Kagome金属化合物CsV3Sb5和CsTi3Bi5的物性调控和电子结构研究

凝聚态物理学中，晶体的物理性质与其结构密切相关。其中kagome晶格由于独特的晶体结构，成为研究几何阻挫、电子关联、能带拓扑等性质的理想平台。由V构成kagome晶格的AV₃Sb₅（A = K, Rb, Cs）家族为近年来实验上发现的代表性kagome材料。AV₃Sb₅由于78 K - 103 K的电荷密度波和0.75 K - 2.5 K的超导态共存而引发了研究者们的极大兴趣，同时还存在条纹序、电子向列相和配对密度波等有序态，表现出极其丰富的物理内涵。在这些有序态中，电荷密度波出现的温度最高，研究电荷密度波的相关机理对于全面理解AV3Sb5家族有着重要意义，通过多种手段调控电荷密度波和超导态也有助于我们揭开这些新奇物态间的有趣关联。

在本论文中，我们通过不同类型的化学掺杂对CsV₃Sb₅中的电荷密度波、超导态和能带结构进行调控。Ti替换V的空穴掺杂会导致费米能级下降，逐渐抑制CsV₃Sb₅中的电荷密度波，而Cr替换V的电子掺杂会引入磁性杂质，并迅速抑制超导态，由此我们展开对电荷密度波和超导态相关问题的研究。此外，还合成了一种新型kagome“135”材料CsTi₃Bi₅，并详细研究了相关的物性和能带结构，展现出kagome“135”材料丰富的物理性质。

本论文取得的具体研究成果如下：

一、通过Ti的空穴掺杂对CsV₃Sb₅中的电荷密度波、超导态和能带结构进行调控，研究了电荷密度波的形成机理等问题。对Cs(V_1-xTi_x)₃Sb₅的物性测试发现随着掺杂浓度的增加，电荷密度波逐渐被抑制，而超导态被加强，表现出电荷密度波和超导态之间的竞争关系。结合ARPES测试和第一性原理计算，发现空穴掺杂导致能带结构向上移动，当M点范霍夫奇点被抬高至费米面以上时，Cs(V_1-xTi_x)₃Sb₅中的电荷密度波消失，这些结果揭示了范霍夫奇点在CsV₃Sb₅的电荷密度波中不可或缺的作用。理论计算不同掺杂浓度的声子谱表明声子谱虚频随着空穴掺杂逐渐减弱，当声子谱虚频消失时，对应着系统中电荷密度波的消失，表明声子谱虚频对应的晶格不稳定性同样起着重要作用。此外，我们发现在无电荷密度波样品中，T_C和Sb衍生的电子口袋有效质量变化规律符合良好，表明超导态与Sb衍生能带有关。

二、通过Cr的磁性掺杂抑制CsV₃Sb₅中的超导态，研究了常压下和高压下磁性掺杂系统Cs(V_1-xCr_x)₃Sb₅中超导态的演化。对Cs(V_1-xCr_x)₃Sb₅的磁化率测试和低温下居里外斯拟合证明Cr掺杂引入了局域磁矩，是一种有效的磁性掺杂方法。物性测试发现超导态被磁性杂质迅速抑制，而电荷密度波则相对受影响较小。能带结构的研究也证明Cr掺杂为电子掺杂，随着掺杂浓度的增加能带结构逐渐往下移动。特别的，我们对x = 3.1%和x = 5.3%样品进行加压电输运测试，发现了x = 3.1%在0.99 GPa下电荷密度波的异常增强。随着压力的进一步增加，两个样品中均出现超导转变，类似于CsV₃Sb₅在高压下出现的第二个超导“穹顶”，且对于掺杂浓度更高的样品，超导态在更低的温度和更高的压强出现。理论计算发现压力会抑制Cr离子的局域磁矩，当局域磁矩逐渐被压力抑制时，超导态重新出现，且局域磁矩越小时T_C越高。CsV₃Sb₅中超导态对磁性的敏感性暗示着系统中可能存在s波超导。

三、合成了新型kagome“135”材料CsTi₃Bi₅，并详细研究了其物性和电子结构。我们通过Bi的助熔剂法成功合成了与CsV₃Sb₅同构的新型kagome“135”材料CsTi₃Bi₅，并对其晶体结构进行了详细表征。物性测试表明CsTi₃Bi₅的基态为费米液体态，ARPES测试和第一性原理计算则揭示了CsTi₃Bi₅中靠近费米面的平带以及Z₂拓扑性。此外，对CsTi₃Bi₅在高压下的结构研究发现在P = 3.3 GPa附近存在六方到单斜的结构相变。这些结果表明了kagome“135”材料实现丰富物理现象的潜力，也为后续探索更多可能的新型kagome“135”材料提供了参考。

In condensed matter physics, the physical properties of crystals are closely related to their crystal structures. The kagome lattice has emerged as an ideal platform for studying properties such as geometric frustration, electronic correlation, and band topology, owing to its unique crystal structure.

