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Andrej Pustogow

Publications and source records attributed to Andrej Pustogow.

At least 19 recordsLinked to original sources

Antiferromagnetic order and magnetic polarons in lightly doped Li$_x$CoO$_2$ (x $\sim$ 0.9)

We investigate the magnetic properties of Li$_x$CoO$_2$ (x$\sim$0.9) using bulk magnetization, specific heat, nuclear magnetic resonance (NMR) and electron paramagnetic resonance (EPR) spectroscopy measurements. The dc magnetization, specific heat and NMR measurements, which probe the macroscopic response, indeed show that this compound partially undergoes an antiferromagnetic transition below $T_N \sim$ 10 K. In addition, we observed a weak ferromagnetic response, which gives rise to the history dependence in magnetization measurements at low fields and is observed at temperatures above room temperature. We propose that there are ferromagnetic clusters at high temperatures due to the formation of magnetic polarons out of doped holes. In EPR measurements performed at the $X$-band frequency, only a fraction of the total spins contribute and show Curie-like paramagnetic behavior as reflected in the temperature dependence of the EPR intensity. The temperature variation of the EPR spectra can be understood in the framework of the diffusion of magnetic polarons.

cond-mat.str-el

Mott Intermittency at the Metal-Insulator Boundary

The resistivity maximum at a temperature $T=T_{\mathrm{max}}$ is a recurring feature of bandwidth-tuned Mott systems, yet its meaning remains controversial: is it a coherence-incoherence crossover of an electronically homogeneous metal, or does it mark the onset of transport through a mixed landscape of metallic and insulating regions? Even more debated is whether a true phase-coexistence regime survives in the relevant parameter range, or whether apparent inhomogeneity is merely extrinsic. Here we address these questions by moving beyond temperature sweeps and probe charge transport in the time domain. Near $T=T_{\mathrm{max}}$, we find that the resistance of a model system, a quasi-two-dimensional Mott spin liquid material, exhibits clear random-telegraph switching between discrete levels over long timescales. The statistics of the switching - sharp two-level behavior with thermally activated dwell times - point to a mesoscopic "current-controlling" region that dynamically toggles between metallic and insulating states, intermittently opening and closing the dominant conduction channel. This characteristic fluctuating dynamics provides direct evidence for intrinsic metal-insulator coexistence and establishes $T\sim T_{\mathrm{max}}$ as the regime of Mott intermittency, where transport is governed by stochastic domain switching rather than quasiparticle decoherence.

cond-mat.str-el

$P$-type Ru$_2$Ti$_{1-x}$Hf$_x$Si full-Heusler bulk thermoelectrics with $zT = 0.7$

Heusler compounds have emerged as important thermoelectric materials due to their combination of promising electronic transport properties, mechanical robustness and chemical stability -- key aspects for practical device integration. While a wide range of XYZ-type half-Heusler compounds have been studied for high-temperature applications, X$_2$YZ-type full-Heuslers, often characterized by narrower band gaps, may offer potential advantages at different temperature regimes but remain less explored. In this work, we report the discovery of $p$-type Ru$_2$Ti$_{1-x}$Hf$_x$Si full-Heusler thermoelectrics, exhibiting a high figure of merit $zT \sim 0.7$ over a broad range of temperatures $700-1000$ K. These results not only represent the largest values known to date among full-Heusler materials but confirm earlier theoretical predictions that $p$-type Ru$_2$TiSi systems would be superior to their $n$-type counterparts. Moreover, using a two-band model, we unveil electronic structure changes induced by the Hf substitution at the Ti site and outline strategies to further improve $zT$ up to $zT > 1$. Our findings highlight the untapped potential of new semiconducting full-Heusler phases and the crucial need for continued exploration of this rich materials class for thermoelectric applications.

cond-mat.mtrl-sci

Universal relation between residual resistivity and A coefficient in correlated metals

