Chemical Physics Reviews最新文献

{"title":"Data-driven insights into the fluorescence of asphaltene aggregates using extended Frenkel exciton model","authors":"Fangning Ren, Fang Liu","doi":"10.1063/5.0175581","DOIUrl":"https://doi.org/10.1063/5.0175581","url":null,"abstract":"The origin of the fluorescence redshift during asphaltene aggregation remains debated due to the great diversity of asphaltene molecules, while the extended Frenkel exciton model provided a theoretical framework for studying multi-chromophore systems, such as asphaltene aggregates. We investigated the fluorescence energy of hundreds of asphaltene dimers based on 133 experimental revealed asphaltene monomer structures. Our result shows that the dimer's fluorescence energy is always lower than both of its monomers regardless of its intermolecular conformation, with its redshift dominated by superexchange. The dimer oscillator strength predominantly depends on the monomer with the lower fluorescence energy, and the involvement of charge-transfer states and the cancellation between monomer transition dipole moments suppressed the fluorescence especially when two monomers have similar fluorescence energy. The above-mentioned findings hold for all asphaltene dimers despite their diversity, which offers a theoretical interpretation for comprehending the relationship between asphaltene aggregation and its fluorescence variation. Furthermore, this work provides theoretical guidance to other research areas related to organic planar conjugated systems with multiple chromophores.","PeriodicalId":502275,"journal":{"name":"Chemical Physics Reviews","volume":"9 4","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139188738","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"The anisotropic nature of singlet fission in single crystalline organic semiconductors","authors":"Gang-Hua Deng, Jesse B. Brown, Haley Fisher, Zhi-Chao Huang-Fu, Yuqin Qian, Tong Zhang, A. Harutyunyan, Hanning Chen, Gugang Chen, Y. Rao","doi":"10.1063/5.0166062","DOIUrl":"https://doi.org/10.1063/5.0166062","url":null,"abstract":"The escalating global energy predicament implores for a revolutionary resolution—one that converts sunlight into electricity—holding the key to supreme conversion efficiency. This comprehensive review embarks on the exploration of the principle of generating multiple excitons per absorbed photon, a captivating concept that possesses the potential to redefine the fundamental confines of conversion efficiency, albeit its application remains limited in photovoltaic devices. At the nucleus of this phenomenon are two principal processes: multiple exciton generation (MEG) within quantum-confined environments, and singlet fission (SF) inside molecular crystals. The process of SF, characterized by the cleavage of a single photogenerated singlet exciton into two triplet excitons, holds promise to potentially amplify photon-to-electron conversion efficiency twofold, thereby laying the groundwork to challenge the detailed balance limit of solar cell efficiency. Our discourse primarily dissects the complex nature of SF in crystalline organic semiconductors, laying special emphasis on the anisotropic behavior of SF and the diffusion of the subsequent triplet excitons in single-crystalline polyacene organic semiconductors. We initiate this journey of discovery by elucidating the principles of MEG and SF, tracing their historical genesis, and scrutinizing the anisotropy of SF and the impact of quantum decoherence within the purview of functional mode electron transfer theory. We present an overview of prominent techniques deployed in investigating anisotropic SF in organic semiconductors, including femtosecond transient absorption microscopy and imaging as well as stimulated Raman scattering microscopies, and highlight recent breakthroughs linked with the anisotropic dimensions of Davydov splitting, Herzberg–Teller effects, SF, and triplet transport operations in single-crystalline polyacenes. Through this comprehensive analysis, our objective is to interweave the fundamental principles of anisotropic SF and triplet transport with the current frontiers of scientific discovery, providing inspiration and facilitating future ventures to harness the anisotropic attributes of organic semiconductor crystals in the design of pioneering photovoltaic and photonic devices.","PeriodicalId":502275,"journal":{"name":"Chemical Physics Reviews","volume":"37 9","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139188427","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Rapid synthesis of nanomaterials by solvent-free laser irradiation for energy storage and conversion","authors":"Winda Devina, Iyan Subiyanto, D. T. Dung, Seong Ok Han, Hyung Chul Yoon, Do Van Lam, Seung-Mo Lee, Hyunuk Kim","doi":"10.1063/5.0150598","DOIUrl":"https://doi.org/10.1063/5.0150598","url":null,"abstract":"Nanomaterials synthesized through