmalle Dubbel, Westmalle Tripel, Guinness Draft) shows that this low-frequency β-sheet feature near 1610–1620 cm–1 recurs across very different beer styles. Foams of natural samples thus emerge as a route to 2D IR of protein films in H2O.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"45 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218955","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

Interfacial Solvation and Spin-Selective Electron Transfer Govern CO/MeOH Selectivity at a Graphene–CoPc Interface 界面溶剂化和自旋选择性电子转移影响石墨烯- copc界面上CO/MeOH的选择性

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-19 DOI: 10.1021/acs.jpclett.6c03065

Kong Meng,Run Long

{"title":"Interfacial Solvation and Spin-Selective Electron Transfer Govern CO/MeOH Selectivity at a Graphene–CoPc Interface","authors":"Kong Meng,Run Long","doi":"10.1021/acs.jpclett.6c03065","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c03065","url":null,"abstract":"Electrochemical CO2-to-methanol conversion over noncopper single-atom catalysts is limited by competition between further *CO reduction and CO desorption. Here, constant-potential ab initio molecular dynamics and nonadiabatic molecular dynamics elucidate how applied potential, interfacial solvation, and spin-resolved electron transfer control CO/MeOH selectivity at a graphene-supported cobalt phthalocyanine interface. At −0.6 V versus the reversible hydrogen electrode, frequent Co–C bond elongation favors CO release. By contrast, −1.0 V strengthens *CO retention and extends the hydrogen-bond-network lifetime from 171.0 to 282.1 fs, establishing a persistent proton-delivery pathway for subsequent proton-coupled electron transfer. Unsupported CO@CoPc exhibits predominantly spin-down electron transfer, whereas graphene coupling enhances nonadiabatic coupling and activates an ultrafast spin-up channel with an injection time of 20.3 fs at −1.0 V. Thus, potential-dependent *CO residence, solvent organization, and spin-selective charge injection act cooperatively to govern CO/MeOH selectivity, with graphene serving as an active regulator of interfacial dynamics.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"3 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218899","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

Strain-Gradient Engineering of Topological, Nonlinear Optical, and Spin Chiral Responses in MnBi2Te4 MnBi2Te4中拓扑、非线性光学和自旋手性响应的应变梯度工程

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-19 DOI: 10.1021/acs.jpclett.6c02756

Hongtao Yan,Dongliang Jia,Bolun Zhang,Xinming Guo,Dan Tan

{"title":"Strain-Gradient Engineering of Topological, Nonlinear Optical, and Spin Chiral Responses in MnBi2Te4","authors":"Hongtao Yan,Dongliang Jia,Bolun Zhang,Xinming Guo,Dan Tan","doi":"10.1021/acs.jpclett.6c02756","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02756","url":null,"abstract":"Strain gradients arising from nonuniform interlayer expansion in layered van der Waals materials simultaneously modulate interlayer coupling and break inversion symmetry, yet their potential as a control knob for topological quantum materials remains unexplored. Using first-principles calculations, we demonstrate that graded interlayer expansion characterized by an effective gap-strain gradient in five-septuple-layer MnBi2Te4 drives three distinct physical responses: a topological phase transition from a quantum anomalous Hall state (C = 1) to a trivial insulator (C = 0), a second-harmonic-generation response in the mid-to-far-infrared spectral range, and a Rashba-type chiral spin texture with opposite inner–outer helicities. All three responses share a common microscopic origin in the layer-selective redistribution of interlayer hybridization, which weakens the Bi–Te orbital inversion near the Γ point and generates an out-of-plane polar field. Our findings establish strain-gradient engineering as a design principle for coordinating topological, nonlinear optical, and spin-textural functionalities in layered quantum materials.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"162 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210896","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

Probing Optical Response and Surface Conductance in Mixed-Halide Perovskites Using Terahertz Spectroscopy 用太赫兹光谱探测混合卤化物钙钛矿的光响应和表面电导

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-19 DOI: 10.1021/acs.jpclett.6c02805

Sarvani Jowhar Khanam,Naveen Periketi,Sushma Kumari,Arunkumar Meghavath,Srinivasa Rao Konda,Chaudhary Anil Kumar,Banavoth Murali

