Intercalated chalcogenides Fe1/4TaS2 and Fe1/3TaS2 under extreme pressure—temperature conditions
Year: 2025
Type: article
Abstract: Intercalation is an important strategy for enhancing functionality in complex chalcogenides. This is because layered materials can be endowed with intriguing properties by filling the van der Waals gap with various ions and molecules, which, in addition to their unique chemistry, break symmetry in new ways. In order to explore the properties of intercalated metal dichalcogenides under extreme pressure-temperature conditions, we combine diamond anvil cell techniques, Raman scattering spectroscopy, magnetic susceptibility, and first-principles calculations to reveal the pressure–temperature phase diagram of Fe 1/3 TaS 2 . This system hosts a compression-driven structural phase transition to a polar state as well as remnant charge density wave signatures deriving from the host lamella of the 2H-parent compound. We also explore the role of different A -site patterns and determine that, by comparison, Fe 1/4 TaS 2 is soft and flexible due to the lower metal density inside the van der Waals gap. These findings open the door to entirely new states of matter with exciting property combinations, including metallicity, polarity, chirality, and altermagnetism – depending upon the conditions – that can support a wide range of spintronics and phononics applications.
Authors: J. L. Musfeldt, Junjie Yang, R. E. Putnam Jr, Shengzhi Zhang, J. T. Haraldsen, S. -W. Cheong, Z. Liu
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $3,405
Awards: THE CHICAGO/DOE ALLIANCE CENTER (CDAC)IS DEDICATED TO BASIC RESEARCH, TRAINING, AND TECHNIQUE DEVELOPMENT IN THE STUDY OF MATERIALS IN EXTREME CONDITIONS. THE CENTER HAS ENABLED NUMEROUS ADVANCES IN HIGH P-T SCIENCE, TECHNOLOGY, AND TRAINING SINCE ITS INCEPTION 16 YEARS AGO AS THE CARNEGIE/DOE ALLIANCE CENTER. THESE ADVANCES INCLUDE STUDENT AND POSTDOC-LED SCIENTIFIC DISCOVERIES AND A SUCCESSFUL TRACK RECORD IN TRAINING EARLY CAREER SCIENTISTS FOR WORK IN THE NNSA COMPLEX.
MATERIALS OF INTEREST ENCOMPASS CRYSTALLINE SOLIDS, FLUIDS AND GLASSES, NANOSTRUCTURED TO MESOSTRUCTURED MATERIALS, AND COMPLEX COMPOSITES. CHEMICALLY THESE MATERIALS INCLUDE D- AND F-ELECTRON ELEMENTS AND ALLOYS, LOW-Z MOLECULAR COMPOUNDS, ENERGETIC MATERIALS AND DETONATION PRODUCTS, DENSE GASES, METAL OXIDES AND HYDRIDES, AND CHEMICALLY HETEROGENEOUS SUBSTANCES. CDAC WILL ADVANCE UNDERSTANDING OF THESE STEWARDSHIP-RELATED CLASSES OF MATERIALS IN EXTREME CONDITIONS IN THE FOLLOWING SIX MATERIAL PROPERTY THRUSTS (1) HIGH P-T STRUCTURES AND PHASE RELATIONS; (2) P-V-T EQUATIONS OF STATE; (3) PHONONS, VIBRATIONAL THERMODYNAMICS, AND ELASTICITY; (4) PLASTICITY, YIELD STRENGTH, AND DEFORMATION; (5) ELECTRONIC AND MAGNETIC STRUCTURE AND DYNAMICS; AND (6) HIGH P-T CHEMISTRY. FOR EACH OF THESE ABOVE MATERIALS AND PROPERTIES THRUSTS, CDAC WILL ADDRESS NEW QUESTIONS, INCLUDING THE FOLLOWING:
• HOW CAN WE UNDERSTAND, PREDICT, AND CONTROL MATTER AND MATERIALS TO VERY HIGH COMPRESSIONS?
• WHAT NEW PHYSICS MAY EMERGE IN ‘COLD’ TO ‘WARM’ DENSE MATTER?
• HOW CAN WE ACCURATELY DETERMINE FUNDAMENTAL THERMODYNAMIC PROPERTIES TO VERY HIGH P AND T?
