Ab initio thermodynamics assessment based on data-driven structure modelling

• Project Area: High Entropy Alloys - Science of New Class of Materials Based on Elemental Multiplicity and Heterogeneity
• Project/Area Number: 19H05169
• Research Category: Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)
• Allocation Type: Single-year Grants
• Review Section: Science and Engineering
• Research Institution: Japan Advanced Institute of Science and Technology
• Principal Investigator: 本郷 研太 北陸先端科学技術大学院大学, 情報社会基盤研究センター, 准教授 (60405040)
• Project Period (FY): 2019-04-01 – 2021-03-31
• Project Status: Completed (Fiscal Year 2020)
• Budget Amount: ¥5,850,000 (Direct Cost: ¥4,500,000、Indirect Cost: ¥1,350,000); Fiscal Year 2020: ¥3,250,000 (Direct Cost: ¥2,500,000、Indirect Cost: ¥750,000); Fiscal Year 2019: ¥2,600,000 (Direct Cost: ¥2,000,000、Indirect Cost: ¥600,000)
• Keywords: ハイエントロピー合金 / 第一原理熱力学アセスメント / マテリアルズ・インフォマティクス / 機械学習 / クラスタリング / 第一原理計算 / データ駆動型構造探索 / XRD

Outline of Research at the Start

本研究は、ハイエントロピー(HEA)合金の微視的構造モデルに対するシミュレーションを大量に実施し、得られた諸物性とXRDパターンを学習データとして、動的時間伸縮法を非類似度とするクラスタリング識別モデルを構築する。当該手法は、XRDデータから構成相を同定する従来型の機械学習適用を超えて、構成相における組成配分と微視的原子配列を識別する枠組みを構築する。本研究は、最終的には、多相HEA合金系を対象として、構築したXRD分類器によって多相合金における組成配分や偏析に伴う非均一性を取り除いて主相組成のみならず占有サイトを同定し、得られた微視的構造を入力とする第一原理熱力学アセスメントを展開する。

Outline of Annual Research Achievements

本研究は、ハイエントロピー合金(HEA)系の特異物性の理解に向け、組成配分や偏析に伴う非均一性を考慮したミクロ組織解析を目的とする。解析手法として、「XRD分類による機械学習的構造推定法」と「第一原理熱力学アセスメント」を開発する。まず、大量の微視的構造モデルと呼応するXRDシミュレーションの構造・XRDパターンのデータを学習データとするクラスタリング識別モデルを構築する。昨年度の段階で、当該モデルに関する予備的成果を原著論文として出版した。この推定構造と実験を照合して得られた微視的原子配列構造を入力とする第一原理熱力学アセスメントを実施し、微視的構造の寄与を解明する。典型的な単相固溶体系HEAであるAlxCoCrFeNi(x<2)を対象系とする。
昨年度から今年度にかけて、x=0の場合の４元系CoCrFeNiにおいて、Cr原子にL12短距離秩序を持つ（部分的な）ランダム原子配置の方が自由エネルギー的に安定であることが確認できた。そこで、当初の研究方針とは異なり、3d遷移金属からなる４元系（全１５組成パターン）を対象として、ヘルムホルツ自由エネルギーを算定し、完全ランダム系とL12短距離秩序を持つ部分ランダム系の（温度に対する）相安定性を検証した。その結果、いくつかの組成に対して、L12短距離秩序を持つ方が完全ランダム系よりも安定であることを発見した。HEAに関する先行研究論文調査を行ったが、４元系HEAですら、このような系統的研究は行われておらず、本研究で初めて見出された知見である。当該成果を原著論文にまとめて投稿し、現在、査読中となっている（arXiv:2110.02587）。第一原理熱力学的アセスメントでは、対象合金系に含まれる全ての二元及び三元系合金の自由エネルギー計算が必要であるため、全てのパターンについての計算は完了しておらず、現在も計算を継続している。

