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S. Krämer

Publications and source records attributed to S. Krämer.

At least 19 recordsLinked to original sources

Magnetic-field-induced Tomonaga-Luttinger liquid and Bose-Einstein condensate phases in an organic S=1 Haldane chain

We present a comprehensive low-temperature $^1$H nuclear magnetic resonance (NMR) study of magnetic field-induced phases and spin fluctuations in an isotropic Haldane chain system $m$-NO$_2$PhBNO (BoNO) in fields up to 34 T. NMR spectral and $T_1^{-1}$ relaxation rate data are used to map out the transition temperature $T_c(B)$ and we show that it defines a complete phase boundary between the field-induced Bose-Einstein condensate (BEC) and Tomonaga-Luttinger liquid (TLL) phases by reproducing its shape via quantum Monte Carlo calculations. We also observe the theoretical critical behavior $T_c (B) \propto (B-B_\text{c2})^ν$ with $ν= 2/3$ and universal quasiparticle scaling in the low-temperature limit close to $B_\text{c2}$. The extensive Bayesian inference analysis of the temperature and field dependence of $T_1 ^{-1} (T,B)$ reveals attractive interactions across the TLL phase of a Haldane chain. Our results are further corroborated by magnetostriction measurements in pulsed magnetic fields and density matrix renormalization group calculations.

cond-mat.str-el↗

Signatures of a high-temperature collective electronic phase with superconductivity-like characteristics and a giant pressure effect in networks of boron-doped ultrathin carbon nanotubes

We present data consistent with a high-temperature collective electronic phase with superconductivity-like characteristics in three dimensional networks of boron doped, ultrathin carbon nanotubes (CNTs) grown inside the 5 Angstrom channels of ZSM-5 zeolite. Confinement stabilizes (2,1) CNTs that are otherwise dynamically unstable, while boron doping shifts the Fermi level towards a van Hove singularity, as supported by ab-initio calculations. The resulting CNT network exhibits multiple, mutually consistent signatures of an electronic condensate with the typical characteristics of a high temperature superconductor at ambient pressure. DC magnetization and AC susceptibility measurements reveal the onset of a Meissner response between 220 and 250K, with compacted samples achieving up to 93 percent of full diamagnetic screening. Electrical transport shows a sharp resistive transition with extrapolated Tc = 239K and vanishing resistance in optimized samples. Specific heat measurements display a reproducible anomaly at 233 to 236 K that broadens under magnetic field, consistent with strong fluctuations. Point contact spectroscopy identifies three energy gaps, including a leading gap of 30 meV whose temperature dependence follows BCS expectations for Tc = 224K, and exhibits particle-hole symmetry and Andreev reflection. Remarkably, applying pressures below 0.1 kbar enhances Tc by nearly 100K and modulates the room temperature resistance by more than three orders of magnitude, suggesting a pressure driven 1D to 3D crossover in the CNT network. These results identify boron doped ultrathin CNT networks as a promising carbon-based platform for near ambient temperature superconductivity and reveal an unusually large pressure sensitivity with potential technological relevance.

cond-mat.supr-con↗

Field-induced antiferromagnetic transition in CeIrIn$_5$

We report low-temperature $^{115}$In nuclear magnetic resonance (NMR) study of the prototypical heavy-fermion compound CeIrIn$_5$ in high magnetic fields applied close to the crystallographic $c$ axis. For this orientation, a field-induced transition was previously reported to take place at about 28 T. Although we do not observe any change of the NMR spectrum above the transition, the intensity of the NMR lines drastically decreases as a consequence of a considerable shortening of the $T_2$ relaxation time. In addition, $1/T_1$ shows a pronounced maximum at the transition. Taking into account previous high-field de Haas-van Alphen results in conjunction with band-structure calculations, our NMR results are most naturally explained by the field-induced transition into an antiferromagnetic state with the propagation vector $\mathbf{Q} = (1/2, 1/2, 0)$ and magnetic moments aligned antiferromagnetically along the $c$ axis. This makes CeIrIn$_5$ a unique case where the application of the magnetic field induces an ordered state with moments antiferromagnetically aligned along the field direction.

