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Effect of local chain stiffness on oligomer crystallization from a melt 局部链刚度对熔体低聚物结晶的影响
IF 3.4 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-23 DOI: 10.1103/physrevmaterials.8.075606
Pierre Kawak, Christopher Akiki, Douglas R. Tree
While the process by which a polymer crystal nucleates from the melt has been extensively studied via molecular simulation, differences in polymer models and simulated crystallization conditions have led to seemingly contradictory results. We make steps to resolve this controversy by computing low-temperature phase diagrams of oligomer melts using Wang-Landau Monte Carlo simulations. Two qualitatively different crystallization mechanisms are possible depending on the local bending stiffness potential. Polymers with a discrete bending potential crystallize via a single-step mechanism, whereas polymers with a continuous bending potential can crystallize via a two-step mechanism that includes an intermediate nematic phase. Other model differences can be quantitatively accounted for using an effective volume fraction and a temperature scaled by the bending stiffness. These results suggest that at least two universality classes of nucleation exist for melts and that local chain stiffness is a key determining factor in the mechanism of nucleation.
虽然通过分子模拟对聚合物晶体从熔体中成核的过程进行了广泛研究,但聚合物模型和模拟结晶条件的差异导致了看似矛盾的结果。我们利用 Wang-Landau 蒙特卡洛模拟计算了低聚物熔体的低温相图,从而解决了这一争议。根据局部弯曲刚度势的不同,可能存在两种性质不同的结晶机制。具有离散弯曲势的聚合物通过单步机制结晶,而具有连续弯曲势的聚合物可通过包括中间向列相的两步机制结晶。其他模型差异可使用有效体积分数和按弯曲刚度缩放的温度来定量解释。这些结果表明,熔体至少存在两种成核普遍性,而局部链刚度是成核机制的关键决定因素。
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引用次数: 0
Probing intrinsic magnetization dynamics of the Y3Fe5O12/Bi2Te3 interface at low temperature 低温下 Y3Fe5O12/Bi2Te3 界面的内在磁化动力学探测
IF 3.4 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-23 DOI: 10.1103/physrevmaterials.8.074409
A. R. Will-Cole, Valeria Lauter, Alexander Grutter, Carsten Dubs, David A. Lidsky, Morris Lindner, Timmy Reimann, Nirjhar Bhattacharjee, Tzu-Ming Lu, Peter Sharma, Nichole R. Valdez, Charles J. Pearce, Todd C. Monson, Matthew Matzelle, Arun Bansil, Don Heiman, Nian X. Sun
Topological insulator–magnetic insulator (TI–MI) heterostructures hold significant promise in the field of spintronics, offering the potential for manipulating magnetization through topological surface state–enabled spin-orbit torque. However, many TI–MI interfaces are plagued by issues such as contamination within the magnetic insulator layer and the presence of a low-density transitional region of the topological insulator. These interfacial challenges often obscure the intrinsic behavior of the TI–MI system. In this study, we addressed these challenges by depositing sputtered Bi2Te3 on liquid phase epitaxy grown Y3Fe5O12/Gd3Ga5O12. The liquid phase epitaxy grown Y3Fe5O12 has been previously shown to have exceptional interface quality, without an extended transient layer derived from interdiffusion processes of the substrate or impurity ions, thereby eliminating rare-earth impurity-related losses in the MI at low temperatures. At the TI–MI interface, high-resolution depth-sensitive polarized neutron reflectometry confirmed the absence of a low-density transitional growth region of the TI. By overcoming these undesirable interfacial effects, we isolate and probe the intrinsic low-temperature magnetization dynamics and transport properties of the TI–MI interface. Our findings revealed strong spin pumping at low temperatures, accompanied by an additional in-plane anisotropy. The enhanced spin pumping at low temperatures is correlated with the observed suppression of bulk conduction and the weak antilocalization in the TI film, highlighting the interplay between the transport and spin pumping behavior in the TI–MI system.
