Pub Date : 2023-12-04DOI: 10.1088/2515-7639/ad0f2f
Ruiqi Wu, Alex M Ganose
Antiperovskites are a rich family of compounds with applications in battery cathodes, superconductors, solid-state lighting, and catalysis. Recently, a novel series of antimonide phosphide antiperovskites (A3SbP, where A = Ca, Sr Ba) were proposed as candidate photovoltaic absorbers due to their ideal band gaps, small effective masses and strong optical absorption. In this work, we explore this series of compounds in more detail using relativistic hybrid density functional theory. We reveal that the proposed cubic structures are dynamically unstable and instead identify a tilted orthorhombic Pnma phase as the ground state. Tilting is shown to induce charge localisation that widens the band gap and increases the effective masses. Despite this, we demonstrate that the predicted maximum photovoltaic efficiencies remain high (24%–31% for 200 nm thin films) by bringing the band gaps into the ideal range for a solar absorber. Finally, we assess the band alignment of the series and suggest hole and electron contact materials for efficient photovoltaic devices.
反掺杂磷酸盐是一个丰富的化合物家族，可应用于电池阴极、超导体、固态照明和催化等领域。最近，人们提出了一系列新型磷化锑系反穿晶石（A3SbP，其中 A = Ca、Sr Ba），由于它们具有理想的带隙、较小的有效质量和较强的光吸收能力，因此被认为是候选的光伏吸收体。在这项研究中，我们利用相对论混合密度泛函理论对这一系列化合物进行了更详细的探讨。我们发现所提出的立方结构在动力学上是不稳定的，并确定了倾斜正方 Pnma 相作为基态。研究表明，倾斜会引起电荷局域化，从而扩大带隙并增加有效质量。尽管如此，我们仍然证明，通过将带隙引入太阳能吸收器的理想范围，预测的最大光电效率仍然很高（200 nm 薄膜的光电效率为 24%-31%）。最后，我们评估了该系列的能带排列，并为高效光伏设备的空穴和电子接触材料提出了建议。
{"title":"Tilt-induced charge localisation in phosphide antiperovskite photovoltaics","authors":"Ruiqi Wu, Alex M Ganose","doi":"10.1088/2515-7639/ad0f2f","DOIUrl":"https://doi.org/10.1088/2515-7639/ad0f2f","url":null,"abstract":"Antiperovskites are a rich family of compounds with applications in battery cathodes, superconductors, solid-state lighting, and catalysis. Recently, a novel series of antimonide phosphide antiperovskites (<italic toggle=\"yes\">A</italic>\u0000<sub>3</sub>SbP, where <italic toggle=\"yes\">A</italic> = Ca, Sr Ba) were proposed as candidate photovoltaic absorbers due to their ideal band gaps, small effective masses and strong optical absorption. In this work, we explore this series of compounds in more detail using relativistic hybrid density functional theory. We reveal that the proposed cubic structures are dynamically unstable and instead identify a tilted orthorhombic <italic toggle=\"yes\">Pnma</italic> phase as the ground state. Tilting is shown to induce charge localisation that widens the band gap and increases the effective masses. Despite this, we demonstrate that the predicted maximum photovoltaic efficiencies remain high (24%–31% for 200 nm thin films) by bringing the band gaps into the ideal range for a solar absorber. Finally, we assess the band alignment of the series and suggest hole and electron contact materials for efficient photovoltaic devices.","PeriodicalId":501825,"journal":{"name":"Journal of Physics: Materials","volume":"17 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138693333","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}
Pub Date : 2023-11-30DOI: 10.1088/2515-7639/ad0f31
Nolan Lassaline
Scanning probe microscopy (SPM) uses a sharp tip to interrogate surfaces with atomic precision. Inputs such as mechanical, electrical, or thermal energy can activate highly localized interactions, providing a powerful class of instruments for manipulating materials on small length scales. Thermal scanning-probe lithography (tSPL) is an advanced SPM variant that uses a silicon tip on a heated cantilever to locally sublimate polymer resist, acting as a high-resolution lithography tool and a scanning probe microscope simultaneously. The main advantage of tSPL is the ability to electrically control the temperature and applied force of the tip, which can produce smooth topographical surfaces that are unattainable with conventional nanofabrication techniques. Recent investigations have exploited these surfaces to generate potential landscapes for enhanced control of photons, electrons, excitons, and nanoparticles, demonstrating a broad range of experimental possibilities. This paper outlines the principles, procedures, and limitations of tSPL for generating smooth potentials and discusses the prospective impact in photonics, electronics, and nanomaterials science.
