A rare earth magnetic single crystal material, a preparation method and application thereof

By preparing the rare earth magnetic single crystal material HoAuSi2, the limitations of the coordinated regulation of low-temperature physical properties and crystal structure were solved, efficient conductivity and stability at low temperatures were achieved, and its application in quantum computing, low-temperature electronics and magnetic sensors was expanded.

CN119956495BActive Publication Date: 2025-10-10HEFEI INSTITUTE OF PHYSICAL SCIENCE CHINESE ACADEMY OF SCIENCES
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Patent Information

Application Number
CN202510120416.5
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2025-01-25
Publication Date
2025-10-10
Estimated Expiration
2045-01-25

AI Technical Summary

Technical Problem

Existing material systems have limitations in the coordinated regulation of low-temperature physical properties and crystal structure, making it difficult to meet the requirements of emerging technologies for special electrical and magnetic properties.

Method used

The rare earth magnetic single crystal material HoAuSi2 is prepared with a hexagonal crystal structure and a Curie temperature of 8K. It is grown by the flux method to ensure the crystal uniformity and purity, and is used to manufacture low-temperature quantum devices and sensors.

Benefits of technology

HoAuSi2 single crystals exhibit good conductivity and stability at low temperatures and are used in low-temperature quantum devices and sensors to detect physical quantities in extremely low-temperature environments and to study the physical phenomena of strongly correlated electronic systems.

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Abstract

The application relates to a rare earth magnetic single crystal material, a preparation method and application thereof, the chemical formula of the rare earth magnetic single crystal material is HoAuSi2, the rare earth magnetic single crystal material has a hexagonal crystal structure, the lattice constant is a=b=4.09 angstrom, c=4.03 angstrom, electric transport shows metallicity, and the Curie temperature is 8K. The rare earth magnetic single crystal material HoAuSi2 provided by the application has a unique hexagonal crystal structure, exhibits a Curie temperature of 8K and a resistance characteristic of metal behavior at low temperature, and provides a new possibility and research direction for further exploring potential applications of new functional materials in frontier fields such as quantum computing, low-temperature electronics, spin electronics and new magnetic sensors.
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Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of functional materials, in particular to a rare earth magnetic single crystal material and a preparation method and application thereof. BACKGROUND

[0002] In the field of modern materials science, the exploration and research of new functional materials have always been a research hotspot, aiming to meet the increasingly stringent requirements of the high-tech industry on material performance.

[0003] Rare earth metals and their compounds often exhibit a wide range of fascinating physical properties due to their unique 4f electron structure, which have potential applications in magnetic, electrical, optical, and other fields, thus attracting widespread attention. Among them, gold (Au) is a noble metal with excellent electrical conductivity and chemical stability, which has important application basis in electronic devices and other aspects. Silicon (Si) is the cornerstone of the semiconductor industry, and its electrical properties and controllable crystal structure make it a key element for building various electronic and optoelectronic devices.

[0004] In recent years, researchers have been working to combine rare earth elements with other metals and metalloid elements in order to develop novel material systems with unique properties, in order to fill the gaps in existing materials in certain specific performance aspects and expand the application range of materials. However, the existing material systems still have limitations in the synergistic regulation of low-temperature physical properties and crystal structure, making it difficult to meet the needs of some emerging technologies for materials with special electrical and magnetic properties. SUMMARY

[0005] Therefore, the purpose of the present application is to provide a rare earth magnetic single crystal material and a preparation method and application thereof, which has a hexagonal crystal structure, exhibits metallic electrical transport, has a Curie temperature of 8K, and has good electrical conductivity and stability at low temperatures, providing new possibilities and research directions for further exploration of the potential applications of new functional materials in the fields of quantum computing, low-temperature electronics, spintronics, and new magnetic sensors.

[0006] To achieve the above-mentioned purpose, the present application adopts the following technical solutions:

[0007] The present application first provides a rare earth magnetic single crystal material with a chemical formula of HoAuSi2, which has a hexagonal crystal structure with lattice constants of a=b=4.09 Å and c=4.03 Å, and exhibits metallic electrical transport with a Curie temperature of 8K.