拓扑绝缘体-磁性绝缘体(TI-MI)异质结构在自旋电子学领域大有可为,它为通过拓扑表面态支持的自旋轨道力矩操纵磁化提供了潜力。然而,许多 TI-MI 界面都存在磁绝缘体层污染和拓扑绝缘体低密度过渡区等问题。这些界面难题往往会掩盖 TI-MI 系统的内在行为。在本研究中,我们通过在液相外延生长的 Y3Fe5O12/Gd3Ga5O12 上沉积溅射 Bi2Te3 来解决这些难题。液相外延生长的 Y3Fe5O12 此前已被证明具有优异的界面质量,没有因衬底或杂质离子的相互扩散过程而产生的扩展瞬态层,从而消除了低温下 MI 中与稀土杂质相关的损耗。在 TI-MI 界面上,高分辨率深度敏感偏振中子反射仪证实 TI 不存在低密度过渡生长区。通过克服这些不良的界面效应,我们分离并探测了 TI-MI 界面的内在低温磁化动力学和传输特性。我们的研究结果表明,低温下的自旋泵很强,并伴有额外的面内各向异性。低温下增强的自旋泵与在 TI 薄膜中观察到的体传导抑制和微弱的反聚焦相关,突出了 TI-MI 系统中传输和自旋泵行为之间的相互作用。
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引用次数: 0
Nodal line induced large transverse thermoelectric response in the D03-type Heusler compound Fe3Si D03 型 Heusler 化合物 Fe3Si 中节点线诱导的大横向热电响应
IF 3.4 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-23 DOI: 10.1103/physrevmaterials.8.075403
Susumu Minami, Sota Hogaki, Takahiro Shimada
Giant magnetic transverse thermoelectric effect, anomalous Nernst effect (ANE), was theoretically and experimentally observed in 3d-transition metal compounds. The intrinsic components of ANE can be described from the electronic structure based on the Berry phase concept. The topological electronic structure, such as the Weyl node and nodal lines, induces large Berry curvature, one origin of giant ANE. We investigated transverse thermoelectric properties on ferromagnetic D03-type Heusler compounds Fe3Si based on first-principles calculations. We found large transverse thermoelectric conductivity αxy5AK1m1 is realized with hole carrier doping at room temperature. We also clarified that the nodal line and its stationary point enhance transverse thermoelectric conductivity. These results give us a clue to design high-performance ANE-based magnetic thermoelectric materials.
在 3d 过渡金属化合物中从理论和实验上观测到了巨磁横向热电效应,即反常奈恩斯特效应(ANE)。ANE 的内在成分可以根据贝里相概念从电子结构中描述出来。拓扑电子结构,如韦尔节点和节点线,会诱发大贝里曲率,这是巨型 ANE 的起源之一。我们基于第一原理计算研究了铁磁性 D03 型 Heusler 化合物 Fe3Si 的横向热电特性。我们发现,在室温下掺杂空穴载流子时,可实现较大的横向热电导率 αxy∼5AK-1m-1。我们还阐明了节点线及其静止点可提高横向热电导率。这些结果为我们设计基于 ANE 的高性能磁性热电材料提供了线索。
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引用次数: 0
Possible Wigner states in CrI3 heterostructures with graphene: A tight-binding model perspective 带有石墨烯的 CrI3 异质结构中可能存在的维格纳态:紧束缚模型视角
IF 3.4 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-23 DOI: 10.1103/physrevmaterials.8.074007
Igor Rozhansky, Vladimir Fal'ko
In this study, we present an effective tight-binding model for an accurate description of the lowest energy quadruplet of a conduction band in a ferromagnetic CrX3 monolayer, tuned to the complementary ab initio density functional theory simulations. This model, based on a minimum number of chromium orbitals, captures a distinctively flat dispersion in those bands but requires taking into account hoppings beyond nearest neighbors, revealing ligand-mediated electron pathways connecting remote chromium sites. Doping of states in the lowest conduction band of CrX3 requires charge transfer, which, according to recent studies [Tenasini et al., Nano Lett. 22, 6760 (2022); Tseng et al., Nano Lett. 22, 8495 (2022); Cardoso et al., Phys. Rev. B 108, 184423 (2023)], can occur in graphene(G)/CrX3 heterostructures. Here, we use the detailed description of the lowest conduction band in CrI3 to show that G/CrI3/G and G/CrI3 are type-II heterostructures where light holes in graphene would coexist with heavy electrons in the magnetic layer, where the latter can be characterized by Wigner-Seitz radius rs2535 (as estimated for hBN-encapsulated structures).
在这项研究中,我们提出了一种有效的紧密结合模型,用于准确描述铁磁性 CrX3 单层中导带的最低能量四元组,并根据互补的 ab initio 密度泛函理论模拟进行了调整。该模型以最低数量的铬轨道为基础,捕捉到了这些带中明显平坦的色散,但需要考虑近邻之外的跳变,揭示了配体介导的连接偏远铬位点的电子路径。CrX3 最低导带中的掺杂态需要电荷转移,根据最近的研究[Tenasini 等人,Nano Lett.在这里,我们利用对 CrI3 最低导带的详细描述来说明 G/CrI3/G 和 G/CrI3 是 II 型异质结构,其中石墨烯中的轻空穴将与磁层中的重电子共存,后者可以用 Wigner-Seitz 半径 rs∼25-35 来描述(根据对 hBN 封装结构的估计)。
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引用次数: 0
Proximate Tomonaga-Luttinger liquid in a spin-1/2 ferromagnetic XXZ chain compound 自旋-1/2 铁磁 XXZ 链化合物中的近似友永-鲁丁格液体
IF 3.4 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-23 DOI: 10.1103/physrevmaterials.8.074410
Boqiang Li, Xun Chen, Yuqian Zhao, Zhaohua Ma, Zongtang Wan, Yuesheng Li
The spin-1/2 ferromagnetic XXZ chain is a prototypical many-body quantum model, exactly solvable via the integrable Bethe ansatz method, hosting a Tomonaga-Luttinger spin liquid. However, its clear experimental realizations remain absent. Here, we present a thorough investigation of the magnetism of the structurally disorder-free compound LuCu(OH)3SO4. By conducting magnetization and electron-spin-resonance measurements on the single-crystal sample, we establish that the title compound approximates the spin-1/2 ferromagnetic XXZ chain model with a nearest-neighbor exchange strength of J165K and an easy-plane anisotropy of 0.994. The specific heat demonstrates a distinctive power-law behavior at low magnetic fields (with energy scales 0.02J1) and low temperatures (T0.03J1). This behavior is consistent with the expectations of the ideal spin-1/2 ferromagnetic XXZ chain model, thereby supporting the formation of a gapless Tomonaga-Luttinger spin liquid in LuCu(OH)3SO4.