The effects of strong electronic correlations and disorder are crucial for emergent phenomena such as unconventional superconductivity, metal-insulator transitions, and quantum criticality. While both are omnipresent in real materials, their individual impacts on charge transport remain elusive. To disentangle their respective roles, we have independently varied the degree of randomness and the strength of electronic correlations -- by chemical substitution and physical pressure, respectively -- within the metallic phase nearby a Mott-insulating state. We find a distinct correlation dependence of the disorder-dependent residual resistivity $\rho_0$ in the Fermi-liquid regime $\rho(T)=\rho_0 + A T^2$, where $A\propto (m^{\star}/m)^2$ quantifies the electronic mass enhancement. Contrary to conventional expectations, we observe that at fixed disorder level $\rho_0$ grows linearly with $A$. This scaling can be understood in terms of chemical-potential fluctuations with variance $\sigma_\mu^2$, yielding $\rho_0 \propto A\,\sigma_\mu^2$. By comparing our findings to transport data on other organic Mott systems, oxides, heavy-fermion compounds, and moir\'e materials, we demonstrate that this new relation between residual resistivity and mass enhancement is a universal feature of correlated metals.

cond-mat.str-el

Tracking flat bands via phonon-mediated interband scattering

Flat-band (FB) materials have emerged as promising platforms for exploring exotic quantum phases. While numerous candidates have recently been identified through spectroscopic techniques such as angle-resolved photoemission spectroscopy, central challenges remain on how to tune FBs towards the Fermi level $E_F$ and to understand their impact on low-energy excitations probed in electronic transport experiments. Here, we show that, by attributing the temperature dependence of the electrical resistivity at elevated temperatures to electron-phonon interband scattering, one can infer the position of FBs near $E_F$ across diverse material classes. As charge carriers scatter off phonons, interband transitions into FB states lead to distinctive sub- or superlinear resistivity at elevated temperatures, governed by the proximity of the FB to $E_F$. Our phenomenological model captures these universal transport behaviors observed across several recently studied FB compounds and offers a simple, broadly applicable method for detecting flat bands.

cond-mat.str-el

Failed superconductivity in a Mott spin liquid material

A central challenge for understanding unconventional superconductivity in most strongly correlated electronic materials is their complicated band structure and presence of competing orders. In contrast, quasi-two-dimensional organic spin liquids are single-band systems with superconductivity arising near the bandwidth-tuned Mott metal-insulator transition in the absence of other orders. Here, we study chemically substituted $\kappa$-organics in which superconducting fluctuations emerge in the phase coexistence region between the Mott insulator and the Fermi liquid. Using magnetotransport and ac susceptibility measurements, we find that global superconductivity fails to set in as temperature $T\rightarrow 0$. Our results indicate instead the presence of superconducting domains embedded in the metallic percolating cluster that undergo a magnetic field-tuned quantum superconductor-to-metal phase transition. Surprisingly, albeit consistent with the percolation picture, universal conductance fluctuations are seen at high fields in macroscopic samples. The observed interplay of the intrinsic inhomogeneity and quantum phase fluctuations provides a new insight into failed superconductivity, a phenomenon seen in various conventional and unconventional superconductors, including cuprates.

cond-mat.supr-con

Emergence of a Fluctuating Ground State in Y-kapellasite under Pressure

Y-kapellasite (Y$_3$Cu$_9$(OH)$_{19}$Cl$_8$), which hosts an original anisotropic kagome sublattice, is a promising candidate for studying elusive and complex correlated physics. It exhibits a theoretically predicted in-plane $(1/3, 1/3)$ magnetic order [1] but its magnetic interaction values place it close to a phase boundary to a spin liquid state [2]. Our $\mu$SR measurements under hydrostatic pressure demonstrate the complete suppression of static magnetism in favor of a fully dynamical ground state at $2.3$~GPa. Complementary high-pressure x-ray and optical phonon measurements reveal a gradual reduction of the kagome anisotropy, enhancing magnetic frustration without structural transitions. Our results establish Y-kapellasite as a rare clean kagome model in which long-range order is suppressed by pressure-tuned frustration, the first fingerprint for the realization of a quantum spin liquid without strong disorder.