cond-mat.str-el↗

Spin-stripe order tied to the pseudogap phase in La1.8-xEu0.2SrxCuO4

Although spin and charge stripes in high-Tc cuprates have been extensively studied, the exact range of carrier concentration over which they form a static order remains uncertain, complicating efforts to understand their significance. In La2-xSrxCuO4 (LSCO) and in zero external magnetic field, static spin stripes are confined to a doping range well below p*, the pseudogap boundary at zero temperature. However, when high fields suppress the competing effect of superconductivity, spin stripe order is found to extend up to p*. Here, we investigated La1.8-xEu0.2SrxCuO4 (Eu-LSCO) using 139La nuclear magnetic resonance and observe field-dependent spin fluctuations suggesting a similar competition between superconductivity and spin order as in LSCO. Nevertheless, we find that static spin stripes are present practically up to p* irrespective of field strength: the stronger stripe order in Eu-LSCO prevents superconductivity from enforcing a non-magnetic ground state, except very close to p*. Thus, spin-stripe order is consistently bounded by p* in both LSCO and Eu-LSCO, despite their differing balances between stripe order and superconductivity. This indicates that the canonical stripe order, where spins and charges are intertwined in a static pattern, is fundamentally tied to the pseudogap phase, though the exact nature of this connection has yet to be elucidated. Any stripe order beyond the pseudogap endpoint must then be of a different nature: either spin and charge orders remain intertwined, but both fluctuating, or only spin order fluctuates while charge order remains static. The presence of spin-stripe order up to p*, the pervasive, slow, and field-dependent spin-stripe fluctuations, as well as the electronic inhomogeneity documented in this work, must all be carefully considered in discussions of Fermi surface transformations, quantum criticality, and strange metal behavior.

cond-mat.supr-con↗

Signatures of two gaps in the spin susceptibility of a cuprate superconductor

A major obstacle to understanding high-Tc cuprates is that superconductivity precludes observing normal-state properties at low temperatures. One prime example is the normal-state spin susceptibility \c{hi}spin: although its decrease upon cooling far above Tc typifies pseudogap behavior, its behavior at low temperatures is generally unknown. Here, our measurements in high magnetic fields expose \c{hi}spin of YBa2Cu3Oy down to low temperatures. Even though superconductivity is suppressed by the field, we uncover two thermally-activated contributions alongside a residual \c{hi}spin(T=0) due to gapless excitations. We relate these two distinct gaps to short-range charge-density waves and to the formation of singlets as in certain quantum spin systems. Both phenomena thus contribute to the pseudogap at low temperature, supplementing short-lived antiferromagnetism that initiates pseudogap behavior at high temperatures. We therefore propose that the pseudogap ought to be regarded as a composite property and that, when not undergoing spin-stripe ordering, underdoped cuprates tend to form short-ranged spin singlets.

cond-mat.supr-con↗

Competition between spin ordering and superconductivity near the pseudogap boundary in La2-xSrxCuO4: insights from NMR

When superconductivity is suppressed by high magnetic fields in La2-xSrxCuO4, striped antiferromagnetic (AFM) order becomes the magnetic ground state of the entire pseudogap regime, up to its end at the doping p* [M. Frachet, I. Vinograd et al., Nat. Phys. 16, 1064 (2020)]. Glass-like freezing of this state is detected in 139La NMR measurements of the spin-lattice relaxation rate 1/T1. Here, we present a quantitative analysis of 1/T1 data in the hole-doping range p=x=0.12-0.171, based on the Bloembergen-Purcell-Pound (BPP) theory, modified to include statistical distribution of parameters arising from strong spatial inhomogeneity. We observe spin fluctuations to slow down at temperatures T near the onset of static charge order and, overall, the effect of the field B may be seen as equivalent to strengthening stripe order by approaching p=0.12 doping. In details however, our analysis reveals significant departure from usual field-induced magnetic transitions. The continuous growth of the amplitude of the fluctuating moment with increasing B suggests a nearly-critical state in the B->0 limit, with very weak quasi-static moments possibly confined in small areas like vortex cores. Further, the nucleation of spin order in the vortex cores is shown to account quantitatively for both the value and the p dependence of a field scale characterizing bulk spin freezing. The correlation time of the fluctuating moment appears to depend exponentially on B/T (over the investigated range). This explains the timescale dependence of various experimental manifestations, including why, for transport measurements, the AFM moments may be considered static over a considerable range of B and T. These results make the high-field magnetic ground state up to p* an integral part of the discussion on putative quantum criticality.

