A narrowband detection photodetector (PD) serves as a rapid identifier of specific wavebands, holding immense significance in secure communication and spectral recognition. Herein, after carbon is doped into GaN, an acceptor energy level emerges in its band structure, which will compensate with donor states in GaN to reduce carrier concentration and make GaN semi-insulating, and it affected the dark current and electric field distribution of the GaN p-i-n PD. Operating at a bias of 0 V, the C-doped GaN p-i-n PD demonstrates an ultralow dark current density and a high light-to-dark current ratio compared to the undoped intrinsic i-layer GaN p-i-n PD. Moreover, the narrowband response’s full width at half-maximum of the PD is only 8.11 nm and displays rapid signal feedback capabilities. Consequently, this prepared C-doped GaN p-i-n PD, which obviates the need for integrating optical filters or employing sophisticated processes, stands to be capable of accurately distinguishing UVA radiation.
{"title":"Enhanced Ultra-narrowband Fast Response Ultraviolet Photodetector based on GaN Homojunction with a Carbon-Doped Semi-insulating Intermediate Layer","authors":"Shihao Fu, Danyang Xia, Rongpeng Fu, Yuefei Wang, Yurui Han, Chong Gao, Weizhe Cui, Bingsheng Li, Zhendong Fu, Si Shen, Aidong Shen","doi":"10.1021/acs.jpclett.5c00026","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00026","url":null,"abstract":"A narrowband detection photodetector (PD) serves as a rapid identifier of specific wavebands, holding immense significance in secure communication and spectral recognition. Herein, after carbon is doped into GaN, an acceptor energy level emerges in its band structure, which will compensate with donor states in GaN to reduce carrier concentration and make GaN semi-insulating, and it affected the dark current and electric field distribution of the GaN p-i-n PD. Operating at a bias of 0 V, the C-doped GaN p-i-n PD demonstrates an ultralow dark current density and a high light-to-dark current ratio compared to the undoped intrinsic i-layer GaN p-i-n PD. Moreover, the narrowband response’s full width at half-maximum of the PD is only 8.11 nm and displays rapid signal feedback capabilities. Consequently, this prepared C-doped GaN p-i-n PD, which obviates the need for integrating optical filters or employing sophisticated processes, stands to be capable of accurately distinguishing UVA radiation.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"25 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560903","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}
Pub Date : 2025-03-06DOI: 10.1021/acs.jpclett.5c00125
Yifan Cheng, Xian Lin, Chunwei Wang, Zeyu Zhang, Chen Wang, Long Geng, Peng Suo, Juan Du, Guohong Ma
Heterostructures composed of graphene (Gr) and transition metal dichalcogenides (TMDs) establish a new platform for optoelectronic applications. A substantial amount of research has concentrated on the interfacial charge transfer (CT) within heterostructures, yet investigations into the nonlinear effects occurring within these heterostructures have been relatively scarce. Utilizing terahertz (THz) emission spectroscopy, we demonstrate the synergistic interaction between interfacial CT and nonlinear photocurrent within the Gr/MoS2 heterostructure. Our study shows that despite the cancellation of photocurrents from CT in the MoS2/Gr/MoS2 sandwich heterostructure, THz emissions are still observable, indicating additional photocurrents from other effects. By conducting experiments that involved varying the pump fluence, sample azimuthal angle, incidence angle, and pump polarization states, we determined that the THz radiation in the MoS2/Gr/MoS2 heterostructure is dominated by the photon drag effect (PDE), particularly dominated by the photon drag injection current. For the case of the Gr/MoS2 heterostructure, both CT and PDE play a role in THz emission, and the contribution of CT to THz emission is dominant, with an estimated CT:PDE ratio of 5:2. The study provides a foundation for the application of these heterostructures in next-generation optoelectronic devices.