cond-mat.str-el

Energy filtering-induced ultrahigh thermoelectric power factors in Ni$_3$Ge

Traditional thermoelectric materials rely on low thermal conductivity to enhance their efficiency but suffer from inherently limited power factors. Novel pathways to optimize electronic transport are thus crucial. Here, we achieve ultrahigh power factors in Ni$_3$Ge through a new materials design principle. When overlapping flat and dispersive bands are engineered to the Fermi level, charge carriers can undergo intense interband scattering, yielding an energy filtering effect similar to what has long been predicted in certain nanostructured materials. Via a multi-step DFT-based screening method developed herein, we discover a new family of L1$_2$-ordered binary compounds with ultrahigh power factors up to 11 mW m$^{-1}$ K$^{-2}$ near room temperature, which are driven by an intrinsic phonon-mediated energy filtering mechanism. Our comprehensive experimental and theoretical study of these new intriguing materials paves the way for understanding and designing high-performance scattering-tuned metallic thermoelectrics.

cond-mat.mtrl-sci

Thermoelectric transport in Ru$_2$TiSi full-Heusler compounds

Heusler compounds with six valence electrons per atom have attracted interest as thermoelectric materials owing to their semimetallic and semiconducting properties. Here, we theoretically and experimentally investigate electronic transport in Ru$_2$TiSi-based full-Heuslers. We show that electronic transport in this system can be well captured by a two-parabolic band model. The larger band gap of Ru$_2$TiSi promises a higher thermoelectric performance, compared to its isovalent family member Fe$_2$VAl, which has been studied as a thermoelectric material for over two decades. Additionally, we identify $p$-type Ru$_2$TiSi as far more efficient than previously studied $n$-type compounds and demonstrate that this can be traced back to much lighter and more mobile holes originating from dispersive valence bands. Our findings demonstrate that an exceptionally high dimensionless figure of merit $zT > 1$ can be realized in these $p$-type compounds around 700 K upon proper reduction of the lattice thermal conductivity, e.g., by substituting Zr or Hf for Ti.

cond-mat.mtrl-sci

Gapped magnetic ground state in the spin-liquid candidate $\kappa$-(BEDT-TTF)$_2$Ag$_2$(CN)$_3$ suggested by magnetic spectroscopy

The nature of the magnetic ground state of highly frustrated systems remained puzzling to this day. Here, we have performed multifrequency electron spin resonance (ESR) measurements on a putative quantum spin liquid compound $\kappa$-(BEDT-TTF)$_2$Ag$_2$(CN)$_3$, which is a rare example of $S = 1/2$ spins on a triangular lattice. At high temperatures, the spin susceptibility exhibits a weak temperature dependence which can be described by the Heisenberg model with an antiferromagnetic exchange interaction of strength $J/k_B \approx 175$ K. At low temperatures, however, the rapid drop of the static spin susceptibility, together with monotonic decrease of the ESR linewidth indicates that strong singlet correlations develop below a pairing energy scale $T^*$ accompanied by a spin gap. On the other hand, a weak Curie-like spin susceptibility and the angular dependence of the linewidth suggest additional contribution from impurity spins. We propose the gradual formation of spin singlets with an inhomogeneous spin gap at low temperatures.

cond-mat.str-el

High thermoelectric power factor through topological flat bands

Thermoelectric (TE) materials are useful for applications such as waste heat harvesting or efficient and targeted cooling. While various strategies towards superior thermoelectrics through a reduction of the lattice thermal conductivity have been developed, a path to enhance the power factor is pressing. Here, we report large power factors up to 5 mW m$^{-1}$ K$^{-2}$ at room temperature in the kagome metal Ni$_3$In$_{1-x}$Sn$_x$. This system is predicted to feature almost dispersionless flat bands in conjunction with highly dispersive Dirac-like bands in its electronic structure around the Fermi energy $E_\text{F}$ [L. Ye et al., Nature Physics 1-5 (2024)]. Within this study, we experimentally and theoretically showcase that tuning this flat band precisely below $E_\text{F}$ by chemical doping $x$ boosts the Seebeck coefficient and power factor, as highly mobile charge carriers scatter into the flat-band states. Our work demonstrates the prospect of engineering extremely flat and highly dispersive bands towards the Fermi energy in kagome metals and introduces topological flat bands as a novel tuning knob for thermoelectrics.