cond-mat.supr-con↗

Competing magnetic phases in the frustrated spin-1/2 chain compound $β$-TeVO$_4$ probed by NMR

In frustrated spin-1/2 chains the competition between the nearest- and next-nearest-neighbor exchange interactions leads to a rich phase diagram that becomes even richer in the presence of perturbations in their material realizations. These effects are still largely unexplored, so that new insight into static and dynamic magnetism, in particular by sensitive local probes, is highly desired. Here we present a comprehensive $^{17}$O nuclear magnetic resonance study of $β$-TeVO$_4$, where the anisotropy of the main exchange interactions and additional weak interchain exchange interactions complement the theoretical phase diagram. Our results confirm the dynamical nature of the intriguing spin-stripe phase that has been reported in previous studies. In addition, we find that the magnetic order in the high-field phase, which develops just below the magnetization saturation, is consistent with an unusual type of spin-density-wave (SDW) order with different alignments of the magnetic moments on the neighboring chains. This is reminiscent of the ordering in the SDW phase, realized in the absence of the magnetic field, and is thus most likely stabilized by magnetic anisotropy.

cond-mat.str-el↗

Locally commensurate charge-density wave with three-unit-cell periodicity in YBCO

In order to identify the mechanism responsible for the formation of charge-density waves (CDW) in cuprate superconductors, it is important to understand which aspects of the CDW's microscopic structure are generic and which are material-dependent. Here, we show that, at the local scale probed by NMR, long-range CDW order in YBa2Cu3Oy is unidirectional with a commensurate period of three unit cells (lambda = 3b), implying that the incommensurability found in X-ray scattering is ensured by phase slips (discommensurations). Furthermore, NMR spectra reveal a predominant oxygen character of the CDW with an out-of-phase relationship between certain lattice sites but no specific signature of a secondary CDW with lambda = 6b associated with a putative pair-density wave. These results shed light on universal aspects of the cuprate CDW. In particular, its spatial profile appears to generically result from the interplay between an incommensurate tendency at long length scales, possibly related to properties of the Fermi surface, and local commensuration effects, due to electron-electron interactions or lock-in to the lattice.

cond-mat.supr-con↗

High magnetic field ultrasound study of spin freezing in La$_{1.88}$Sr$_{0.12}$CuO$_4$

High-$T_{\rm{c}}$ cuprate superconductors host spin, charge and lattice instabilities. In particular, in the antiferromagnetic glass phase, over a large doping range, lanthanum based cuprates display a glass-like spin freezing with antiferromagnetic correlations. Previously, sound velocity anomalies in La$_{2-x}$Sr$_{x}$CuO$_4$ (LSCO) for hole doping $p\geq 0.145$ were reported and interpreted as arising from a coupling of the lattice to the magnetic glass [Frachet, Vinograd et al., Nat. Phys. 16, 1064-1068 (2020)]. Here we report both sound velocity and attenuation in LSCO $p=0.12$, i.e. at a doping level for which the spin freezing temperature is the highest. Using high magnetic fields and comparing with nuclear magnetic resonance (NMR) measurements, we confirm that the anomalies in the low temperature ultrasound properties of LSCO are produced by a coupling between the lattice and the spin glass. Moreover, we show that both sound velocity and attenuation can be simultaneously accounted for by a simple phenomenological model originally developed for canonical spin glasses. Our results point towards a strong competition between superconductivity and spin freezing, tuned by the magnetic field. A comparison of different acoustic modes suggests that the slow spin fluctuations have a nematic character.

