Award Abstract # 1905499
Probing Effects of Pressure, Mixed Valence, and Spin Frustration on Itinerant Magnets

NSF Org: DMR
Division Of Materials Research
Recipient: FLORIDA STATE UNIVERSITY
Initial Amendment Date: July 19, 2019
Latest Amendment Date: July 19, 2019
Award Number: 1905499
Award Instrument: Standard Grant
Program Manager: Robert Meulenberg
rmeulenb@nsf.gov
 (703)292-2499
DMR
 Division Of Materials Research
MPS
 Directorate for Mathematical and Physical Sciences
Start Date: August 15, 2019
End Date: April 30, 2023 (Estimated)
Total Intended Award Amount: $488,287.00
Total Awarded Amount to Date: $488,287.00
Funds Obligated to Date: FY 2019 = $488,287.00
History of Investigator:
  • Mykhailo Shatruk (Principal Investigator)
    shatruk@chem.fsu.edu
Recipient Sponsored Research Office: Florida State University
874 TRADITIONS WAY
TALLAHASSEE
FL  US  32306-0001
(850)644-5260
Sponsor Congressional District: 02
Primary Place of Performance: Florida State University
95 Chieftan Way
Tallahassee
FL  US  32306-4390
Primary Place of Performance
Congressional District:
02
Unique Entity Identifier (UEI): JF2BLNN4PJC3
Parent UEI:
NSF Program(s): SOLID STATE & MATERIALS CHEMIS
Primary Program Source: 01001920DB NSF RESEARCH & RELATED ACTIVIT
Program Reference Code(s):
Program Element Code(s): 176200
Award Agency Code: 4900
Fund Agency Code: 4900
Assistance Listing Number(s): 47.049

ABSTRACT

PART I: NON-TECHNICAL SUMMARY

This project focuses on investigation of itinerant magnets, a unique class of materials used in societally important clean-energy technologies, including electric vehicles, wind turbines, and magnetic refrigerators. Early studies offered understanding of magnetism in simple metals -- iron, cobalt, and nickel. Currently, however, the state of knowledge and theoretical tools available to materials scientists affords insight into magnetic behavior of more complex intermetallic systems, consisting of two or more elements. This project, supported by the Solid State and Materials Chemistry program in the Division of Materials Research, will combine advanced theoretical methods with experimental studies of itinerant magnets. Chemical synthesis, applied pressure, and high magnetic fields will be used to trigger changes in magnetic behavior. A detailed analysis of the changes observed will establish how itinerant magnets respond to variations in their crystal and electronic structures. The outcome of these studies will be improved understanding of itinerant magnets for the design of advanced magnetic materials to be used in clean-energy technologies and other applications. The diversity of theoretical and experimental tools employed in this project will provide unique research training for graduate and undergraduate students, who will become proficient in solid state chemistry, materials synthesis and characterization, and quantum-chemical calculations. For broader outreach, the project PI will also organize nationwide undergraduate summer schools in magnetism and magnetic materials.

PART II: TECHNICAL SUMMARY

Itinerant magnetism has been a fascinating area of research in condensed-matter physics for many decades. Currently, however, such magnetic systems are receiving renewed attention from solid-state chemists, due to the broader availability of theoretical tools for investigation of electronic structure and improved insight into peculiarities of chemical bonding in the solid state. This project aims to uncover correlations between the nature of magnetic ordering and chemical bonding in itinerant magnets by exploring the interplay between the crystal and electronic structure and magnetic properties as a function of chemical substitution, applied pressure, or magnetic field. One aspect of the project will focus on complex transition metal pnictides, with an emphasis on effects of pressure and light-induced excitations that may lead to drastic changes in metallic behavior. The project will also investigate behavior of spin-frustrated systems with metallic or strongly covalent bonding. These studies target the next level of complexity in the spin-frustrated systems, where the addition of itinerant magnetic behavior can lead to the discovery of exotic spin textures and unconventional spin dynamics. The proposed research activities will provide versatile training to graduate and undergraduate students in materials synthesis, investigation of structural and magnetic properties, and studies of the electronic band structure. Undergraduate students and students from underrepresented groups will be involved in the project, both as researchers and through participation in national undergraduate summer schools in magnetism and magnetic materials organized by the PI. This project is supported by the Solid State and Materials Chemistry program in the Division of Materials Research.

