The Journal of Physical Chemistry Letters最新文献_第6页

Odd–Even Effects in the Structure and Thermal Stability of Carboxylic Acid Anchored Monolayers on Naturally Oxidized Aluminum Surface

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-25 DOI: 10.1021/acs.jpclett.5c0050010.1021/acs.jpclett.5c00500

Daria M. Cegiełka*, Łukasz Bodek, Michael Zharnikov and Piotr Cyganik*,

{"title":"Odd–Even Effects in the Structure and Thermal Stability of Carboxylic Acid Anchored Monolayers on Naturally Oxidized Aluminum Surface","authors":"Daria M. Cegiełka*, Łukasz Bodek, Michael Zharnikov and Piotr Cyganik*, ","doi":"10.1021/acs.jpclett.5c0050010.1021/acs.jpclett.5c00500","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00500https://doi.org/10.1021/acs.jpclett.5c00500","url":null,"abstract":"Self-assembled monolayers (SAMs) are broadly used for molecular engineering of surfaces and interfaces, which demands control over their structure and properties. An important tool in this context is the so-called odd–even effects exploiting the dependence of the SAM structure on the parity of the number of building blocks forming the backbone of SAM-building molecules. Even though these effects influence parameters crucial for SAM applications, they have been mainly studied on coinage metals (Au and Ag) until now. Here, using the series of biphenyl-substituted carboxylic acids (BPnCOO, n = 0–4), we show that structural odd–even behavior occurs as well on technologically relevant surface of naturally oxidized aluminum (representative of other oxide surfaces), with the even-numbered monolayers exhibiting higher packing density and lower molecular inclination than the odd-numbered analogs. Despite these structural changes, the SAM desorption energy remains nearly constant at a high value (∼1.5 eV) making BPnCOO/AlOx a promising system for organic electronics applications.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 13","pages":"3343–3350 3343–3350"},"PeriodicalIF":4.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.jpclett.5c00500","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758917","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

Unveiling Interactions of a Peptide-Bound Monolayer-Protected Metal Nanocluster with a Lipid Bilayer

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-25 DOI: 10.1021/acs.jpclett.5c0054810.1021/acs.jpclett.5c00548

Soumya Mondal, and , Tarak Karmakar*,

{"title":"Unveiling Interactions of a Peptide-Bound Monolayer-Protected Metal Nanocluster with a Lipid Bilayer","authors":"Soumya Mondal,  and , Tarak Karmakar*, ","doi":"10.1021/acs.jpclett.5c0054810.1021/acs.jpclett.5c00548","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00548https://doi.org/10.1021/acs.jpclett.5c00548","url":null,"abstract":"Monolayer-protected atomically precise nanoclusters (MPCs) are potential candidates for drug delivery because of their unique, versatile, and tunable physiochemical properties. The rational design of nanosized drug carriers relies on a deep understanding of their molecular-level interactions with cell membranes and other biological entities. In this work, we applied coarse-grained molecular dynamics and umbrella sampling simulations to investigate the interactions between the magainin 2 (MG2)-loaded Au144(MPA)60 (MPA = 5-mercaptopentanoic acid) nanocluster (MG2-MPC) and a model anionic tumor cell membrane. Electrostatic interactions between MPC ligands and MG2’s positively charged residues with the polar headgroups of lipids play a crucial role in the adhesion of the MG2-MPC complex to the membrane surface. Furthermore, MG2-MPCs self-assemble in the linear trimeric supramolecular aggregate on the bilayer surface, indicating a possible mechanism of MPC’s action in peptide delivery to the membrane.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 13","pages":"3351–3358 3351–3358"},"PeriodicalIF":4.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758910","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

Screening and Design of Aqueous Zinc Battery Electrolytes Based on the Multimodal Optimization of Molecular Simulation

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-25 DOI: 10.1021/acs.jpclett.5c00341

Wei Feng, Luyan Zhang, Yaobo Cheng, Jin Wu, Chunguang Wei, Junwei Zhang, Kuang Yu