自旋-1/2 铁磁 XXZ 链是一个典型的多体量子模型,可通过可积分的贝特安萨特方法精确求解,其中寄存着一个 Tomonaga-Luttinger 自旋液体。然而,其明确的实验实现仍然缺失。在此,我们对结构无序的化合物 LuCu(OH)3SO4 的磁性进行了深入研究。通过对单晶样品进行磁化和电子自旋共振测量,我们确定了标题化合物近似于自旋-1/2 铁磁性 XXZ 链模型,其最近邻交换强度为 J1∼65K,易平面各向异性为 ∼0.994。在低磁场(能量尺度≤0.02J1)和低温(T≤0.03J1)条件下,比热表现出独特的幂律行为。这种行为与理想的自旋-1/2 铁磁 XXZ 链模型的预期一致,从而支持在 LuCu(OH)3SO4 中形成无间隙的 Tomonaga-Luttinger 自旋液体。
{"title":"Proximate Tomonaga-Luttinger liquid in a spin-1/2 ferromagnetic XXZ chain compound","authors":"Boqiang Li, Xun Chen, Yuqian Zhao, Zhaohua Ma, Zongtang Wan, Yuesheng Li","doi":"10.1103/physrevmaterials.8.074410","DOIUrl":"https://doi.org/10.1103/physrevmaterials.8.074410","url":null,"abstract":"The spin-<math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mn>1</mn><mo>/</mo><mn>2</mn></mrow></math> ferromagnetic XXZ chain is a prototypical many-body quantum model, exactly solvable via the integrable Bethe ansatz method, hosting a Tomonaga-Luttinger spin liquid. However, its clear experimental realizations remain absent. Here, we present a thorough investigation of the magnetism of the structurally disorder-free compound <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi>LuCu</mi><msub><mrow><mo>(</mo><mi>OH</mi><mo>)</mo></mrow><mn>3</mn></msub><msub><mi>SO</mi><mn>4</mn></msub></mrow></math>. By conducting magnetization and electron-spin-resonance measurements on the single-crystal sample, we establish that the title compound approximates the spin-<math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mn>1</mn><mo>/</mo><mn>2</mn></mrow></math> ferromagnetic XXZ chain model with a nearest-neighbor exchange strength of <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><msub><mi>J</mi><mn>1</mn></msub><mo>∼</mo><mn>65</mn><mspace width=\"0.16em\"></mspace><mi mathvariant=\"normal\">K</mi></mrow></math> and an easy-plane anisotropy of <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mo>∼</mo><mn>0.994</mn></mrow></math>. The specific heat demonstrates a distinctive power-law behavior at low magnetic fields (with energy scales <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mo>≤</mo><mn>0.02</mn><msub><mi>J</mi><mn>1</mn></msub></mrow></math>) and low temperatures <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mo>(</mo><mi>T</mi><mo>≤</mo><mn>0.03</mn><msub><mi>J</mi><mn>1</mn></msub><mo>)</mo></mrow></math>. This behavior is consistent with the expectations of the ideal spin-<math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mn>1</mn><mo>/</mo><mn>2</mn></mrow></math> ferromagnetic XXZ chain model, thereby supporting the formation of a gapless Tomonaga-Luttinger spin liquid in <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi>LuCu</mi><msub><mrow><mo>(</mo><mi>OH</mi><mo>)</mo></mrow><mn>3</mn></msub><msub><mi>SO</mi><mn>4</mn></msub></mrow></math>.","PeriodicalId":20545,"journal":{"name":"Physical Review Materials","volume":"65 1","pages":""},"PeriodicalIF":3.4,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141754127","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Probing the interface and individual layers in cuprate/manganite heterostructures by Raman spectroscopy 利用拉曼光谱探测铜绿石/锰矿异质结构中的界面和单个层
IF 3.4 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-22 DOI: 10.1103/physrevmaterials.8.074804
F. Lyzwa, A. Chan, K. Fürsich, B. Keimer, C. Faugeras, Yu. G. Pashkevich, C. Bernhard, M. Minola, B. P. P. Mallett
We report a comprehensive set of polarized Raman spectra on thin-film multilayers of the high-Tc superconductor YBa2Cu3O7 and electrically insulating manganites RMnO3 (R= rare-earth partially substituted with group-II elements) hosting magnetic, charge and orbital order (COO). Such multilayers have been shown to exhibit a unique insulating-to-superconducting transition that is induced by magnetic field, electric field, or by tailoring the chemical composition of the R site of the manganite. The Raman spectra show significant Jahn-Teller distortions of the manganite structure, which correlate with COO, approximately 90 K above the magnetic ordering temperature of 140 K. Based on the Raman data and earlier electrical transport studies of single-layer manganite films, we argue that the manganite layers in our heterostructures remain electrically insulating across the range of investigated temperatures, dopings, and magnetic fields. The Raman spectra show a pronounced redshift and broadening of lattice vibrations around 200 cm1 in the multilayers compared to those of manganite films, which may indicate hybridization with YBa2Cu3O7 phonons. We also observe additional excitations at 690 cm1 and 830 cm1 that are absent in the single films or bulk responses, which we discuss to originate from the cuprate/manganite interface. These observations demonstrate that the phonon spectrum is significantly modified in our multilayer samples. This is expected to play an important role in the mechanism of the insulating-to-superconducting transition found in these cuprate-manganite multilayers.