{"title":"Revealing a Nonlinear Photocurrent in the Graphene/MoS2 Heterostructure via Terahertz Emission Spectroscopy","authors":"Yifan Cheng, Xian Lin, Chunwei Wang, Zeyu Zhang, Chen Wang, Long Geng, Peng Suo, Juan Du, Guohong Ma","doi":"10.1021/acs.jpclett.5c00125","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00125","url":null,"abstract":"Heterostructures composed of graphene (Gr) and transition metal dichalcogenides (TMDs) establish a new platform for optoelectronic applications. A substantial amount of research has concentrated on the interfacial charge transfer (CT) within heterostructures, yet investigations into the nonlinear effects occurring within these heterostructures have been relatively scarce. Utilizing terahertz (THz) emission spectroscopy, we demonstrate the synergistic interaction between interfacial CT and nonlinear photocurrent within the Gr/MoS<sub>2</sub> heterostructure. Our study shows that despite the cancellation of photocurrents from CT in the MoS<sub>2</sub>/Gr/MoS<sub>2</sub> sandwich heterostructure, THz emissions are still observable, indicating additional photocurrents from other effects. By conducting experiments that involved varying the pump fluence, sample azimuthal angle, incidence angle, and pump polarization states, we determined that the THz radiation in the MoS<sub>2</sub>/Gr/MoS<sub>2</sub> heterostructure is dominated by the photon drag effect (PDE), particularly dominated by the photon drag injection current. For the case of the Gr/MoS<sub>2</sub> heterostructure, both CT and PDE play a role in THz emission, and the contribution of CT to THz emission is dominant, with an estimated CT:PDE ratio of 5:2. The study provides a foundation for the application of these heterostructures in next-generation optoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560904","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}
Pub Date : 2025-03-06DOI: 10.1021/acs.jpclett.5c0034510.1021/acs.jpclett.5c00345
Zhihua Wu, Jian-Feng Li* and Zhong-Qun Tian*,
{"title":"Celebrating 10 Years of the Collaborative Innovation Center of Chemistry for Energy Materials (iChEM)","authors":"Zhihua Wu, Jian-Feng Li* and Zhong-Qun Tian*, ","doi":"10.1021/acs.jpclett.5c0034510.1021/acs.jpclett.5c00345","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00345https://doi.org/10.1021/acs.jpclett.5c00345","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 9","pages":"2417–2418 2417–2418"},"PeriodicalIF":4.8,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143547775","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}
Pub Date : 2025-03-06DOI: 10.1021/acs.jpclett.5c00086
Aniket Mandal, John M. Herbert
Range-separated hybrid functionals have dramatically improved the description of charge-transfer excitations in time-dependent density functional theory (TD-DFT), especially when the range-separation parameter is adjusted in order to satisfy the ionization energy (IE) criterion, εHOMO = −IE. However, this “optimal tuning” procedure is molecule-specific, inconvenient, expensive for large systems, and problematic in extended or periodic systems. Here, we consider an alternative procedure known as global density-dependent (GDD) tuning, which sets the range-separation parameter in an automated way based on properties of the exchange hole. In small molecules, we find that long-range corrected functionals with either IE or GDD tuning afford remarkably similar TD-DFT excitation energies, for both valence and charge-transfer excitations. However, GDD tuning is more efficient and is well-behaved even for large systems. It provides a black-box solution to the optimal-tuning problem that can replace IE tuning for many applications of TD-DFT.
{"title":"Simplified Tuning of Long-Range Corrected Time-Dependent Density Functional Theory","authors":"Aniket Mandal, John M. Herbert","doi":"10.1021/acs.jpclett.5c00086","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00086","url":null,"abstract":"Range-separated hybrid functionals have dramatically improved the description of charge-transfer excitations in time-dependent density functional theory (TD-DFT), especially when the range-separation parameter is adjusted in order to satisfy the ionization energy (IE) criterion, ε<sub>HOMO</sub> = −IE. However, this “optimal tuning” procedure is molecule-specific, inconvenient, expensive for large systems, and problematic in extended or periodic systems. Here, we consider an alternative procedure known as global density-dependent (GDD) tuning, which sets the range-separation parameter in an automated way based on properties of the exchange hole. In small molecules, we find that long-range corrected functionals with either IE or GDD tuning afford remarkably similar TD-DFT excitation energies, for both valence and charge-transfer excitations. However, GDD tuning is more efficient and is well-behaved even for large systems. It provides a black-box solution to the optimal-tuning problem that can replace IE tuning for many applications of TD-DFT.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560902","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}
Plasmonic nanoparticles (NPs), characterized by significant localized surface plasmon excitations, can generate exceptionally large electromagnetic fields. In the plasmonic cavity, the enhancement of population and energy transfer across closely spaced metallic NPs significantly influence the optical response of the emitter. The theoretical investigation of transport properties in plasmonic nanocavities in atomic-scale level of calculation is important to characterize the optical response of the system. We model the coupling of plasmonic excitations of silver NPs in a bowtie configuration and generate new bright and dark states according to symmetry. By varying the separation distance, the rate of population and energy transfer between two NPs are analyzed within the framework of quantum dynamics multiconfiguration time-dependent Hartree (MCTDH) algorithm. The coupling of the emitter with bright and dark states of the plasmonic cavity is investigated based on the dipole–dipole approximation. The Hermitian Hamiltonian parametrized with first-principles calculations is applied to model the whole system. These results can reveal a connection between atomistic properties and optical response in the subnanometric-scale.