[0008] The rare earth magnetic single crystal material HoAuSi2 provided by the present invention has a unique hexagonal crystal structure and exhibits a Curie temperature of 8K and metallic resistance characteristics at low temperatures. The Curie temperature of 8K and the metallic resistance behavior of the HoAuSi2 single crystal give it good conductivity and stability at low temperatures. It can be used to manufacture electrodes, connecting wires and other components in low-temperature quantum devices to ensure the efficient operation of quantum computing systems in low-temperature environments. Based on its magnetic and resistive properties that change with temperature, it can also be used to make low-temperature sensors for detecting physical quantities such as temperature changes or magnetic field changes in extremely low-temperature environments. The Ho ions in HoAuSi2 may cause the material to have a strongly correlated electron effect, which can be used to study physical phenomena in strongly correlated electron systems, such as the interaction between the electron's spin, charge and orbital degrees of freedom. Therefore, the discovery of the HoAuSi2 single crystal provides new possibilities and research directions for further exploring the potential applications of new functional materials in cutting-edge fields such as quantum computing, low-temperature electronics, spin electronics and new magnetic sensors.

[0009] As a further improvement of the above solution of the present invention, the longitudinal resistivity of the rare earth magnetic single crystal material at room temperature is 1.53×10 2 μΩcm.

[0010] As a further improvement of the above solution of the present invention, the naturally grown surface of the rare earth magnetic single crystal material is a (010) crystal plane.

[0011] The present invention also provides a method for preparing the rare earth magnetic single crystal material as described above, which comprises the following steps: mixing the self-fluxing agent Sn powder with Ho powder, Au powder and Si powder, vacuum sealing, calcining, cooling to a predetermined temperature and immediately centrifuging to obtain the rare earth magnetic single crystal material.

[0012] As a further improvement of the above solution of the present invention, the molar ratio of Ho powder, Au powder, Si powder and Sn powder is 1:1:1-2:10-15.

[0013] As a further improvement of the above-mentioned solution of the present invention, the process of using Sn powder as a self-flux and mixing it with Ho powder, Au powder and Si powder and then vacuum sealing it includes the following steps: in an argon-protected glove box, placing Ho powder, Au powder, Si powder and Sn powder into a pretreated alumina crucible, then placing the alumina crucible in a quartz tube and vacuum sealing it with an oxyhydrogen flame.

[0014] As a further improvement of the above-mentioned solution of the present invention, the pretreatment method of the alumina crucible is: rinse the alumina crucible with deionized water, then place the alumina crucible in deionized water for ultrasonic cleaning for 30-35 minutes, then place it at 1000-1050°C for 10-15 hours, and then take it out of the furnace for cooling.

[0015] As a further improvement of the above solution of the present invention, the calcination is carried out at 1050-1100° C. for 10-15 hours.

[0016] As a further improvement of the above solution of the present invention, the cooling rate is 1-1.5°C / h, the predetermined temperature is 850-900°C; and / or the centrifugal speed is 1500-2000r / min, and the centrifugal time is 5-10min.

[0017] The present invention also provides an application of the rare earth magnetic single crystal material as described above in low-temperature quantum devices, magnetic sensors, and strongly correlated materials.

[0018] Compared with the prior art, the present invention has the following beneficial effects:

[0019] 1. The rare earth magnetic single crystal material HoAuSi2 provided by the present invention has a unique hexagonal crystal structure and exhibits a Curie temperature of 8K and metallic resistance characteristics at low temperatures. The Curie temperature of 8K and metallic resistance behavior of HoAuSi2 single crystal give it good conductivity and stability at low temperatures. It can be used to manufacture electrodes, connecting wires and other components in low-temperature quantum devices, ensuring the efficient operation of quantum computing systems in low-temperature environments. The resistivity of HoAuSi2 single crystal at room temperature (T=300K) is 1.53×10 2 μΩcm, as the temperature decreases, the resistivity also decreases. Based on the magnetic and resistive properties of HoAuSi2 single crystals that change with temperature, it can also be used to make low-temperature sensors to detect physical quantities such as temperature changes or magnetic field changes in extremely low temperature environments; the Ho ions in HoAuSi2 can cause the material to have a strongly correlated electron effect, which can be used to study physical phenomena in strongly correlated electron systems, such as the interaction between the electron's spin, charge and orbital degrees of freedom; therefore, the discovery of HoAuSi2 single crystals provides new possibilities and research directions for further exploring the potential applications of new functional materials in cutting-edge fields such as quantum computing, low-temperature electronics, spin electronics and new magnetic sensors.

[0020] 2. The present invention uses Sn as a flux, places the raw material and flux powder in an alumina crucible and vacuum seals it in a quartz tube, melts it at high temperature and then slowly cools it down to precipitate HoAuSi2 single crystals, and then centrifuges to remove the flux at a specific temperature to obtain HoAuSi2 single crystals. The self-fluxing method does not introduce other impurities, can ensure the uniformity of the grown crystals, has simple equipment, and is easy to implement. BRIEF DESCRIPTION OF THE DRAWINGS

[0021] Figure 1 A physical picture of the HoAuSi2 single crystal prepared in an embodiment of the present invention;

[0022] Figure 2 XRD patterns of HoAuSi2 single crystal and powder prepared in the embodiment of the present invention;

[0023] Figure 3 Schematic diagram of the structure of the HoAuSi2 single crystal prepared in an embodiment of the present invention;

[0024] Figure 4 The SEM morphology and element distribution diagram of the HoAuSi2 single crystal prepared in the embodiment of the present invention;

[0025] Figure 5 χ-T (a) and MH (b) curves of the magnetic field of the HoAuSi2 single crystal prepared in an embodiment of the present invention along different directions;

[0026] Figure 6 The longitudinal resistivity of the HoAuSi2 single crystal prepared in the embodiment of the present invention is ρ xx Temperature variation diagram. DETAILED DESCRIPTION

[0027] To facilitate understanding of the present invention, the present invention will be described more fully below in conjunction with specific embodiments. However, the present invention can be implemented in many different forms and is not limited to the embodiments described herein. On the contrary, the purpose of providing these embodiments is to provide a more thorough and comprehensive understanding of the disclosure of the present invention.

[0028] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as those commonly understood by those skilled in the art of the present invention. The terms used in the specification of the present invention herein are only for the purpose of describing specific embodiments and are not intended to limit the present invention.

[0029] This embodiment provides a rare earth magnetic single crystal material, which is grown using a flux method, specifically comprising the following steps:

[0030] S1. Pretreatment of the alumina crucible: Clean the alumina crucible with deionized water. Then, ultrasonically clean the cleaned alumina crucible in a beaker of deionized water for 30 minutes to remove impurities adhering to the wall of the alumina crucible. Finally, dry the alumina crucible in a high-temperature box furnace at 1000°C for 10 hours to remove moisture from the crucible, thereby obtaining a pretreated alumina crucible.

[0031] S2. Raw material weighing and packaging: In a high-purity argon-protected glove box (water content <0.1 ppm, oxygen content <0.1 ppm), weigh high-purity Ho powder (purity: 99.9%), Au powder (purity: 99.99%), Si powder (purity: 99.9%), and flux Sn powder (purity: 99.9%) in a molar ratio of 1:1:2:15 and place them into a pretreated alumina crucible; place the loaded alumina crucible into a quartz tube, and evacuate the quartz tube to 10 -3 After Pa, it is sealed by oxyhydrogen flame.

[0032] S3. Single Crystal Growth: Place the sealed quartz tube in a high-temperature box furnace and heat it to 1100°C at 100°C / h and maintain it for 10 hours to fully melt and mix the raw materials. Then, slowly cool it to 900°C at 1°C / h. During this process, the crystals spontaneously nucleate and crystallize from the saturated melt and gradually grow.