我们报告了一组关于高锝超导体 YBa2Cu3O7 和电绝缘锰矿 RMnO3(R=部分被第二族元素取代的稀土)薄膜多层的偏振拉曼光谱,这些薄膜多层具有磁序、电荷序和轨道序 (COO)。研究表明,磁场、电场或通过调整锰矿 R 位点的化学成分,可诱导这种多层膜发生从绝缘到超导的独特转变。拉曼光谱显示,锰酸盐结构发生了明显的贾恩-泰勒(Jahn-Teller)畸变,这与 COO 有关,比 140 K 的磁有序温度高出约 90 K。根据拉曼数据和早期对单层锰酸盐薄膜的电传输研究,我们认为,在所研究的温度、掺杂和磁场范围内,我们的异质结构中的锰酸盐层仍然是电绝缘的。拉曼光谱显示,与锰矿薄膜的拉曼光谱相比,多层膜中 200 cm-1 附近的晶格振动有明显的重移和拓宽,这可能表明与 YBa2Cu3O7 声子的杂化。我们还在 690 cm-1 和 830 cm-1 处观察到了单层薄膜或块体响应中所没有的额外激发,我们认为这些激发来自于杯状石/锰矿石界面。这些观察结果表明,声子谱在我们的多层样品中发生了显著变化。预计这将在这些铜锰酸盐多层膜的绝缘到超导转变机制中发挥重要作用。
{"title":"Probing the interface and individual layers in cuprate/manganite heterostructures by Raman spectroscopy","authors":"F. Lyzwa, A. Chan, K. Fürsich, B. Keimer, C. Faugeras, Yu. G. Pashkevich, C. Bernhard, M. Minola, B. P. P. Mallett","doi":"10.1103/physrevmaterials.8.074804","DOIUrl":"https://doi.org/10.1103/physrevmaterials.8.074804","url":null,"abstract":"We report a comprehensive set of polarized Raman spectra on thin-film multilayers of the high-<math xmlns=\"http://www.w3.org/1998/Math/MathML\"><msub><mi>T</mi><mi>c</mi></msub></math> superconductor <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><msub><mrow><mi>YBa</mi></mrow><mn>2</mn></msub><msub><mrow><mi>Cu</mi></mrow><mn>3</mn></msub><msub><mrow><mi mathvariant=\"normal\">O</mi></mrow><mn>7</mn></msub></math> and electrically insulating manganites <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi>R</mi><msub><mi>MnO</mi><mn>3</mn></msub></mrow></math> (<math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi>R</mi><mo>=</mo></mrow></math> rare-earth partially substituted with group-II elements) hosting magnetic, charge and orbital order (COO). Such multilayers have been shown to exhibit a unique insulating-to-superconducting transition that is induced by magnetic field, electric field, or by tailoring the chemical composition of the <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mi>R</mi></math> site of the manganite. The Raman spectra show significant Jahn-Teller distortions of the manganite structure, which correlate with COO, approximately 90 K above the magnetic ordering temperature of 140 K. Based on the Raman data and earlier electrical transport studies of single-layer manganite films, we argue that the manganite layers in our heterostructures remain electrically insulating across the range of investigated temperatures, dopings, and magnetic fields. The Raman spectra show a pronounced redshift and broadening of lattice vibrations around 200 <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><msup><mrow><mi>cm</mi></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msup></math> in the multilayers compared to those of manganite films, which may indicate hybridization with <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><msub><mrow><mi>YBa</mi></mrow><mn>2</mn></msub><msub><mrow><mi>Cu</mi></mrow><mn>3</mn></msub><msub><mrow><mi mathvariant=\"normal\">O</mi></mrow><mn>7</mn></msub></math> phonons. We also observe additional excitations at 690 <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><msup><mrow><mi>cm</mi></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msup></math> and 830 <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><msup><mrow><mi>cm</mi></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msup></math> that are absent in the single films or bulk responses, which we discuss to originate from the cuprate/manganite interface. These observations demonstrate that the phonon spectrum is significantly modified in our multilayer samples. This is expected to play an important role in the mechanism of the insulating-to-superconducting transition found in these cuprate-manganite multilayers.","PeriodicalId":20545,"journal":{"name":"Physical Review Materials","volume":"39 1","pages":""},"PeriodicalIF":3.4,"publicationDate":"2024-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141743325","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tetragonal phases in Fe-Ga alloys: A quantitative study 铁-镓合金中的四方相:定量研究
