arXiv subjects

C. Petrovic

Publications and source records attributed to C. Petrovic.

At least 19 recordsLinked to original sources

arXiv2026

Superconductivity and fractionalized magnetic excitations in CeCoIn5

Recent experiments on CeCoIn5 -- a prototypical d-wave superconductor -- indicate that its normal state lies near an unconventional quantum critical point (QCP). One intriguing hypothesis is that quantum-critical fluctuations promote fractionalization of localized 4f moments into fermionic spinons. This fractionalized Fermi liquid (FL*) scenario provides a comprehensive framework for the unconventional QCP and superconductivity, and can reconcile a "missing" Fermi-surface volume relative to the Luttinger count in the normal state of CeCoIn5. To test this possibility, we performed inelastic neutron scattering (INS) measurements on CeCoIn5 across the superconducting transition and corresponding theoretical analysis. Our high-precision spectra reveal detailed momentum and temperature dependence of the spin resonance and a structured spin excitation continuum persisting even in the normal state, placing stringent constraints on the physical picture of pairing in a d-wave superconductor. We show that a Kondo-lattice framework incorporating proximity to FL* physics and d-wave pairing reproduces key features of the data. The model suggests that both the quasi-localized nature of the f-moments above Tc and the resonance below Tc arise from common underlying gauge dynamics, implying a unifying organizing principle linking spin fractionalization and unconventional superconductivity in strongly correlated metals.

cond-mat.str-el↗

arXiv2024

Anisotropic excitonic magnetism from discrete $\mathrm{C}_{4}$ symmetry in CeRhIn$_{5}$

Anisotropy in strongly correlated materials is a central parameter in determining the electronic ground state and is tuned through the local crystalline electric field. This is notably the case in the CeCo$_{x}$Rh$_{1-x}$In$_{5}$ system where the ground-state wave function can provide the basis for antiferromagnetism and/or unconventional superconductivity. We develop a methodology to understand the local magnetic anisotropy and experimentally investigate with neutron spectroscopy applied to antiferromagnetic ($T_{N}$=3.8 K) CeRhIn$_{5}$ which is isostructural to $d$-wave superconducting ($T_{c}$=2.3 K) CeCoIn$_{5}$. Through diagonalizing the local crystal field Hamiltonian with discrete tetragonal $\mathrm{C}_{4}$ point group symmetry and coupling these states with the Random Phase Approximation (RPA), we find two distinct modes polarized along the crystallographic $c$ and $a-b$ planes, agreeing with experiment. The anisotropy and bandwidth, underlying the energy scale of these modes, are tuneable with a magnetic field which we use experimentally to separate in energy single and multiparticle excitations thereby demonstrating the instability of excitations polarized within the crystallographic $a-b$ plane in CeRhIn$_{5}$. We compare this approach to a $S_{eff}={1\over 2}$ parameterizations and argue for the need to extend conventional SU(2) theories of magnetic excitations to utilize the multi-level nature of the underlying crystal-field basis states constrained by the local point-group $\mathrm{C}_{4}$ symmetry.

cond-mat.str-el↗

arXiv2023

Superconducting pairing symmetry in MoTe$_{2}$

Topological superconductors have long been sought for their potential use in quantum computing. The type-II Weyl semimetal MoTe$_{2}$ is an obvious candidate, exhibiting a superconducting state below 500 mK at ambient pressure, but the question remains whether the pairing is conventional $s^{++}$ or topological $s^{+-}$. The application of external pressure favors the superconducting state in MoTe$_{2}$ and suppresses the structural transition from $1T'$ to $T_{d}$. The competition between the two structures leads to a mixed phase that strongly enhances the disorder present in the system, remarkably without affecting the superconducting transition temperature, in contrast to the expectation of $s^{+-}$ pairing superconductivity. Our thorough analysis of the electrical and Hall resistivities as a function of pressure yields the most accurate temperature-pressure phase diagram available to date for MoTe$_{2}$ and a detailed view of the relationship between disorder and superconductivity, supporting a conventional $s^{++}$ pairing symmetry.

