Crystal Growth & Design最新文献

{"title":"Comparative Studies of Synthesis, Performance, and Applications of Recently Developed CL-20 Based Co-crystals","authors":"Qamar-un-Nisa Tariq,&nbsp;Maher-un-Nisa Tariq,&nbsp;Wen-Shuai Dong,&nbsp;Saira Manzoor,&nbsp;Faiza Arshad and Jian-Guo Zhang*,&nbsp;","doi":"10.1021/acs.cgd.3c00340","DOIUrl":"https://doi.org/10.1021/acs.cgd.3c00340","url":null,"abstract":"<p >Owing to promising characteristics including a high heat of formation (100 kcal·mol^–1), high density (2.04 g·cm^–3), and powerful explosive nature (14–20% more potent than 1,3,5,7-tetranitro-1,3,5,7-tetrazocane (HMX)), the hollow cage-type molecular structure of polycyclic nitramine 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (HNIW/CL-20) has recently attained significant attention from scientists. Its high sensitivity toward mechanical stimuli raises safety concerns. The safety–power contradiction of high-energy explosives can be alleviated to a certain extent via a co-crystallization method. It is possible to modify the properties of energetic materials such as melting and decomposition point, density, detonation properties (detonation velocity and detonation pressure), and mechanical sensitivities (friction and impact) by forming a new chemical composition from the new/existing molecules through noncovalent interactions (π–π stacking, hydrogen bonds, and van der Waals forces). Energetic co-crystals have been developed by various approaches such as solvent evaporation, solvent/nonsolvent, grinding, slurry, resonant acoustic mixing, etc. This Review highlights an interesting overview of HNIW/CL-20 based energetic co-crystals, including their synthetic methods, intermolecular interactions, and physicochemical and energetic properties. Moreover, their applications, existing problems, and challenges for future work on CL-20-based co-crystals are also discussed.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":"23 9","pages":"6974–6987"},"PeriodicalIF":3.8,"publicationDate":"2023-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"183997","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}

{"title":"First Finding of High-Pressure Modifications of Na2CO3 and K2CO3 with sp3-Hybridized Carbon Atoms","authors":"Pavel N. Gavryushkin*,&nbsp;Nursultan E. Sagatov,&nbsp;Dinara N. Sagatova,&nbsp;Altyna Bekhtenova,&nbsp;Maksim V. Banaev,&nbsp;Eugeny V. Alexandrov and Konstantin D. Litasov,&nbsp;","doi":"10.1021/acs.cgd.3c00507","DOIUrl":"https://doi.org/10.1021/acs.cgd.3c00507","url":null,"abstract":"<p >The transition from structures with classical [CO₃] triangles to structures with [CO₄] tetrahedra, corresponding to the transition from sp² to sp³ hybridization of carbon atoms, is quite well established for alkaline earth carbonates CaCO₃ and MgCO₃. Here, using a crystal structure prediction technique, we show that alkali carbonates Na₂CO₃ and K₂CO₃ follow the same trend. Both compounds form isostructural sp³-hybridized phases, Na₂CO₃–<i>C</i>2/<i>m</i> and K₂CO₃–<i>C</i>2/<i>m</i>, which became thermodynamically stable at pressures above 125 and 150 GPa, respectively. The automated topological search through ICSD has shown that the found <i>C</i>2/<i>m</i> structures, as well as sp³-structures of CaCO₃ and MgCO₃ do not have topological analogs among silicates and phosphates. Transitions of Na₂CO₃ and K₂CO₃ to <i>C</i>2/<i>m</i> structures are realized without sufficient perturbation of the initial Na₂CO₃–<i>P</i>2₁/<i>m</i> and K₂CO₃–<i>P</i>1̅ structures and require relatively small atomic displacements of carbon and oxygen atoms. These transitions are realized through simple energy optimization. This indicates the absence or low height of the energy barrier. In the wide interval of pressures before the transition to the sp³ structures, carbon atoms of [CO₃] triangles are gradually displaced from the plane defined by three oxygen atoms due to the interaction with the fourth oxygen atom. In the case of Na₂CO₃, the dihedral angle C–O–O–O describing the degree of this displacement increases from 5 to 12°, when the pressure increases from 60 to 127 GPa. At pressures above 130 GPa, the angle abruptly increases to the value of 31°, which corresponds to the formation of the sp³-hybridized phase Na₂CO₃–<i>C</i>2/<i>m</i>. Based on the examples of alkali and alkaline earth carbonates, we show that the transition from a sp²-hybridized [CO₃] triangle to a sp³-hybridized [CO₄] tetrahedron is realized when the fourth oxygen atom approaches the carbon atom at a distance less than 2.0 Å, which is usually realized at pressures of around 100 GPa. The stable structures with sp³-hybridized carbon atoms have not been found for Li₂CO₃ in the considered pressure range up to 200 GPa, and we show that the <i>P</i>6₃/<i>mcm</i> structure of this compound is stable in sp² form up to a pressure of 700 GPa or even higher. This indicates that not all the structures of carbonates adopt sp³ form even at extreme pressures.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":"23 9","pages":"6589–6596"},"PeriodicalIF":3.8,"publicationDate":"2023-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"183304","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}

