The Journal of Physical Chemistry Letters最新文献_第10页

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

IF 6.475 2区化学

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

Mikhail R. Samatov, Dongyu Liu, Long Zhao, Elena A. Kazakova, Dmitrii A. Abrameshin, Abinash Das, Andrey S. Vasenko, 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, Oleg V. Prezhdo","doi":"10.1021/acs.jpclett.4c03332","DOIUrl":"https://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":"777 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793346","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 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-09 DOI: 10.1021/acs.jpclett.4c0307710.1021/acs.jpclett.4c03077

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

{"title":"Revealing the Dynamic Aspects of Photoinduced Halide Segregation in Mixed-Halide Cs0.15FA0.85PbI2Br Perovskite Films Using a Hyperspectral Imaging Technique","authors":"Yusuke Daikoku, Takumi Yamada, Ai Shimazaki, Tomoya Nakamura, Atsushi Wakamiya and Yoshihiko Kanemitsu*, ","doi":"10.1021/acs.jpclett.4c0307710.1021/acs.jpclett.4c03077","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03077https://doi.org/10.1021/acs.jpclett.4c03077","url":null,"abstract":"The band gap energy of halide perovskite semiconductors is manipulated by controlling the halide composition, and mixed halide perovskites are receiving much attention as top cell materials for tandem solar cells. To understand dynamic aspects of photoinduced halide segregation in mixed-halide perovskite films, we use a hyperspectral imaging technique. We reveal the space- and time-resolved photoluminescence (PL) spectra of Cs0.15FA0.85PbI2Br perovskite films during prolonged light illumination. Under applied electric fields, we observe photoinduced phase segregation at the excitation laser spot, with a line-shape I-rich region of low PL efficiency appearing near the anode electrode. This I-rich region moves from the anode to the cathode electrodes and stops at the laser excitation spot. We discuss the significant enhancement of halide ion migration under light illumination and the dynamical changes of photoinduced halide segregation.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 50","pages":"12341–12347 12341–12347"},"PeriodicalIF":4.8,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842914","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

Charge Transfer and Retention in 2D Passivated Perovskite–C60 Systems

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-07 DOI: 10.1021/acs.jpclett.4c02898

Hannu P. Pasanen, Vladyslav Hnapovskyi, Anand Selvin Subbiah, Stefaan De Wolf, Frédéric Laquai

引用次数: 0

Charge Transfer and Retention in 2D Passivated Perovskite–C60 Systems

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-07 DOI: 10.1021/acs.jpclett.4c0289810.1021/acs.jpclett.4c02898

Hannu P. Pasanen*, Vladyslav Hnapovskyi, Anand Selvin Subbiah, Stefaan De Wolf and Frédéric Laquai,

{"title":"Charge Transfer and Retention in 2D Passivated Perovskite–C60 Systems","authors":"Hannu P. Pasanen*, Vladyslav Hnapovskyi, Anand Selvin Subbiah, Stefaan De Wolf and Frédéric Laquai, ","doi":"10.1021/acs.jpclett.4c0289810.1021/acs.jpclett.4c02898","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02898https://doi.org/10.1021/acs.jpclett.4c02898","url":null,"abstract":"2D perovskites and organic ligands are often implemented as passivating interlayers in perovskite solar cells. Herein, five such passivates are evaluated by using time-resolved spectroscopy to study the carrier dynamics at the perovskite–C60 interface. The impact of passivation on factors such as charge transfer rate, charge retention in the acceptor layers, surface recombination, and uniformity are mapped onto the solar cell performance. The charge transfer was found to take place in tens of nanoseconds, and the charge retention without any passivate lasted a few hundred nanoseconds. The passivate that produced the best solar cells, ethylenediammonium iodide, extended the charge retention time up to one microsecond, which significantly increased the open-circuit voltage. It also had the best uniformity and hence least variance in power conversion efficiency. Curiously, it did not merely adjust surface energy states to enhance charge transfer but also extracted charges by itself without the C60, resulting in higher short-circuit current.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 50","pages":"12334–12340 12334–12340"},"PeriodicalIF":4.8,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842063","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

Prediction and Measurement of Resonant and Nonresonant Shake Effects in the Core-Level X-ray Emission Spectra of 3d0 Transition Metal Compounds

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-06 DOI: 10.1021/acs.jpclett.4c02583

Charles A. Cardot, Joshua J. Kas, John J. Rehr, Jared E. Abramson, Gerald T. Seidler