cond-mat.supr-con↗

arXiv2023

Coherent Spin-Phonon Coupling in the Layered Ferrimagnet Mn3Si2Te6

We utilize ultrafast photoexcitation to drive coherent lattice oscillations in the layered ferrimagnetic crystal Mn3Si2Te6, which significantly stiffen below the magnetic ordering temperature. We suggest that this is due to an exchange-mediated contraction of the lattice, stemming from strong magneto-structural coupling in this material. Additionally, simulations of the transient incoherent dynamics reveal the importance of spin relaxation channels mediated by optical and acoustic phonon scattering. Our findings highlight the importance of spin-lattice coupling in van der Waals magnets and a promising route for their dynamic optical control through their intertwined electronic, lattice, and spin degrees of freedom.

cond-mat.mtrl-sci↗

arXiv2023

Electronic transport and thermoelectricity in selenospinel Cu$_{6-x}$Fe$_{4+x}$Sn$_{12}$Se$_{32}$

We report a study of selenospinel Cu$_{6-x}$Fe$_{4+x}$Sn$_{12}$Se$_{32}$ ($x$ = 0, 1, 2) single crystals, which crystalize in a cubic structure with the $Fd\overline{3}m$ space group, and show typical semiconducting behavior. The large discrepancy between the activation energy for electrical conductivity $E_ρ$ (32.3 $\sim$ 69.8 meV), and for thermopower $E_\textrm{S}$ (3.2 $\sim$ 11.5 meV), indicates a polaronic transport mechanism between 350 and 50 K. With decreasing temperature, it evolves into variable-range hopping conduction. Furthermore, the heat capacity shows a hump around 25(5) K and diverges from the Debye $T^3$ law at low temperatures, indicating the observation of structural glassy features in these crystalline solids.

cond-mat.mtrl-sci↗

arXiv2023

Interplay of Hidden Orbital Order and Superconductivity in CeCoIn5

Visualizing atomic-orbital degrees of freedom is a frontier challenge in scanned microscopy. Some types of orbital order are virtually imperceptible to normal scattering techniques because they do not reduce the overall crystal lattice symmetry. A good example is dxz/dyz (π,π) orbital order in tetragonal lattices. For enhanced detectability, here we consider the quasiparticle scattering interference (QPI) signature of such (π,π) orbital order in both normal and superconducting phases. The theory reveals that sublattice-specific QPI signatures generated by the orbital order should emerge strongly in the superconducting phase. Sublattice-resolved QPI visualization in superconducting CeCoIn5 then reveals two orthogonal QPI patterns at lattice-substitutional impurity atoms. We analyze the energy dependence of these two orthogonal QPI patterns and find the intensity peaked near E=0, as predicted when such (π) orbital order is inte,πrtwined with d-wave superconductivity. Sublattice-resolved superconductive QPI techniques thus represent a new approach for study of hidden orbital order.

cond-mat.str-el↗

arXiv2023

Optical conductivity and vibrational spectra of the narrow-gap semiconductor FeGa$_3$

Intermetallic narrow-gap semiconductors have been intensively explored due to their large thermoelectric power at low temperatures and a possible role of strong electronic correlations in their unusual thermodynamic and transport properties. Here we study the optical spectra and vibrational properties of $\mathrm{FeGa_3}$ single crystal. The optical conductivity indicates that $\mathrm{FeGa_3}$ has a direct band gap of $\sim 0.7$\,eV, consistent with density functional theory (DFT) calculations. Most importantly, we find a substantial spectral weight also below 0.4~eV, which is the energy of the indirect (charge) gap found in resistivity measurements and ab initio calculations. We find that the spectral weight below the gap decreases with increasing temperature, which indicates that it originates from the impurity states and not from the electronic correlations. Interestingly, we did not find any signatures of the impurity states in vibrational spectra. The infrared and Raman vibrational lines are narrow and weakly temperature dependent. The vibrational frequencies are in excellent agreement with our DFT calculations, implying a modest role of electronic correlations. Narrow M\" ossbauer spectral lines also indicate high crystallinity of the sample.