{"title":"Modulating Organic/Inorganic Segregation in Columnar Mesophases","authors":"Estela de Domingo,&nbsp;Gregorio García,&nbsp;César L. Folcia,&nbsp;Josu Ortega,&nbsp;Jesús Etxebarria and Silverio Coco*,&nbsp;","doi":"10.1021/acs.cgd.3c00660","DOIUrl":"https://doi.org/10.1021/acs.cgd.3c00660","url":null,"abstract":"<p >This work reports an uncommon modulation of columnar segregation of metal–organic triphenylene liquid crystals by blending two structurally dissimilar metallomesogens that can self-associate through complementary electron donor–acceptor interactions. The constituent molecules are <i>cis</i>-[PtCl₂(CNR)₂] (CNR = 2-(6-(4-isocyanophenoxy)hexyloxy)-3,6,7,10,11-pentakisdodecyloxytriphenylene) that displays an organic/inorganic segregated columnar mesophase and [PtCl₂(Bipy)] (Bipy = didodecyl 2,2′-bipyridyl-4,4′-dicarboxylate) that shows a lamellar mesomorphism. The phase diagram of this system was constructed using polarized optical microscopy (POM), differential scanning calorimetry (DSC), and X-ray scattering data. The phase diagram corresponds to a typical binary system with an intermediate compound (in this case a supramolecular aggregate) of stoichiometry [PtCl₂(CNR)₂]/2[PtCl₂(Bipy)], which is maintained in solution. This species shows an unusual columnar mesophase formed by the stacking of alternating organic/inorganic fragments. Quantum chemical calculations show that the columnar structure is mainly supported by complementary π electron donor–acceptor interactions between each triphenylene group of the isocyanide complex and a platinum-bipyridine molecule. This induces the elimination of the organic/inorganic columnar segregation of the isocyano parent component and constitutes an unconventional example of modulation of organic/inorganic segregation in columnar mesophases by the intercalation of metal complexes into hexaalkoxytriphenylene stacks.</p><p >Modulation of columnar segregation in metal−organic triphenylene liquid crystals is accomplished by blending two structurally dissimilar metallomesogens able to self-associate through complementary electron donor−acceptor interactions.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":"23 9","pages":"6812–6821"},"PeriodicalIF":3.8,"publicationDate":"2023-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.cgd.3c00660","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"181275","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}