{"title":"Quantum Dynamics of Plasmonic Coupling in Silver Nanoparticle Dimers: Enhanced Energy and Population Transfer via Emitter Interaction","authors":"Fatemeh Khalili, Oriol Vendrell, Maryam Sadat Hosseini, Zahra Jamshidi","doi":"10.1021/acs.jpclett.4c03609","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03609","url":null,"abstract":"Plasmonic nanoparticles (NPs), characterized by significant localized surface plasmon excitations, can generate exceptionally large electromagnetic fields. In the plasmonic cavity, the enhancement of population and energy transfer across closely spaced metallic NPs significantly influence the optical response of the emitter. The theoretical investigation of transport properties in plasmonic nanocavities in atomic-scale level of calculation is important to characterize the optical response of the system. We model the coupling of plasmonic excitations of silver NPs in a bowtie configuration and generate new bright and dark states according to symmetry. By varying the separation distance, the rate of population and energy transfer between two NPs are analyzed within the framework of quantum dynamics multiconfiguration time-dependent Hartree (MCTDH) algorithm. The coupling of the emitter with bright and dark states of the plasmonic cavity is investigated based on the dipole–dipole approximation. The Hermitian Hamiltonian parametrized with first-principles calculations is applied to model the whole system. These results can reveal a connection between atomistic properties and optical response in the subnanometric-scale.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"47 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560901","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}
Pub Date : 2025-03-06DOI: 10.1021/acs.jpclett.5c00345
Zhihua Wu, Jian-Feng Li, Zhong-Qun Tian
Published as part of <i>The Journal of Physical Chemistry Letters</i> special issue “Celebrating 10 Years of the Collaborative Innovation Center of Chemistry for Energy Materials (iChEM)”. The Collaborative Innovation Center of Chemistry for Energy Materials (<i>i</i>ChEM) was approved in October 2014, jointly by Xiamen University (XMU), Fudan University (FDU), the University of Science and Technology of China (USTC), and the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS). The mission of the consortium is to integrate key innovative elements from universities, research institutes, and enterprises both in China and abroad. In addition, <i>i</i>ChEM leverages the strengths in chemistry and materials sciences of the four member-institutions to further advance cutting-edge energy-related research while also training younger generations for research excellence by strengthening collaboration between the research community and industry. Over the past decade, <i>i</i>ChEM has focused on common scientific issues in energy chemistry by jointly tackling energy chemistry and energy material systems and introducing a number of core key technologies. Researchers at <i>i</i>ChEM focus on three main areas: the optimal utilization of carbon resources, chemical energy storage and conversion, and solar energy conversion chemistry. Investigations in these energy-oriented areas use a number of approaches: basic research in synthesis and fabrication, theory and simulation, and instrumentation and methodology. As a result, we are able to make advances in the approaches themselves, as well as in the aforementioned three research areas. To realize the new energy strategic objectives, <i>i</i>ChEM has adhered to the principle of “chemistry as the foundation, materials as the carrier, and energy as the goal”, addressing critical scientific issues in the development of petroleum alternatives. This approach has led to a series of original results that are both urgently needed by the country and recognized as world-class. In order to celebrate the 10th anniversary of the <i>i</i>ChEM, The Journal of Physical Chemistry C (JPC C), The Journal of Physical Chemistry Letters (JPCL), and ACS Energy Letters are publishing a joint Special Issue (SI). This SI, organized by the center’s directors, Zhong-Qun Tian (Xiamen Univ.), Dongyuan Zhao (Fudan Univ.), Can Li (DICP, CAS), and Jinlong Yang (USTC), brings together 37 articles on energy materials and chemistry. It is with great pride and reflection that we look back on a decade of groundbreaking research, collaboration, and innovation. <i>i</i>ChEM has grown into a world-class hub for scientific exploration, fostering multidisciplinary partnerships and pioneering advancements in energy materials chemistry. Since its inception, <i>i</i>ChEM has been driven by a vision to address the critical challenges facing our world’s energy future. Our researchers, drawn from diverse backgrounds and expertise,
