arXiv subjects

P. Rogl

Publications and source records attributed to P. Rogl.

At least 19 recordsLinked to original sources

arXiv2023

Ce$_3$Bi$_4$Ni$_3$ $-$ A large hybridization-gap variant of Ce$_3$Bi$_4$Pt$_3$

The family of cubic noncentrosymmetric 3-4-3 compounds has become a fertile ground for the discovery of novel correlated metallic and insulating phases. Here, we report the synthesis of a new heavy fermion compound, Ce$_3$Bi$_4$Ni$_3$. It is an isoelectronic analog of the prototypical Kondo insulator Ce$_3$Bi$_4$Pt$_3$ and of the recently discovered Weyl-Kondo semimetal Ce$_3$Bi$_4$Pd$_3$. In contrast to the volume-preserving Pt-Pd substitution, structural and chemical analyses reveal a positive chemical pressure effect in Ce$_3$Bi$_4$Ni$_3$ relative to its heavier counterparts. Based on the results of electrical resistivity, Hall effect, magnetic susceptibility, and specific heat measurements, we identify an energy gap of 65-70 meV, about eight times larger than that in Ce$_3$Bi$_4$Pt$_3$ and about 45 times larger than that of the Kondo-insulating background hosting the Weyl nodes in Ce$_3$Bi$_4$Pd$_3$. We show that this gap as well as other physical properties do not evolve monotonically with increasing atomic number, i.e., in the sequence Ce$_3$Bi$_4$Ni$_3$-Ce$_3$Bi$_4$Pd$_3$-Ce$_3$Bi$_4$Pt$_3$, but instead with increasing partial electronic density of states of the $d$ orbitals at the Fermi energy. To understand under which condition topological states form in these materials is a topic for future studies.

cond-mat.str-el↗

arXiv2019

Nanostructured clathrates and clathrate-based nanocomposites

Intermetallic clathrates are candidate materials for thermoelectric applications above room temperature. Here we explore whether their intrinsically low lattice thermal conductivities can be further reduced by nanostructuring and whether this can further enhance their thermoelectric performance.}{As bulk nanostructuring routes we studied melt spinning and ball milling. To optimize the compaction process and/or stabilize the nanostructure we varied the process parameters, used additives, and studied clathrate-based composites. Initial results on clathate nanowires as simpler model nanostructures are also presented.

cond-mat.mtrl-sci↗

arXiv2019

Physical properties of CeIrSi with trillium-lattice frustrated magnetism

Magnetic ($χ$), transport ($ρ$) and heat capacity ($C_m$)properties of CeIrSi are investigated to elucidate the effect of geometric frustration in this compound with trillium type structure because, notwithstanding its robust effective moment, $μ_{\rm eff}\approx 2.46μ_B$, this Ce-lattice compound does not undergo a magnetic transition. In spite of that it shows broad $C_m(T)/T$ and $χ(T)$ maxima centered at $T_{max}\approx 1.5$\,K, while a $ρ\propto T^2$ thermal dependence, characteristic of electronic spin coherent fluctuations, is observed below $T_{coh} \approx 2.5$\,K. Magnetic field does not affect significantly the position of the mentioned maxima up to $\approx 1$\,T, though $χ(T)$ shows an incipient structure that completely vanishes at $μ_0 H \approx 1$\,T. Concerning the $ρ\propto T^2$ dependence, it is practically not affected by magnetic field up to $μ_0 H = 9$\,T, with the residual resistivity $ρ_0(H)$ slightly decreasing and $T_{coh}(H)$ increasing. These results are compared with the physical properties observed in other frustrated intermetallic compounds

cond-mat.str-el↗

arXiv2017

New bulk p-type skutterudites DD0.7Fe2.7Co1.3Sb12-xXx (X = Ge, Sn) reaching ZT>1.3

The best p-type skutterudites so far are didymium filled, Fe/Co substituted, Sb-based skutterudites. Substitution at the Sb-sites influences the electronic structure, deforms the Sb4-rings, enhances the scattering of phonons on electrons and impurities and this way reduces the lattice thermal conductivity. In this paper we study structural and transport properties of p-type skutterudites with the nominal composition DD0.7Fe2.7Co1.3Sb11.7{Ge/Sn}0.3, which were prepared by a rather fast reaction-annealing-melting technique. The Ge-doped sample showed impurities, which did not anneal out completely and even with ZT > 1 the result was not satisfying. However, the single-phase Sn-doped sample, DD0.7Fe2.7Co1.3Sb11.8Sn0.2, showed a lower thermal and lattice thermal conductivity than the undoped skutterudite leading to a higher ZT=1.3, hitherto the highest ZT for a p-type skutterudite. Annealing at 570 K for 3 days proved the stability of the microstructure. After severe plastic deformation (SPD), due to additionally introduced defects, an enhancement of the electrical resistivity was compensated by a significantly lower thermal conductivity and the net effect led to a record high figure of merit: ZT = 1.45 at 850 K for DD0.7Fe2.7Co1.3Sb11.8Sn0.2.