{"title":"Screening and Design of Aqueous Zinc Battery Electrolytes Based on the Multimodal Optimization of Molecular Simulation","authors":"Wei Feng, Luyan Zhang, Yaobo Cheng, Jin Wu, Chunguang Wei, Junwei Zhang, Kuang Yu","doi":"10.1021/acs.jpclett.5c00341","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00341","url":null,"abstract":"Aqueous batteries, such as aqueous zinc-ion batteries (AZIB), have garnered significant attention because of their advantages in intrinsic safety, low cost, and eco-friendliness. However, aqueous electrolytes tend to freeze at low temperatures, which limits their potential industrial applications. Thus, one of the core challenges in aqueous electrolyte design is optimizing the formula to prevent freezing while maintaining good ion conductivity. However, the experimental trial-and-error approach is inefficient for this purpose, and existing simulation tools are either inaccurate or too expensive for high-throughput phase transition predictions. In this work, we employ a small amount of experimental data and differentiable simulation techniques to develop a multimodal optimization workflow. With minimal human intervention, this workflow significantly enhances the prediction power of classical force fields for electrical conductivity. Most importantly, the simulated electrical conductivity can serve as an effective predictor of electrolyte freezing at low temperatures. Generally, the workflow developed in this work introduces a new paradigm for electrolyte design. This paradigm leverages both easily measurable experimental data and fast simulation techniques to predict properties that are challenging to access by using either approach alone.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"47 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695693","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

Odd–Even Effects in the Structure and Thermal Stability of Carboxylic Acid Anchored Monolayers on Naturally Oxidized Aluminum Surface

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-25 DOI: 10.1021/acs.jpclett.5c00500

Daria M. Cegiełka, Łukasz Bodek, Michael Zharnikov, Piotr Cyganik

{"title":"Odd–Even Effects in the Structure and Thermal Stability of Carboxylic Acid Anchored Monolayers on Naturally Oxidized Aluminum Surface","authors":"Daria M. Cegiełka, Łukasz Bodek, Michael Zharnikov, Piotr Cyganik","doi":"10.1021/acs.jpclett.5c00500","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00500","url":null,"abstract":"Self-assembled monolayers (SAMs) are broadly used for molecular engineering of surfaces and interfaces, which demands control over their structure and properties. An important tool in this context is the so-called odd–even effects exploiting the dependence of the SAM structure on the parity of the number of building blocks forming the backbone of SAM-building molecules. Even though these effects influence parameters crucial for SAM applications, they have been mainly studied on coinage metals (Au and Ag) until now. Here, using the series of biphenyl-substituted carboxylic acids (BPnCOO, n = 0–4), we show that structural odd–even behavior occurs as well on technologically relevant surface of naturally oxidized aluminum (representative of other oxide surfaces), with the even-numbered monolayers exhibiting higher packing density and lower molecular inclination than the odd-numbered analogs. Despite these structural changes, the SAM desorption energy remains nearly constant at a high value (∼1.5 eV) making BPnCOO/AlOx a promising system for organic electronics applications.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"6 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695695","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

Non-adiabatic Dynamical Simulations to the Radiative and Non-radiative Recombinations of the Non-fullerene Acceptor Excited State To Optimize Its Photoluminescence Quantum Yield

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-25 DOI: 10.1021/acs.jpclett.5c0042710.1021/acs.jpclett.5c00427

