The Journal of Physical Chemistry Letters最新文献_第9页

Amplified Detection of Threading Dislocations in n-Type 4H-SiC Epilayers Enabled by Time-Resolved Photoluminescence Mapping

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-09 DOI: 10.1021/acs.jpclett.4c03297

Zhaoxia Yang, Fengke Sun, Jing Leng, Wenming Tian, Shengye Jin

引用次数: 0

Ion Migration at Metal Halide Perovskite Grain Boundaries Elucidated with a Machine Learning Force Field

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-09 DOI: 10.1021/acs.jpclett.4c0333210.1021/acs.jpclett.4c03332

Mikhail R. Samatov, Dongyu Liu*, Long Zhao, Elena A. Kazakova, Dmitrii A. Abrameshin, Abinash Das, Andrey S. Vasenko and Oleg V. Prezhdo*,

{"title":"Ion Migration at Metal Halide Perovskite Grain Boundaries Elucidated with a Machine Learning Force Field","authors":"Mikhail R. Samatov, Dongyu Liu*, Long Zhao, Elena A. Kazakova, Dmitrii A. Abrameshin, Abinash Das, Andrey S. Vasenko and Oleg V. Prezhdo*, ","doi":"10.1021/acs.jpclett.4c0333210.1021/acs.jpclett.4c03332","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03332https://doi.org/10.1021/acs.jpclett.4c03332","url":null,"abstract":"Metal halide perovskites are promising optoelectronic materials with excellent defect tolerance in carrier recombination, believed to arise largely from their unique soft lattices. However, weak lattice interactions also promote ion migration, leading to serious stability issues. Grain boundaries (GBs) have been experimentally identified as the primary migration channels, but the relevant mechanism remains elusive. Using molecular dynamics with a machine learning force field, we directly model ion migration at a common CsPbBr3 GB. We demonstrate that the as-built GB model, containing 6400 atoms, experiences structural reconstruction over several nanoseconds, and only Br atoms diffuse after that. A fraction of Br atoms near the GB either migrate toward the GB center or along the GB through different migration channels. Increasing the temperature not only accelerates the ion migration via the Arrhenius activation but also allows more Br atoms to migrate. The activation energies are much lower at the GB than in the bulk due to large-scale structural distortions and favorable non-stoichiometric local environments available at GBs. Making the local GB composition more stoichiometric by doping or annealing can suppress the ion migration. The reported results provide valuable atomistic insights into the GB properties and ion migration in metal halide perovskites.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 50","pages":"12362–12369 12362–12369"},"PeriodicalIF":4.8,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.jpclett.4c03332","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842816","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

Chiral-Polar Alternating Cation Intercalation-Type Perovskite Enables Sensitive Self-Driven X-ray Detection with an Ultralow Detection Limit

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-09 DOI: 10.1021/acs.jpclett.4c0297610.1021/acs.jpclett.4c02976

Qiuxiao Yin, Jianbo Wu, Zeng-Kui Zhu, Huang Ye, Ruiqing Li, Tingting Zhu, Yaru Geng, Lijun Xu, Zhangtong Han, Chengshu Zhang and Junhua Luo*,