This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

PUBLICATIONS PRODUCED AS A RESULT OF THIS RESEARCH

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(Showing: 1 - 10 of 19)
Mann, Dallas K. and Wang, YiXu and Marks, Jeanette D. and Strouse, Geoffrey F. and Shatruk, Michael "Microwave Synthesis and Magnetocaloric Effect in AlFe 2 B 2" Inorganic Chemistry , v.59 , 2020 https://doi.org/10.1021/acs.inorgchem.0c01731 Citation Details
Adams, Milo and Huang, Chen and Shatruk, Michael "Effect of electron- and hole-doping on properties of kagomé-lattice ferromagnet Fe 3 Sn 2" Journal of Physics: Condensed Matter , v.35 , 2023 https://doi.org/10.1088/1361-648X/acc91e Citation Details
Clark, Judith and Pak, Chongin and Cao, Huibo and Shatruk, Michael "Helimagnetism in MnBi2Se4 Driven by Spin-Frustrating Interactions Between Antiferromagnetic Chains" Crystals , v.11 , 2021 https://doi.org/10.3390/cryst11030242 Citation Details
Clark, Judith K. and Tan, Xiaoyan and Garlea, V. Ovidiu and Arico, Alexandra A. and Ramirez, Arthur P. and Yannello, Vincent and Thompson, Corey M. and Kovnir, Kirill and Shatruk, Michael "Reentrant spin glass state induced by structural phase transition in La0.4Ce" Physical Review Materials , v.4 , 2020 10.1103/PhysRevMaterials.4.074412 Citation Details
Clark, Judith K. and Yannello, Vincent and Samarakoon, Anjana M. and Ross, Cyris and Uible, Madeleine C. and Garlea, V. Ovidiu and Shatruk, Michael "Inelastic Neutron Scattering Study of Magnetic Exchange Pathways in MnS" The Journal of Physical Chemistry C , v.125 , 2021 https://doi.org/10.1021/acs.jpcc.1c02956 Citation Details
Gamage, Eranga H. and Greenfield, Joshua T. and Unger, Colin and Kamali, Saeed and Clark, Judith K. and Harmer, Colin P. and Luo, Liang and Wang, Jigang and Shatruk, Michael and Kovnir, Kirill "Tuning FeSe Tetrahedral Frameworks by a Combination of [Fe(en) 3 ] 2+ Cations and Cl Anions" Inorganic Chemistry , v.59 , 2020 https://doi.org/10.1021/acs.inorgchem.0c01727 Citation Details
Gamage, Eranga H. and Kamali, Saeed and Clark, Judith K. and Lee, Yongbin and Yox, Philip and Shafer, Padraic and Yaroslavtsev, Alexander A. and Ke, Liqin and Shatruk, Michael and Kovnir, Kirill "AsSe Pentagonal Linkers to Induce Chirality and Polarity in Mixed-Valent FeSe Tetrahedral Chains Resulting in Hidden Magnetic Ordering" Journal of the American Chemical Society , v.144 , 2022 https://doi.org/10.1021/jacs.2c02936 Citation Details
Jo, Minyoung and Dragulescu-Andrasi, Alina and Miller, L. Zane and Pak, Chongin and Shatruk, Michael "Nucleophilic Activation of Red Phosphorus for Controlled Synthesis of Polyphosphides" Inorganic Chemistry , v.59 , 2020 10.1021/acs.inorgchem.0c00108 Citation Details
Kumar, Govind Sasi and Xin, Yan and Raaj Vellore Winfred, J. S. and Clark, Judith K. and Shatruk, Michael "2D spin glass MnIn 2 Se 4 : application of liquid-phase exfoliation to a layered structure with seven-atom-thick layers" Journal of Materials Chemistry C , v.11 , 2023 https://doi.org/10.1039/D2TC03776A Citation Details
Macy, Juan and Ratkovski, Danilo and Balakrishnan, Purnima P. and Strungaru, Mara and Chiu, Yu-Che and Flessa Savvidou, Aikaterini and Moon, Alex and Zheng, Wenkai and Weiland, Ashley and McCandless, Gregory T. and Chan, Julia Y. and Kumar, Govind S. and "Magnetic field-induced non-trivial electronic topology in Fe 3x GeTe 2" Applied Physics Reviews , v.8 , 2021 https://doi.org/10.1063/5.0052952 Citation Details
Mann, Dallas K. and Díez, Aida M. and Xu, Junyuan and Lebedev, Oleg I. and Kolenko, Yury V. and Shatruk, Michael "Polar Layered Intermetallic LaCo 2 P 2 as a Water Oxidation Electrocatalyst" ACS Applied Materials & Interfaces , v.14 , 2022 https://doi.org/10.1021/acsami.1c19858 Citation Details
(Showing: 1 - 10 of 19)