Research Progress Status

令和2年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

令和2年度が最終年度であるため、記入しない。

Research Products

• [Int'l Joint Research] Indian Institute of Technology,(インド)
• [Journal Article] Anomalies in the bulk and surface electronic properties of SnS: effects of native defects (2022)
  • Author(s): Dahule Rohit、Singh Chetan C.、Hongo Kenta、Maezono Ryo、Panda Emila
  • Journal Title: Journal of Materials Chemistry C Volume: 10 Issue: 14 Pages: 5514-5525
  • DOI: 10.1039/d1tc04738h
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] High-Pressure Mg-Sc-H Phase Diagram and Its Superconductivity from First-Principles Calculations (2022)
  • Author(s): Song Peng、Hou Zhufeng、Baptista de Castro Pedro、Nakano Kousuke、Hongo Kenta、Takano Yoshihiko、Maezono Ryo
  • Journal Title: The Journal of Physical Chemistry C Volume: 126 Issue: 5 Pages: 2747-2755
  • DOI: 10.1021/acs.jpcc.1c08743
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] The Systematic Study on the Stability and Superconductivity of Y‐Mg‐H Compounds under High Pressure (2022)
  • Author(s): Song Peng、Hou Zhufeng、de Castro Pedro Baptista、Nakano Kousuke、Takano Yoshihiko、Maezono Ryo、Hongo Kenta
  • Journal Title: Advanced Theory and Simulations Volume: 5 Issue: 3 Pages: 2100364-2100364
  • DOI: 10.1002/adts.202100364
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Diffusion Monte Carlo evaluation of disiloxane linearisation barrier (2022)
  • Author(s): Hanindriyo Adie Tri、Yadav Amit Kumar Singh、Ichibha Tom、Maezono Ryo、Nakano Kousuke、Hongo Kenta
  • Journal Title: Physical Chemistry Chemical Physics Volume: 24 Issue: 6 Pages: 3761-3769
  • DOI: 10.1039/d1cp01471d
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Candidate structure for the H2-PRE phase of solid hydrogen (2021)
  • Author(s): Ichibha Tom、Zhang Yunwei、Hongo Kenta、Maezono Ryo、Reboredo Fernando A.
  • Journal Title: Physical Review B Volume: 104 Issue: 21 Pages: 214111-214111
  • DOI: 10.1103/physrevb.104.214111
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] High-Tc Superconducting Hydrides Formed by LaH24 and YH24 Cage Structures as Basic Blocks (2021)
  • Author(s): Song Peng、Hou Zhufeng、Castro Pedro Baptista de、Nakano Kousuke、Hongo Kenta、Takano Yoshihiko、Maezono Ryo
  • Journal Title: Chemistry of Materials Volume: 33 Issue: 24 Pages: 9501-9507
  • DOI: 10.1021/acs.chemmater.1c02371
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Site-Selective Eu3+ Luminescence in the Monoclinic Phase of YSiO2N (2021)
  • Author(s): Kitagawa Yuuki、Ueda Jumpei、Fujii Kotaro、Yashima Masatomo、Funahashi Shiro、Nakanishi Takayuki、Takeda Takashi、Hirosaki Naoto、Hongo Kenta、Maezono Ryo、Tanabe Setsuhisa
  • Journal Title: Chemistry of Materials Volume: 33 Issue: 22 Pages: 8873-8885
  • DOI: 10.1021/acs.chemmater.1c03139
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Importance of Van der Waals Interactions in Hydrogen Adsorption on a Silicon-carbide Nanotube Revisited with vdW-DFT and Quantum Monte Carlo (2021)
  • Author(s): Prayogo Genki I.、Shin Hyeondeok、Benali Anouar、Maezono Ryo、Hongo Kenta
  • Journal Title: ACS Omega Volume: 6 Issue: 38 Pages: 24630-24636
  • DOI: 10.1021/acsomega.1c03318
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] High-Throughput Evaluation of Discharge Profiles of Nickel Substitution in LiNiO2 by Ab Initio Calculations (2021)
  • Author(s): Yoshio Satoshi、Hongo Kenta、Nakano Kousuke、Maezono Ryo