{"title":"Chiral-Polar Alternating Cation Intercalation-Type Perovskite Enables Sensitive Self-Driven X-ray Detection with an Ultralow Detection Limit","authors":"Qiuxiao Yin, Jianbo Wu, Zeng-Kui Zhu, Huang Ye, Ruiqing Li, Tingting Zhu, Yaru Geng, Lijun Xu, Zhangtong Han, Chengshu Zhang and Junhua Luo*, ","doi":"10.1021/acs.jpclett.4c0297610.1021/acs.jpclett.4c02976","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02976https://doi.org/10.1021/acs.jpclett.4c02976","url":null,"abstract":"Metal halide perovskites (MHPs) have shown great potential for direct X-ray detection, but achieving high sensitivity without external bias remains challenging. Chiral-polar alternating cation intercalation (ACI)-type MHPs, with excellent optoelectronic properties and a robust chirality-induced bulk photovoltaic effect (BPVE), offer a promising platform for self-driven X-ray detection. Herein, impressive self-driven X-ray detection performance was achieved by utilizing chiral-polar 2D ACI-type perovskite single crystals of (R-PPA)PAPbBr4 (1R; R-PPA = R-1-phenylpropylamine; PA = propylamine). The chiral R-PPA cations induce the crystallization of 1R in the chiral-polar space group P21, wherein its spontaneous electric polarization further induces a strong BPVE. Consequently, 1R shows remarkable radiation photovoltaics of 0.75 V, which endows its excellent self-driven X-ray detection with a high sensitivity of 417.2 μC Gy–1 cm–2 and a low detection limit of 24.1 nGy s–1, meeting the state-of-the-art level by leveraging its intrinsic photovoltaic effect. These findings highlight the huge potential of chiral-polar ACI-type MHPs in self-driven X-ray detection applications.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 50","pages":"12348–12356 12348–12356"},"PeriodicalIF":4.8,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842817","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

Chiral-Polar Alternating Cation Intercalation-Type Perovskite Enables Sensitive Self-Driven X-ray Detection with an Ultralow Detection Limit

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-09 DOI: 10.1021/acs.jpclett.4c02976

Qiuxiao Yin, Jianbo Wu, Zeng-Kui Zhu, Huang Ye, Ruiqing Li, Tingting Zhu, Yaru Geng, Lijun Xu, Zhangtong Han, Chengshu Zhang, Junhua Luo

{"title":"Chiral-Polar Alternating Cation Intercalation-Type Perovskite Enables Sensitive Self-Driven X-ray Detection with an Ultralow Detection Limit","authors":"Qiuxiao Yin, Jianbo Wu, Zeng-Kui Zhu, Huang Ye, Ruiqing Li, Tingting Zhu, Yaru Geng, Lijun Xu, Zhangtong Han, Chengshu Zhang, Junhua Luo","doi":"10.1021/acs.jpclett.4c02976","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02976","url":null,"abstract":"Metal halide perovskites (MHPs) have shown great potential for direct X-ray detection, but achieving high sensitivity without external bias remains challenging. Chiral-polar alternating cation intercalation (ACI)-type MHPs, with excellent optoelectronic properties and a robust chirality-induced bulk photovoltaic effect (BPVE), offer a promising platform for self-driven X-ray detection. Herein, impressive self-driven X-ray detection performance was achieved by utilizing chiral-polar 2D ACI-type perovskite single crystals of (R-PPA)PAPbBr4 (1R; R-PPA = R-1-phenylpropylamine; PA = propylamine). The chiral R-PPA cations induce the crystallization of 1R in the chiral-polar space group P21, wherein its spontaneous electric polarization further induces a strong BPVE. Consequently, 1R shows remarkable radiation photovoltaics of 0.75 V, which endows its excellent self-driven X-ray detection with a high sensitivity of 417.2 μC Gy–1 cm–2 and a low detection limit of 24.1 nGy s–1, meeting the state-of-the-art level by leveraging its intrinsic photovoltaic effect. These findings highlight the huge potential of chiral-polar ACI-type MHPs in self-driven X-ray detection applications.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"20 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793341","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 the Dynamic Aspects of Photoinduced Halide Segregation in Mixed-Halide Cs0.15FA0.85PbI2Br Perovskite Films Using a Hyperspectral Imaging Technique

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-09 DOI: 10.1021/acs.jpclett.4c03077

Yusuke Daikoku, Takumi Yamada, Ai Shimazaki, Tomoya Nakamura, Atsushi Wakamiya, Yoshihiko Kanemitsu

引用次数: 0

Unraveling Photoinduced Desorption Dynamics of π-Conjugated Ligands in ZnS Nanocrystals via Pump–Push–Probe Spectroscopy

