arXiv subjects

F. O. von Rohr

Publications and source records attributed to F. O. von Rohr.

At least 19 recordsLinked to original sources

arXiv2026

Correlated charge order intertwined with time-reversal symmetry-breaking nodal superconductivity in the dual flat band kagome superconductor CeRu$_{3}$Si$_{2}$

Kagome materials provide a powerful platform for exploring how flat electronic bands promote symmetry-breaking quantum states, yet studies have so far focused mainly on kagome-derived $d$-electron flat bands. In this paper, we introduce CeRu$_{3}$Si$_{2}$, a kagome superconductor in which our first-principles calculations show the coexistence of Ru $d$-orbital kagome flat bands and heavy-fermion flat bands derived from Ce$^{4+}$ $4f$-states. X-ray diffraction reveals a dominant 1/2 charge order with a much weaker 1/3 component persisting up to room temperature. Theoretical calculations further highlight the correlated nature of these charge-order states. Deep within the charge-ordered state, magnetoresistance emerges below 80 K and strengthens further below 30 K. Zero-field muon spin-rotation measurements show no time-reversal symmetry (TRS) breaking in the normal state, in contrast to LaRu$_{3}$Si$_{2}$ and YRu$_{3}$Si$_{2}$. However, an applied magnetic field induces weak magnetism. Across the $A$Ru$_{3}$Si$_{2}$ family ($A$ = La, Y, and Ce), the superconducting transition temperature $T_{\rm c}$ scales linearly with the onset temperature of normal-state TRS breaking $T_{\rm {TRSB}}$ and the magnitude of the field-induced magnetic response, revealing a direct positive correlation between normal-state symmetry breaking and superconductivity. Furthermore, we identify that CeRu$_{3}$Si$_{2}$ is the first 132-type kagome compound to host nodal superconductivity together with spontaneous internal magnetic fields, providing clear evidence for intrinsic TRS breaking in the superconducting state. These results establish CeRu$_{3}$Si$_{2}$ as a unique platform where intertwined kagome $d$- and heavy fermion $f$-electron flat bands generate a rich hierarchy of electronic orders.

cond-mat.supr-con↗

arXiv2025

Ultrafast recovery dynamics of dimer stripes in IrTe2

The transition metal dichalcogenide IrTe2 displays a remarkable series of first-order phase transitions below room temperature, involving lattice displacements as large as 20 percents of the initial bond length. This is nowadays understood as the result of strong electron-phonon coupling leading to the formation of local multicentre dimers that arrange themselves into one-dimensional stripes. In this work, we study the out-of-equilibrium dynamics of these dimers and track the time evolution of their population following an infrared photoexcitation using free-electron lased-based time-resolved X-ray photoemission spectroscopy. First, we observe that the dissolution of dimers is driven by the transfer of energy from the electronic subsystem to the lattice subsystem, in agreement with previous studies. Second, we observe a surprisingly fast relaxation of the dimer population on the timescale of a few picoseconds. By comparing our results to published ultrafast electron diffraction and angle-resolved photoemission spectroscopy data, we reveal that the long-range order needs tens of picoseconds to recover, while the local dimer distortion recovers on a short timescale of a few picoseconds.

cond-mat.str-el↗

arXiv2025

Discovery of High-Temperature Charge Order and Time-Reversal Symmetry-Breaking in the Kagome Superconductor YRu3Si2