cond-mat.str-el↗

arXiv2023

Enhanced Magnetization from Proton Irradiated Bulk van der Waals Magnet CrSiTe3

Van der Waals (vdWs) crystals have attracted a great deal of scientific attention due to their interesting physical properties and widespread practical applications. Among all, CrSiTe3 (CST) is a ferromagnetic semiconductor with the Curie temperature (TC) of ~32 K. In this letter, we study the magnetic properties of bulk CST single-crystal upon proton irradiation with the fluence of 1x1018 protons/cm2. Most significantly, we observed an enhancement (23%) in the saturation magnetization from 3.9 μB to 4.8 μB and is accompanied by an increase in the coercive field (465-542 Oe) upon proton irradiation. Temperature-dependent X-band electron paramagnetic resonance measurements show no additional magnetically active defects/vacancies that are generated upon proton irradiation. The findings from X-ray photoelectron spectroscopy and Raman measurements lead us to believe that modification in the spin-lattice coupling and introduction of disorder could cause enhancement in saturation magnetization. This work demonstrates that proton irradiation is a feasible method in modifying the magnetic properties of vdWs crystals, which represents a significant step forward in designing future spintronic and magneto-electronic applications.

cond-mat.mtrl-sci↗

arXiv2023

Proton-fluence dependent magnetic properties of exfoliable quasi-2D van der Waals Cr2Si2Te6 magnet

The discovery of long-range magnetic ordering in atomically thin materials catapulted the van der Waals (vdW) family of compounds into an unprecedented popularity. In particular, with a current push in space exploration, it is beneficial to study how the properties of such materials evolve under proton irradiation. Owing to their robust intra-layer stability and sensitivity to external perturbations, these materials provide excellent opportunities for studying proton irradiation as a non-destructive tool for controlling their magnetic properties. Specifically, the exfoliable Cr2Si2Te6 (CST) is a ferromagnetic semiconductor with the Curie temperature (TC) of ~32 K. Here, we have investigated the magnetic properties of CST upon proton irradiation as a function of fluence (1 x 1015, 5 x 1015, 1 x 1016, 5 x 1016, and 1 x 1018 H+/cm2) by employing variable-temperature, variable-field magnetization measurements coupled with electron paramagnetic resonance (EPR) spectroscopy and detail how the magnetization, magnetic anisotropy and EPR spectral parameters vary as a function of proton fluence across the magnetic phase transition. While the TC remains constant as a function of proton fluence, we observed that the saturation magnetization and magnetic anisotropy diverge at the proton fluence of 5 x 1016 H+/cm2, which is prominent in the ferromagnetic phase, in particular. This work demonstrates that proton irradiation is a feasible method for modifying the magnetic properties and local magnetic interactions of vdWs crystals, which represents a significant step forward in the design of future spintronic and magneto-electronic applications.

cond-mat.mtrl-sci↗

arXiv2023

Optical fingerprints of the electronic band reconstruction in van der Waals magnetic materials

We report a broadband study of the charge dynamics in the van der Waals (vdW) magnetic materials 2H-$M_x$TaS$_2$ ($M$ = Mn and Co), which span the onset of both long-range antiferromagnetic (AFM) and ferromagnetic (FM) order, depending on the intercalation $M$ and its concentration $x$. We discover a spectral weight ($SW$) shift from high to low energy scales for FM compositions, while reversely $SW$ is removed from low towards high spectral energies for AFM compounds. This maps the related reconstruction of the electronic band structure along the crossover from the FM to AFM order, which restores an occupation balance in the density of states between spin majority and minority bands of the intercalated 3$d$ elements.

cond-mat.mtrl-sci↗

arXiv2022

Thermal transport properties of IrSbSe

We report a thermal transport study of IrSbSe, which crystallizes in a noncentrosymmetric cubic structure with the $P2_13$ space group and shows a narrow-gap semiconducting behavior. The large discrepancy between the activation energy for conductivity [$E_ρ$ = 128(2) meV] and for thermopower [$E_S$ = 17.7(9) meV] from 200 to 300 K indicates the polaronic transport mechanism. Electrical resistivity varies as $exp(T_0/T)^{1/4}$ and thermopower varies as $T^{1/2}$ at low temperatures, indicating that it evolves into the Mott's variable-range hopping dominant conduction with decreasing temperature. IrSbSe shows relatively low value of thermal conductivity ($\sim$ 1.65 W/K$\cdot$m) and thermopower of about 0.24 mV/K around 100 K, yet poor electrical conductivity. On the other hand, high vacancy defect concentration on both Ir and Sb atomic sites of up to 15\%, suggests high defect tolerance and points to possibility of future improvement of carrier density by chemical substitution or defect optimization.