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-09 DOI: 10.1021/acs.jpclett.4c0326010.1021/acs.jpclett.4c03260

Daisuke Yoshioka, Jessica M. de la Perrelle, Andrew Dolan, Zi Goh, Tak W. Kee and Yoichi Kobayashi*,

{"title":"Unraveling Photoinduced Desorption Dynamics of π-Conjugated Ligands in ZnS Nanocrystals via Pump–Push–Probe Spectroscopy","authors":"Daisuke Yoshioka, Jessica M. de la Perrelle, Andrew Dolan, Zi Goh, Tak W. Kee and Yoichi Kobayashi*, ","doi":"10.1021/acs.jpclett.4c0326010.1021/acs.jpclett.4c03260","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03260https://doi.org/10.1021/acs.jpclett.4c03260","url":null,"abstract":"The photoinduced ligand desorption from nanocrystal (NC) surfaces plays a critical role in the diverse functionalities of NCs. However, this reaction is inherently complex because photophysical and photochemical reactions are involved, and many aspects remain elusive. In this study, using ZnS NCs coordinated with perylenebisimide (PBI) ligands as a model system, we revealed that pump–push–probe spectroscopy provides detailed insights into the transient species following photoinduced ligand desorption reactions. This method successfully isolated the signal of the PBI radical anion, generated by photoinduced charge separation, which was difficult to identify by conventional pump–probe spectroscopy. Furthermore, pump–push–probe spectroscopy also revealed that the transiently formed aggregation of PBI after PBI desorption is the H-type aggregate. This research is expected to contribute to the analysis of complex photochemical reaction processes in composite nanomaterials and is important for the development of highly efficient NC photocatalysts and photodurable NCs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 50","pages":"12370–12375 12370–12375"},"PeriodicalIF":4.8,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842988","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

Photosynthetic Energy Transfer: Missing in Action (Detected Spectroscopy)? 光合作用能量转移：行动中的缺失（检测光谱学）？

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-09 DOI: 10.1021/acs.jpclett.4c02665

Ariba Javed, Julian Lüttig, Kateřina Charvátová, Stephanie E. Sanders, Rhiannon Willow, Muyi Zhang, Alastair T. Gardiner, Pavel Malý, Jennifer P. Ogilvie

{"title":"Photosynthetic Energy Transfer: Missing in Action (Detected Spectroscopy)?","authors":"Ariba Javed, Julian Lüttig, Kateřina Charvátová, Stephanie E. Sanders, Rhiannon Willow, Muyi Zhang, Alastair T. Gardiner, Pavel Malý, Jennifer P. Ogilvie","doi":"10.1021/acs.jpclett.4c02665","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02665","url":null,"abstract":"In recent years, action-detected ultrafast spectroscopies have gained popularity offering distinct advantages over their coherently detected counterparts, such as spatially resolved and operando measurements with high sensitivity. However, there are also fundamental limitations connected to the process of signal generation in action-detected experiments. Here we perform fluorescence-detected two-dimensional electronic spectroscopy (F-2DES) of the light-harvesting II (LH2) complex from purple bacteria. We demonstrate that the B800–B850 energy transfer process in LH2 is weak but observable in F-2DES, unlike in coherently detected 2DES where the energy transfer is visible with 100% contrast. We explain the weak signatures using a disordered excitonic model that accounts for experimental conditions. We further derive a general formula for the presence of excited-state signals in multichromophoric aggregates, dependent on the aggregate geometry, size, excitonic coupling and disorder. We find that the prominence of excited-state dynamics in action-detected spectroscopy offers a unique probe of excitonic delocalization in multichromophoric systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"19 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797850","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

Amplified Detection of Threading Dislocations in n-Type 4H-SiC Epilayers Enabled by Time-Resolved Photoluminescence Mapping

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-09 DOI: 10.1021/acs.jpclett.4c0329710.1021/acs.jpclett.4c03297

Zhaoxia Yang, Fengke Sun, Jing Leng, Wenming Tian* and Shengye Jin*,

引用次数: 0

Photosynthetic Energy Transfer: Missing in Action (Detected Spectroscopy)?