laser irradiation have numerous applications in the field of energy storage and conversion. Conventional methods for fabricating nanomaterials often involve extended reaction times, making them susceptible to issues such as reproducibility, impurities, and inhomogeneity. To address these issues, a novel strategy of synthesizing nanomaterials via solvent-free laser irradiation in the gas phase is proposed as a potential solution. This innovative strategy offers ultrafast heating and cooling processes compared to conventional time-consuming methods, resulting in the formation of homogeneous nanosystems within femto- to nanosecond timeframes. The focused laser beam induces rapid photothermal and photochemical effects in either air or an inert gas atmosphere, enabling the rapid production of nanomaterials with precise control over geometry, chemistry, crystallinity, and defect density by adjusting processing conditions and sintering mediums. This review provides insights into the rapid solvent-free laser-assisted synthesis of nanomaterials using natural carbon-based materials, polymers, metal–organic frameworks, and inorganic species in both air and inert atmospheres. The introduction of photo-irradiation across a wide range of precursors facilitates phase transitions and surface functionalization in the resulting nanoproducts. We also discuss the effects of altering laser wavelengths, pulse widths, fluences, and repetition rates on both surface and bulk properties of the final products. Finally, we explore the applications of laser-induced nanomaterials in areas such as rechargeable batteries, supercapacitors, solar cells, and catalysis.","PeriodicalId":502275,"journal":{"name":"Chemical Physics Reviews","volume":"41 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139217205","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Advances in polymerized small-molecule acceptors for improved performance in all-polymer solar cells","authors":"Wissem Khelifi, C. Luscombe","doi":"10.1063/5.0169728","DOIUrl":"https://doi.org/10.1063/5.0169728","url":null,"abstract":"This mini-review discusses the progress made in the development of polymerized small-molecule acceptors (PSMAs) for use in all-polymer solar cells (all-PSCs). These PSMAs combine the advantages of both small-molecule acceptors (SMAs) and polymers. Various studies have been conducted using different building blocks to synthesize these acceptors, including indacenodithiophene and indacenodithienothiophene. They exhibit many advantages such as strong absorption in the near infrared region, high electron mobility, and appropriate energy levels, making them good candidate for PSAMs. The improved efficiency of all-PSCs is attributed to several factors, including stronger absorption, improved blend morphology, and redistribution of composition in the film. Additionally, new materials have been incorporated as third components in ternary organic photovoltaics, with some achieving high power conversion efficiencies of up to 17.0%. The development of new acceptors with different building blocks has resulted in improved stability and reproducibility in all-PSCs, paving the way toward high-performance and stable devices. Overall, these developments demonstrate significant potential for further advancements in the field.","PeriodicalId":502275,"journal":{"name":"Chemical Physics Reviews","volume":"51 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139248468","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Large-area single-crystal hexagonal boron nitride: From growth mechanism to potential applications","authors":"Joo Song Lee, Nilanjan Basu, Hyeon Suk Shin","doi":"10.1063/5.0165422","DOIUrl":"https://doi.org/10.1063/5.0165422","url":null,"abstract":"To date, chemical vapor deposition has been employed to grow large-area polycrystalline (PC) films of hexagonal boron nitride (hBN). However, PC hBN thin films exhibit abundant grain boundaries, small grain sizes, and structural imperfections, which collectively degrade the performance as well as hinder the scalability and potential applications of hBN films. Recently, demonstrated deposition methods for growing large-area single-crystalline (SC) hBN films can break through these bottlenecks and have opened avenues for new opportunities. Large-area SC hBN films outperform their PC counterparts owing to the presence of fewer grain boundaries and a more homogeneous surface morphology. This review article presents a consolidated overview of the growth mechanisms of SC hBN films and role of metal catalysts (substrates) in the growth process. Applications, in which SC hBN outperforms PC hBN as well as the potential applications of SC hBN, are also discussed.","PeriodicalId":502275,"journal":{"name":"Chemical Physics Reviews","volume":"33 1-2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139273873","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}