{"title":"Probing Optical Response and Surface Conductance in Mixed-Halide Perovskites Using Terahertz Spectroscopy","authors":"Sarvani Jowhar Khanam,Naveen Periketi,Sushma Kumari,Arunkumar Meghavath,Srinivasa Rao Konda,Chaudhary Anil Kumar,Banavoth Murali","doi":"10.1021/acs.jpclett.6c02805","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02805","url":null,"abstract":"Mixed halide perovskite single crystals (MHPSCs) have attracted considerable attention as promising building blocks for next-generation photovoltaic technologies due to their exceptional optoelectronic properties, low fabrication cost, and facile processability. However, their practical implementation remains limited by phase segregation, which severely undermines the material stability and device scalability. Among the various crystal growth strategies, additive engineering has emerged as an effective approach to address these challenges by facilitating the formation of passivating interfacial layers, enhancing nanoscale crystallinity, and reducing the defect density. In this study, the optical response and surface conductance of MHPSCs were investigated by using terahertz spectroscopy in both reflection and transmission geometries. The influence of choline bromide (CB) and the heterocyclic additive 3-aminopiperidine (API) on the phonon modes and terahertz response were also examined. X-ray photoelectron spectroscopy (XPS) revealed that the suppression of phase segregation, associated with stronger chemical bonding, contributes to an enhanced THz transmission in the modified MHPSCs. In addition, the THz response of the crystals was examined after approximately six months of ambient aging, revealing changes in the reflection response compared with measurements performed shortly after synthesis. Since the fresh and aged samples were characterized by using different THz spectroscopy configurations, the aging-related changes are interpreted qualitatively. Overall, combined time- and frequency-domain imaging provides a comprehensive assessment of spatial and spectral heterogeneity, complementing bulk THz spectroscopy and highlighting the impact of additive-induced microstructural modifications on the THz dielectric response.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"42 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210897","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

Competitive Desorption Enables Room-Temperature CO and H2O Co-release in Reverse Water–Gas Shift over Noble-Metal-Free Cluster Co3O2– 竞争解吸使室温CO和H2O在反水气转换中在无贵金属簇Co3O2 -上共同释放

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-19 DOI: 10.1021/acs.jpclett.6c02811

Hai Zhu,Yi Liu,Guang-Sheng Tao,Xiao-Na Li

{"title":"Competitive Desorption Enables Room-Temperature CO and H2O Co-release in Reverse Water–Gas Shift over Noble-Metal-Free Cluster Co3O2–","authors":"Hai Zhu,Yi Liu,Guang-Sheng Tao,Xiao-Na Li","doi":"10.1021/acs.jpclett.6c02811","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02811","url":null,"abstract":"Reverse water–gas shift (RWGS, CO2 + H2 → CO + H2O) represents a pivotal strategy for CO2 hydrogenation. Although noble-metal (NM) catalysts are efficient, their scarcity necessitates the development of non-noble alternatives, while the mechanisms of elementary steps involved in RWGS over non-NM systems remains elusive. Herein, by combining mass spectrometry and quantum-chemical calculations, we demonstrate the room-temperature cogeneration of CO and H2O via competitive desorption on the reaction of cobalt oxide cluster Co3O2– with H2 followed by CO2. The comparable intensities of signals of Co3O3H2– (from CO desorption) and Co3O2CO– (from H2O desorption) in mass spectra provide solid experimental evidence for this phenomenon. Note that only one RWGS product (CO or H2O) typically desorbs at a given temperature owing to thermodynamic constraints, and rhodium is widely considered essential for driving RWGS. The synergistic and comparable electron-withdrawing abilities of both adsorbates, arising from orbital delocalization across Co and two species on Co3O2–, are emphasized to promote the desorption of either CO or H2O.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"28 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218901","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

Interplay ofDepletion Interaction and Viscosity DrivesNon-monotonic Ligand Binding to DNA G-Quadruplex under Crowding 拥挤条件下耗竭相互作用和黏度驱动非单调配体与DNA g -四重体的结合

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-18 DOI: 10.1021/acs.jpclett.6c02779

