Experiments on the $Gd^{3+}$ Electron Spin Resonance (ESR) in the filled skutterudite $Ce_{1-x}Gd_{x}Fe_{4}P_{12}$ ($x \approx 0.001$), at temperatures where the host resistivity manifests a smooth insulator-metal crossover, provides evidence of the underlying Kondo physics associated with this system. At low temperatures (below $T \approx K$), $Ce_{1-x}Gd_{x}Fe_{4}P_{12}$ behaves as a Kondo-insulator with a relatively large hybridization gap, and the $Gd^{3+}$ ESR spectra displays a fine structure with lorentzian line shape, typical of insulating media. The electronic gap is attributed to the large hybridization present in the coherent regime of a Kondo lattice, when Ce 4f-electrons cooperate with band properties at half-filling. Mean-field calculations suggest that the electron-phonon interaction is fundamental at explaining the strong 4f-electron hybridization in this filled skutterudite. The resulting electronic structure is strongly temperature dependent, and at about $T^{*} \approx 160 K$ the system undergoes an insulator-to-metal transition induced by the withdrawal of 4f-electrons from the Fermi volume, the system becoming metallic and non-magnetic. The $Gd^{3+}$ ESR fine structure coalesces into a single dysonian resonance, as in metals. Still, our simulations suggest that exchange-narrowing via the usual Korringa mechanism, alone, is not capable of describing the thermal behavior of the ESR spectra in the entire temperature region ($4.2$ - $300$ K). We propose that temperature activated fluctuating-valence of the Ce ions is the missing ingredient that, added to the usual exchange-narrowing mechanism, fully describes this unique temperature dependence of the $Gd^{3+}$ ESR fine structure observed in $Ce_{1-x}Gd_{x}Fe_{4}P_{12}$.
The dynamic magnetic properties of the Kondo-insulator state in CeFe2Al10 (spin gap, resonance mode) have been investigated using polarized neutrons on a single crystal of pure CeFe2Al10. The results indicate that the magnetic excitations are polarized mainly along the orthorhombic a axis and their dispersion along the orthorhombic c direction could be determined. Polycrystalline samples of Nd- and Rh-doped CeFe2Al0 were also studied by the time-of-flight technique, with the aim of finding out how the low-energy magnetic excitation spectra change upon isoelectronic substitution of the rare-ear…
Direct determination of the crystal field parameters of Dy, Er and Yb impurities in the skutterudite compound CeFe$_{4}$P$_{12}$ by Electron Spin Resonance
尽管在过去的十年里对方钴矿进行了广泛的研究,但它们的电晶体场基态仍然是一个有争议的问题。我们表明,电子自旋共振(ESR)测量可以确定完整的晶场参数(CFPs)的Th立方对称性(Im 3)的Ce $_{1-x}$ R $_{x}$ Fe $_{4}$ P $_{12}$(R = Dy,Er,Yb,$x\lesssim 0.003$)方钴矿化合物。根据ESR数据的分析,确定了Ce $^{3+}$位点上这些稀土中的每一种的三个CFPs,B4c,B6c和B6t。场和温度依赖性的掺杂晶体的测量磁化强度是在一个很好的协议与来自ESR的CFPs Bnm预测。
Anisotropic Electronic Structure of the Kondo Semiconductor CeFe2Al10 Studied by Optical Conductivity
我们报告了CeFe $_2$ Al $_{10}$的温度依赖性极化光学电导率[ $σ(ω)$ ]光谱,该光谱是CeRu $_2$ Al $_{10}$和CeOs $_2$ Al $_{10}$在28 K下发生异常磁转变的参考材料。沿b轴的$σ(ω)$谱与在$ac$平面中的谱有很大不同,表明该材料具有各向异性的电子结构。在低温下,在所有轴上,在55 meV处出现了由于穿过导带和局部$4f$状态之间的杂化间隙的光学跃迁(即$c$ - $f$杂化)而引起的肩部结构。然而,间隙打开温度和准粒子Drude重量的出现温度是强烈的各向异性,表明各向异性的近藤温度。CeRu $_2$ Al $_{10}$和CeOs $_2$ Al $_{10}$的电子结构和近藤温度的强各向异性与反常磁相变有关。