{"title":"Amorphous Solid Forms of Ranolazine and Tryptophan and Their Relaxation to Metastable Polymorphs","authors":"Joana F. C. Silva,&nbsp;Pedro S. Pereira Silva,&nbsp;Manuela Ramos Silva,&nbsp;Elvira Fantechi,&nbsp;Laura Chelazzi,&nbsp;Samuele Ciattini,&nbsp;M. Ermelinda S. Eusébio* and Mário T. S. Rosado*,&nbsp;","doi":"10.1021/acs.cgd.3c00565","DOIUrl":"https://doi.org/10.1021/acs.cgd.3c00565","url":null,"abstract":"<p >Different methods were explored for the amorphization of ranolazine, a sparingly soluble anti-anginal drug, such as mechanochemistry, quench-cooling, and solvent evaporation from solutions. Amorphous phases, with <i>T</i>_g values lower than room temperature, were obtained by cryo-milling and quench-cooling. New forms of ranolazine, named II and III, were identified from the relaxation of the ranolazine amorphous phase produced by cryo-milling, which takes place within several hours after grinding. At room temperature, these metastable polymorphs relax to the lower energy polymorph I, whose crystal structure was solved in this work for the first time. A binary co-amorphous mixture of ranolazine and tryptophan was produced, with three important advantages: higher glass transition temperature, increased kinetic stability preventing relaxation of the amorphous to crystalline phases for at least two months, and improved aqueous solubility. Concomitantly, the thermal behavior of amorphous tryptophan obtained by cryo-milling was studied by DSC. Depending on experimental conditions, it was possible to observe relaxation directly to the lower energy form or by an intermediate metastable crystalline phase and the serendipitous production of the neutral form of this amino acid in the pure solid phase.</p><p >Amorphous phases of ranolazine, tryptophan, and co-amorphous mixtures were produced and their stepwise relaxations toward low-energy crystals were investigated. Unprecedently, three polymorphs of ranolazine were discovered and the crystal structure of the most stable solved. Amorphous tryptophan relaxation led to the serendipitous appearance of its neutral form. A co-amorphous mixture showed enhanced thermal and kinetical stability and improved ranolazine aqueous solubility.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":"23 9","pages":"6679–6691"},"PeriodicalIF":3.8,"publicationDate":"2023-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.cgd.3c00565","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"180493","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}

{"title":"Electrochemistry-Induced Direct Deposition of Nanoscale Thin Zeolitic Imidazolate Framework-8 Films on Insulator Substrates","authors":"Takashi Ito*,&nbsp;Samantha G. Jenkins,&nbsp;Soenke Seifert and Ahmet Uysal,&nbsp;","doi":"10.1021/acs.cgd.3c00329","DOIUrl":"https://doi.org/10.1021/acs.cgd.3c00329","url":null,"abstract":"<p >Electrochemical approaches have been explored as controlled means to prepare thin films of metal–organic frameworks (MOFs) on electrodes but have rarely been used to form insulator films on insulator surfaces. Herein, we report an electrochemistry-based approach to direct deposition of a thin film of zeolitic imidazolate framework-8 (ZIF-8) onto an insulator surface. The film deposition was induced by a cathodic reaction at an electrode that was placed above the insulator with a separation of ≈100 μm in a methanol solution containing ZnCl₂ and 2-methylimidizole. The effects of the electrode and insulator material, applied potential, electrode–substrate distance, deposition time, and the number of deposition cycles were systematically investigated to gain insight into the deposition mechanism. The results of these measurements were consistent with a hypothesized mechanism involving cathodic base generation at the working electrode for ligand deprotonation, formation of intermediate species, their diffusion toward the substrate, and the formation of ZIF-8 on the substrate. Interestingly, the size, shape, and position of the film on the substrate replicated those of the working electrode, showing the applicability of this approach to the patterned deposition of a ZIF-8 film. In addition, film thickness could be easily controlled in the range of tens to hundreds of nanometers by adjusting the potential application conditions. This electrochemistry-induced method will provide a simple means for the patterned formation of a MOF film of controlled thickness on an insulator without metal precoating and thus will open the possibility of designing unique devices for various applications including chemical sensing and separations.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":"23 9","pages":"6369–6377"},"PeriodicalIF":3.8,"publicationDate":"2023-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"180340","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}