cond-mat.str-el

SrCu(OH)$_3$Cl, an ideal isolated equilateral triangle spin $S$ = 1/2 model system

We have investigated the magnetic ground state properties of the quantum spin trimer compound strontium hydroxy copper chloride SrCu(OH)$_3$Cl using bulk magnetization, specific heat measurements, nuclear magnetic resonance (NMR), and electron spin resonance (ESR) spectroscopy. SrCu(OH)$_3$Cl consists of layers with isolated Cu$^{2+}$ triangles and hence provides an opportunity to understand the magnetic ground state of an isolated system of \textit{S} = 1/2 arranged on an equilateral triangle. Although magnetization measurements do not exhibit a phase transition to a long-range ordered state down to \textit{T} = 2 K, they reveal the characteristic behavior of isolated trimers with an exchange of $J = 154$~K. The Curie-Weiss behavior changes around 50--80~K, as is also seen in the NMR spin-lattice relaxation rate. In zero magnetic field, our specific heat data establish a second-order phase transition to an antiferromagnetic ground state below \textit{T}= 1.2 K. We have drawn a magnetic field-temperature ($H$-$T$) phase diagram based on the specific heat measurements. The ESR data show divergence of the linewidth at lower temperatures, which precedes the phase transition to an antiferromagnetic long-range ordered state with unconventional critical exponents. The temperature variation of the $g$-factor further confirms the antiferromagnetic phase transition and reflects the underlying magneto-crystalline anisotropy of the compound.

cond-mat.str-el

High thermoelectric performance in metallic NiAu alloys

Thermoelectric (TE) materials seamlessly convert thermal into electrical energy and vice versa, making them promising for applications such as power generation or cooling. Although historically the TE effect was first discovered in metals, state-of-the-art research mainly focuses on doped semiconductors with large figure of merit, $zT$, that determines the conversion efficiency of TE devices. While metallic alloys have superior functional properties, such as high ductility and mechanical strength, they have mostly been discarded from investigation in the past due to their small Seebeck effect. Here, we realize unprecedented TE performance in metals by tuning the energy-dependent electronic scattering. Based on our theoretical predictions, we identify binary NiAu alloys as promising candidate materials and experimentally discover colossal power factors up to 34 mWm$^{-1}$K$^{-2}$ (on average 30 mWm$^{-1}$K$^{-2}$ from 300 to 1100 K), which is more than twice larger than in any known bulk material above room temperature. This system reaches a $zT$ up to 0.5, setting a new world record value for metals. NiAu alloys are not only orders of magnitude more conductive than heavily doped semiconductors, but also have large Seebeck coefficients originating from an inherently different physical mechanism: within the Au s band conduction electrons are highly mobile while holes are scattered into more localized Ni d states, yielding a strongly energy-dependent carrier mobility. Our work challenges the common belief that good metals are bad thermoelectrics and presents an auspicious paradigm for achieving high TE performance in metallic alloys through engineering electron-hole selective s-d scattering.

cond-mat.mtrl-sci

Thermodynamic Properties of the Mott Insulator-Metal Transition in a Triangular Lattice System Without Magnetic Order

The organic system, $κ$-[(BEDT-TTF)$_{1-x}$(BEDT-STF)$_x$]$_2$Cu$_2$(CN)$_3$, showing the Mott transition between a nonmagnetic Mott insulating (NMI) state and a Fermi liquid (FL), is systematically studied by calorimetric measurements. An increase of the electronic heat capacity at the transition from the NMI state to the FL state which keeps the triangular dimer lattice demonstrates that the charge sector lost in the Mott insulating state is recovered in the FL state. We observed that the remaining low-energy spin excitations in the Mott insulating state show unique temperature dependence, and that the NMI state has a larger lattice entropy originating from the frustrated lattice, which leads to the Pomeranchuk-like effect on the electron localization. Near the Mott boundary, an unexpected enhancement and magnetic-field dependence of heat capacity are observed. This anomalous heat capacity is different from the behavior in the typical first-order Mott transition and shows similarities with quantum critical behavior. To reconcile our results with previously reported scenarios about a spin gap and the first-order Mott transition, further studies are desired.