The identification of high-temperature unconventional charge order and superconductivity in kagome quantum materials is pivotal for deepening our understanding of geometrically frustrated and correlated electron systems, and for harnessing their exotic properties in future quantum technologies. Here, we report the discovery of a remarkably rich phase diagram in the kagome superconductor YRu$_{3}$Si$_{2}$, uncovered through a unique combination of muon spin rotation ($μ$SR), magnetotransport, X-ray diffraction (XRD), and density functional theory (DFT) calculations. Our study reveals the emergence of a charge-ordered state with a propagation vector of (1/2, 0, 0), setting a record onset temperature of 800 K for such an order in a kagome system and for quantum materials more broadly. In addition, we observe time-reversal symmetry (TRS) breaking below $T_{2}^{*}$ ${\simeq}$ 25 K and field-induced magnetism below $T_{1}^{*}$ ${\simeq}$ 90 K, indicating the presence of a hidden magnetic state. These transitions are mirrored in the magnetoresistance data, which show a clear onset at ${\sim}$ $T_{1}^{*}$ and a pronounced increase below ${\sim}$ $T_{2}^{*}$, ultimately reaching a maximum magnetoresistance of 45${\%}$. Band structure calculations identify two van Hove singularities (VHSs) near the Fermi level, one of which resides within a flat band, suggesting a strong interplay between electronic correlations and emergent orders. At low temperatures, we find bulk superconductivity below $T_{\rm c}$ = 3.4 K, characterized by a pairing symmetry with either two isotropic full gaps or an anisotropic nodeless gap. Together, our findings point to a coexistence of high-temperature charge order, tunable magnetism, and multigap superconductivity in YRu$_{3}$Si$_{2}$, positioning it as a compelling platform for exploring correlated kagome physics.

cond-mat.supr-con↗

arXiv2025

Competing Quantum Orders in 6R-TaS$_2$: Unconventional Superconductivity, Charge Order, and an Anomalous Hall Effect phase

The transition metal dichalcogenide 6R-TaS$_{2}$ offers a natural platform for studying the interplay among charge density wave (CDW) order, superconductivity, and transport anomalies. Recent findings reveal that, in the intermediate temperature range between charge order and superconductivity, a hidden order emerges around $T^{*}$ ${\simeq}$ 35 K-as evidenced by strong magnetoresistance and an anomalous Hall effect (AHE). However, the nature of the superconducting pairing, the hidden order, and their relationship with the CDW remain unclear. Using $μ$SR, magnetotransport, susceptibility, and hydrostatic pressure techniques, we identify a nodal superconducting state with low superfluid density at ambient pressure, with no spontaneous magnetic order detected below $T^{*}$. This indicates that the AHE originates from the band structure rather than magnetism. Under pressures up to 2 GPa, the superfluid density rises markedly in correlation with the superconducting transition temperature, the nodal pairing shifts to a nodeless state, and the CDW onset is reduced by half. Notably, AHE is fully suppressed and magnetoresistance drops by 50${\%}$ within just 0.2 GPa, highlighting the fragility of the hidden order. These results reveal an unconventional superconducting pairing in 6R-TaS$_{2}$, competing with both CDW and hidden orders through weakened interlayer coupling and competition for the same electronic states. With a multifaceted approach, we establish a comprehensive phase diagram that reveals the intricate interplay and competition between the intertwined quantum orders in 6R-TaS$_{2}$.

cond-mat.supr-con↗

arXiv2024

Pressure-Induced Enhancement of Superfluid Density in Transition Metal Dichalcogenides with and without Charge Density Wave

Gaining a deeper understanding of the interplay between charge density wave (CDW) order and superconductivity in transition metal dichalcogenides (TMDs), particularly within the (4H/2H)-NbX$_{2}$ (X=Se,S) family, remains an open and intriguing challenge. A systematic microscopic study across various compounds in this family is therefore required to unravel this complex interplay. Here, we report on muon spin rotation and magnetotransport experiments investigating the effects of hydrostatic pressure on the superconducting transition temperature ($T_{\rm c}$), the temperature-dependent magnetic penetration depth ($λ_\mathrm{eff}$), and the charge density wave order (CDW) in two layered chalcogenide superconductors: 4H-NbSe$_{2}$, which exhibits CDW order, and 2H-NbS$_{2}$, which lacks such order. Our observations reveal a substantial 75$\%$ enhancement of the superfluid density ($n_{s}/m^{*}$) in 4H-NbSe$_{2}$ upon maximum applied pressure of 2 GPa, surpassing that of 2H-NbSe$_{2}$. Despite the absence of CDW order, a sizeable 20$\%$ growth in superfluid density is also observed for 2H-NbS$_{2}$ under an applied pressure of 1.8 GPa. Notably, the evaluated superconducting gaps in all these TMDs remain largely unaffected by changes in applied pressure, irrespective of pressure-induced partial suppression of CDW order in (4H/2H)-NbSe$_{2}$ or its general absence in 2H-NbS$_{2}$. These results underscore the complex nature of pressure-induced behaviors in these TMDs, challenging a simplistic view of competition solely between CDW order and superconductivity. Remarkably, the relationship between $n_{s}/m^{*}$ and $T_{\rm c}$ exhibits an unconventional correlation, indicating a noteworthy similarity with the behavior observed in cuprate, kagome, and iron-based superconductors.