{"title":"Cocrystal or Salt Crystallization for Active Pharmaceutical Ingredients By Using Deep Eutectic Solvents","authors":"Masataka Ito*,&nbsp;Yuriko Iwata,&nbsp;Hiroyasu Iwasaki,&nbsp;Kyu Hayashi,&nbsp;Taku Nakayama,&nbsp;Hidemasa Hikawa,&nbsp;Isao Azumaya,&nbsp;Hironori Suzuki and Shuji Noguchi,&nbsp;","doi":"10.1021/acs.cgd.3c00155","DOIUrl":"https://doi.org/10.1021/acs.cgd.3c00155","url":null,"abstract":"<p >Active pharmaceutical ingredients (APIs) often exhibit physicochemical problems that one can remedy by various methods (e.g., salt formation, grinding, ordered mixtures, and cocrystal or amorphous formation). Crystallizing salts or cocrystals from solutions of an API and a coformer is widely used today. In recent years, green chemistry and sustainable development goals have been an active area of research, and a production method is required for reducing the use of organic solvents and implementing a low environmental load. In this study, deep eutectic solvents (DESs) were used as the mother liquids for crystallization and environmentally friendly solvents. The DESs were made by combining three types of choline salts and a coformer compound of malonic acid. Nine model APIs were then dissolved in each DES and crystals precipitated from the DESs. As a result, five kinds of cocrystals or salts precipitated in 10 conditions, two of which were identified for the first time in this study. Crystallization by using DESs is a potent alternative for discovering novel cocrystals or salts with low environmental impact.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":"23 9","pages":"6298–6307"},"PeriodicalIF":3.8,"publicationDate":"2023-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"180664","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}

{"title":"Postdecorated Polyoxometalate Metal–Organic Framework-Constructed Ternary Electrocatalysts for Hydrogen Evolution","authors":"Jiao Li,&nbsp;Rui Wang,&nbsp;Zongyan Dong,&nbsp;Xuejian Zhang,&nbsp;Xiao Li,&nbsp;Yongtao Li and Zhongmin Su,&nbsp;","doi":"10.1021/acs.cgd.3c00391","DOIUrl":"https://doi.org/10.1021/acs.cgd.3c00391","url":null,"abstract":"<p >Metal–organic frameworks (MOFs) are widely used as precursor materials for electrocatalysts in the hydrogen evolution reaction (HER) because of the various and adjustable metal sites with long-ranged order and porous structures. In this paper, polyoxometalate-based MOF (POMOF) ([Ni(H₂O)₂(bth)(Mo₈O₂₆)_0.5·3H₂O], JLJZ-1) was synthesized by ammonium molybdate hydrate, Ni²⁺, and a flexible chain ligand (bth, 1,6-bis(1,2,4-triazol-1-yl)hexane) via a hydrothermal method. Then, JLJZ-1 decorated with polyvinylpyrrolidone (PVP), phytic acid (PA) as the composite precursor, and carbon-coated ternary hydrogen evolution electrocatalyst (Mo₂C/MoP/MoNiP@C) was prepared via one-step calcination. In acidic medium, Mo₂C/MoP/MoNiP@C exhibits good catalytic activity with an overpotential of 154 mV at the current density of 10 mA cm^–2, and it shows good stability within 14 h. After characterization and tests, the satisfactory HER performance is mainly attributed to the synergistic effects among multiple components. Furthermore, the mesoporous structures help to expose more active sites, and the graphitic carbon layers protect the catalyst nanoparticles from corrosion. This work provides a guiding strategy of postdecorated POMOF-based composites as precursors for multicomponent electrocatalysts used in energy conversion fields.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":"23 9","pages":"6403–6409"},"PeriodicalIF":3.8,"publicationDate":"2023-08-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"177861","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}

{"title":"Optimal Control and Communication Strategies in Multi-Energy Generation Grid","authors":"Muhammad Waseem Khan;Guojie Li;Keyou Wang;Muhammad Numan;Linyun Xiong;Muhammad Azam Khan","doi":"10.1109/COMST.2023.3304982","DOIUrl":"10.1109/COMST.2023.3304982","url":null,"abstract":"Multi-energy generation grids (MEGGs) provide a promising solution for reliable operations of cooperative various distributed energy resources (DERs), supply environmentally friendly energy to remote/off-grid areas, and improve overall system performance in terms of efficiency, reliability, flexibility, and resiliency. However, with the penetration of grids and the presence of various DERs with unpredictable renewables-based power generation and intermittent power loads, the operational coordination and supervision tasks become more complex. The communication-based optimal distributed control approach plays a significant role in MEGGs for coordinating an assembly of spatially and heterogeneous DERs, which improves reliability, efficiency, scalability, robustness, and privacy-preserving compared with traditional centralized-based controls. Therefore, this article aims to study different grid architectures and provide a comprehensive survey of optimal control and communication strategies/systems (CCS) in MEGG. A well-organized and systematic discussion related to the topic has been provided and elaborated on: 1) energy production and distribution with various grid architectures and distributed generating units (DGUs) integration for sustainable power generation, importance of unit sizing and technologies selection, and their implementations and operations; 2) classification on numerous control architectures and techniques, their prominent features and impact on MEGG stability; 3) multiple advanced intelligent control strategies and their essential aspects and merits; 4) different promising communication networks and technologies with optimal communication protocols and standards along with their computational mechanism and potential operational objectives in MEGGs; 5) communication strategies features and reliability issues concerning data volume, data availability, data accuracy, data security and authentication, time synchronization, and the growth of countermeasures; and 6) finally, key research gaps are highlighted and some recommendations are provided for future research works to efficiently handle the MEGG control, security, and communication network requirements.","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":"25 4","pages":"2599-2653"},"PeriodicalIF":35.6,"publicationDate":"2023-08-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"125556838","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}