{"title":"Celebrating 10 Years of the Collaborative Innovation Center of Chemistry for Energy Materials (iChEM)","authors":"Zhihua Wu, Jian-Feng Li, Zhong-Qun Tian","doi":"10.1021/acs.jpclett.5c00345","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00345","url":null,"abstract":"Published as part of <i>The Journal of Physical Chemistry Letters</i> special issue “Celebrating 10 Years of the Collaborative Innovation Center of Chemistry for Energy Materials (iChEM)”. The Collaborative Innovation Center of Chemistry for Energy Materials (<i>i</i>ChEM) was approved in October 2014, jointly by Xiamen University (XMU), Fudan University (FDU), the University of Science and Technology of China (USTC), and the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS). The mission of the consortium is to integrate key innovative elements from universities, research institutes, and enterprises both in China and abroad. In addition, <i>i</i>ChEM leverages the strengths in chemistry and materials sciences of the four member-institutions to further advance cutting-edge energy-related research while also training younger generations for research excellence by strengthening collaboration between the research community and industry. Over the past decade, <i>i</i>ChEM has focused on common scientific issues in energy chemistry by jointly tackling energy chemistry and energy material systems and introducing a number of core key technologies. Researchers at <i>i</i>ChEM focus on three main areas: the optimal utilization of carbon resources, chemical energy storage and conversion, and solar energy conversion chemistry. Investigations in these energy-oriented areas use a number of approaches: basic research in synthesis and fabrication, theory and simulation, and instrumentation and methodology. As a result, we are able to make advances in the approaches themselves, as well as in the aforementioned three research areas. To realize the new energy strategic objectives, <i>i</i>ChEM has adhered to the principle of “chemistry as the foundation, materials as the carrier, and energy as the goal”, addressing critical scientific issues in the development of petroleum alternatives. This approach has led to a series of original results that are both urgently needed by the country and recognized as world-class. In order to celebrate the 10th anniversary of the <i>i</i>ChEM, The Journal of Physical Chemistry C (JPC C), The Journal of Physical Chemistry Letters (JPCL), and ACS Energy Letters are publishing a joint Special Issue (SI). This SI, organized by the center’s directors, Zhong-Qun Tian (Xiamen Univ.), Dongyuan Zhao (Fudan Univ.), Can Li (DICP, CAS), and Jinlong Yang (USTC), brings together 37 articles on energy materials and chemistry. It is with great pride and reflection that we look back on a decade of groundbreaking research, collaboration, and innovation. <i>i</i>ChEM has grown into a world-class hub for scientific exploration, fostering multidisciplinary partnerships and pioneering advancements in energy materials chemistry. Since its inception, <i>i</i>ChEM has been driven by a vision to address the critical challenges facing our world’s energy future. Our researchers, drawn from diverse backgrounds and expertise, ","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"67 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560906","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}
Pub Date : 2025-03-05DOI: 10.1021/acs.jpclett.5c00172
Miguel de la Puente, Axel Gomez, Damien Laage
Excess proton diffusion at aqueous interfaces is crucial for applications including electrocatalysis, aerosol chemistry, and biological energy conversion. While interfaces have been proposed as pathways for channeling protons, proton diffusion at interfaces remains far less understood than in the bulk. Here we focus on the air–water interface and use density functional theory-based deep potential molecular dynamics simulations to reveal the contrasting interface’s impacts: excess proton diffusion slows down compared to the bulk, while water diffusion accelerates. This contrast stems from reduced hydrogen-bond coordination at the interface, which facilitates water diffusion and transient unstable proton rattling but impedes the stable proton hops central to Grotthuss diffusion. As a result, at the interface, excess protons and water molecules diffuse at comparable rates, in stark departure from bulk behavior. This mechanistic insight delineates distinct limiting regimes for bulk-enhanced interfacial proton diffusion, with important implications for interfacial chemistry.