IF 3.4 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-22 DOI: 10.1103/physrevmaterials.8.073604
A. M. Balagurov, I. A. Bobrikov, D. Yu. Chernyshov, A. S. Sohatsky, S. V. Sumnikov, B. Yerzhanov, I. S. Golovin
Currently, the dominant model for the formation of enhanced magnetostriction of Fe-Ga alloys is based on the assumption of the presence of microscopic inclusions with a tetragonal L60 structure in the cubic matrix of the alloy. However, no evidence for the presence of this phase in the bulk of the alloys in amounts sufficient to have a noticeable effect on the magnitude of magnetostriction has been obtained so far. To test this hypothesis, a detailed scanning of the reciprocal space of Fe81Ga19Tb0.1 and Fe73Ga27 single crystals was carried out at ESRF at high photon flux stations. In particular, it was possible to reliably record superstructure diffraction peaks, the intensity of which was at a level of 2×106 from the intensity of the fundamental peaks. Nevertheless, neither the presence of superstructure diffraction peaks obviously belonging to the L60 phase nor the tetragonal splitting of the fundamental diffraction peaks into components, which could indicate the presence of this phase in the samples, was detected. Similar results were obtained using complementary methods (electron and neutron diffraction). Based on the performed analysis of the background level in the places of the expected positions of superstructure peaks of the L60 phase, it was found that the volume fraction of this phase in the Fe81Ga19Tb0.1 alloy cannot exceed 0.2 %. The presence of a previously discovered X phase with hexagonal or orthorhombic symmetry in a crystal with 27 at. % Ga was confirmed.
目前,Fe-Ga 合金磁致伸缩增强形成的主要模型是基于合金立方基体中存在具有四方 L60 结构的微观夹杂物这一假设。然而,迄今为止还没有证据表明在合金块体中存在这种相,其数量足以对磁致伸缩的大小产生明显的影响。为了验证这一假设,我们在 ESRF 的高光子通量站对 Fe81Ga19Tb0.1 和 Fe73Ga27 单晶的倒易空间进行了详细扫描。特别是可以可靠地记录到超结构衍射峰,其强度与基本峰的强度相差 2×10-6。不过,既没有检测到明显属于 L60 相的超结构衍射峰,也没有检测到基本衍射峰的四方分裂成分,而这可能表明样品中存在该相。使用补充方法(电子衍射和中子衍射)也得到了类似的结果。根据对 L60 相上结构峰预期位置的背景水平进行的分析,发现该相在 Fe81Ga19Tb0.1 合金中的体积分数不能超过 0.2%。之前发现的具有六方或正方对称性的 X 相在含 27 at.%镓的晶体中存在六方或正方对称的 X 相。
{"title":"Tetragonal phases in Fe-Ga alloys: A quantitative study","authors":"A. M. Balagurov, I. A. Bobrikov, D. Yu. Chernyshov, A. S. Sohatsky, S. V. Sumnikov, B. Yerzhanov, I. S. Golovin","doi":"10.1103/physrevmaterials.8.073604","DOIUrl":"https://doi.org/10.1103/physrevmaterials.8.073604","url":null,"abstract":"Currently, the dominant model for the formation of enhanced magnetostriction of Fe-Ga alloys is based on the assumption of the presence of microscopic inclusions with a tetragonal <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi>L</mi><msub><mn>6</mn><mn>0</mn></msub></mrow></math> structure in the cubic matrix of the alloy. However, no evidence for the presence of this phase in the bulk of the alloys in amounts sufficient to have a noticeable effect on the magnitude of magnetostriction has been obtained so far. To test this hypothesis, a detailed scanning of the reciprocal space of <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi mathvariant=\"normal\">F</mi><msub><mi mathvariant=\"normal\">e</mi><mn>81</mn></msub><mi mathvariant=\"normal\">G</mi><msub><mi mathvariant=\"normal\">a</mi><mn>19</mn></msub><mi mathvariant=\"normal\">T</mi><msub><mi mathvariant=\"normal\">b</mi><mrow><mn>0.1</mn></mrow></msub></mrow></math> and <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><msub><mi>Fe</mi><mn>73</mn></msub><msub><mi>Ga</mi><mn>27</mn></msub></mrow></math> single crystals was carried out at ESRF at high photon flux stations. In particular, it was possible to reliably record superstructure diffraction peaks, the intensity of which was at