论文标题

吉塔夫旋转液体候选者Cu $ _2 $ IRO $ _3 $:X射线,拉曼,磁敏感性,电阻率和第一原理分析

Pressure tuning of structure, magnetic frustration and carrier conduction in Kitaev spin liquid candidate Cu$_2$IrO$_3$: X-ray, Raman, magnetic susceptibility, resistivity and first-principles analysis

论文作者

Pal, Srishti, Malavi, Pallavi, Sinha, Arijit, Ali, Anzar, Sakrikar, Piyush, Joseph, Boby, Waghmare, Umesh V., Singh, Yogesh, Muthu, D. V. S., Karmakar, S., Sood, A. K.

论文摘要

分层的蜂窝状晶格irate cu $ _2 $ iro $ _3 $是Kitaev量子旋转液体的最接近的实现,这主要是由于增强的层间间隔和几乎理想的蜂窝状晶格。我们报告了压力引起的结构演变,cu $ _2 $ iro $ _3 $ ty Powder X射线衍射(PXRD)最多可达$ \ sim $ 17 GPA和拉曼散射测量值,最高$ \ sim $ 25 gpa。结构相变(单斜$ C2/C \:\ Rightarrow $ Triclinic $ p \ bar {1} $)在宽阔的混合相压范围内观察到($ \ sim $ 4至15 GPA)。三斜阶段由带有IR-IR二聚体形成的严重扭曲的蜂窝状晶格和塌陷的层间分离组成。在低压单斜相相的稳定性范围内,结构进化可维持高达4 GPA的基塔耶ev构型。观察到的DC易感性增强的磁性挫败感支持了这一点,而没有出现任何磁性顺序和增强的动态拉曼敏感性。在温度范围内,高压电阻测量值1.4---300 K显示出弹性的非金属$ r $($ t $)行为,在高压阶段的电阻率大大降低。 Mott 3D变量范围的传导传导大量降低了特征能量$ T_0 $,这表明高压阶段位于局部 - 互换交叉的边界。使用第一原理密度的功能理论(DFT)计算,我们发现在环境压力$ \ rm cu_2iro_3 $中存在单纤维胶质$ p2_1/c $相位,在能量上低于$ c2/c $相位(两种结构都与实验XRD模式保持一致)。 DFT揭示了与实验观察到的过渡压力一致的7 GPA(涉及IR-IR债券的二聚化)在7 GPA(涉及IR-IR键的二聚化)的结构过渡到$ P \ bar {1} $结构。

The layered honeycomb lattice iridate Cu$_2$IrO$_3$ is the closest realization of the Kitaev quantum spin liquid, primarily due to the enhanced interlayer separation and nearly ideal honeycomb lattice. We report pressure-induced structural evolution of Cu$_2$IrO$_3$ by powder x-ray diffraction (PXRD) up to $\sim$17 GPa and Raman scattering measurements up to $\sim$25 GPa. A structural phase transition (monoclinic $C2/c \: \rightarrow$ triclinic $P\bar{1}$) is observed with a broad mixed phase pressure range ($\sim$4 to 15 GPa). The triclinic phase consists of heavily distorted honeycomb lattice with Ir-Ir dimer formation and a collapsed interlayer separation. In the stability range of the low-pressure monoclinic phase, structural evolution maintains the Kitaev configuration up to 4 GPa. This is supported by the observed enhanced magnetic frustration in dc susceptibility without emergence of any magnetic ordering and an enhanced dynamic Raman susceptibility. High-pressure resistance measurements up to 25 GPa in the temperature range 1.4--300 K show resilient non-metallic $R$($T$) behaviour with significantly reduced resistivity in the high-pressure phase. The Mott 3D variable-range-hopping conduction with much reduced characteristic energy scale $T_0$ suggests that the high-pressure phase is at the boundary of localized-itinerant crossover. Using first-principles density functional theoretical (DFT) calculations, we find that at ambient pressure $\rm Cu_2IrO_3$ exists in monoclinic $P2_1/c$ phase which is energetically lower than $C2/c$ phase (both the structures are consistent with experimental XRD pattern). DFT reveals structural transition from $P2_1/c$ to $P\bar{1}$ structure at 7 GPa (involving dimerization of Ir-Ir bonds) in agreement with experimentally observed transition pressure.

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