{"title":"Why Proton Grotthuss Diffusion Slows down at the Air–Water Interface while Water Diffusion Accelerates","authors":"Miguel de la Puente, Axel Gomez, Damien Laage","doi":"10.1021/acs.jpclett.5c00172","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00172","url":null,"abstract":"Excess proton diffusion at aqueous interfaces is crucial for applications including electrocatalysis, aerosol chemistry, and biological energy conversion. While interfaces have been proposed as pathways for channeling protons, proton diffusion at interfaces remains far less understood than in the bulk. Here we focus on the air–water interface and use density functional theory-based deep potential molecular dynamics simulations to reveal the contrasting interface’s impacts: excess proton diffusion slows down compared to the bulk, while water diffusion accelerates. This contrast stems from reduced hydrogen-bond coordination at the interface, which facilitates water diffusion and transient unstable proton rattling but impedes the stable proton hops central to Grotthuss diffusion. As a result, at the interface, excess protons and water molecules diffuse at comparable rates, in stark departure from bulk behavior. This mechanistic insight delineates distinct limiting regimes for bulk-enhanced interfacial proton diffusion, with important implications for interfacial chemistry.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"11 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546855","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}
Pub Date : 2025-03-04DOI: 10.1021/acs.jpclett.5c00219
Xiao-Hang He, Feng-Lei Jiang
Shell coating of quantum dots (QDs) is a widely implemented strategy to enhance the optical properties and stability. Typically, binary QDs, such as CdSe and CdS, are able to be precisely coated by several layers of shell material because their molar concentrations and radii could be empirically calculated from UV–vis absorption spectra. When it comes to ternary or alloyed QDs, such as CdSeS, there is not even one empirical formula to calculate them. Therefore, the method mentioned above is no longer available. However, complex alloyed QDs are prevalent in both research and industry since they exhibit more color gamut and tunability than binary QDs. Here, a “mass-method” was proposed to solve the problem of precise shell coating for complex alloyed QDs by mass and size (via TEM characterization). This method bypasses the necessity of the step of measuring the QD molar quantity before shell coating. After verification with CdSe and CdS QDs, this method was applicable with CdSeS alloyed QDs. The error of shell thickness coated onto the QD surface in this work was less than 0.1 monolayers. This work has filled the gap of precise shell coating for complex QDs, and it could be extended to any QD system.
{"title":"Universal “Mass-Method” for Precise Shell Coating of Quantum Dots by Mass and Size","authors":"Xiao-Hang He, Feng-Lei Jiang","doi":"10.1021/acs.jpclett.5c00219","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00219","url":null,"abstract":"Shell coating of quantum dots (QDs) is a widely implemented strategy to enhance the optical properties and stability. Typically, binary QDs, such as CdSe and CdS, are able to be precisely coated by several layers of shell material because their molar concentrations and radii could be empirically calculated from UV–vis absorption spectra. When it comes to ternary or alloyed QDs, such as CdSeS, there is not even one empirical formula to calculate them. Therefore, the method mentioned above is no longer available. However, complex alloyed QDs are prevalent in both research and industry since they exhibit more color gamut and tunability than binary QDs. Here, a “mass-method” was proposed to solve the problem of precise shell coating for complex alloyed QDs by mass and size (via TEM characterization). This method bypasses the necessity of the step of measuring the QD molar quantity before shell coating. After verification with CdSe and CdS QDs, this method was applicable with CdSeS alloyed QDs. The error of shell thickness coated onto the QD surface in this work was less than 0.1 monolayers. This work has filled the gap of precise shell coating for complex QDs, and it could be extended to any QD system.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"2 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546856","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}
Pub Date : 2025-03-04DOI: 10.1021/acs.jpclett.5c00376
Ning-Jing Hao, Rui Dai, Chuan-Jia Tong
Defect-assisted ion migration is one of the important issues that results in instability and non-radiative losses in hybrid organic–inorganic metal halide perovskite solar cells. In this work, based on the deep potential (DP) model, a long-time-scale molecular dynamics (MD) simulation has been employed to capture the interstitial-assisted iodine migration process. The results indicate that, when interstitial iodine (Ii) begins to migrate, the serious structural distortion becomes mild, weakening the electron–vibration interaction. The deep trap state induced by the iodine trimer undergoes a “deep–shallow–deep” dynamic process, which ultimately leads to an improvement of the carrier lifetime during the interstitial-assisted iodine migration process. Our work confirms that different dynamic processes are strongly correlated in halide perovskites and demonstrates that ion migration, considered to be detrimental, can become benign in a particular case. The reported results provide new fundamental insight to improve the efficiency of CH3NH3PbI3 perovskite solar cells.