cond-mat.mtrl-sci↗

arXiv2017

Clathrate formation in the systems Sr-Cu-Ge and {Ba,Sr}-Cu-Ge

In the ternary system Sr-Cu-Ge, a clathrate type-I phase, Sr8Cu5.3Ge40.7 (a = 1.06311(3), exists close to the Zintl limit in a small temperature interval. Sr8Cu5.3Ge40.7 decomposes eutectoidally on cooling at 730°C into (Ge), SrGe2 and tau1-SrCu2-xGe2+x. Phase equilibria at 700°C have been established for the Ge rich part and are characterized by the appearance of only one ternary compound, tau1-SrCu2-xGe2+x, which crystallizes with the ThCr2Si2 structure type and forms a homogeneity range up to x=0.4 (a = 0.42850(4), c = 1.0370(1) nm). Additionally, the extent of the clathrate type-I solid solution Ba8-xSrxCuyGe46-y (5.2 < y < 5.4) has been studied at various temperatures. The clathrate type-I crystal structure (space group ) has been proven by X-ray single crystal diffraction on two single crystals with composition Sr8Cu5.3Ge40.7 (a = 1.06368(2) nm) and Ba4.9Sr3.1Cu5.3Ge40.7 (a = 1.06748(2) nm) measured at 300, 200 and 100 K. From the temperature dependency of the lattice parameters and the atomic displacement parameters, the thermal expansion coefficients, the Debye- and Einstein-temperatures and the speed of sound have been determined. From heat capacity measurements of Sr8Cu5.3Ge40.7 at low temperatures, the Sommerfeld coefficient and the Debye temperature have been extracted, whereas from a detailed analysis of these data at higher temperatures, Einstein branches of the phonon dispersion relation have been derived and compared with those obtained from the atomic displacement parameters. Electrical resistivity measurements of Sr8Cu5.3Ge40.7 reveal a rather metallic behaviour in the low temperature range (< 300 K).

cond-mat.mtrl-sci↗

arXiv2012

Optimizing thermoelectric properties of filled MPt$_4$Ge$_{12-x}$Sb$_x$ skutterudites by band engineering

On the basis of density functional theory (DFT) calculations thermoelectric properties are derived for Sb-doped skutterudites MPt$_4$Ge$_{12-x}$Sb$_x$ with M=Ba,La,Th. It is predicted that the originally very small absolute values of Seebeck coefficients $|S|$ of the undoped compounds is increased by factors of 10 or more for suitable dopings. The optimal dopings correspond to a "magic" valence electron number for which all electronic states up to a (pseudo)gap are filled. The theoretical findings are corroborated by measurements of $S$ for LaPt$_4$Ge$_{12-x}$Sb$_x$ skutterudites. DFT derived vibrational rattling-like modes for LaPt$_4$Ge$_{12}$ indicate a small value for the lattice thermal conductivity which in combination with a large value of $S^2$ makes the La-based skutterudites appear as promising thermoelectric materials.

cond-mat.mtrl-sci↗

arXiv2011

Thermoelectric properties of Ba-Cu-Si clathrates

Thermoelectric properties of the type-I clathrates Ba$_8$Cu$_x$Si$_{46-x}$ ($3.6 \leq x \leq 7$, $x$ = nominal Cu content) are investigated both experimentally and theoretically. The polycrystalline samples are prepared either by melting, ball milling and hot pressing or by melt spinning, hand milling and hot pressing techniques. Temperature-dependent electrical resistivity, $ρ(T)$, and the Seebeck coefficient, $S(T)$, measurements reveal metal-like behavior for all samples. For $x = 5$ and 6, density functional theory calculations are performed for deriving the enthalpy of formation and the electronic structure which is exploited for the calculation of Seebeck coefficients and conductivity within Boltzmann's transport theory. For simulating the properties of doped clathrates the rigid band model is applied. On the basis of the density functional theory results the experimentally observed compositional dependence of $ρ(T)$ and $S(T)$ of the whole sample series is analyzed. The highest dimensionless thermoelectric figure of merit $ZT$ of 0.28 is reached for a melt-spun sample at $600^{\circ}$C. The relatively low $ZT$ values in this system are attributed to the too high charge carrier concentrations.

cond-mat.mtrl-sci↗

arXiv2010

Unconventional superconductivity in weakly correlated, non-centrosymmetric $\rm{Mo_3Al_2C}$