{"title":"Prediction and Measurement of Resonant and Nonresonant Shake Effects in the Core-Level X-ray Emission Spectra of 3d0 Transition Metal Compounds","authors":"Charles A. Cardot, Joshua J. Kas, John J. Rehr, Jared E. Abramson, Gerald T. Seidler","doi":"10.1021/acs.jpclett.4c02583","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02583","url":null,"abstract":"Shake effects, resulting from sudden core potential changes during photoexcitation, are well-known in X-ray photoelectron spectroscopy (XPS) and often produce satellite peaks due to many-body excitations. It has been thought, however, that they are negligible in core-to-core X-ray emission spectroscopy (CTC-XES), where the difference in core–hole potentials upon radiative decay is rather small. We demonstrate that shake effects are significant in Kα XES from 3d transition metal systems with nominally zero valence electrons. We show that valence level shake satellites are amplified via interference due to a resonance between the 2p3/2-hole (Kα1) plus valence level shake state and the 2p1/2-hole (Kα2) state. Additionally, while the Kα2 shake satellite is indeed predicted to be weak, we observe it experimentally, providing further independent verification of our model. This prediction includes a detailed analysis of 2p to 1s Kα XES using density functional theory (DFT)-augmented multiplet ligand field theory (MLFT).","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"97 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142783105","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

Ultrafast Carrier Diffusion in Perovskite Monocrystalline Films

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-06 DOI: 10.1021/acs.jpclett.4c03063

Xiayuan Xu, Yan Chen, Yijie Luo, Yuxin Zhang, Yiqun Duan, Yaobin Li, Guanyu Zhang, Zhijian Chen, Shufeng Wang, Guowei Lu

{"title":"Ultrafast Carrier Diffusion in Perovskite Monocrystalline Films","authors":"Xiayuan Xu, Yan Chen, Yijie Luo, Yuxin Zhang, Yiqun Duan, Yaobin Li, Guanyu Zhang, Zhijian Chen, Shufeng Wang, Guowei Lu","doi":"10.1021/acs.jpclett.4c03063","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03063","url":null,"abstract":"Monocrystalline perovskite materials exhibit superior properties compared with polycrystalline perovskites, including lower defect density, minimal grain boundaries, and enhanced carrier mobility. Nevertheless, the preparation of large-area, high-quality single-crystal films, which could prove invaluable for photoelectronic applications, remains a significant challenge. The study of how their unique properties go beyond polycrystalline thin films is still missing. In our experiment, using polarization-selective transient absorption microscopy, we directly observed the spatial carrier transportation in methylammonium lead iodide (CH3NH3PbI3, MAPbI3) strip-shaped monocrystalline ultrathin films. Ultrafast carrier diffusion transportation was observed. The monocrystalline carrier diffusion coefficient D (∼22 cm2 s–1) is an order of magnitude higher than that in polycrystalline films. Anisotropic carrier diffusion of the MAPbI3 single crystal has been discovered. It is also discovered that the electrons and holes are of different anisotropy and diffusion speed. This ultralong carrier transport inside the monocrystalline film provides solid support for the development of perovskite based photoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"20 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782963","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

High-Throughput Computing of Janus Chalcogenides as Photocatalysts and Piezoelectric Materials for Overall Water Splitting

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-06 DOI: 10.1021/acs.jpclett.4c03062

Jiali Wang, Xiuwen Zhao, Guichao Hu, Xiaobo Yuan, Junfeng Ren, Siyun Qi

{"title":"High-Throughput Computing of Janus Chalcogenides as Photocatalysts and Piezoelectric Materials for Overall Water Splitting","authors":"Jiali Wang, Xiuwen Zhao, Guichao Hu, Xiaobo Yuan, Junfeng Ren, Siyun Qi","doi":"10.1021/acs.jpclett.4c03062","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03062","url":null,"abstract":"The presence of the intrinsic fields in two-dimensional (2D) materials holds promise for photocatalysts, as it diminishes the band gap requirements of 1.23 eV and accelerates the separation of the photogenerated carriers. Inspired by the extensive application in MA2X4 families, we predict Janus ZMXAY derived from MA2X4 materials to introduce intrinsic fields suitable for photocatalysts from 512 candidates. These monolayers also exhibit high mobilities up to ∼104 cm2V–1s–1 with strong anisotropy, and are accompanied by the inherent piezoelectric properties. Notably, all monolayers, except Janus SMoPGeAs, SeMoPSiAs, and SeMoPGeAs, demonstrate suitable band gaps (0.88–1.43 eV) and appropriate band edge positions without the need for any external potential to drive spontaneous overall water splitting. It also demonstrates visible optical absorption capacity and high solar-to-hydrogen conversion efficiency (16.06–41.08%). Our work identifies ideal candidates for multifunctional devices and provides theoretical guidance for future experimental research and application development.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"19 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142783097","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

Prediction and Measurement of Resonant and Nonresonant Shake Effects in the Core-Level X-ray Emission Spectra of 3d0 Transition Metal Compounds

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-06 DOI: 10.1021/acs.jpclett.4c0258310.1021/acs.jpclett.4c02583

Charles A. Cardot, Joshua J. Kas, John J. Rehr, Jared E. Abramson and Gerald T. Seidler*,