{"title":"Machine-Learning-Assisted Investigation on Benign Ion Migration in Metal Halide Perovskites","authors":"Ning-Jing Hao, Rui Dai, Chuan-Jia Tong","doi":"10.1021/acs.jpclett.5c00376","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00376","url":null,"abstract":"Defect-assisted ion migration is one of the important issues that results in instability and non-radiative losses in hybrid organic–inorganic metal halide perovskite solar cells. In this work, based on the deep potential (DP) model, a long-time-scale molecular dynamics (MD) simulation has been employed to capture the interstitial-assisted iodine migration process. The results indicate that, when interstitial iodine (I<sub>i</sub>) begins to migrate, the serious structural distortion becomes mild, weakening the electron–vibration interaction. The deep trap state induced by the iodine trimer undergoes a “deep–shallow–deep” dynamic process, which ultimately leads to an improvement of the carrier lifetime during the interstitial-assisted iodine migration process. Our work confirms that different dynamic processes are strongly correlated in halide perovskites and demonstrates that ion migration, considered to be detrimental, can become benign in a particular case. The reported results provide new fundamental insight to improve the efficiency of CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub> perovskite solar cells.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"6 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539160","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}
Pub Date : 2025-03-04DOI: 10.1021/acs.jpclett.4c03568
Yong-Hyun Kim, Jungho Kim, Jung-Fu Lin, Sung Keun Lee
Electronic structures of iron in glasses are essential for unraveling the effect of transition metals on amorphous networks and controlling the electro-optical and transport properties of advanced glasses and amorphous energy-storing materials. The electronic configurations around iron in glasses, however, remain not well understood due to the structural disorders arising from multiple iron species with distinct valence, coordination, and spin states. Here, the first 1s3p resonant inelastic X-ray scattering (RIXS) for oxide glasses identifies hidden electronic configurations for Fe2+ and Fe3+ in amorphous networks. The results allow us to quantify the composition-induced evolution of oxygen ligand–field interactions of high-spin Fe 3d states with varying valence and coordination environments in complex glasses. The distinct electronic structures account for the electronic origins of iron-induced changes in the glass properties. The results offer prospects for a simultaneous probing of valence, coordination, and spin states of transition metals in diverse multicomponent oxide glasses and functional amorphous solids via 1s3p RIXS.
{"title":"Electronic Structures of Iron in Oxide Glasses via 1s3p Resonant Inelastic X-ray Scattering","authors":"Yong-Hyun Kim, Jungho Kim, Jung-Fu Lin, Sung Keun Lee","doi":"10.1021/acs.jpclett.4c03568","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03568","url":null,"abstract":"Electronic structures of iron in glasses are essential for unraveling the effect of transition metals on amorphous networks and controlling the electro-optical and transport properties of advanced glasses and amorphous energy-storing materials. The electronic configurations around iron in glasses, however, remain not well understood due to the structural disorders arising from multiple iron species with distinct valence, coordination, and spin states. Here, the first 1s3p resonant inelastic X-ray scattering (RIXS) for oxide glasses identifies hidden electronic configurations for Fe<sup>2+</sup> and Fe<sup>3+</sup> in amorphous networks. The results allow us to quantify the composition-induced evolution of oxygen ligand–field interactions of high-spin Fe 3d states with varying valence and coordination environments in complex glasses. The distinct electronic structures account for the electronic origins of iron-induced changes in the glass properties. The results offer prospects for a simultaneous probing of valence, coordination, and spin states of transition metals in diverse multicomponent oxide glasses and functional amorphous solids via 1s3p RIXS.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"1 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539234","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}
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