Electrical resistivity, specific heat and NMR measurements classify non-centrosymmetric $\rm Mo_3Al_2C$ ($β$-Mn type, space group $P4_132$) as a strong-coupled superconductor with $T_c = 9$~K deviating notably from BCS-like behaviour. The absence of a Hebbel-Slichter peak, a power law behaviour of the spin-lattice relaxation rate (from $^{27}$Al NMR), a $T^3$ temperature dependence of the specific heat and a pressure enhanced $T_c$ suggest unconventional superconductivity with a nodal structure of the superconducting gap. Relativistic DFT calculations reveal a splitting of degenerate electronic bands due to the asymmetric spin-orbit coupling, favouring a mix of spin-singlet and spin triplet components in the superconducting condensate, in absence of strong correlations among electrons.

cond-mat.supr-con↗

arXiv2007

Superconductivity in novel Ge-based skutterudites: {Sr,Ba}Pt_4Ge_{12}

Combining experiments and ab initio models we report on $\rm SrPt_4Ge_{12}$ and $\rm BaPt_4Ge_{12}$ as members of a novel class of superconducting skutterudites, where Sr or Ba atoms stabilize a framework entirely formed by Ge-atoms. Below $T_c=5.35$ K, and 5.10 K for $\rm BaPt_4Ge_{12}$ and $\rm SrPt_4Ge_{12}$, respectively, electron-phonon coupled superconductivity emerges, ascribed to intrinsic features of the Pt-Ge framework, where Ge-$p$ states dominate the electronic structure at the Fermi energy.

cond-mat.supr-con↗

arXiv2006

Ab initio prediction of half-metallic properties for the ferromagnetic Heusler alloys Co$_2$MSi (M=Ti, V, Cr)

By means of density functional calculations the magnetic and electronic properties and phase stabilities of the Heusler compounds Co$_2$MSi (with M=Ti, V, Cr, Mn, Fe, Co, Ni) were investigated. Based on the calculated results we predict the ferromagnetic phases of the compounds Co$_2$TiSi, Co$_2$VSi and Co$_2$CrSi to be half-metals. Of particular interest is Co$_2$CrSi because of its high density of majority spin states at Fermi energy in combination with a reasonably high estimated Curie temperature of 747K. The compounds Co$_2$TiSi and Co$_2$VSi are thermodynamically stable, whereas Co$_2$CrSi is a metastable phase which might be stabilized by suitable experimental techniques.

cond-mat.mtrl-sci↗

arXiv2005

Ferromagnetism and possible heavy fermion behavior in single crystals of NdOs$_4$Sb$_{12}$

Single crystals of the filled-skutterudite compound NdOs$_4$Sb$_{12}$ have been investigated by means of electrical resistivity, magnetization, and specific heat measurements. The NdOs$_4$Sb$_{12}$ crystals have the LaFe$_4$P$_{12}$-type cubic structure with a lattice parameter of 9.3 Å. Possible heavy-fermion behavior is inferred from specific heat measurements, which reveal a large electronic specific heat coefficient $γ\approx 520$ mJ/mol-K$^2$, corresponding to an effective mass $m^* \sim$ 98 $m_e$. Features related to a ferromagnetic transition at {$\sim$ 0.9 K} can be observed in electrical resistivity, magnetization and specific heat. Conventional Arrott-plot analysis indicates that NdOs$_4$Sb$_{12}$ conforms to mean-field ferromagnetism.

cond-mat.str-el↗

arXiv2004

Heavy Fermion Behavior, Crystalline Electric Field Effects, and Weak Ferromagnetism in SmOs_{4}Sb_{12}

The filled skutterudite compound SmOs_{4}Sb_{12} was prepared in single crystal form and characterized. The SmOs_{4}Sb_{12} crystals have the LaFe_{4}P_{12}-type structure with lattice parameter a = 9.3085 Angstroms. Specific heat measurements indicate a large electronic specific heat coefficient of ~880 mJ/mol K^{2}, from which an enhanced effective mass m^{*} ~ 170 m_{e} is estimated. The specific heat data also suggest crystalline electric field (CEF) splitting of the Sm^{3+} J = 5/2 multiplet into a Gamma_{7} doublet ground state and a Gamma_{8} quartet excited state separated by 37 K. Electrical resistivity rho(T) measurements reveal a decrease in rho(T) below ~50 K that is consistent with CEF splitting of ~33 K between a Gamma_(7) doublet ground state and Gamma_{8} quartet excited state. Specific heat and magnetic susceptibility measurements display a possible weak ferromagnetic transition at ~2.6 K, which could be an intrinsic property of SmOs_4Sb_{12} or possibly due to an unknown impurity phase.