cond-mat.supr-con↗

arXiv2024

Dome-Shaped Superconducting Phase Diagram Linked to Charge Order in LaRu$_{3}$Si$_{2}$

The interplay between superconductivity and charge order is a central focus in condensed matter research, with kagome lattice systems offering unique insights. The kagome superconductor LaRu$_{3}$Si$_{2}$ ($T_{\rm c}$ ${\simeq}$ 6.5 K) exhibits a hierarchy of charge order transitions: primary ($T_{\rm co,I}$ ${\simeq}$ 400 K), secondary ($T_{\rm co,II}$ ${\simeq}$ 80 K), and an additional transition at ($T^{*}$ $\simeq$ 35 K). The transitions at $T_{\rm co,II}$ and $T^{*}$ are linked to electronic and magnetic responses as revealed by muon-spin rotation and magnetotransport experiments. However, the connection between superconductivity, charge order, and electronic responses has remained elusive. By employing magnetotransport and X-ray diffraction techniques under pressures of up to 40 GPa, we observe that $T_{\rm c}$ rises to 9 K at 2 GPa, remains nearly constant up to 12 GPa, and then decreases to 2 K at 40 GPa, resulting in a dome-shaped phase diagram. The resistivity anomaly at $T^{*}$ and magnetoresistance also exhibit a similar dome-shaped pressure dependence. Furthermore, we find that charge order transitions from long-range to short-range above 12 GPa, correlating with the suppression of $T_{\rm c}$, suggesting superconductivity is closely tied to the charge-ordered state. Specifically, $T_{\rm c}$ peaks when charge order and the normal-state electronic responses are optimized. In contrast to systems like the cuprates, transition metal dichalcogenides, and other kagome materials, where superconductivity typically competes with charge order, LaRu$_{3}$Si$_{2}$ displays a pronounced interdependence between these two phenomena. This distinctive behavior sheds new light on the connection between superconductivity and charge order, offering avenues for theoretical advancements in understanding superconductivity.

cond-mat.supr-con↗

arXiv2024

Nature of metallic and insulating domains in the CDW system 1T-TaSe2

We study the electronic structure of bulk 1T-TaSe$_2$ in the charge density wave phase at low temperature. Our spatially and angle resolved photoemission (ARPES) data show insulating areas coexisting with metallic regions characterized by a chiral Fermi surface and moderately correlated quasiparticle bands. Additionally, high-resolution laser ARPES reveals variations in the metallic regions, with series of low-energy states, whose energy, number and dispersion can be explained by the formation of quantum well states of different thicknesses. Dynamical mean field theory calculations show that the observed rich behaviour can be rationalized by assuming occasional stacking faults of the charge density wave. Our results indicate that the diverse electronic phenomena reported previously in 1T-TaSe$_2$ are dictated by the stacking arrangement and the resulting quantum size effects while correlation effects play a secondary role.

cond-mat.str-el↗

arXiv2024

Bonding states underpinning structural transitions in IrTe$_2$ observed with micro-ARPES

Competing interactions in low-dimensional materials can produce nearly degenerate electronic and structural phases. We investigate the staircase of structural phase transitions in layered IrTe$_2$ for which a number of potential transition mechanisms have been postulated. The spatial coexistence of multiple phases on the micron scale has prevented a detailed analysis of the electronic structure. By exploiting micro-ARPES obtained with synchrotron radiation we extract the electronic structure of the multiple structural phases in IrTe$_2$ in order to address the mechanism underlying the phase transitions. We find direct evidence of lowered energy states that appear in the low-temperature phases, states previously predicted by \textit{ab initio} calculations and extended here. Our results validate a proposed scenario of bonding and anti-bonding states as the driver of the phase transitions.