Ajay Kumar Chand,Pramod Kumar,Harsh Sahu,Shubham Kumar Sharma,Sobhan Sen

{"title":"Interplay of\u0000Depletion Interaction and Viscosity Drives\u0000Non-monotonic Ligand Binding to DNA G-Quadruplex under Crowding","authors":"Ajay Kumar Chand,Pramod Kumar,Harsh Sahu,Shubham Kumar Sharma,Sobhan Sen","doi":"10.1021/acs.jpclett.6c02779","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02779","url":null,"abstract":"Abstract Study of ligand binding to G-quadruplex (G4) DNA under molecular crowding is essential for understanding its implications in cellular contexts; however, the underlying mechanism remains largely unresolved. We investigate the binding of 5,10,15,20-tetrakis(1-methyl-4-pyridinio)porphyrin tetra(p-toluenesulfonate) (TMPyP4) to parallel c-MYC G4-DNA under ethylene glycol/poly(ethylene glycol) (EG/PEG) crowding using steady-state and fluorescence correlation spectroscopy (FCS). The ligand binding affinity to G4 (K) exhibits a pronounced non-monotonic, U-shaped dependence on crowder size─first decreasing due to viscosity-induced hindrance and then recovering for larger PEGs. Kinetic analysis of FCS data reveals that this arises from competing effects of crowder-induced viscosity and depletion interactions on ligand association (kon) and dissociation (koff) rates. A modified Collins–Kimball–Debye formalism combined with hybrid molecular dynamics (MD) simulations shows that larger crowders create polymer-free depletion cavities that accelerate ligand–G4 association, counteracting viscous drag. These results provide a generalizable framework connecting polymer physics to nucleic acid–ligand recognition that will be useful for G4-targeted drug design in crowded cellular milieu.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"11 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210176","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

Secondary Fragmentationof Benzylpyridinium ThermometerIons Bearing a 4-Trifluoromethyl Group Extends the InternalEnergy Calibration Range of Gas-Phase Ions 含4-三氟甲基的苄基吡啶温度离子的二次破碎扩展了气相离子的内部能量校准范围

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-16 DOI: 10.1021/acs.jpclett.6c02447

Daiki Asakawa,Akira Matsugi

{"title":"Secondary Fragmentation\u0000of Benzylpyridinium Thermometer\u0000Ions Bearing a 4-Trifluoromethyl Group Extends the Internal\u0000Energy Calibration Range of Gas-Phase Ions","authors":"Daiki Asakawa,Akira Matsugi","doi":"10.1021/acs.jpclett.6c02447","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02447","url":null,"abstract":"Abstract Secondary fragmentation of substituted benzylpyridinium “thermometer ions” has been observed previously, but they have not been used as quantitative probes for internal energy calibration. Here, we demonstrate that the secondary fragmentation of 4-trifluoromethyl-substituted benzylpyridiniums provides a high-energy survival-yield probe that extends the measurable internal energy range in collision-induced dissociation (CID). CID of 4-trifluoromethyl-substituted benzylpyridiniums proceeds by N–C bond cleavage to form the corresponding benzyl cation, followed by secondary CF2 loss. This secondary fragmentation can be incorporated into internal energy calibration, provided that the effective dissociation energy for the secondary fragmentation is assigned by considering how excess energy is partitioned during the primary N–C bond cleavage. Using the secondary-fragmentation survival yield extended the CID calibration range from 30 to 60 eV, revealing that internal energy distributions shift toward higher energies and broaden with increasing collision energy. This approach also provide a quantitative probe of high-energy regions inaccessible through primary fragmentation alone.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"39 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209831","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

Multi-channelNon-radiative Dynamics to Reveal Δ E ST as the Key Efficiency Descriptor for Deep-BluePt(II) Phosphors 多通道非辐射动力学揭示Δ E ST是深蓝色（II）荧光粉的关键效率描述符

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-16 DOI: 10.1021/acs.jpclett.6c03198

Xiao Chen,Weitang Li,Wenjie Zhang,Yulong Li,Yaxin Wang,Zhigang Shuai

{"title":"Multi-channel\u0000Non-radiative Dynamics to Reveal Δ\u0000 E\u0000 ST as the Key Efficiency Descriptor for Deep-Blue\u0000Pt(II) Phosphors","authors":"Xiao Chen,Weitang Li,Wenjie Zhang,Yulong Li,Yaxin Wang,Zhigang Shuai","doi":"10.1021/acs.jpclett.6c03198","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c03198","url":null,"abstract":"Abstract Tetradentate platinum(II) complexes are promising candidates for phosphorescent organic light-emitting diodes (OLEDs), combining deep-blue emission, high color purity, and potential for near-unity photoluminescence quantum yields (PLQYs). However, despite their rigid structures, which should suppress non-radiative decay, many of these complexes still show surprisingly low PLQYs, and the mechanism underlying this discrepancy has remained unclear. Here, through first-principle calculations of multi-channel transition rates for 25 tetradentate Pt(II) complexes, we show that this apparent paradox arises from a thermally activated S1 non-radiative channel (T1 → S1 → S0) that dominates the non-radiative decay. The rate of this channel depends exponentially on the singlet–triplet gap ΔEST, establishing ΔEST as a key descriptor for PLQY. Electronic structural analysis reveals that donors on the pyridine unit can delocalize LUMO, increase HOMO–LUMO overlap, and help enlarge ΔEST and PLQY. These results provide a unified mechanistic picture and a direct design rule for high-efficiency deep-blue Pt(II) emitters.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"292 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210177","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

