Abstract The class ofAV3Sb5(A=K, Rb, Cs) kagome metals hosts unconventional charge density wave states seemingly intertwined with their low temperature superconducting phases. The nature of the coupling between these two states and the potential presence of nearby, competing charge instabilities however remain open questions. This phenomenology is strikingly highlighted by the formation of two ‘domes’ in the superconducting transition temperature upon hole-doping CsV3Sb5. Here we track the evolution of charge correlations upon the suppression of long-range charge density wave order in the first dome and into the second of the hole-doped kagome superconductor CsV3Sb5−xSnx. Initially, hole-doping drives interlayer charge correlations to become short-ranged with their periodicity diminished along the interlayer direction. Beyond the peak of the first superconducting dome, the parent charge density wave state vanishes and incommensurate, quasi-1D charge correlations are stabilized in its place. These competing, unidirectional charge correlations demonstrate an inherent electronic rotational symmetry breaking in CsV3Sb5, and reveal a complex landscape of charge correlations within its electronic phase diagram. Our data suggest an inherent 2kfcharge instability and competing charge orders in theAV3Sb5class of kagome superconductors.
more »
« less
Electron hole asymmetry in the phase diagram of carrier-tuned CsV3Sb5
In this work, we study the effect of electron doping on the kagome superconductor CsV3Sb5. Single crystals and powders of CsV3Sb5−xTexare synthesized and characterized via magnetic susceptibility, nuclear quadrupole resonance, and x-ray diffraction measurements, where we observe a slight suppression of the charge density wave transition temperature and superconducting temperature with the introduction of electron dopants. In contrast to hole doping, both transitions survive relatively unperturbed up to the solubility limit of Te within the lattice. A comparison is presented between the electronic phase diagrams of electron- and hole-tuned CsV3Sb5.
more »
« less
- Award ID(s):
- 1905532
- PAR ID:
- 10539687
- Publisher / Repository:
- Frontiers
- Date Published:
- Journal Name:
- Frontiers in Electronic Materials
- Volume:
- 3
- ISSN:
- 2673-9895
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Kagome metals have emerged as a frontier in condensed matter physics due to their potential to host exotic quantum states. Among these, CsV3Sb5has attracted significant attention for the unusual coexistence of charge density wave (CDW) order and unconventional superconductivity, presenting an ideal system for exploring the emergent phenomena from the interplay of phonons, electronic fluctuations, and topological effects. The nature of CDW formation in CsV3Sb5is unconventional and has sparked considerable debate. In this study, we examine the origin of the CDW state via ab initio finite-temperature simulations of the lattice dynamics. Through a comparative study of CsV3Sb5and 2H-NbSe2, we demonstrate that the experimental absence of phonon softening—a hallmark of conventional CDW transition—in CsV3Sb5along with the presence of a weakly first-order transition, can be attributed to quantum zero-point atomic motion. This zero-point motion smears the free energy landscape of CDW, effectively stabilizing the pristine structure even below the CDW transition temperature. We argue that this surprising behavior could cause coexistence of pristine and CDW structures across the transition and lead to a weak first-order transition. Our predicted lattice dynamical behavior is supported by coherent phonon spectroscopy in single-crystalline CsV3Sb5. Our results provide crucial insights into the formation mechanism of CDW materials that exhibit little to no phonon softening, including cuprates, and highlight the surprising role of quantum effects in emergent properties of relatively heavy-element materials like CsV3Sb5.more » « less
-
Recent, and somewhat surprising, successful n-type doping of Mg 3 Sb 2 was the key to realizing high thermoelectric performance in this material. Herein, we use first-principles defect calculations to investigate different extrinsic n-type doping strategies for Mg 3 Sb 2 and to reveal general chemical trends in terms of dopant solubilities and maximal achievable electron concentrations. In agreement with experiments, we find that Sb substitution is an effective doping strategy, with Se and Te doping predicted to yield up to ∼8 × 10 19 cm −3 electrons. However, we also find that Mg substitution with trivalent (or higher) cations can be even more effective; in particular, the predicted highest achievable electron concentration (∼5 × 10 20 cm −3 ) with La as an extrinsic dopant exceeds that of Se and Te doping. Interstitial doping (Li, Zn, Cu, Be) is found to be largely ineffective either due to self-compensation (Li) or high formation energy (Zn, Cu, Be). Our results offer La as an alternative dopant to Te and Se and reinforce the need for careful phase boundary mapping in achieving high electron concentrations in Mg 3 Sb 2 .more » « less
-
Abstract We report a theoretical investigation of effects of Mn and Co substitution in the transition metal sites of the kagomé-lattice ferromagnet, Fe3Sn2. Herein, hole- and electron-doping effects of Fe3Sn2have been studied by density-functional theory calculations on the parent phase and on the substituted structural models of Fe3−xMxSn2(M = Mn, Co;x= 0.5, 1.0). All optimized structures favor the ferromagnetic ground state. Analysis of the electronic density of states (DOS) and band structure plots reveals that the hole (electron) doping leads to a progressive decrease (increase) in the magnetic moment per Fe atom and per unit cell overall. The high DOS is retained nearby the Fermi level in the case of both Mn and Co substitutions. The electron doping with Co results in the loss of nodal band degeneracies, while in the case of hole doping with Mn emergent nodal band degeneracies and flatbands initially are suppressed in Fe2.5Mn0.5Sn2but re-emerge in Fe2MnSn2. These results provide key insights into potential modifications of intriguing coupling between electronic and spin degrees of freedom observed in Fe3Sn2.more » « less
-
Abstract The discovery of a semiconducting ground stateXyYZ(y= 0.8 or 0.75) in nominally 19‐electron half‐Heusler materials warrants a closer look at their apparently metallic properties that often make them good thermoelectric (TE) materials. By systematically investigating the temperature dependence of off‐stoichiometry (x) in V0.8+xCoSb, Nb0.8+xCoSb, and Ti0.75+xNiSb it is found thatxinvariably increases with increasing temperature, leading to an n‐type self‐doping behavior. In addition, there is also a large phase width (range ofx) associated with each phase that is temperature dependent. Thus, unlike in typical 18‐electron half‐Heuslers (e,g, TiNiSn), the temperature dependence of vacancy and carrier concentration (n) in nominally 19‐electron half‐Heuslers links its transport properties to synthesis conditions. The temperature dependence ofxandnare understood using density functional theory based defect energies (Ed) and phase diagrams.Edare calculated for 21 systems which can be used in predicting solubility in this family of compounds. Using this simple strategy, suitable composition and temperature synthesis conditions are devised for obtaining an optimizednto engineer TE properties in phase‐pure V0.8+xCoSb, and the previously unexplored Ta0.8+xCoSb.more » « less
An official website of the United States government