cond-mat.mtrl-sci↗

arXiv2024

Anomalous Shubnikov-de Haas effect and observation of the Bloch-Grüneisen temperature in the Dirac semimetal ZrTe5

Appearance of quantum oscillations (QO) in both thermodynamic and transport properties of metals at low temperatures is the most striking experimental consequence of the existence of a Fermi surface (FS). The frequency of these oscillations and the temperature dependence of their amplitude provides essential information about the FS topology and fermionic quasiparticle properties. Here, we report the observation of an anomalous suppression of the QO amplitude seen in resistivity (Shubnikov de-Haas effect) at sub-kelvin temperatures in ZrTe5 samples with a single small FS sheet comprising less than 5% of the first Brillouin zone. By comparing these results with measurements of the magneto-acoustic QO and the recovery of the usual Lifshitz-Kosevich behavior of the Shubnikov de-Haas (SdH) effect in ZrTe$_5$ samples with a multi-sheet FS, we show that the suppression of the SdH effect originates from a decoupling of the electron liquid from the lattice. On crossing the so-called Bloch-Grüneisen temperature, T$_BG$, electron-phonon scattering becomes strongly suppressed and in the absence of Umklapp scattering the electronic liquid regains Galilean invariance. In addition, we show, using a combination of zero-field electrical conductivity and ultrasonic-absorption measurements, that entering this regime leads to an abrupt increase of electronic viscosity.

cond-mat.mtrl-sci↗

arXiv2022

The Duel of Magnetic Interactions & Structural Instabilities: Itinerant Frustration in the Triangular Lattice Compound LiCrSe$_2$

The recent synthesis of the chromium selenide compound LiCrSe$_2$ constitutes a valuable addition to the ensemble of two-dimensional triangular lattice antiferromagnets (2D-TLA). In this work we present the very first comprehensive study of the combined low temperature nuclear and magnetic structure established in this material. Details on the connection between Li-ion dynamics and structural changes are also presented along with a direct link between atomic structure and spin order via a strong magnetoelastic coupling. LiCrSe$_2$ was found to undergo a first order structural transition from a trigonal crystal system with space group $P\bar{3}m1$ to a monoclinic one with space group $C2/m$ at $T_{\rm s}=30$~K. Such restructuring of the lattice is accompanied by a magnetic transition at $T_{\rm N}=30$~K, with the formation of a complex spin arrangement for the Cr$^{3+}$ moments. Refinement of the magnetic structure with neutron diffraction data and complementary muon spin rotation analysis reveal the presence of two incommensurate magnetic domains with a up-up-down-down arrangement of the spins with ferromagnetic (FM) double chains coupled antiferromagnetically (AFM). In addition to this unusual arrangement, the spin axial vector is modulated both in direction and modulus, resulting in a spin density wave-like order with periodic suppression of the Cr moment along the chains. This behavior is believed to appear as a result of strong competition between direct exchange AFM and superexchange FM couplings established between both nearest neighbor and next nearest neighbor Cr$^{3+}$ ions. We finally conjecture that the resulting magnetic order is stabilized via subtle vacancy/charge order within the Li layers, potentially causing a mix of two different magnetic phases within the sample.

cond-mat.str-el↗

arXiv2022

Nuclear and magnetic spin structure of the antiferromagnetic triangular lattice compound LiCrTe$_2$ investigated by $μ^+$SR as well as neutron and X-ray diffraction

Two$-$dimensional (2D) triangular lattices antiferromagnets (2D$-$TLA) often manifest intriguing physical and technological properties, due to the strong interplay between lattice geometry and electronic properties. The recently synthesized 2$-$dimensional transition metal dichalcogenide LiCrTe$_2$, being a 2D$-$TLA, enriched the range of materials which can present such properties. In this work, muon spin rotation ($μ^+$SR) and neutron powder diffraction (NPD) have been utilized to reveal the true magnetic nature and ground state of LiCrTe$_2$. From high$-$resolution NPD the magnetic spin order at base$-$temperature is not, as previously suggested, helical, but rather collinear antiferromagnetic (AFM) with ferromagnetic (FM) spin coupling within the $ab-$plane and AFM coupling along the $c-$axis. The ordered magnetic Cr moment is established as $μ_{\rm Cr}=$ 2.36 $μ_{\rm B}$. From detailed $μ^+$SR measurements we observe an AFM ordering temperature $T_{\rm N}\approx$ 125 K. This value is remarkably higher than the one previously reported by magnetic bulk measurements. From $μ^+$SR we are able to extract the magnetic order parameter, whose critical exponent allows us to categorize LiCrTe$_2$ in the 3D Heisenberg AFM universality class. Finally, by combining our magnetic studies with high$-$resolution synchrotron X$-$ray diffraction (XRD), we find a clear coupling between the nuclear and magnetic spin lattices. This suggests the possibility for a strong magnon$-$phonon coupling, similar to what has been previously observed in the closely related compound LiCrO$_2$.