Direct All-ElectronRelativistic Framework for Nuclear-ClockField Shifts: 229Th in CaF2 核时钟场位移的直接全电子相对论框架：第229期

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-16 DOI: 10.1021/acs.jpclett.6c02774

Han Wang,Rundong Zhao

{"title":"Direct All-Electron\u0000Relativistic Framework for Nuclear-Clock\u0000Field Shifts: 229Th in CaF2","authors":"Han Wang,Rundong Zhao","doi":"10.1021/acs.jpclett.6c02774","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02774","url":null,"abstract":"Abstract Recent progress toward nuclear clocks based on 229Th-doped crystals has made it increasingly important to understand how the local crystal environment affects the nuclear transition frequency. Based on the quasi-four-component (Q4C) relativistic density-functional method we have developed, we establish a direct all-electron framework for calculating nuclear-clock field shifts in periodic solids: by combining a finite-nucleus model with a Hellmann–Feynman formulation, the method directly evaluates the electronic response to a change in nuclear size. Q4C can describe both the large and small spinor components near a heavy nucleus while reducing the final eigenvalue problem to two-component dimensions, making fully relativistic calculations feasible for large defect supercells. We systematically validate the method through benchmarks on one-electron atoms, many-electron atoms, and molecules; we then apply it to 229Th-doped CaF2, focusing on the widely discussed but still controversial charge-compensation configurations, i.e., F-90 and F-180. The calculated field-shift difference is δν(180°) – δν(90°) = −16.8 × (1.00 ± 0.27) MHz. The predicted frequency separation provides direct theoretical evidence for distinguishing these two local structures and places an important constraint on the assignment of the observed 229Th:CaF2 spectra. More generally, the present work provides a practical first-principles relativistic tool for solid-state nuclear-clock studies.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"33 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209830","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

Wavelength-DependentPhotoluminescence Mapping ofDepth-Dependent Degradation Under Thermal Stress in PhenethylammoniumTetrafluoroborate Treated Perovskite Solar Cells 热应力下四氟硼酸苯乙铵处理钙钛矿太阳能电池深度降解的波长依赖性光致发光映射

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-16 DOI: 10.1021/acs.jpclett.6c01989

Julisa Juarez,Akash Dasgupta,Alan Zhan,Lamtiur P. Samosir,David S. Ginger

{"title":"Wavelength-Dependent\u0000Photoluminescence Mapping of\u0000Depth-Dependent Degradation Under Thermal Stress in Phenethylammonium\u0000Tetrafluoroborate Treated Perovskite Solar Cells","authors":"Julisa Juarez,Akash Dasgupta,Alan Zhan,Lamtiur P. Samosir,David S. Ginger","doi":"10.1021/acs.jpclett.6c01989","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c01989","url":null,"abstract":"Abstract Studying real-time degradation in perovskite semiconductors remains an important challenge. Conventional methods often cannot separate interfacial and bulk processes or rely on destructive analysis. Here, we demonstrate multiwavelength excitation photoluminescence (PL) as a nondestructive approach to distinguish interface- and bulk-dominated recombination losses. Using phenethylammonium tetrafluoroborate (PEABF4) treatment as a model, we use PL to show that PEABF4 passivates the electron transport layer (ETL)/perovskite interface, reducing interfacial recombination losses from fullerene deposition. However, upon thermal aging, PEABF4-treated stacks degrade more rapidly, with recombination losses broadening from the ETL/perovskite interface into the absorber. Diffusion–recombination simulations support interpreting excitation-wavelength-dependent PL decay signatures consistent with changes in surface recombination velocity and bulk lifetime, providing a framework for depth-sensitive comparisons during aging. Collectively, these results further establish multiwavelength excitation PL as a platform for studying recombination losses during aging of perovskite films.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"13 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209832","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