cond-mat.supr-con↗

Thermal effects versus spin nematicity in a frustrated spin-1/2 chain

The spin-nematic phase is an intriguing state of matter that lacks usual long-range dipolar order, yet it exhibits higher multipolar order. This makes its detection extremely difficult and controversial. Recently, nuclear magnetic resonance (NMR) has been proposed as one of the most suitable techniques to confirm its existence. We report a $^{17}$O NMR observation of the reduction of the local magnetization in the polarized state of the frustrated spin-1/2 chain $β$-TeVO$_4$, which was previously proposed to be a fingerprint of the spin-nematic behavior. However, our detailed study shows that the detected missing fraction of the magnetization, probed by NMR frequency shift, is thermally activated, thus undermining the presence of the spin-nematic phase in the investigated compound. This highlights the importance of careful considerations of temperature-dependent NMR shift that has been overlooked in previous studies of spin nematicity.

cond-mat.str-el↗

Pre-saturation phase in the frustrated ferro-antiferromagnet Pb$_2$VO(PO$_4$)$_2$

Magnetization, magnetic torque, neutron diffraction and NMR experiments are used to map out the $H$$-$$T$ phase diagram of the prototypical quasi-two-dimensional ferro-antiferromagnet Pb$_2$VO(PO$_4$)$_2$ in magnetic fields up to 27 T. When the field is applied perpendicular to the axis of magnetic anisotropy, a new magnetic state emerges through a discontinuous transition and persists in a narrow field range just below saturation. The measured NMR spectra suggest a complex and possibly incommensurate magnetic order in that regime.

cond-mat.str-el↗

NMR study of charge density waves under hydrostatic pressure in YBa2Cu3Oy

The effect of hydrostatic pressure (P) on charge density waves (CDW) in YBa2Cu3Oy has recently been controversial. Using NMR, we find that both the short-range CDW in the normal state and the long-range CDW in high fields are, at most, slightly weakened at P=1.9 GPa. This result is in contradiction with x-ray scattering results finding complete suppression of the CDW at ~1 GPa and we discuss possible explanations of this discrepancy. Quantitative analysis, however, shows that the NMR data is not inconsistent with a disappearance of the CDW on a larger pressure scale, typically ~10-20 GPa. We also propose a simple model reconciling transport data with such a hypothesis, provided the pressure-induced change in doping is taken into account. We conclude that it is therefore possible that most of the spectacular increase in Tc upon increasing pressure up to ~15~GPa arises from a concomitant decrease of CDW strength.

cond-mat.supr-con↗

Detection of a Disorder-Induced Bose-Einstein Condensate in a Quantum Spin Material at High Magnetic Fields

The coupled spin-1 chains material NiCl$_2$-4SC(NH$_2$)$_2$ (DTN) doped with Br impurities is expected to be a perfect candidate for observing many-body localization at high magnetic field: the so-called "Bose glass", a zero-temperature bosonic fluid, compressible, gapless, incoherent, and short-range correlated. Using nuclear magnetic resonance (NMR), we critically address the stability of the Bose glass in doped DTN, and find that it hosts a novel disorder-induced ordered state of matter, where many-body physics leads to an unexpected resurgence of quantum coherence emerging from localized impurity states. An experimental phase diagram of this new "order-from-disorder" phase, established from NMR $T_1^{-1}$ relaxation rate data in the (13 $\pm$ 1)% Br-doped DTN, is found to be in excellent agreement with the theoretical prediction from large-scale quantum Monte Carlo simulations.

cond-mat.str-el↗

Spin susceptibility of charge ordered YBa2Cu3Oy across the upper critical field

The value of the upper critical field Hc2, a fundamental characteristic of the superconducting state, has been subject to strong controversy in high-Tc copper-oxides. Since the issue has been tackled almost exclusively by macroscopic techniques so far, there is a clear need for local-probe measurements. Here, we use 17O NMR to measure the spin susceptibility $χ_{spin}$ of the CuO2 planes at low temperature in charge ordered YBa2Cu3Oy. We find that $χ_{spin}$ increases (most likely linearly) with magnetic field H and saturates above field values ranging from 20 to 40 T. This result is consistent with Hc2 values claimed by G. Grissonnanche et al. [Nat. Commun. 5, 3280 (2014)] and with the interpretation that the charge-density-wave (CDW) reduces Hc2 in underdoped YBa2Cu3Oy. Furthermore, the absence of marked deviation in $χ_{spin}(H)$ at the onset of long-range CDW order indicates that this Hc2 reduction and the Fermi-surface reconstruction are primarily rooted in the short-range CDW order already present in zero field, not in the field-induced long-range CDWorder. Above Hc2, the relatively low values of $χ_{spin}$ at T=2 K show that the pseudogap is a ground-state property, independent of the superconducting gap.