PROJECT OUTCOMES REPORT

Disclaimer

This Project Outcomes Report for the General Public is displayed verbatim as submitted by the Principal Investigator (PI) for this award. Any opinions, findings, and conclusions or recommendations expressed in this Report are those of the PI and do not necessarily reflect the views of the National Science Foundation; NSF has not approved or endorsed its content.

Intellectual Merit. This project has continued to advance our expertise in itinerant magnets, which represent a fundamentally and technologically important group of magnetic materials. To achieve better understanding of correlations between the structure and properties of these materials, we have used diverse synthetic methods in conjunction with a variety of characterization techniques, including X-ray crystallography, magnetometry, X-ray absorption spectroscopy, and neutron diffraction. In addition, theoretical methods were used to establish correlations between the electronic and crystal structures of solids and their magnetic behavior. We have demonstrated that the interplay between the crystal and electronic structure can be used to tune magnetic properties via judicious variation of chemical composition, as well as by application of applied pressure or magnetic field. Moreover, these developments have led us to propose novel approaches to generating magnetic structures with non-collinear arrangement of magnetic moments. Such materials can be very useful for the future quantum, sensing, and data storage technologies.

We used a combination of X-ray and neutron scattering to detect an intermediate phase involved in martensitic phase transition between cubic and hexagonal polymorphs of MnSe. This transition is one of the most fundamental structural transformations in crystallography. The detection of the intermediate orthorhombic phase provides a rare experimental visualization of this transformation, which plays important role in a variety of physical disciplines.

We also discovered an unusual reversal of magnetic ordering in La0.4Ce0.6Co2P2, where the initial ferromagnetic ordering that takes place below 225 K is lost as the temperature is lowered below 190 K. Such a behavior is rather unusual, because lowering the temperature typically makes magnetically ordered states more robust. By using a combination of various experimental techniques and theoretical studies, we have demonstrated that the loss of magnetic ordering was caused by a structural phase transition at 190 K. Thus, this study has provided yet another demonstration of the intimate relationship between the crystal and electronic structures of itinerant magnets and their magnetic properties.

Broader Impacts. The project activities have provided research training and education to 1 postdoctoral scholar, 8 graduate students (3 of them have already defended the PhD dissertations), and 10 undergraduate students (5 of them females and 4 minority students). In addition to the research training in the lab, the students also participated in various scientific meetings to build their professional networks and in summer schools and workshops to broaden their research skills.

In summer of 2021, the PI organized the 3rd Undergraduate Summer School on Magnetism and Magnetic Materials (US-MMM) that provided introduction to magnetism to 14 students selected from a nationwide pool and coming from disciplines of chemistry, physics, and engineering (see the attached program and participant photo).


Last Modified: 07/18/2023
Modified by: Mykhailo Shatruk

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