a level of <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mn>2</mn><mo>×</mo><msup><mrow><mn>10</mn></mrow><mrow><mo>−</mo><mn>6</mn></mrow></msup></mrow></math> from the intensity of the fundamental peaks. Nevertheless, neither the presence of superstructure diffraction peaks obviously belonging to the <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi>L</mi><msub><mn>6</mn><mn>0</mn></msub></mrow></math> phase nor the tetragonal splitting of the fundamental diffraction peaks into components, which could indicate the presence of this phase in the samples, was detected. Similar results were obtained using complementary methods (electron and neutron diffraction). Based on the performed analysis of the background level in the places of the expected positions of superstructure peaks of the <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi>L</mi><msub><mn>6</mn><mn>0</mn></msub></mrow></math> phase, it was found that the volume fraction of this phase in the <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi mathvariant=\"normal\">F</mi><msub><mi mathvariant=\"normal\">e</mi><mn>81</mn></msub><mi mathvariant=\"normal\">G</mi><msub><mi mathvariant=\"normal\">a</mi><mn>19</mn></msub><mi mathvariant=\"normal\">T</mi><msub><mi mathvariant=\"normal\">b</mi><mrow><mn>0.1</mn></mrow></msub></mrow></math> alloy cannot exceed 0.2 %. The presence of a previously discovered <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mi>X</mi></math> phase with hexagonal or orthorhombic symmetry in a crystal with 27 at. % Ga was confirmed.","PeriodicalId":20545,"journal":{"name":"Physical Review Materials","volume":"7 1","pages":""},"PeriodicalIF":3.4,"publicationDate":"2024-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141743108","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tuning the electronic and magnetic states of Ca2RuO4 with proton evolution 用质子演化调节 Ca2RuO4 的电子和磁态
IF 3.4 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-22 DOI: 10.1103/physrevmaterials.8.074408
Di Tian, Ludi Miao, Liang Si, Nathaniel J. Schreiber, Shengchun Shen, Jianbing Zhang, Xinyu Shu, Xiaochao Wang, Hari P. Nair, Jacob P. Ruf, Darrell G. Schlom, Kyle M. Shen, Pu Yu
With strong correlations between lattice, spin, and charge degrees of freedom, the layered ruthenate Ca2RuO4 has attracted considerable interest over the past few decades due to its metal-insulator transition, antiferromagnetic-to-ferromagnetic transition, metamagnetic transition, and orbital ordering. Much effort has been devoted to manipulating its crystalline structure through epitaxial strain, chemical substitution, and pressure to clarify the underlying many-body physics and related quantum critical phenomena. Here we report a comprehensive proton intercalation study of Ca2RuO4 thin films and investigate their magneto-transport properties arising from structural deformations and carrier doping. It reveals a rich phase diagram with distinct electronic and magnetic ground states. Specifically, with increasing gate voltage during ionic liquid gating, the film first evolves from an insulating state into a metallic state and then gradually turns towards an exotic Mott insulator. Furthermore, we observed an emergent metamagnetic transition from a canted antiferromagnetic to a nearly ferromagnetic state, a characteristic feature conventionally triggered by external magnetic field, but here with electron doping. Our first-principles calculations reveal that these unexpected features could be attributed to the proton evolution-induced synergistic structural distortion and electron doping during ionic liquid gating. Our findings highlight the important role of both lattice and charge degrees of freedom in the intriguing electronic states of Ca2RuO4 and provide an effective approach to uncover different properties in quantum materials.