• HOW DO DEFECTS, GRAIN BOUNDARIES, AND INTERFACES RESPOND TO HIGH P-T CONDITIONS AND STRAIN RATES?
• HOW CAN WE BETTER MEASURE TIME-DEPENDENT TRANSFORMATIONS, AND BRIDGE STRAIN-RATE GAPS BETWEEN STATIC, QUASI-STATIC, AND DYNAMIC COMPRESSION?
• CAN WE BETTER DETERMINE STRENGTH, PLASTICITY, AND RHEOLOGY AT VERY HIGH P-T CONDITIONS?
• CAN WE EXPAND THE HIGH P-T SYNTHETIC CHEMISTRY FRONTIER TO PRODUCE NEW, OPTIMIZED MATERIALS?
CDAC WILL ADDRESS THESE QUESTIONS WITH BOTH STATIC AND DYNAMIC COMPRESSION EXPERIMENTS TOGETHER WITH THEORY, MODELING, AND SIMULATION IN CDAC UNIVERSITY LABORATORIES AS WELL AS DOE/SC AND DOE/NNSA FACILITIES. THE WORK WILL BE ENABLED BY CONTINUED ACCESS TO CDAC’S PARTNER SYNCHROTRON RADIATION FACILITIES, HIGH PRESSURE COLLABORATIVE ACCESS TEAM (HPCAT) AT THE ADVANCED PHOTON SOURCE, ARGONNE NATIONAL LABORATORY (ANL) AND THE FRONTIER INFRARED SPECTROSCOPY (FIS) BEAMLINE AT THE NATIONAL SYNCHROTRON LIGHT SOURCE II, BROOKHAVEN NATIONAL LABORATORY (BNL), AS WELL AS OTHER FACILITIES. THE OVERARCHING SCIENTIFIC OUTCOME IS ADVANCING FUNDAMENTAL UNDERSTANDING OF MATERIALS BEHAVIOR IN EXTREME CONDITIONS, WHICH IN TURN WILL LEAD TO IMPROVED UNDERSTANDING OF MATERIALS AGING, PERFORMANCE OF NEWLY MANUFACTURED MATERIALS, MATERIALS IN MULTIPLE EXTREME ENVIRONMENTS, AND THE CREATION OF NEW MATERIALS.
CDAC ENGAGEMENT WITH NNSA PROGRAMS AT ANL AND WITH ITS PARTNER GROUPS IN ILLINOIS WILL BE SIGNIFICANTLY ENHANCED BY ITS MOVE TO THE UNIVERSITY OF ILLINOIS (UIC). CDAC WILL CONTINUE ITS ACTIVE PROGRAM IN EDUCATION AND TRAINING OF NEXT-GENERATION RESEARCHERS FOR STEWARDSHIP SCIENCE. IN SO DOING, CDAC WILL HOST STUDENT WORKSHOPS AND SPONSOR MEETINGS AND SYMPOSIA FOR THE BROADER COMMUNITY. THE CENTER WILL FACILITATE STUDENT ENGAGEMENT WITH NNSA LABORATORIES AND BE A VEHICLE FOR INTRODUCING EARLY CAREER SCIENTISTS TO NNSA LABORATORY PROGRAMS. THE CENTER WILL CONTINUE TO CLOSELY COLLABORATE WITH OTHER ACADEMIC GROUPS, OTHER SSAA AWARDEES, AND NATIONAL LABORATORY SCIENTISTS. CDAC WILL CONTINUE TO LEVERAGE THE SSAA COOPERATIVE AGREEMENT WITH ADDITIONAL GRANTS, WHICH SO FAR HAVE MULTIPLIED BY SEVERAL TIMES THE IMPACT AND INVESTMENT OF NNSA IN THE CENTER. FINALLY, CDAC WILL CONTINUE TO SUPPORT USE OF NNSA FACILITIES, INCLUDING NIF, Z, AND LANSCE, AND FEASIBILITY STUDIES FOR NEXT-GENERATION NNSA FACILITIES., G1639680140, G2388925162, G4038517476, COMPLEX CHALCOGENIDES UNDER PRESSURE, G490166620, G7098706596, EXOTIC MAGNETIC ORDERS AND DYNAMICS IN CHIRAL MAGNETS, G7707297413
OpenAlex ID: W7110038438