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-09 DOI: 10.1021/acs.jpclett.4c0266510.1021/acs.jpclett.4c02665

Ariba Javed, Julian Lüttig, Kateřina Charvátová, Stephanie E. Sanders, Rhiannon Willow, Muyi Zhang, Alastair T. Gardiner, Pavel Malý* and Jennifer P. Ogilvie*,

{"title":"Photosynthetic Energy Transfer: Missing in Action (Detected Spectroscopy)?","authors":"Ariba Javed, Julian Lüttig, Kateřina Charvátová, Stephanie E. Sanders, Rhiannon Willow, Muyi Zhang, Alastair T. Gardiner, Pavel Malý* and Jennifer P. Ogilvie*, ","doi":"10.1021/acs.jpclett.4c0266510.1021/acs.jpclett.4c02665","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02665https://doi.org/10.1021/acs.jpclett.4c02665","url":null,"abstract":"In recent years, action-detected ultrafast spectroscopies have gained popularity offering distinct advantages over their coherently detected counterparts, such as spatially resolved and operando measurements with high sensitivity. However, there are also fundamental limitations connected to the process of signal generation in action-detected experiments. Here we perform fluorescence-detected two-dimensional electronic spectroscopy (F-2DES) of the light-harvesting II (LH2) complex from purple bacteria. We demonstrate that the B800–B850 energy transfer process in LH2 is weak but observable in F-2DES, unlike in coherently detected 2DES where the energy transfer is visible with 100% contrast. We explain the weak signatures using a disordered excitonic model that accounts for experimental conditions. We further derive a general formula for the presence of excited-state signals in multichromophoric aggregates, dependent on the aggregate geometry, size, excitonic coupling and disorder. We find that the prominence of excited-state dynamics in action-detected spectroscopy offers a unique probe of excitonic delocalization in multichromophoric systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 50","pages":"12376–12386 12376–12386"},"PeriodicalIF":4.8,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842986","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

Unraveling Photoinduced Desorption Dynamics of π-Conjugated Ligands in ZnS Nanocrystals via Pump–Push–Probe Spectroscopy

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-09 DOI: 10.1021/acs.jpclett.4c03260

Daisuke Yoshioka, Jessica M. de la Perrelle, Andrew Dolan, Zi Goh, Tak W. Kee, Yoichi Kobayashi

{"title":"Unraveling Photoinduced Desorption Dynamics of π-Conjugated Ligands in ZnS Nanocrystals via Pump–Push–Probe Spectroscopy","authors":"Daisuke Yoshioka, Jessica M. de la Perrelle, Andrew Dolan, Zi Goh, Tak W. Kee, Yoichi Kobayashi","doi":"10.1021/acs.jpclett.4c03260","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03260","url":null,"abstract":"The photoinduced ligand desorption from nanocrystal (NC) surfaces plays a critical role in the diverse functionalities of NCs. However, this reaction is inherently complex because photophysical and photochemical reactions are involved, and many aspects remain elusive. In this study, using ZnS NCs coordinated with perylenebisimide (PBI) ligands as a model system, we revealed that pump–push–probe spectroscopy provides detailed insights into the transient species following photoinduced ligand desorption reactions. This method successfully isolated the signal of the PBI radical anion, generated by photoinduced charge separation, which was difficult to identify by conventional pump–probe spectroscopy. Furthermore, pump–push–probe spectroscopy also revealed that the transiently formed aggregation of PBI after PBI desorption is the H-type aggregate. This research is expected to contribute to the analysis of complex photochemical reaction processes in composite nanomaterials and is important for the development of highly efficient NC photocatalysts and photodurable NCs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793344","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