层状钌酸盐 Ca2RuO4 具有晶格、自旋和电荷自由度之间的强相关性,由于其金属-绝缘体转变、反铁磁-铁磁转变、元磁转变和轨道有序性,在过去几十年中引起了人们的极大兴趣。人们一直致力于通过外延应变、化学置换和压力来操纵其晶体结构,以阐明其潜在的多体物理学和相关的量子临界现象。在此,我们报告了对 Ca2RuO4 薄膜的质子插层综合研究,并探讨了其因结构变形和载流子掺杂而产生的磁传输特性。研究揭示了具有不同电子和磁基态的丰富相图。具体来说,在离子液体浇注过程中,随着栅极电压的增加,薄膜首先从绝缘态演变为金属态,然后逐渐转向奇异的莫特绝缘体。此外,我们还观察到了从斜向反铁磁态到近铁磁态的新兴元磁性转变,这种特征通常由外部磁场触发,但在这里是由电子掺杂触发的。我们的第一原理计算显示,这些意想不到的特征可归因于离子液体浇注过程中质子演化引起的协同结构畸变和电子掺杂。我们的研究结果凸显了晶格和电荷自由度在 Ca2RuO4 奇妙的电子状态中的重要作用,并为揭示量子材料的不同性质提供了一种有效的方法。
{"title":"Tuning the electronic and magnetic states of Ca2RuO4 with proton evolution","authors":"Di Tian, Ludi Miao, Liang Si, Nathaniel J. Schreiber, Shengchun Shen, Jianbing Zhang, Xinyu Shu, Xiaochao Wang, Hari P. Nair, Jacob P. Ruf, Darrell G. Schlom, Kyle M. Shen, Pu Yu","doi":"10.1103/physrevmaterials.8.074408","DOIUrl":"https://doi.org/10.1103/physrevmaterials.8.074408","url":null,"abstract":"With strong correlations between lattice, spin, and charge degrees of freedom, the layered ruthenate <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi mathvariant=\"normal\">C</mi><msub><mi mathvariant=\"normal\">a</mi><mn>2</mn></msub><mi>Ru</mi><msub><mi mathvariant=\"normal\">O</mi><mn>4</mn></msub></mrow></math> has attracted considerable interest over the past few decades due to its metal-insulator transition, antiferromagnetic-to-ferromagnetic transition, metamagnetic transition, and orbital ordering. Much effort has been devoted to manipulating its crystalline structure through epitaxial strain, chemical substitution, and pressure to clarify the underlying many-body physics and related quantum critical phenomena. Here we report a comprehensive proton intercalation study of <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi mathvariant=\"normal\">C</mi><msub><mi mathvariant=\"normal\">a</mi><mn>2</mn></msub><mi>Ru</mi><msub><mi mathvariant=\"normal\">O</mi><mn>4</mn></msub></mrow></math> thin films and investigate their magneto-transport properties arising from structural deformations and carrier doping. It reveals a rich phase diagram with distinct electronic and magnetic ground states. Specifically, with increasing gate voltage during ionic liquid gating, the film first evolves from an insulating state into a metallic state and then gradually turns towards an exotic Mott insulator. Furthermore, we observed an emergent metamagnetic transition from a canted antiferromagnetic to a nearly ferromagnetic state, a characteristic feature conventionally triggered by external magnetic field, but here with electron doping. Our first-principles calculations reveal that these unexpected features could be attributed to the proton evolution-induced synergistic structural distortion and electron doping during ionic liquid gating. Our findings highlight the important role of both lattice and charge degrees of freedom in the intriguing electronic states of <math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow><mi mathvariant=\"normal\">C</mi><msub><mi mathvariant=\"normal\">a</mi><mn>2</mn></msub><mi>Ru</mi><msub><mi mathvariant=\"normal\">O</mi><mn>4</mn></msub></mrow></math> and provide an effective approach to uncover different properties in quantum materials.","PeriodicalId":20545,"journal":{"name":"Physical Review Materials","volume":"57 1","pages":""},"PeriodicalIF":3.4,"publicationDate":"2024-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141743222","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Optical properties of metallic MXene multilayers through advanced first-principles calculations 通过先进的第一原理计算研究金属 MXene 多层膜的光学特性
IF 3.4 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-22 DOI: 10.1103/physrevmaterials.8.075201
Zafer Kandemir, Pino D'Amico, Giacomo Sesti, Claudia Cardoso, Milorad V. Milošević, Cem Sevik
Having a strong electromagnetic absorption, MXene multilayers are readily envisaged for applications in electromagnetic shields and related prospective technology. However, an ab initio characterization of the optical properties of MXenes is still lacking, due in part to major difficulties with the treatment of metallicity in the first-principles approaches. Here we addressed the latter challenge, after a careful treatment of intraband transitions, to present a thorough analysis of the electronic and optical properties of a selected set of metallic MXene layers based on density functional theory (DFT) and many-body perturbation theory calculations. Our results reveal that the GW corrections are particularly important in regions of the band structure where d and p states hybridize. For some systems, we show that GW corrections open a gap between occupied states, resulting in a band structure that closely resembles that of an intrinsic transparent conductor, thereby opening an additional line of prospective applications for the MXenes family. Nevertheless, GW and Bethe-Salpeter corrections have a minimal influence on the absorption spectra, in contrast to what is typically observed in semiconductor layers. Our present results suggest that calculations within the independent particle approximation (IPA) calculations are sufficiently accurate for assessing the optical characteristics of bulk-layered MXene materials. Finally, our calculated dielectric properties and absorption spectra, in agreement with existing experimental data, confirm the potential of MXenes as effective infrared emitters.