cond-mat.str-el↗

arXiv2022

Enhanced Superconductivity and Electron Correlations in Intercalated ZrTe$_3$

Charge density waves (CDWs) with superconductivity, competing Fermi surface instabilities and collective orders, have captured much interest in two-dimensional van der Waals (vdW) materials. Understanding of CDW suppression mechanism, its connection to emerging superconducting state and electronic correlations provides opportunities for engineering the electronic properties of vdW heterostructures and thin film devices. Using combination of the thermal transport, X-ray photoemission spectroscopy, Raman measurements, and first-principle calculations, we observe an increase in electronic correlations of the conducting states as CDW is suppressed in ZrTe$_3$ with 5\% Cu and Ni intercalation in the vdW gap. As superconductivity emerges, intercalation brings decoupling of quasi-one-dimensional conduction electrons with phonons as a consequence of intercalation-induced lattice expansion but also a drastic increase in Zr$^{2+}$ at the expense of Zr$^{4+}$ metal atoms. These observation demonstrate the potential of atomic intercalates in vdW gap for ground state tuning but also illustrate the crucial role of Zr metal valence in formation of collective electronic orders.

cond-mat.supr-con↗

arXiv2022

Room temperature ferromagnetism in intercalated Fe3-xGeTe2 van der Waals magnet

Among several well-known transition metal-based compounds, the van der Waals (vdW) Fe3-xGeTe2 (FGT) magnet is a strong candidate for use in two-dimensional (2D) magnetic devices due to its strong perpendicular magnetic anisotropy, sizeable Curie temperature (TC ~ 154 K), and versatile magnetic character that is retained in the low-dimensional limit. While the TC remains far too low for practical applications, there has been a successful push toward improving it via external driving forces such as pressure, irradiation, and doping. Here we present experimental evidence of a novel room-temperature (RT) ferromagnetic phase induced by the electrochemical intercalation of common tetrabutylammonium cations (TBA+) into FGT bulk crystals. We obtained Curie temperatures as high as 350 K with chemical and physical stability of the intercalated compound. The temperature-dependent Raman measurements in combination with vdW-corrected ab initio calculations suggest that charge transfer (electron doping) upon intercalation could lead to the observation of RT ferromagnetism. This work demonstrates that molecular intercalation is a viable route in realizing high-temperature vdW magnets in an inexpensive and reliable manner.

cond-mat.mtrl-sci↗

arXiv2022

Sub-Phases in the Superconducting State of CeIrIn$_5$ Revealed by Low Temperature $c$-axis Heat Transport

Low-temperature (down to $\sim$ 50 mK) thermal conductivity measurements with the heat flow direction along the inter-plane tetragonal $c$-axis, $κ_c$, were used to study the superconducting state of heavy fermion CeIrIn$_5$. Measurements were performed in the magnetic fields both parallel to the heat flow direction, $H\parallel c$, and transverse to it, $H \parallel a$. Inter-plane heat conductivity in $H \parallel c$ configuration shows negligible initial increase with magnetic field and a rapid rise on approaching $H_{c2}$ from below, similar to the expectations for the superconducting gap without line nodes. This observation is in stark contrast to monotonic increase found in the previous in-plane heat transport measurements. In the configuration with the magnetic field breaking the tetragonal symmetry of the lattice, $H \parallel a$, $κ_c$ reveals non-monotonic evolution with temperature and magnetic field suggesting sub-phase boundary in the superconducting state. The characteristic temperature $T_{kink} \sim$ 0.07~K of the sub-boundary is well within the domain of bulk superconductivity $T_c \sim$ 0.4~K and $H_{c2}\sim$ 1.0~T. These results are consistent with a superconducting gap with an equatorial line node and polar point nodes, a gap symmetry of the D$_{4h}$ point group, for which magnetic field along the tetragonal plane breaks the degeneracy of the multi-component order parameter and induces a phase transition with nodal topology change.

cond-mat.supr-con↗

arXiv2022

The scaled-invariant Planckian metal and quantum criticality in Ce$_{1-x}$Nd$_x$CoIn$_5$