cond-mat.str-el↗

arXiv2004

Unconventional superconductivity and magnetism in $\rm CePt_3Si_{1-x}Ge_x$

$\rm CePt_3Si$ is a novel ternary compound exhibiting antiferromagnetic order at $T_N \approx 2.2$ K and superconductivity (SC) at $T_c \approx 0.75$ K. Large values of $H_{c2}' \approx -8.5$ T/K and $H_{c2}(0) \approx 5$ T indicate Cooper pairs formed out of heavy quasiparticles. The mass enhancement originates from Kondo interaction with a characteristic temperature $T_K \approx 8$ K. NMR and $μ$SR measurements evidence coexistence of SC and long range magnetic order on a microscopic scale. Moreover, $\rm CePt_3Si$ is the first heavy fermion SC without an inversion symmetry. This gives rise to a novel type of the NMR relaxation rate $1/T_1$ which is very unique and never reported before for other heavy fermion superconductors. Studies of Si/Ge substitution allow us to establish a phase diagram.

cond-mat.supr-con↗

arXiv2004

Intermediate valence behavior in CeCo9Si4

The novel ternary compound CeCo$_9$Si$_4$ has been studied by means of specific heat, magnetisation, and transport measurements. Single crystal X-ray Rietveld refinements reveal a fully ordered distribution of Ce, Co and Si atoms with the tetragonal space group I4/mcm isostructural with other RCo9Si4. The smaller lattice constants of CeCo9Si4 in comparison with the trend established by other RCo9Si4 is indicative for intermediate valence of cerium. While RCo9Si4 with R= Pr, .. Tb, and Y show ferromagnetism and LaCo9Si4 is nearly ferromagnetic, CeCo9Si4 remains paramagnetic even in external fields as large as 40 T, though its electronic specific heat coefficient (g~190 mJ/molK^2) is of similar magnitude as that of metamagnetic LaCo9Si4 and weakly ferromagnetic YCo9Si4.

cond-mat.str-el↗

arXiv2004

Weak itinerant ferromagnetism in YCo9Si4

Weak itinerant ferromagnetism in YCo9Si4 below about 25 K is studied by means of magnetisation, specific heat, and resistivity measurements. Single crystal X-ray Rietveld refinements at room temperature reveal a fully ordered distribution of Y, Co and Si atoms within the tetragonal space group I4/mcm isostructural with LaCo9Si4. The latter exhibits itinerant electron metamagnetism with an induced moment of about 1 mu_B/f.u. above 6 T, whereas YCo9Si4 exhibits a spontaneous magnetisation M0~12 Am^2/kg at 2 K which corresponds to an ordered moment of about 1.6 mu_B/f.u. indicating weak itinerant ferromagnetism.

cond-mat.str-el↗

arXiv2004

Evidence for a Novel State of Superconductivity in Noncentrosymmetric CePt3Si : A 195Pt-NMR Study

We report on novel antiferromagnetic (AFM) and superconducting (SC) properties of noncentrosymmetric CePt3Si through measurements of the 195Pt nuclear spin-lattice relaxation rate 1/T_1. In the normal state, the temperature (T) dependence of 1/T1 unraveled the existence of low-lying levels in crystal-electric-field multiplets and the formation of a heavy fermion (HF) state. The coexistence of AFM and SC phases, that emerge at TN = 2.2 K and Tc = 0.75 K, respectively, takes place on a microscopic level. CePt3Si is the first HF superconductor that reveals a peak in 1/T1 just below Tc and, additionally, does not follow the T^3 law that used to be reported for most unconventional HF superconductors. We remark that this unexpected SC characteristics may be related with the lack of an inversion center in its crystal structure.

cond-mat.supr-con↗

arXiv2004

A new polymorphic material? Structural degeneracy of ZrMn_2

Based on density functional calculations, we propose that ZrMn_2 is a polymorphic material. We predict that at low temperatures the cubic C15, and the hexagonal C14 and C36 structures of the Laves phase compound ZrMn_2 are nearly equally stable within 0.3 kJmol^{-1} or 30 K. This degeneracy occurs when the Mn atoms magnetize spontaneously in a ferromagnetic arrangement forming the states of lowest energy. From the temperature dependent free energies at T approx 160K we predict a transition from the most stable C15 to the C14 structure, which is the experimentally observed structure at elevated temperatures.

cond-mat.mtrl-sci↗

arXiv2003

Itinerant electron metamagnetism in LaCo$_9$Si$_4$

The strongly exchange enhanced Pauli paramagnet LaCo$_9$Si$_4$ is found to exhibit an itinerant metamagnetic phase transition with indications for metamagnetic quantum criticality. Our investigation comprises magnetic, specific heat, and NMR measurements as well as ab-initio electronic structure calculations. The critical field is about 3.5 T for $H||c$ and 6 T for $H\bot c$, which is the lowest value ever found for rare earth intermetallic compounds. In the ferromagnetic state there appears a moment of about 0.2 $μ_B$/Co at the $16k$ Co-sites, but sigificantly smaller moments at the 4d and $16l$ Co-sites.

cond-mat.str-el↗