Xinyu Mu, Dongrui Wang, Xue Yang, Yiwen Ji, Wenjing Wang and Kun Gao*,

{"title":"Non-adiabatic Dynamical Simulations to the Radiative and Non-radiative Recombinations of the Non-fullerene Acceptor Excited State To Optimize Its Photoluminescence Quantum Yield","authors":"Xinyu Mu, Dongrui Wang, Xue Yang, Yiwen Ji, Wenjing Wang and Kun Gao*, ","doi":"10.1021/acs.jpclett.5c0042710.1021/acs.jpclett.5c00427","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00427https://doi.org/10.1021/acs.jpclett.5c00427","url":null,"abstract":"Optimizing the photoluminescence quantum yield (PLQY) of non-fullerene acceptor (NFA) molecules is critical for reducing the non-radiative recombination energy loss in NFA-based organic solar cells. In this letter, by developing a non-adiabatic dynamical method combined with different electron population rate equations, we separately simulate the radiative and non-radiative recombination process of the NFA molecular excited state, and thus clarify the quantitative correlations of typical characteristics of NFA molecules with their PLQY, including the analyses for the corresponding mechanisms directed against the conventional “energy gap law”. The main findings include: weakening the intramolecular electron–phonon coupling and electronic push–pull potential can optimize the competition between radiative and non-radiative recombinations, thus improving PLQY; furthermore, increasing the intermolecular J-aggregation ratio should be an effective strategy to alleviate the aggregation-induced reduction in PLQY. These findings provide clear directions for the rational design of NFA molecules and morphology optimization toward a higher PLQY.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 13","pages":"3359–3365 3359–3365"},"PeriodicalIF":4.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758892","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

Enhancing the Photoexcited Carrier Spin Relaxation Lifetime in CsPbBr3 Perovskite Quantum Dots by 208Pb Isotope Enrichment

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-25 DOI: 10.1021/acs.jpclett.5c0012310.1021/acs.jpclett.5c00123

Vivien L. Cherrette, David Zeitz, Mariam Khvichia, Jason K. Cooper, Yuan Ping and Jin Z. Zhang*,

{"title":"Enhancing the Photoexcited Carrier Spin Relaxation Lifetime in CsPbBr3 Perovskite Quantum Dots by 208Pb Isotope Enrichment","authors":"Vivien L. Cherrette, David Zeitz, Mariam Khvichia, Jason K. Cooper, Yuan Ping and Jin Z. Zhang*, ","doi":"10.1021/acs.jpclett.5c0012310.1021/acs.jpclett.5c00123","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00123https://doi.org/10.1021/acs.jpclett.5c00123","url":null,"abstract":"CsPbBr3 perovskite quantum dot (PQD) films enriched with 208Pb (I = 0) or 207Pb (I = 1/2) isotope were used to study the effect of nuclear spin on the photoexcited carrier spin relaxation using circularly polarized femtosecond transient absorption spectroscopy at 293 and 77 K. At 293 K, the short carrier spin relaxation lifetimes of 208Pb-enriched PQDs (2.0 ps) and natPb PQDs (0.70 ps) indicate that electron–phonon interactions dominate. At 77 K, the 207Pb-enriched PQD carrier spin relaxation lifetime was not detectible within the instrumental limit (<0.30 ps). However, the carrier spin relaxation lifetime increased to 5.0 ps for natPb PQDs and 170 ps for 208Pb-enriched PQDs. The dramatic increase in the 208Pb-enriched PQD carrier spin relaxation lifetime suggests that decreasing the concentration of 207Pb in the PQDs can reduce spin decoherence from nuclear spin–carrier spin coupling and enhance the lifetime.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 13","pages":"3336–3342 3336–3342"},"PeriodicalIF":4.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758787","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

Electronic Spectroscopy of YbNH2 and the Potential for Laser Cooling

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-25 DOI: 10.1021/acs.jpclett.5c0040010.1021/acs.jpclett.5c00400

Sophia Vadachkoria, Qingqing Lei, Timothy C. Steimle and Michael C. Heaven*,

{"title":"Electronic Spectroscopy of YbNH2 and the Potential for Laser Cooling","authors":"Sophia Vadachkoria, Qingqing Lei, Timothy C. Steimle and Michael C. Heaven*, ","doi":"10.1021/acs.jpclett.5c0040010.1021/acs.jpclett.5c00400","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00400https://doi.org/10.1021/acs.jpclett.5c00400","url":null,"abstract":"YbNH2 has been recognized as a suitable platform for observations of parity and time-reversal symmetry violations. Gas phase electronic spectra for YbNH2 were obtained for the Ã2B2-X̃2A1 and B̃2B1-X̃2A1 band systems. Both upper states are derived from the Yb+(4f146s)NH2– → Yb+(4f146p)NH2– electron promotion. Laser excitation and dispersed fluorescence measurements yielded band origins, vibrational constants and rotational band contours. Data for the Ã-X̃ system show a Franck–Condon distribution that is favorable for laser cooling. An upper bound for the vibrational branching fraction for the 000 transition in emission was found to be 0.94, assuming negligible radiation to the low-energy Yb+(4f136s2)NH2– states. Quantum chemical calculations for the Ã–X̃ vibronic bands are reported.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 13","pages":"3309–3315 3309–3315"},"PeriodicalIF":4.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.jpclett.5c00400","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758784","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