  • Journal Title: The Journal of Physical Chemistry C Volume: 125 Issue: 27 Pages: 14517-14524
  • DOI: 10.1021/acs.jpcc.0c11589
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Peculiar Atomic Bond Nature in Platinum Monatomic Chains (2021)
  • Author(s): Zhang Jiaqi、Ishizuka Keisuke、Tomitori Masahiko、Arai Toyoko、Hongo Kenta、Maezono Ryo、Tosatti Erio、Oshima Yoshifumi
  • Journal Title: Nano Letters Volume: online Issue: 9 Pages: 1-7
  • DOI: 10.1021/acs.nanolett.1c00564
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Surface Study of Cu2SnS3 Using First‐Principles Density Functional Theory (2021)
  • Author(s): Dahule Rohit、Raghav Abhishek、Hanindriyo Adie Tri、Hongo Kenta、Maezono Ryo、Panda Emila
  • Journal Title: Advanced Theory and Simulations Volume: 4 Issue: 6 Pages: 2000315-2000315
  • DOI: 10.1002/adts.202000315
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Insights into the Mechanical and Electrical Properties of a Metal?Phosphorene Interface: An Ab Initio Study with a Wide Range of Metals (2021)
  • Author(s): Ghaffar Abdul、Ganeriwala Mohit D.、Hongo Kenta、Maezono Ryo、Mohapatra Nihar R.
  • Journal Title: ACS Omega Volume: 6 Issue: 11 Pages: 7795-7803
  • DOI: 10.1021/acsomega.0c06255
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] GaN bandgap bias caused by semi-core treatment in pseudopotentials analyzed by the diffusion Monte Carlo method (2021)
  • Author(s): Nikaido Yutaka、Ichibha Tom、Nakano Kousuke、Hongo Kenta、Maezono Ryo
  • Journal Title: AIP Advances Volume: 11 Issue: 2 Pages: 025225-025225
  • DOI: 10.1063/5.0035047
  • Peer Reviewed / Open Access
• [Journal Article] Exploring Heat-Shielding Nanoparticle-Based Materials via First-Principles Calculations and Transfer Learning (2021)
  • Author(s): Yoshida Tomohiro、Maezono Ryo、Hongo Kenta
  • Journal Title: ACS Applied Nano Materials Volume: 4 Issue: 2 Pages: 1932-1939
  • DOI: 10.1021/acsanm.0c03298
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Intrinsic carbon-doping induced synthesis of oxygen vacancies-mediated TiO2 nanocrystals: Enhanced photocatalytic NO removal performance and mechanism (2021)
  • Author(s): Gu Zhanyong、Cui Zhitao、Wang Zijing、Sinkou Qin Ken、Asakura Yusuke、Hasegawa Takuya、Hongo Kenta、Maezono Ryo、Yin Shu
  • Journal Title: Journal of Catalysis Volume: 393 Pages: 179-189
  • DOI: 10.1016/j.jcat.2020.11.025
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Synthesis, Electronic Structure, and Physical Properties of Layered Oxypnictides Sr2ScCrAsO3 and Ba3Sc2Cr2As2O5 (2021)
  • Author(s): Pavan Kumar Naik Sugali、Iwasa Yuki、Kuramochi Kenta、Ichihara Yoshihisa、Kishio Kohji、Hongo Kenta、Maezono Ryo、Nishio Taichiro、Ogino Hiraku
  • Journal Title: Inorganic Chemistry Volume: 60 Issue: 3 Pages: 1930-1936
  • DOI: 10.1021/acs.inorgchem.0c03404
  • Peer Reviewed / Open Access
• [Journal Article] Octahedral morphology of NiO with (111) facet synthesized from the transformation of NiOHCl for the NOx detection and degradation: experiment and DFT calculation (2020)
  • Author(s): Hermawan Angga、Hanindriyo Adie Tri、Ramadhan Erland Rachmad、Asakura Yusuke、Hasegawa Takuya、Hongo Kenta、Inada Miki、Maezono Ryo、Yin Shu
  • Journal Title: Inorganic Chemistry Frontiers Volume: 7 Issue: 18 Pages: 3431-3442
  • DOI: 10.1039/d0qi00682c
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Two-Dimensional Perovskite Oxynitride K2LaTa2O6N with an H+/K+ Exchangeability in Aqueous Solution to Form Stable Photocatalyst for Visible-Light H2 Evolution (2020)