Perfect $T$-linear resistivity associated with universal scattering rate: $1/τ=αk_B T/\hbar$ with $α\sim 1$, so-called Planckian metal state, has been observed in the normal state of a variety of strongly correlated superconductors close to a quantum critical point. However, the microscopic origin of this intriguing phenomena and its link to quantum criticality still remains an outstanding open problem. In this work, we observe the quantum-critical $T/B$-scaling of the Planckian metal state in the resistivity and heat capacity of heavy-electron superconductor Ce$_{1-x}$Nd$_x$CoIn$_5$ in magnetic fields near the edge of antiferromagnetism, driven by critical Kondo hybridization at the critical doping $x_c \sim 0.03$. We further provide the first microscopic mechanism to account for the Planckian state in a quantum critical system based on the critical charge fluctuations near Kondo breakdown transition at $x_c$ within the quasi-two-dimensional Kondo-Heisenberg lattice model. This mechanism simultaneously captures the observed universal Planckian scattering rate as well as the quantum-critical scaling and power-law divergence in thermodynamic observables near criticality. Our mechanism is generic to Planckian metal states in a variety of quantum critical superconductors near Kondo destruction.

cond-mat.str-el↗

arXiv2022

Polaronic Conductivity in Cr$_2$Ge$_2$Te$_6$ Single Crystals

Intrinsic, two-dimensional (2D) ferromagnetic semiconductors are an important class of materials for spin-charge conversion applications. Cr$_2$Ge$_2$Te$_6$ retains long-range magnetic order in bilayer at cryogenic temperatures and shows complex magnetic interactions with considerable magnetic anisotropy. Here, we performed a series of structural, magnetic, X-ray scattering, electronic, thermal transport and first-principles calculation studies which reveal that localized electronic charge carriers in Cr$_2$Ge$_2$Te$_6$ are dressed by surrounding lattice and are involved in polaronic transport via hopping that is sensitive on details of magnetocrystalline anisotropy. This opens possibility for manipulation of charge transport in Cr$_2$Ge$_2$Te$_6$ - based devices by electron-phonon- and spin-orbit coupling-based tailoring of polaron properties.

cond-mat.mtrl-sci↗

arXiv2022

Thermal transport and mixed valence in ZrTe$_3$ doped with Hf and Se

Two-dimensional transition metal trichalcogenides (TMTC's) feature covalently bonded metal-chalcogen layers separated by the van der Waals (vdW) gap. Similar to transition metal dichalcogenides (TMDCs), TMTCs often host charge density waves (CDWs) and superconductivity but unlike TMDCs atomic chains in the crystal structure give rise to quasi one-dimensional (quasi 1D) conduction. ZrTe$_3$ features CDW below $T_{\textrm{CDW}}$ = 63 K and filamentary superconductivity below 2 K that can be enhanced by pressure or chemical substitution. Here we report the presence of mixed valent Zr$^{2+}$ and Zr$^{4+}$ atoms in ZrTe$_3$ crystals that is reduced by doping in ZrTe$_{3-x}$Se$_x$ and Zr$_{1-y}$Hf$_y$Te$_3$. Superconductivity is enhanced via disorder in Te2-Te3 atomic chains that are associated with CDW formation. Hf substitution on Zr atomic site enhances $T_{\textrm{CDW}}$ due to unperturbed Te2-Te3 chain periodicity and enhanced electron-phonon coupling. Weak electronic correlations in ZrTe$_{3-x}$Se$_x$ are likely governed by the lattice contraction effects.

cond-mat.str-el↗

arXiv2022

Thermoelectricity and electronic correlations enhancement in FeS by slight Se substitution

We report thermoelectric studies of FeS$_{1-x}$Se$_x$ ($x$ = 0, 0.06) superconducting single crystals that feature high irreversibility fields and critical current density $J_c$ comparable to materials with much higher superconducting critical temperatures ($T_c$'s). The ratio of $T_c$ to the Fermi temperature $T_F$ is very small indicating weak electronic correlations. With a slight selenium substitution on sulfur site in FeS both $T_c$/$T_F$ and the effective mass $m^*$ rise considerably, implying increase in electronic correlation of the bulk conducting states. The first-principle calculations show rise of the density of states at the Fermi level in FeS$_{0.94}$Se$_{0.06}$ when compared to FeS which is related not only to Fe but also to chalcogen-derived electronic states.

cond-mat.supr-con↗