{"title":"Generating smooth potential landscapes with thermal scanning-probe lithography","authors":"Nolan Lassaline","doi":"10.1088/2515-7639/ad0f31","DOIUrl":"https://doi.org/10.1088/2515-7639/ad0f31","url":null,"abstract":"Scanning probe microscopy (SPM) uses a sharp tip to interrogate surfaces with atomic precision. Inputs such as mechanical, electrical, or thermal energy can activate highly localized interactions, providing a powerful class of instruments for manipulating materials on small length scales. Thermal scanning-probe lithography (tSPL) is an advanced SPM variant that uses a silicon tip on a heated cantilever to locally sublimate polymer resist, acting as a high-resolution lithography tool and a scanning probe microscope simultaneously. The main advantage of tSPL is the ability to electrically control the temperature and applied force of the tip, which can produce smooth topographical surfaces that are unattainable with conventional nanofabrication techniques. Recent investigations have exploited these surfaces to generate potential landscapes for enhanced control of photons, electrons, excitons, and nanoparticles, demonstrating a broad range of experimental possibilities. This paper outlines the principles, procedures, and limitations of tSPL for generating smooth potentials and discusses the prospective impact in photonics, electronics, and nanomaterials science.","PeriodicalId":501825,"journal":{"name":"Journal of Physics: Materials","volume":"2 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138693334","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}
Pub Date : 2023-11-23DOI: 10.1088/2515-7639/ad0d7c
Nattaphon Hongrutai, Saurav Ch Sarma, Yuxiang Zhou, Simon Kellner, Angus Pedersen, Kari Adourian, Helen Tyrrell, Mary P Ryan, Joongjai Panpranot, Jesús Barrio
Tandem CO2 reduction electrocatalysts that combine a material that selectively produces CO with Cu are capable of producing hydrocarbons at low overpotentials and high selectivity. However, controlling the spatial distribution and the catalytic activity of the CO-making catalyst remains a challenge. In this work, a novel tandem electrocatalyst that overcomes limitations of simple Cu catalysts, namely selectivity and efficiency at low overpotential, is presented. The tandem electrocatalysts are prepared through a sequential spray coating protocol, using a single atom Fe in N-doped C (FeNC) as the selective CO-producing catalyst and commercial Cu nanopowder. The high faradaic efficiency towards CO of FeNC (99% observed at −0.60 V vs. RHE) provides a high CO coverage to the Cu particles, leading to reduced hydrogen evolution and the selective formation of ethanol and n-propanol at a much low overpotential than that of bare Cu.