cond-mat.str-el

Upper Critical Field of Sr$_2$RuO$_4$ under In-Plane Uniaxial Pressure

In-plane uniaxial pressure has been shown to strongly tune the superconducting state of Sr2RuO4 by approaching a Lifshitz transition and associated Van Hove singularity (VHS) in the density of states. At the VHS, $T_c$ and the in- and out-of-plane upper critical fields are all strongly enhanced, and the latter has changed its curvature as a function of temperature from convex to concave. However, due to strain inhomogeneity it has not been possible so far to determine how the upper critical fields change with strain. Here, we show the strain dependence of both upper critical fields, which was achieved due to an improved sample preparation. We find that the in-plane upper critical field is mostly linear in $T_c$. On the other hand, the out-of-plane upper critical field varies with a higher power in $T_c$, and peaks strongly at the VHS. The strong increase in magnitude and the change in form of $H_\mathrm{c2||c}$ occur very close to the Van Hove strain, and points to a strong enhancement of both the density of states and the gap magnitude at the Lifshitz transition.

cond-mat.supr-con

Multi-Center Magnon Excitations Open the Entire Brillouin Zone to Terahertz Magnetometry of Quantum Magnets

Due to the small photon momentum, optical spectroscopy commonly probes magnetic excitations only at the center of the Brillouin zone; however, there are ways to override this restriction. In the case of the distorted kagome quantum magnet Y-kapellasite, Y$_3$Cu$_9$(OH)$_{19}$Cl$_8$, under scrutiny here, the magnon density of states can be accessed over the entire Brillouin zone through three-center magnon excitations. This mechanism is aided by the three different magnetic sublattices and strong short-range correlations in the distorted kagome lattice. The results of THz time-domain experiments agree remarkably well with linear spin-wave theory. Relaxing the conventional zone-center constraint of photons gives a new aspect to probe magnetism in matter.

cond-mat.str-el

Tuning the Fermi Liquid Crossover in Sr$_2$RuO$_4$ with Uniaxial Stress

We perform nuclear magnetic resonance (NMR) measurements of the oxygen-17 Knight shifts for Sr$_2$RuO$_4$, while subjected to uniaxial stress applied along [100] direction. The resulting strain is associated with a strong variation of the temperature and magnetic field dependence of the inferred magnetic response. A quasi-particle description based on density-functional theory calculations, supplemented by many-body renormalizations, is found to reproduce our experimental results, and highlights the key role of a van-Hove singularity. The Fermi liquid coherence scale is shown to be tunable by strain, and driven to low values as the associated Lifshitz transition is approached.

cond-mat.str-el

Magnetic terahertz resonances above the Néel temperature in the frustrated kagome antiferromagnet averievite

Time-domain magneto-THz spectroscopy is utilized to study the frustrated magnet averievite Cu$_{5-x}$Zn$_x$V$_2$O$_{10}$(CsCl). Pronounced THz resonances are observed in unsubstituted samples ($x=0$) when cooling below the onset of short-range magnetic correlations. The influence of external magnetic effects confirms the magnetic origin of these resonances. Increasing Zn substitution suppresses the resonances, as frustration effects dominate, reflecting the non-magnetic phases for $x> 0.25$ compounds. The temperature evolution of the THz spectra is complemented with electron spin resonance spectroscopy. This comparison allows a direct probe of the different contributions from magnetic order, frustration, and structural properties in the phase diagram of averievite. Our results illustrate the effect of magnetic interactions in THz spectra of frustrated magnets.

cond-mat.str-el