cond-mat.str-el↗

arXiv2021

Insensitivity of the striped charge-orders in IrTe$_2$ to alkali surface doping implies their structural origin

We present a combined angle-resolved photoemission spectroscopy and low-energy electron diffraction (LEED) study of the prominent transition metal dichalcogenide IrTe$_2$ upon potassium (K) deposition on its surface. Pristine IrTe$_2$ undergoes a series of charge-ordered phase transitions below room temperature that are characterized by the formation of stripes of Ir dimers of different periodicities. Supported by density functional theory calculations, we first show that the K atoms dope the topmost IrTe$_2$ layer with electrons, therefore strongly decreasing the work function and shifting only the electronic surface states towards higher binding energy. We then follow the evolution of its electronic structure as a function of temperature across the charge-ordered phase transitions and observe that their critical temperatures are unchanged for K coverages of $0.13$ and $0.21$~monolayer (ML). Using LEED, we also confirm that the periodicity of the related stripe phases is unaffected by the K doping. We surmise that the charge-ordered phase transitions of IrTe$_2$ are robust against electron surface doping, because of its metallic nature at all temperatures, and due to the importance of structural effects in stabilizing charge order in IrTe$_2$.

cond-mat.str-el↗

arXiv2021

Ultrafast Dynamics of the Surface Photovoltage in Potassium Doped Black Phosphorus

Black phosphorus is a quasi-two-dimensional layered semiconductor with a narrow direct band gap of 0.3 eV. A giant surface Stark effect can be produced by the potassium doping of black phosphorus, leading to a semiconductor to semimetal phase transition originating from the creation of a strong surface dipole and associated band bending. By using time- and angle-resolved photoemission spectroscopy, we report the partial photoinduced screening of this band bending by the creation of a compensating surface photovoltage. We further resolve the detailed dynamics of this effect at the pertinent timescales and the related evolution of the band structure near the Fermi level. We demonstrate that after a fast rise time, the surface photovoltage exhibits a plateau over a few tens of picoseconds before decaying on the nanosecond timescale. We support our experimental results with simulations based on drift-diffusion equations.

cond-mat.mtrl-sci↗

arXiv2021

Observation of a uniaxial strain-induced phase transition in the 2D topological semimetal IrTe$_2$

Strain is ubiquitous in solid-state materials, but despite its fundamental importance and technological relevance, leveraging externally applied strain to gain control over material properties is still in its infancy. In particular, strain control over the diverse phase transitions and topological states in two-dimensional (2D) transition metal dichalcogenides (TMDs) remains an open challenge. Here, we exploit uniaxial strain to stabilize the long-debated structural ground state of the 2D topological semimetal IrTe$_2$, which is hidden in unstrained samples. Combined angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM) data reveal the strain-stabilized phase has a 6x1 periodicity and undergoes a Lifshitz transition, granting unprecedented spectroscopic access to previously inaccessible type-II topological Dirac states that dominate the modified inter-layer hopping. Supported by density functional theory (DFT) calculations, we show that strain induces a charge transfer strongly weakening the inter-layer Te bonds and thus reshaping the energetic landscape of the system in favor of the 6x1 phase. Our results highlight the potential to exploit strain-engineered properties in layered materials, particularly in the context of tuning inter-layer behavior.