{"title":"Experimental and Computational Study of Solid Solutions Formed between Substituted Nitrobenzoic Acids","authors":"Kristaps Saršu̅ns,&nbsp;Artis Kons,&nbsp;Toms Rekis and Agris Be̅rziņš*,&nbsp;","doi":"10.1021/acs.cgd.3c00529","DOIUrl":"https://doi.org/10.1021/acs.cgd.3c00529","url":null,"abstract":"<p >We present an experimental and computational study of the formation of solid solutions in binary systems of substituted nitrobenzoic acids. Different isomers with a methyl group, hydroxyl group, and chlorine substituents are studied. We show that the solid solution formation likelihood evaluated based on the observed solubility limit is notably affected by both the exchanged functional groups and the location of the substituents in the molecular structure. This demonstrates that the component solubility limit strongly depends on the intermolecular interactions present in the crystal structure and is altered by the molecule replacement. Solid solutions form in all of the studied crystalline phases. Component solubility limits from ∼5% up to 50% were observed. The obtained results indicated that the calculated intermolecular interaction energy change by the functional group replacement does not allow rationalization of the experimentally observed solubilities, considering neither the molecules adjacent to the replace group nor all the molecules within a 15 Å radius. The relative energy of the experimental structures and isostructural phases obtained from the computationally generated structure landscapes calculated at the level providing accurate energy ranking was found to be mostly consistent with the experimentally observed component solubilities.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":"23 9","pages":"6609–6622"},"PeriodicalIF":3.8,"publicationDate":"2023-08-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"177866","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}

{"title":"Parameter Space for Chemical Vapor Deposition Graphene in Cold-Wall Reactors under High Precursor Flow Rate","authors":"Alberto Boscá*,&nbsp;Antonio Ladrón-de-Guevara,&nbsp;Jorge Pedros,&nbsp;Javier Martínez,&nbsp;Rajveer Fandan and Fernando Calle,&nbsp;","doi":"10.1021/acs.cgd.3c00258","DOIUrl":"https://doi.org/10.1021/acs.cgd.3c00258","url":null,"abstract":"<p >Nowadays, promising proof-of-concept graphene technologies already exist, although converting them into a commercial success requires a high-throughput fabrication process providing a high-quality material. Chemical vapor deposition (CVD) has proven to be the enabling technology for this purpose. However, as typical CVD systems are based on laboratory-scale tubular hot-wall reactors, a comprehensive study is required to translate the optimal thermodynamic configuration into industry-ready CVD cold-wall reactors, capable of increasing the growth area and the process efficiency and yield, hence drastically reducing the costs. In this work, a study on how the thermodynamic parameters affect the growth dynamics and the material quality in a cold-wall reactor under high precursor flow rate is presented. The growth dynamics have been assessed in terms of the lateral growth rate and the nucleation density by means of scanning electron microscopy and image-classification techniques, whereas the quality of the single crystals has been evaluated through Raman mapping and electrical measurements. The parameter space defined by the experimental data has been compared with the predictions based on free Gibbs energy minimization, obtaining an overall good qualitative agreement and proving the suitability of the high precursor flow rate regime for achieving a high-quality material at moderate growth times.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":"23 9","pages":"6349–6358"},"PeriodicalIF":3.8,"publicationDate":"2023-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"174701","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}