[0033] S4. Crystal separation: At 900°C, the quartz tube was quickly removed from the high-temperature box furnace and placed upside down in a centrifuge. The crystal was separated from the flux by high-speed centrifugation (speed 1500 r / min, centrifugation time 10 min) to obtain a HoAuSi2 single crystal sample.

[0034] Figure 1 The physical picture of the HoAuSi2 single crystal obtained in this embodiment is as follows: Figure 1 It can be seen that the surface of the HoAuSi2 single crystal prepared in this embodiment presents a very bright metallic luster.

[0035] Using X-ray diffractometer (XRD, PANalytical X'pert, Cu- K α1 ,λ=0.15406 nm) X-ray diffraction was performed on the HoAuSi2 single crystal and its powder prepared in this embodiment, and the following results were obtained: Figure 2 The XRD patterns of the single crystal and powder are shown in Figure 2 It can be seen that the naturally grown surface of the rare earth magnetic single crystal material prepared in this embodiment is the (010) crystal plane; the XRD spectrum of the HoAuSi2 powder prepared in this embodiment is refined to obtain: a=b=4.09Å, c=4.03Å, α=β=90°, γ=120°.

[0036] According to the XRD pattern analysis, Figure 3 The crystal structure of the rare earth magnetic single crystal material prepared in this embodiment is shown, in which Si atoms form a hexagonal close-packed stack, Ho atoms and Au atoms occupy octahedral positions respectively, and the space group is P63 / mmc.

[0037] The chemical composition and element distribution of the HoAuSi2 single crystal prepared in this embodiment were characterized by using a scanning electron microscope (SEM) and its accessory energy dispersive spectrometer (EDS), and the following results were obtained: Figure 4 The SEM morphology and element distribution shown in Figure 4 It can be seen that the surface of the crystal prepared in this embodiment is smooth and flat without obvious defects, and the three elements Ho, Au and Si are evenly distributed in the single crystal.

[0038] The magnetic properties of the HoAuSi2 single crystal prepared in this embodiment were tested by superconducting quantum interference instrument (MPMS-5T, 1.9K≤T≤400K, 0≤H≤5T). The test results are as follows: Figure 5 shown; from Figure 5 As can be seen in (a), the magnetic field along the c-axis and ab-plane shows that: as the temperature T decreases, the magnetic susceptibility χ first gradually increases. Below a certain temperature, the ZFC and FC curves do not overlap, showing glass behavior; the rate of change of the magnetic susceptibility χ along the c-axis and ab-plane with temperature T reaches a peak at 8K, so the Curie temperature T C =8K. Figure 5 As can be seen in (b), when T=3K, the MH curve shows soft magnetic behavior, and the easy magnetization axis is along the c-axis.

[0039] The electrical transport performance of the HoAuSi2 single crystal prepared in this embodiment was tested by means of a low-temperature physical property measurement system (PPMS-9T, 1.8K≤T≤400K, 0≤H≤9T): the electrode leads were made using a four-lead method, and the electrical transport of the rare earth magnetic single crystal material was measured, and the following results were obtained: Figure 6 The longitudinal resistivity ρ shown xx Temperature variation diagram, from Figure 6 It can be seen that at room temperature (T=300K), the longitudinal resistivity of rare earth magnetic single crystal material is 1.53×10 2 μΩcm. As the temperature decreases, the resistivity also decreases, showing metallic behavior. The RRR value is about 1.32, and the turning point at T=8K corresponds to the magnetic phase transition.