In the iron-pnictide material CeFeAsO not only the Fe moments, but also the local 4f moments of the Ce order antiferromagnetically at low temperatures. We elucidate on the peculiar role of the Ce on the emergence of superconductivity. While application of pressure suppresses the iron SDW ordering temperature monotonously up to 4 GPa, the Ce-4f magnetism is stabilized, until both types of magnetic orders disappear abruptly and a narrow SC dome develops. With further increasing pressure characteristics of a Kondo-lattice system become more and more apparent in the electrical resistivity. This su…
We report a systematic study of the $5d$-electron-doped system Ce(Fe$_{1-x}$Ir$_x$)$_2$Al$_{10}$ ($0 \leq x \leq 0.15$). With increasing $x$, the orthorhombic $b$~axis decreases slightly while accompanying changes in $a$ and $c$ leave the unit cell volume almost unchanged. Inelastic neutron scattering, along with thermal and transport measurements, reveal that for the Kondo semiconductor CeFe$_2$Al$_{10}$, the low-temperature energy gap which is proposed to be a consequence of strong $c \mhyphen f$ hybridization, is suppressed by a small amount of Ir substitution for Fe, and that the system ad…
The predicted interplay between Kondo physics and non-trivial topology in SmB$_{6}$ has stimulated many experimental reports, some of which are in apparent contradiction. The origin of the dispute may lie on the fragility of the Kondo insulating phase in the presence of Sm vacancies (Kondo holes) and/or natural impurities, such as Gd$^{3+}$. In this work, we locally investigated this fragility for Al-flux grown Sm$_{1-x}$Gd$_{x}$B$_{6}$ single crystals (0 $\leq$ $x$ $\leq$ 0.02) by combining electron spin resonance (ESR) and complementary bulk measurements. The Gd$^{3+}$ ESR spectra in a highl…
The interplay between non-trivial topological states of matter and strong electronic correlations is one of the most compelling open questions in condensed matter physics. Due to experimental challenges, there is an increasing desire to find more microscopic techniques to complement the results of more traditional experiments. In this work, we locally explore the Kondo insulator Sm$_{1-x}$Gd$_{x}$B$_{6}$ by means of electron spin resonance (ESR) of Gd$^{3+}$ ions at low temperatures. Our analysis reveals that the Gd$^{3+}$ ESR line shape shows an anomalous evolution as a function of temperatur…
Quantitative study of valence and configuration interaction parameters of the Kondo semiconductors CeM2Al10 (M = Ru, Os and Fe) by means of bulk-sensitive hard x-ray photoelectron spectroscopy
We theoretically analyze a state-of-the-art experimental method based on a combination of electron spin resonance and scanning tunneling microscopy (ESR-STM), to directly probe the spin fluctuations in the Kondo effect. The Kondo impurity is exchange coupled to the probe spin, and the ESR-STM setup detects the small level shifts in the probe spin induced by the spin fluctuations of the Kondo impurity. We use the open quantum system approach by regarding the probe spin as the "system" and the Kondo impurity spin as the fluctuating "bath" to evaluate the resonance line shifts in terms of the dyn…
This work reports on the temperature dependence of the electron spin resonance (ESR) of Gd$^{3+}$-doped SmB$_{6}$ single crystals at X- and Q-band microwave frequencies in different crystallographic directions. We found an anomalous inhomogeneous broadening of the Gd$^{3+}$ ESR linewidth ($ΔH$) within 5.3 K $\leq T \leq$ 12.0 K which is attributed to slow crystalline electric field (CEF) fluctuations, slower than the timescale of the ESR microwave frequencies used ($\sim$10 GHz). This linewidth inhomogeneity may be associated to the coupling of the Gd$^{3+}$ $S$-states to the breathing mode of…