cond-mat.supr-con↗

Observation of electronic bound states in charge-ordered YBa$_2$Cu$_3$O$_y$

Observing how electronic states in solids react to a local symmetry breaking provides insight into their microscopic nature. A striking example is the formation of bound states when quasiparticles are scattered off defects. This is known to occur, under specific circumstances, in some metals and superconductors but not, in general, in the charge-density-wave (CDW) state. Here, we report the unforeseen observation of bound states when a magnetic field quenches superconductivity and induces long-range CDW order in YBa$_2$Cu$_3$O$_y$. Bound states indeed produce an inhomogeneous pattern of the local density of states $N(E_F)$ that leads to a skewed distribution of Knight shifts which is detected here through an asymmetric profile of $^{17}$O NMR lines. We argue that the effect arises most likely from scattering off defects in the CDW state, which provides a novel case of disorder-induced bound states in a condensed-matter system and an insightful window into charge ordering in the cuprates.

cond-mat.supr-con↗

Dichotomy between Attractive and Repulsive Tomonaga-Luttinger Liquids in Spin Ladders

We present two methods to determine whether the interactions in a Tomonaga-Luttinger liquid (TLL) state of a spin-$1/2$ Heisenberg antiferromagnetic ladder are attractive or repulsive. The first method combines two bulk measurements, of magnetization and specific heat, to deduce the TLL parameter that distinguishes between the attraction and repulsion. The second one is based on a local-probe, NMR measurements of the spin-lattice relaxation. For the strong-leg spin ladder compound $\mathrm{(C_7H_{10}N)_2CuBr_4}$ we find that the isothermal magnetic field dependence of the relaxation rate, $T_1^{-1}(H)$, displays a concave curve between the two critical fields that bound the TLL regime. This is in sharp contrast to the convex curve previously reported for a strong-rung ladder $\mathrm{(C_5H_{12}N)_2CuBr_4}$. Within the TLL description, we show that the concavity directly reflects the attractive interactions, while the convexity reflects the repulsive ones.

cond-mat.str-el↗

Generalized mean-field approach to simulate large dissipative spin ensembles with long range interactions

We simulate the collective dynamics in spin lattices with long range interactions and collective decay in one, two and three dimensions. Starting from a dynamical mean-field approach derived by local factorization of the density operator we improve the numerical approximation of the full master equation by including pair correlations at any distance. This truncations enable us to drastically increase the number of spins in our numerical simulations from about ten spins in case of the full quantum model to several ten-thousands in the mean-field approximation and a few hundreds if pair correlations are included. Extensive numerical tests help us identify interaction strengths and geometric configurations where these approximations perform well and allow us to state fairly simple error estimates. By simulating systems of increasing size we show that in one and two dimensions we can include as many spins as needed to capture the properties of infinite size systems with high accuracy, while in 3D the method does not converge to desired accuracy within the system sizes we can currently implement. Our approach is well suited to give error estimates of magic wavelength optical lattices for atomic clock applications and corresponding super radiant lasers.

quant-ph↗

One-Third Magnetization Plateau with a Preceding Novel Phase in Volborthite

We have synthesized high-quality single crystals of volborthite, a seemingly distorted kagome antiferromagnet, and carried out high-field magnetization measurements up to 74 T and 51V NMR measurements up to 30 T. An extremely wide 1/3 magnetization plateau appears above 28 T and continues over 74 T at 1.4 K, which has not been observed in previous study using polycrystalline samples. NMR spectra reveal an incommensurate order (most likely a spin-density wave order) below 22 T and a simple spin structure in the plateau phase. Moreover, a novel intermediate phase is found between 23 and 26 T, where the magnetization varies linearly with magnetic field and the NMR spectra indicate an inhomogeneous distribution of the internal magnetic field. This sequence of phases in volborthite bear a striking similarity to those of frustrated spin chains with a ferromagnetic nearest-neighbor coupling J1 competing with an antiferromagnetic next-nearest-neighbor coupling J2.

cond-mat.str-el↗