Electronic Spectroscopy of YbNH2 and the Potential for Laser Cooling

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-25 DOI: 10.1021/acs.jpclett.5c00400

Sophia Vadachkoria, Qingqing Lei, Timothy C. Steimle, Michael C. Heaven

{"title":"Electronic Spectroscopy of YbNH2 and the Potential for Laser Cooling","authors":"Sophia Vadachkoria, Qingqing Lei, Timothy C. Steimle, Michael C. Heaven","doi":"10.1021/acs.jpclett.5c00400","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00400","url":null,"abstract":"YbNH2 has been recognized as a suitable platform for observations of parity and time-reversal symmetry violations. Gas phase electronic spectra for YbNH2 were obtained for the Ã2B2-X̃2A1 and B̃2B1-X̃2A1 band systems. Both upper states are derived from the Yb+(4f146s)NH2– → Yb+(4f146p)NH2– electron promotion. Laser excitation and dispersed fluorescence measurements yielded band origins, vibrational constants and rotational band contours. Data for the Ã-X̃ system show a Franck–Condon distribution that is favorable for laser cooling. An upper bound for the vibrational branching fraction for the 000 transition in emission was found to be 0.94, assuming negligible radiation to the low-energy Yb+(4f136s2)NH2– states. Quantum chemical calculations for the Ã–X̃ vibronic bands are reported.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"71 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695694","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

Unveiling Interactions of a Peptide-Bound Monolayer-Protected Metal Nanocluster with a Lipid Bilayer

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-25 DOI: 10.1021/acs.jpclett.5c00548

Soumya Mondal, Tarak Karmakar

引用次数: 0

Screening and Design of Aqueous Zinc Battery Electrolytes Based on the Multimodal Optimization of Molecular Simulation

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-03-25 DOI: 10.1021/acs.jpclett.5c0034110.1021/acs.jpclett.5c00341

Wei Feng, Luyan Zhang, Yaobo Cheng, Jin Wu, Chunguang Wei, Junwei Zhang and Kuang Yu*,

{"title":"Screening and Design of Aqueous Zinc Battery Electrolytes Based on the Multimodal Optimization of Molecular Simulation","authors":"Wei Feng, Luyan Zhang, Yaobo Cheng, Jin Wu, Chunguang Wei, Junwei Zhang and Kuang Yu*, ","doi":"10.1021/acs.jpclett.5c0034110.1021/acs.jpclett.5c00341","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00341https://doi.org/10.1021/acs.jpclett.5c00341","url":null,"abstract":"Aqueous batteries, such as aqueous zinc-ion batteries (AZIB), have garnered significant attention because of their advantages in intrinsic safety, low cost, and eco-friendliness. However, aqueous electrolytes tend to freeze at low temperatures, which limits their potential industrial applications. Thus, one of the core challenges in aqueous electrolyte design is optimizing the formula to prevent freezing while maintaining good ion conductivity. However, the experimental trial-and-error approach is inefficient for this purpose, and existing simulation tools are either inaccurate or too expensive for high-throughput phase transition predictions. In this work, we employ a small amount of experimental data and differentiable simulation techniques to develop a multimodal optimization workflow. With minimal human intervention, this workflow significantly enhances the prediction power of classical force fields for electrical conductivity. Most importantly, the simulated electrical conductivity can serve as an effective predictor of electrolyte freezing at low temperatures. Generally, the workflow developed in this work introduces a new paradigm for electrolyte design. This paradigm leverages both easily measurable experimental data and fast simulation techniques to predict properties that are challenging to access by using either approach alone.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 13","pages":"3326–3335 3326–3335"},"PeriodicalIF":4.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758783","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