串联二氧化碳还原电催化剂结合了选择性产生二氧化碳的材料和铜，能够在低过电位和高选择性条件下产生碳氢化合物。然而，控制 CO 生成催化剂的空间分布和催化活性仍是一项挑战。本研究提出了一种新型串联电催化剂，它克服了简单铜催化剂的局限性，即在低过电位下的选择性和效率。串联电催化剂是通过顺序喷涂协议制备的，使用掺杂 N 的 C 中的单原子铁（FeNC）作为选择性 CO 生成催化剂，并使用商用纳米铜粉。FeNC 对 CO 的高远电效率（在 -0.60 V 对 RHE 时观察到 99%）为 Cu 颗粒提供了高 CO 覆盖率，从而减少了氢气进化，并以比裸 Cu 低得多的过电位选择性地生成乙醇和正丙醇。
{"title":"Sequential deposition of FeNC–Cu tandem CO2 reduction electrocatalysts towards the low overpotential production of C2+ alcohols","authors":"Nattaphon Hongrutai, Saurav Ch Sarma, Yuxiang Zhou, Simon Kellner, Angus Pedersen, Kari Adourian, Helen Tyrrell, Mary P Ryan, Joongjai Panpranot, Jesús Barrio","doi":"10.1088/2515-7639/ad0d7c","DOIUrl":"https://doi.org/10.1088/2515-7639/ad0d7c","url":null,"abstract":"Tandem CO<sub>2</sub> reduction electrocatalysts that combine a material that selectively produces CO with Cu are capable of producing hydrocarbons at low overpotentials and high selectivity. However, controlling the spatial distribution and the catalytic activity of the CO-making catalyst remains a challenge. In this work, a novel tandem electrocatalyst that overcomes limitations of simple Cu catalysts, namely selectivity and efficiency at low overpotential, is presented. The tandem electrocatalysts are prepared through a sequential spray coating protocol, using a single atom Fe in N-doped C (FeNC) as the selective CO-producing catalyst and commercial Cu nanopowder. The high faradaic efficiency towards CO of FeNC (99% observed at −0.60 V vs. RHE) provides a high CO coverage to the Cu particles, leading to reduced hydrogen evolution and the selective formation of ethanol and <italic toggle=\"yes\">n</italic>-propanol at a much low overpotential than that of bare Cu.","PeriodicalId":501825,"journal":{"name":"Journal of Physics: Materials","volume":"42 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138693337","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}
Pub Date : 2023-11-16DOI: 10.1088/2515-7639/ad08d1
Stijn H M van Leuken, Rolf A T M van Benthem, Remco Tuinier, Mark Vis
Polydispersity affects physical properties of polymeric materials, such as solubility in solvents. Most biobased, synthetic, recycled, mixed, copolymerized, and self-assembled polymers vary in size and chemical structure. Using solvent fractionation, this variety in molecular features can be reduced and a selection of the sizes and molecular features of the polymers can be made. The significant chemical and physical dispersity of these polymers, however, complicates theoretical solubility predictions. A theoretical description of the fractionation process can guide experiments and material design. During solvent fractioning of polymers, a part of the polydisperse distribution of the polymers dissolves. To describe this process, this paper presents a theoretical tool using Flory–Huggins theory combined with molecular mass distributions and distributions in the number of functional groups. This paper quantifies how chemical and physical polydispersity of polymers affects their solubility. Comparison of theoretical predictions with experimental measurements of lignin in a mixture of solvents shows that multiple molecular features can be described well using a single set of parameters, giving a tool to theoretically predict the selective solubility of polymers.
{"title":"Theoretically predicting the solubility of polydisperse polymers using Flory–Huggins theory","authors":"Stijn H M van Leuken, Rolf A T M van Benthem, Remco Tuinier, Mark Vis","doi":"10.1088/2515-7639/ad08d1","DOIUrl":"https://doi.org/10.1088/2515-7639/ad08d1","url":null,"abstract":"Polydispersity affects physical properties of polymeric materials, such as solubility in solvents. Most biobased, synthetic, recycled, mixed, copolymerized, and self-assembled polymers vary in size and chemical structure. Using solvent fractionation, this variety in molecular features can be reduced and a selection of the sizes and molecular features of the polymers can be made. The significant chemical and physical dispersity of these polymers, however, complicates theoretical solubility predictions. A theoretical description of the fractionation process can guide experiments and material design. During solvent fractioning of polymers, a part of the polydisperse distribution of the polymers dissolves. To describe this process, this paper presents a theoretical tool using Flory–Huggins theory combined with molecular mass distributions and distributions in the number of functional groups. This paper quantifies how chemical and physical polydispersity of polymers affects their solubility. Comparison of theoretical predictions with experimental measurements of lignin in a mixture of solvents shows that multiple molecular features can be described well using a single set of parameters, giving a tool to theoretically predict the selective solubility of polymers.","PeriodicalId":501825,"journal":{"name":"Journal of Physics: Materials","volume":"106 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138693336","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：