MXene 多层板具有很强的电磁吸收能力,因此很容易被设想应用于电磁屏蔽和相关的前瞻性技术中。然而,由于第一性原理方法在处理金属性方面存在重大困难,因此目前仍缺乏对 MXene 光学特性的自证表征。在此,我们在仔细处理带内跃迁之后,根据密度泛函理论(DFT)和多体扰动理论计算,对选定的一组金属 MXene 层的电子和光学特性进行了全面分析,从而解决了后一个难题。我们的研究结果表明,GW 修正在带状结构中 d 和 p 态杂化的区域尤为重要。对于某些系统,我们发现 GW 修正在占据态之间打开了一个缺口,导致带状结构与本征透明导体的带状结构非常相似,从而为 MXenes 家族开辟了一条新的应用前景。尽管如此,GW 和 Bethe-Salpeter 修正对吸收光谱的影响微乎其微,这与半导体层中通常观察到的情况截然不同。我们目前的研究结果表明,独立粒子近似(IPA)计算的精确度足以评估体层 MXene 材料的光学特性。最后,我们计算出的介电性能和吸收光谱与现有的实验数据一致,证实了二氧化二烯作为有效红外发射器的潜力。
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引用次数: 0
Multi-mem behavior at reduced voltages in La1/2Sr1/2Mn1/2Co1/2O3−x perovskite modified with Sm:CeO2 用 Sm:CeO2 修饰的 La1/2Sr1/2Mn1/2Co1/2O3-x 包晶在降低电压时的多存储器行为
IF 3.4 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-22 DOI: 10.1103/physrevmaterials.8.075003
Wilson Román Acevedo, Myriam H. Aguirre, Beatriz Noheda, Diego Rubi
The use of machine learning algorithms is exponentially growing and concerns are being raised about their sustainability. Neuromorphic computing aims to mimic the architecture and the information processing mechanisms of the mammalian brain, appearing as the only avenue that offers significant energy savings compared to the standard digital computers. Memcapacitive devices, which can change their capacitance between different nonvolatile states upon the application of electrical stimulation, can significantly reduce the energy consumption of bio-inspired circuitry. In the present work, we study the multi-mem (memristive and memcapacitive) behavior of devices based on thin films of the topotactic redox La1/2Sr1/2Mn1/2Co1/2O3x (LSMCO) perovskite modified with Sm:CeO2 (SCO), grown on Nb:SrTiO3 with (001) and (110) out-of-plane orientations. Either the self-assembling at the nanoscale of both LSMCO and SCO phases or the doping with Ce(Sm) of the LSMCO perovskite were observed for different fabrication conditions and out-of-plane orientations. The impact of these changes on the device electrical behavior was determined. The optimum devices resulted those with (110) orientation and Ce(Sm) doping the perovskite. These devices displayed a multi-mem behavior with robust memcapacitance and significantly lower operation voltages (especially the reset voltage) in comparison with devices based on pristine LSMCO. In addition, they were able to endure electrical cycling—and the concomitant perovskite topotactic redox transition between oxidized and reduced phases—without suffering nanostructural changes nor cationic segregation. We link these properties to an enhanced perovskite reducibility upon Ce(Sm) doping. Our work contributes to increasing the reliability of LSMCO-based multi-mem systems and to reducing their operating voltages closer to the 1 V threshold, which are key issues for the development of nanodevices for neuromorphic or in-memory computing.
机器学习算法的使用呈指数级增长,人们开始关注其可持续性。神经形态计算旨在模仿哺乳动物大脑的架构和信息处理机制,与标准数字计算机相比,它似乎是唯一能显著节约能源的途径。Memcapacitive 器件在施加电刺激时可在不同的非易失性状态之间改变电容,可显著降低生物启发电路的能耗。在本研究中,我们研究了基于用 Sm:CeO2 (SCO) 修饰的拓扑活性氧化还原 La1/2Sr1/2Mn1/2Co1/2O3-x (LSMCO) 包晶石薄膜的器件的多存储器(memristive 和 memcapacitive)行为,该薄膜生长在具有 (001) 和 (110) 面外取向的 Nb:SrTiO3 上。在不同的制造条件和面外取向下,观察到了 LSMCO 和 SCO 相在纳米尺度上的自组装,或 LSMCO 包晶体中的 Ce(Sm)掺杂。确定了这些变化对器件电气行为的影响。最佳器件是那些具有 (110) 方向和掺杂了 Ce(Sm) 的过氧化物。与基于原始 LSMCO 的器件相比,这些器件显示出具有强大记忆电容和显著较低工作电压(尤其是复位电压)的多记忆行为。此外,这些器件还能承受电循环以及氧化相和还原相之间的包晶拓扑氧化还原转变,而不会发生纳米结构变化或阳离子偏析。我们将这些特性与掺杂 Ce(Sm)后增强的包晶还原性联系起来。我们的工作有助于提高基于 LSMCO 的多内存系统的可靠性,并将其工作电压降至接近 1 V 的阈值,这是开发用于神经形态或内存计算的纳米器件的关键问题。
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Physical Review Materials
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