{"title":"Prediction and Measurement of Resonant and Nonresonant Shake Effects in the Core-Level X-ray Emission Spectra of 3d0 Transition Metal Compounds","authors":"Charles A. Cardot, Joshua J. Kas, John J. Rehr, Jared E. Abramson and Gerald T. Seidler*, ","doi":"10.1021/acs.jpclett.4c0258310.1021/acs.jpclett.4c02583","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02583https://doi.org/10.1021/acs.jpclett.4c02583","url":null,"abstract":"Shake effects, resulting from sudden core potential changes during photoexcitation, are well-known in X-ray photoelectron spectroscopy (XPS) and often produce satellite peaks due to many-body excitations. It has been thought, however, that they are negligible in core-to-core X-ray emission spectroscopy (CTC-XES), where the difference in core–hole potentials upon radiative decay is rather small. We demonstrate that shake effects are significant in Kα XES from 3d transition metal systems with nominally zero valence electrons. We show that valence level shake satellites are amplified via interference due to a resonance between the 2p3/2-hole (Kα1) plus valence level shake state and the 2p1/2-hole (Kα2) state. Additionally, while the Kα2 shake satellite is indeed predicted to be weak, we observe it experimentally, providing further independent verification of our model. This prediction includes a detailed analysis of 2p to 1s Kα XES using density functional theory (DFT)-augmented multiplet ligand field theory (MLFT).","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 50","pages":"12326–12333 12326–12333"},"PeriodicalIF":4.8,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850263","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

High-Throughput Computing of Janus Chalcogenides as Photocatalysts and Piezoelectric Materials for Overall Water Splitting

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-06 DOI: 10.1021/acs.jpclett.4c0306210.1021/acs.jpclett.4c03062

Jiali Wang, Xiuwen Zhao, Guichao Hu, Xiaobo Yuan, Junfeng Ren* and Siyun Qi*,

{"title":"High-Throughput Computing of Janus Chalcogenides as Photocatalysts and Piezoelectric Materials for Overall Water Splitting","authors":"Jiali Wang, Xiuwen Zhao, Guichao Hu, Xiaobo Yuan, Junfeng Ren* and Siyun Qi*, ","doi":"10.1021/acs.jpclett.4c0306210.1021/acs.jpclett.4c03062","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03062https://doi.org/10.1021/acs.jpclett.4c03062","url":null,"abstract":"The presence of the intrinsic fields in two-dimensional (2D) materials holds promise for photocatalysts, as it diminishes the band gap requirements of 1.23 eV and accelerates the separation of the photogenerated carriers. Inspired by the extensive application in MA2X4 families, we predict Janus ZMXAY derived from MA2X4 materials to introduce intrinsic fields suitable for photocatalysts from 512 candidates. These monolayers also exhibit high mobilities up to ∼104 cm2V–1s–1 with strong anisotropy, and are accompanied by the inherent piezoelectric properties. Notably, all monolayers, except Janus SMoPGeAs, SeMoPSiAs, and SeMoPGeAs, demonstrate suitable band gaps (0.88–1.43 eV) and appropriate band edge positions without the need for any external potential to drive spontaneous overall water splitting. It also demonstrates visible optical absorption capacity and high solar-to-hydrogen conversion efficiency (16.06–41.08%). Our work identifies ideal candidates for multifunctional devices and provides theoretical guidance for future experimental research and application development.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 50","pages":"12309–12317 12309–12317"},"PeriodicalIF":4.8,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842182","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

Ultrafast Carrier Diffusion in Perovskite Monocrystalline Films

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-12-06 DOI: 10.1021/acs.jpclett.4c0306310.1021/acs.jpclett.4c03063

Xiayuan Xu, Yan Chen, Yijie Luo, Yuxin Zhang, Yiqun Duan, Yaobin Li, Guanyu Zhang, Zhijian Chen, Shufeng Wang* and Guowei Lu*,

{"title":"Ultrafast Carrier Diffusion in Perovskite Monocrystalline Films","authors":"Xiayuan Xu, Yan Chen, Yijie Luo, Yuxin Zhang, Yiqun Duan, Yaobin Li, Guanyu Zhang, Zhijian Chen, Shufeng Wang* and Guowei Lu*, ","doi":"10.1021/acs.jpclett.4c0306310.1021/acs.jpclett.4c03063","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03063https://doi.org/10.1021/acs.jpclett.4c03063","url":null,"abstract":"Monocrystalline perovskite materials exhibit superior properties compared with polycrystalline perovskites, including lower defect density, minimal grain boundaries, and enhanced carrier mobility. Nevertheless, the preparation of large-area, high-quality single-crystal films, which could prove invaluable for photoelectronic applications, remains a significant challenge. The study of how their unique properties go beyond polycrystalline thin films is still missing. In our experiment, using polarization-selective transient absorption microscopy, we directly observed the spatial carrier transportation in methylammonium lead iodide (CH3NH3PbI3, MAPbI3) strip-shaped monocrystalline ultrathin films. Ultrafast carrier diffusion transportation was observed. The monocrystalline carrier diffusion coefficient D (∼22 cm2 s–1) is an order of magnitude higher than that in polycrystalline films. Anisotropic carrier diffusion of the MAPbI3 single crystal has been discovered. It is also discovered that the electrons and holes are of different anisotropy and diffusion speed. This ultralong carrier transport inside the monocrystalline film provides solid support for the development of perovskite based photoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 50","pages":"12318–12325 12318–12325"},"PeriodicalIF":4.8,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842180","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