  • Author(s): Takayoshi Oshima, Tom Ichibha,Kenji Oqmhula, Keisuke Hibino, Hiroto Mogi, Shunsuke Yamashita, Kotaro Fujii, Yugo Miseki, Kenta Hongo, Daling Lu,Ryo Maezono, Kazuhiro Sayama, Masatomo Yashima, Koji Kimoto,Hideki Kato, Masato Kakihana, Hiroshi Kageyama, Kazuhiko Maeda
  • Journal Title: Angewandte Chemie International Edition Volume: - Issue: 24 Pages: 9736-9743
  • DOI: 10.1002/anie.202002534
  • Peer Reviewed / Open Access
• [Journal Article] Light Absorption Properties and Electronic Band Structures of Lead‐Vanadium Oxyhalide Apatites Pb5(VO4)3X (X=F, Cl, Br, I) (2020)
  • Author(s): Masashi Nakamura, Kenji Oqmhula, Keishu Utimula, Miharu Eguchi, Kengo Oka, Kenta Hongo, Ryo Maezono, Kazuhiko Maeda*
  • Journal Title: Chem Asian J. Volume: 15 Issue: 4 Pages: 540-545
  • DOI: 10.1002/asia.201901692
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Carbon vacancies and hydroxyls in graphitic carbon nitride: Promoted photocatalytic NO removal activity and mechanism (2020)
  • Author(s): Gu Zhanyong、Cui Zhitao、Wang Zijing、Qin Ken Sinkou、Asakura Yusuke、Hasegawa Takuya、Tsukuda Satoshi、Hongo Kenta、Maezono Ryo、Yin Shu
  • Journal Title: Applied Catalysis B: Environmental Volume: 279 Pages: 119376-119376
  • DOI: 10.1016/j.apcatb.2020.119376
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] New layered perovskite family built from [CeTa2O7]- layers: coloring mechanism from unique multi-transitions (2020)
  • Author(s): Hasegawa Takuya、Shigee Atsushi、Nishiwaki Yoshinori、Nagasako Makoto、Hanindriyo Adie Tri、Hongo Kenta、Maezono Ryo、Ueda Tadaharu、Yin Shu
  • Journal Title: Chemical Communications Volume: 56 Issue: 61 Pages: 8591-8594
  • DOI: 10.1039/d0cc03466e
  • Peer Reviewed / Open Access
• [Journal Article] Ab Initio Evaluation of Complexation Energies for Cyclodextrin-Drug Inclusion Complexes (2020)
  • Author(s): Oqmhula Kenji、Hongo Kenta、Maezono Ryo、Ichibha Tom
  • Journal Title: ACS Omega Volume: 5 Issue: 31 Pages: 19371-19376
  • DOI: 10.1021/acsomega.0c01059
  • Peer Reviewed / Open Access
• [Journal Article] Synergy of Binary Substitutions for Improving the Cycle Performance in LiNiO2 Revealed by Ab Initio Materials Informatics (2020)
  • Author(s): Yoshida Tomohiro、Maezono Ryo、Hongo Kenta
  • Journal Title: ACS Omega Volume: 5 Issue: 22 Pages: 13403-13408
  • DOI: 10.1021/acsomega.0c01649
  • Peer Reviewed / Open Access
• [Journal Article] Machine‐Learning Clustering Technique Applied to Powder X‐Ray Diffraction Patterns to Distinguish Compositions of ThMn12‐Type Alloys (2020)
  • Author(s): Utimula Keishu、Hunkao Rutchapon、Yano Masao、Kimoto Hiroyuki、Hongo Kenta、Kawaguchi Shogo、Suwanna Sujin、Maezono Ryo
  • Journal Title: Advanced Theory and Simulations Volume: 3 Issue: 7 Pages: 2000039-2000039
  • DOI: 10.1002/adts.202000039
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Electrochemical Properties and Crystal Structure of Li+/H+ Cation-exchanged LiNiO2 (2020)
  • Author(s): T. Toma、 R. Maezono、 K. Hongo
  • Journal Title: ACS Appl. Energy Mater. Volume: - Issue: 4 Pages: 4078-4087
  • DOI: 10.1021/acsaem.0c00602
  • Peer Reviewed / Open Access
• [Journal Article] Ab initio thermodynamic properties of certain compounds in Nd-Fe-B system (2020)
  • Author(s): A.T. Hanindriyo、 S. Sridar、 K.C. Hari Kumar、 K. Hongo、 R. Maezono
  • Journal Title: Comp. Mater. Sci. Volume: 180 Pages: 109696-109696