cond-mat.str-el↗

arXiv2020

Examining the surface phase diagram of IrTe$_2$ with photoemission

In the transition metal dichalcogenide IrTe$_2$, low-temperature charge-ordered phase transitions involving Ir dimers lead to the occurrence of stripe phases of different periodicities, and nearly degenerate energies. Bulk-sensitive measurements have shown that, upon cooling, IrTe$_2$ undergoes two such first-order transitions to $(5\times1\times5)$ and $(8\times1\times8)$ reconstructed phases at $T_{c_1}\sim 280$~K and $T_{c_2}\sim 180$~K, respectively. Here, using surface sensitive probes of the electronic structure of IrTe$_2$, we reveal the first-order phase transition at $T_{c_3}=165$~K to the $(6\times1)$ stripes phase, previously proposed to be the surface ground state. This is achieved by combining x-ray photoemission spectroscopy and angle-resolved photoemission spectroscopy, which give access to the evolution of stripe domains and a particular surface state, the energy of which is dependent on the Ir dimer length. By performing measurements over a full thermal cycle, we also report the complete hysteresis of all these phases.

cond-mat.str-el↗

arXiv2020

Pressure induced topological quantum phase transition in Weyl semimetal T_d-MoTe_2

We report the pressure (p_max = 1.5 GPa) evolution of the crystal structure of the Weyl semimetal T_d-MoTe_2 by means of neutron diffraction experiments. We find that the fundamental non-centrosymmetric structure T_d is fully suppressed and transforms into a centrosymmertic 1T' structure at a critical pressure of p_cr = 1.2 GPa. This is strong evidence for a pressure induced quantum phase transition (QPT) between topological to a trivial electronic state. Although the topological QPT has strong effect on magnetoresistance, it is interesting that the superconducting critical temperature T_c, the superfluid density, and the SC gap all change smoothly and continuously across p_cr and no sudden effects are seen concomitantly with the suppression of the T_d structure. This implies that the T_c, and thus the SC pairing strength, is unaffected by the topological QPT. However, the QPT requires the change in the SC gap symmetry from non-trivial s+- to a trivial s++ state, which we discuss in this work. Our systematic characterizations of the structure and superconducting properties associated with the topological QPT provide deep insight into the pressure induced phase diagram in this topological quantum material.

cond-mat.mtrl-sci↗

arXiv2019

Linear Scaling of the Superfluid Density with the Critical Temperature in the Layered Superconductor 2H-NbSe_2

We report on high-pressure (p_max = 2.1 GPa) muon spin rotation experiments probing the temperature-dependent magnetic penetration depth in the layered superconductor 2H-NbSe_2. Upon increasing the pressure, we observe a substantial increase of the superfluid density n_s, which we find to scale linearly with T_c. This linear scaling is considered a hallmark feature of unconventional superconductivity, especially in high-temperature cuprate superconductors. Our current results, along with our earlier findings on 1T'-MoTe_2 (Z. Guguchia et. al., Nature Communications 8, 1082 (2017)), demonstrate that this linear relation is also an intrinsic property of the superconductivity in transition metal dichalcogenides, whereas the ratio T_c/T_F is approximately a factor of 20 lower than the ratio observed in hole-doped cuprates. We, furthermore, find that the values of the superconducting gaps are insensitive to the suppression of the quasi-two-dimensional CDW state, indicating that the CDW ordering and the superconductivity in 2H-NbSe_2 are independent of each other.

cond-mat.supr-con↗

arXiv2019

Low-energy excitations in type-II Weyl semimetal Td-MoTe2 evidenced through optical conductivity

Molybdenum ditelluride, MoTe2, is a versatile material where the topological phase can be readily tuned by manipulating the associated structural phase transition. The fine details of the band structure of MoTe2, key to understanding its topological properties, have proven difficult to disentangle experientially due to the multi-band character of the material. Through experimental optical conductivity spectra, we detect two strong low-energy interband transitions. Both are linked to excitations between spin-orbit split bands. The lowest interband transition shows a strong thermal shift, pointing to a chemical potential that dramatically decreases with temperature. With the help of ab initio calculations and a simple two-band model, we give qualitative and quantitative explanation of the main features in the temperature-dependent optical spectra up to 400 meV.

cond-mat.mtrl-sci↗