The AV₃Sb₅ (A = K, Rb, Cs) family, composed of kagome lattices with V ions, represents a prominent class of kagome materials discovered experimentally in recent years. The coexistence of charge density waves at 78 K - 103 K and superconducting states at 0.75 K - 2.5 K in AV₃Sb₅ has sparked significant interest among researchers. Additionally, there are other ordered states such as stripe orders, electronic nematic phases, and pairing density waves, exhibiting rich physical implications. Among these ordered states, the charge density wave has the highest appearance temperature. Understanding the mechanisms behind charge density waves is crucial for a comprehensive understanding of the AV₃Sb₅ family. Furthermore, controlling charge density waves and superconducting states through various means helps uncover intriguing correlations among these novel phenomena.

In this paper, we regulated the charge density waves, superconducting states, and band structures in CsV₃Sb₅ through different types of chemical doping. Hole doping by Ti substitution for V results in a lowering of the Fermi level and suppression of charge density waves in CsV₃Sb₅, whereas electron doping by Cr substitution for V introduces magnetic impurities and rapidly suppresses the superconducting state in CsV₃Sb₅. Thus, we delve into the investigation of issues related to charge density waves and superconducting states. Furthermore, we reported a novel kagome “135” material CsTi₃Bi₅, and its associated physical properties and band structure, demonstrating the abundant potential of kagome “135” materials.

Our research achievements are as follows:

1. By modulating the charge density wave, superconducting state, and band structure in CsV₃Sb₅ through Ti hole doping, we conducted research and discussion on the formation mechanism of charge density waves and related issues. Physical properties measurements on Cs(V_1-xTi_x)V₃Sb₅ reveal that with the increase of doping concentration, the charge density wave is gradually suppressed, while the superconducting state is enhanced, showing a competitive relationship between charge density wave and superconducting state. Band structure studies based on ARPES measurements and first-principles calculations unveil that hole doping induces an upward shift in the band structure. When the van Hove singularities at M-point are raised above the Fermi surface due to hole doping, the charge density wave in Cs(V_1-xTi_x)V₃Sb₅ disappears. Our results demonstrate the important role of van Hove singularities in the charge density wave of CsV₃Sb₅. Theoretical calculations of the phonon spectra at different doping concentrations show that the imaginary phonon frequency decreases gradually with hole doping, and the disappearance of imaginary phonon frequency corresponded to the disappearance of charge density wave in the system. Therefore, we propose that the electron instability associated with the van Hove singularities and the lattice instability associated with the imaginary phonon frequency jointly cause the charge density wave in CsV₃Sb₅. Additionally, in samples without charge density waves, we notice a consistent variation pattern in the effective mass of the electronic pocket derived from the Sb orbitals, which parallels that of T_C. This observation implies a possible correlation between the superconducting state and the electronic band originating from the Sb orbitals. It also suggests that the CsV₃Sb₅ system could potentially exhibit s-wave superconductivity.

2. Suppressing the superconducting state in CsV₃Sb₅ through magnetic doping of Cr, we studied the evolution of the superconducting state in Cs(V_1-xCr_x)V₃Sb₅ magnetic doping systems under both ambient and high pressures. Magnetization measurements and low-temperature Curie-Weiss fitting on Cs(V_1-xCr_x)V₃Sb₅ demonstrate that Cr doping introduces local magnetic moments, serving as an effective method for magnetic doping. We find that the superconducting state is rapidly suppressed by magnetic impurities, while charge density waves are relatively less affected. Band structure studies also demonstrate that Cr doping acts as electron doping, with the band structure gradually shifting downwards with increasing doping concentration. In particular, we performed resistivity measurements under various pressures on samples with x = 3.1% and x = 5.3%, and found an anomalous enhancement of charge density wave for x = 3.1% under 0.99 GPa. With further increase in pressure, superconducting transitions occur in both samples, resembling the second superconducting dome observed in CsV₃Sb₅ under pressure, and for samples with higher doping concentration, the superconducting state appears at lower temperatures and higher pressures.Theoretical calculations reveal that pressure suppresses the localized magnetic moments of Cr ions. As the localized magnetic moments are gradually suppressed by pressure, the superconducting state reemerges, and the higher the localized magnetic moment, the higher the critical temperature T_C. The sensitivity of the superconducting state in CsV₃Sb₅ to magnetism suggests the possible presence of an s-wave superconductivity in the system.

3. We synthesized a novel kagome “135” material CsTi₃Bi₅ and thoroughly investigated its physical properties and electronic structure.Using Bi as a flux, the novel kagome “135” material CsTi₃Bi₅, isostructural to CsV₃Sb₅, was successfully synthesized. We characterized its crystal structure and crystallographic information in detail, and through physical properties measurements, we find that the ground state of CsTi₃Bi₅ is Fermi liquid state. ARPES measurements and first-principles calculations reveal flat bands near the Fermi surface and Z2 topological properties in CsTi₃Bi₅. Furthermore, we investigated the structure and transport properties of CsTi₃Bi₅ under high pressure, discovering a structural phase transition from hexagonal to monoclinic around P = 3.3 GPa. These findings underscore the potential of kagome “135” materials to exhibit diverse physical phenomena and provide valuable insights for exploring additional novel kagome “135” materials in the future.

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