[0040] According to the above results, it can be explained that the HoAuSi2 single crystal prepared in this application has a unique hexagonal crystal structure, exhibits a Curie temperature of 8K and metallic resistance characteristics at low temperatures. The Curie temperature of 8K and the metallic resistance behavior of the HoAuSi2 single crystal make it have good conductivity and stability at low temperatures, and can be used to manufacture electrodes, connecting wires and other components in low-temperature quantum devices to ensure the efficient operation of quantum computing systems in low-temperature environments; based on its magnetic and resistance properties that change with temperature, it can also be used to make low-temperature sensors for detecting physical quantities such as temperature changes or magnetic field changes in extremely low-temperature environments; the Ho ions in HoAuSi2 can cause the material to have a strongly correlated electronic effect, which can be used to study physical phenomena in strongly correlated electronic systems, such as the interaction between the spin, charge and orbital freedom of electrons; therefore, the discovery of HoAuSi2 single crystals provides new possibilities and research directions for further exploring the potential applications of new functional materials in cutting-edge fields such as quantum computing, low-temperature electronics, spin electronics and new magnetic sensors.

[0041] The technical features of the above-mentioned embodiments can be combined arbitrarily. In order to make the description concise, not all possible combinations of the technical features in the above-mentioned embodiments are described. However, as long as there is no contradiction in the combination of these technical features, they should be considered to be within the scope of this specification.

[0042] The above-described embodiments merely illustrate several implementations of the present invention, and while their descriptions are relatively specific and detailed, they should not be construed as limiting the scope of the patent. It should be noted that a person skilled in the art would be able to make numerous variations and improvements without departing from the spirit of the present invention, all of which fall within the scope of protection of the present invention. Therefore, the scope of protection of the patent for this invention shall be determined by the appended claims.

Claims

1. A rare earth magnetic single crystal material, characterized in that: Its chemical formula is HoAuSi2, it has a hexagonal crystal structure, its lattice constants are a=b=4.09Å, c=4.03Å, its electrical transport exhibits metallic properties, and its Curie temperature is 8K.

2. The rare earth magnetic single crystal material according to claim 1, characterized in that The rare earth magnetic single crystal material has a longitudinal resistivity of 1.53×10 2 μΩcm.

3. The rare earth magnetic single crystal material according to claim 1, characterized in that The naturally grown surface of the rare earth magnetic single crystal material is a (010) crystal plane.

4. A method for preparing the rare earth magnetic single crystal material according to any one of claims 1 to 3, characterized in that: It includes the following steps: After the self-fluxing agent Sn powder is mixed with Ho powder, Au powder and Si powder, the mixture is vacuum sealed, calcined, cooled to a predetermined temperature and then centrifuged immediately to obtain a rare earth magnetic single crystal material.

5. The method for preparing a rare earth magnetic single crystal material according to claim 4, characterized in that: The molar ratio of Ho powder, Au powder, Si powder and Sn powder is 1:1:1-2:10-15.

6. The method for preparing a rare earth magnetic single crystal material according to claim 4, characterized in that: The method of using Sn powder as a self-flux, mixing it with Ho powder, Au powder and Si powder and then vacuum sealing it includes the following steps: in an argon-protected glove box, placing the Ho powder, Au powder, Si powder and Sn powder into a pretreated alumina crucible, then placing the alumina crucible in a quartz tube, and vacuum sealing it with an oxyhydrogen flame.

7. The method for preparing a rare earth magnetic single crystal material according to claim 6, characterized in that: The pretreatment method of the alumina crucible is as follows: rinse the alumina crucible with deionized water, then ultrasonically clean the alumina crucible in deionized water for 30-35 minutes, then heat-seal the crucible at 1000-1050° C. for 10-15 hours, and then cool the crucible out of the furnace.

8. The method for preparing a rare earth magnetic single crystal material according to claim 4, characterized in that: The calcination is carried out at 1050-1100° C. for 10-15 hours.

9. The method for preparing a rare earth magnetic single crystal material according to claim 4, characterized in that: The cooling rate is 1-1.5°C / h, and the predetermined temperature is 850-900°C; and / or the centrifugal speed is 1500-2000r / min, and the centrifugal time is 5-10min.

10. Use of the rare earth magnetic single crystal material according to any one of claims 1 to 3 in low-temperature quantum devices, magnetic sensors, and strongly correlated materials.

Citation Information

Patent Citations

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  • Growth method for rare earth-ferrite-boron permanent magnet single crystal using fluxing agent

    WO2024045470A1