  • DOI: 10.1016/j.commatsci.2020.109696
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Presentation] XRD スペクトルピークの機械学習的識別 (2022)
  • Author(s): 本郷研太
  • Organizer: 新物質研究会 2022~ハイエントロピー効果や機械学習を取り入れた物質開発~
  • Invited
• [Presentation] 計算材料科学からマテリアルズ・インフォマティクスへの研究展開 (2022)
  • Author(s): 本郷研太
  • Organizer: J第19回凝縮系理論コロキウム
  • Invited
• [Presentation] 機械学習によるXRDパターン認識 (2022)
  • Author(s): 本郷研太
  • Organizer: 日本セラミックス協会 2022年 年会, オンライン
• [Presentation] Autoencoder-based feature space of XRD peak patterns (2022)
  • Author(s): Kenta Hongo
  • Organizer: APS March Meeting 2022,online
  • Int'l Joint Research
• [Presentation] First-principles modeling of water-metal wettability (2022)
  • Author(s): Kenta Hongo
  • Organizer: ACS March Meeting 2022,online
  • Int'l Joint Research
• [Presentation] Computational materials design from materials simulations to informatics (2022)
  • Author(s): Kenta Hongo
  • Organizer: 2nd International Conference on Materials Genome, ACCMS Theme Meeting,ハイブリッド
  • Int'l Joint Research / Invited
• [Presentation] 計算材料科学と材料情報学による材料設計 (2021)
  • Author(s): 本郷研太
  • Organizer: JST-CREST「革新的触媒」触媒インフォマティクス研究会 2021, オンライン
  • Invited
• [Presentation] Ab initio materials informatics approach to materials design and characterization (2021)
  • Author(s): 本郷研太
  • Organizer: JAIST創立30周年記念 マテリアルズインフォマティクス国際シンポジウム
  • Int'l Joint Research
• [Presentation] 材料情報学的アプローチによる物質設計 (2021)
  • Author(s): 本郷研太
  • Organizer: 日本物理学会 第76回年次大会(2021年)
  • Invited
• [Presentation] Computational materials design based on materials simulations and informatics (2021)
  • Author(s): 本郷研太
  • Organizer: 日本化学会第101春季年会(2021) アジア国際シンポジウム
  • Int'l Joint Research / Invited
• [Presentation] 機械学習による機能性材料の設計・探索法の基礎 (2020)
  • Author(s): 本郷研太
  • Organizer: 日本化学会第100春季年会2020
  • Invited
• [Presentation] Computational materials design using materials simulations and informatics (2020)
  • Author(s): 本郷研太
  • Organizer: 日本化学会 第100春季年会 アジア国際シンポジウム(2020)
  • Int'l Joint Research / Invited
• [Presentation] 計算材料設計：材料計算科学から材料情報学への展開 (2020)
  • Author(s): 本郷研太
  • Organizer: 日本物理学会第75回日本物理学会シンポジウム
  • Invited
• [Presentation] 計算科学とデータ科学の協働による物質探索の進展 (2020)
  • Author(s): 本郷 研太
  • Organizer: 「凝縮系の理論化学2020」研究会
  • Invited
• [Presentation] Ab Initio Materials Informatics for Computational Materials Design (2019)
  • Author(s): Kenta Hongo
  • Organizer: The 23rd International Annual Symposium on Computational Science and Engineering: Expanding Your Mind(ANSCSE23)
  • Int'l Joint Research / Invited
• [Presentation] Computational materials design from ab intio simulations to ab initio materials informatics (2019)
  • Author(s): Kenta Hongo
  • Organizer: The 10th Internationa Conference of the Asian Consortium on Computational Materials Science (ACCMS-10)
  • Int'l Joint Research / Invited
• [Presentation] Data-driven approach to computational materials design (2019)
  • Author(s): Kenta Hongo
  • Organizer: 20th International Union of Materials Research Societies Internationl Conference in Asia (IUMRS-ICA)
  • Int'l Joint Research / Invited
• [Presentation] Data-driven approach to molecular design (2019)
  • Author(s): Kenta Hongo
  • Organizer: The 5th International Conference on Molecular Simulation 2019 (ICMS 2019)
  • Int'l Joint Research / Invited
• [Book] マテリアルズ・インフォマティクスによる材料開発と活用集 (2019)
  • Author(s): 本郷 研太
  • Total Pages: 463
  • Publisher: 技術情報協会