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Charles C. Tam

Publications and source records attributed to Charles C. Tam.

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Near itinerancy and slow singlet formation in the triangular lattice NaRuO2

NaRuO$_2$ forms a delafossite-like structure that contains triangular sublattices of edge-sharing RuO$_6$ octahedra. It shows no evidence of magnetic order down to 100 mK and persistent spin fluctuations, suggestive of a quantum disordered magnetic ground state. In order to characterize the physical regime from which this disordered state arises, we use resonant inelastic X-ray scattering (RIXS) and X-ray absorption spectroscopy (XAS) at the Ru-$L_{2,3}$-edge, along with pulsed high-field magnetization to characterize both the local electronic structure and the magnetic interactions. Despite significant spin-orbit coupling inferred from XAS measurements, a spin-orbit exciton, characteristic of a spin-orbit assisted Mott insulator, was not observed with RIXS due to the presence of damped intraorbital excitations, which are characteristic of a metal. Corroborated by models of the high-field magnetization to a random singlet model, we propose a picture of a nearly itinerant system with strong magnetic and charge fluctuations that destabilize long-range magnetic order.

cond-mat.str-el

New Crystal Structures Hide in Plain Sight: A Stress Test for AI-Guided Materials Discovery

New types of crystal structures are discovered only rarely, and the artificial intelligence (AI) models now reshaping materials discovery have so far produced new chemical compositions within known structural families rather than genuinely new structures. We report GdNiSn4 and LuNiSn4, intermetallics that adopt a previously unreported structure type, found not by computation but by exploratory synthesis. Single-crystal diffraction shows that the structure is an intergrowth of two known structural units. We then use this system as a benchmark for two leading generative models, MatterGen and DiffCSP++. For DiffCSP++, the benchmark is performed in its crystallographically constrained setting, using the required space-group and Wyckoff-position inputs. Under our sampling budget, neither model recovers the experimentally reported monoclinic structure within the structural-matching tolerance. The generated structures are evaluated without further structural relaxation using the nonmagnetic analog LuNiSn4, where we rule out 4f magnetism as the cause. Because the new structure is built from familiar building blocks, it should be derivable. We argue that encoding chemical reasoning, such as the stacking of known motifs, is a concrete path toward AI that can discover structurally novel materials.

cond-mat.mtrl-sci

Collinear spin density wave state in distorted square-lattice GdNiSn$_4$

We characterize the magnetic ground state of the newly synthesized lanthanide intermetallic GdNiSn$_4$ via resonant elastic x-ray scattering measurements. This compound forms distorted square nets of Gd that initially order magnetically below 23 K followed by a lower temperature transition at 16 K. Our scattering data identify the ground state order as a single-$q$ incommensurate, collinear order that slides towards a commensurate wave vector above the 16 K transition. Magnetic symmetry analysis combined with azimuthal dependence resolves the ground state magnetic structure as a moment-modulated spin density wave state with Gd moments oriented parallel to the in-plane a-axis. We discuss connections between the observed magnetic order and electronic properties in this square-net compound.

cond-mat.str-el

The doping evolution of the charge density wave and charge density fluctuations in La$_{2-x}$Sr$_x$CuO$_4$

Cuprate superconductors show various collective charge correlations that are intimately connected with their electronic properties. In particular, charge order in the form of an incommensurate charge density wave (CDW) order with an in-plane wavevector $δ_{\text{CDW}} \approx $ 0.23--0.35~r.l.u. appears to be universally present. In addition to CDW, dynamic charge density fluctuations (CDF) are also present with wavevectors comparable to $δ_{\text{CDW}}$. CDFs are present up to $\sim300\;$K and have relatively short correlation lengths of $ξ\sim 20$\;Å. Here we use Cu-$L_3$ and O-$K$ resonant inelastic X-ray scattering (RIXS) to study the doping dependence of CDW and CDFs in La$_{2-x}$Sr$_x$CuO$_4$. We fit our data with (quasi)elastic peaks resulting from the CDW and up to four inelastic modes associated with oxygen phonons that can be strongly coupled to the CDFs. Our analysis allows us to separate the charge correlations into three components: the CDW with wavevector $δ_{4a-\text{CDW}} \approx 0.24$ and two CDF components with $δ_{4a-\text{CDF}} \approx 0.24$ and $δ_{3a-\text{CDF}} \approx 0.30$. We find that for $T \approx T_c$ the CDW coexists with the CDFs for dopings near $x=p \sim 1/8$. The $4a$-CDW disappears beyond $x=0.16$ and the $4a$-CDF beyond $x=0.19$, leaving only a weak $3a$-CDF at the highest doping studied, $x=0.22$. Our data suggest that low-energy charge fluctuations exist up to doping $x=0.19=p^{\star}$, where the pseudogap disappears, however, we find no evidence that they are associated with a quantum critical point.

cond-mat.supr-con

Unified Description of Charge Density Waves in Electron- and Hole-doped Cuprate Superconductors

High-temperature cuprates superconductors are characterised by the complex interplay between superconductivity (SC) and charge density wave (CDW) in the context of intertwined competing orders. In contrast to abundant studies for hole-doped cuprates, the exact nature of CDW and its relationship to SC was much less explored in electron-doped counterparts. Here, we performed resonant inelastic x-ray scattering (RIXS) experiments to investigate the relationship between CDW and SC in electron-doped La$_{2-x}$Ce$_x$CuO$_4$. The short-range CDW order with a correlation length $\sim35$~Å~was found in a wide range of temperature and doping concentration. Near the optimal doping, the CDW order is weakened inside the SC phase, implying an intimate relationship between the two orders. This interplay has been commonly reported in hole-doped La-based cuprates near the optimal doping. We reconciled the diverging behaviour of CDW across the superconducting phase in various cuprate materials by introducing the CDW correlation length as a key parameter. Our study paves the way for establishing a unified picture to describe the phenomenology of CDW and its relationship with SC in the cuprate family.

cond-mat.supr-con

Reply to "Comment on newly found Charge Density Waves in infinite layer Nickelates''

Charge density waves (CDW) have been reported in NdNiO$_2$ and LaNiO$_2$ thin films grown on SrTiO$_3$ substrates using Ni-$L_3$ resonant x-ray scattering in Refs. [1-3]. In their comment [arXiv:2306.15086] on these reports, Pelliciari et al. found no evidence for a CDW in a NdNiO$_2$ film by performing fixed-momentum energy-dependent measurements. Instead, they observed a nearby non-resonant scattering peak, attributed to the (101) substrate reflection, made accessible at Ni-$L_3$ due to third harmonic light contamination. Here we present fixed-momentum energy-dependent resonant inelastic x-ray scattering measurements across Ni-$L_3$ on NdNiO$_2$, used in the preceding study [1]. We see intrinsic Ni-$L_3$ energy profiles at all measured \textbf{Q} values, including a strong resonance effect at $\mathbf{Q}_\mathrm{CDW} = (-1/3, 0, 0.316)$ reciprocal lattice units. Attempts to measure the (101) substrate peak using third harmonic light at Ni-$L_3$ at I21, Diamond were unfruitful. Our results clearly demonstrate the electronic origin of the scattering peak published in Ref. [1] and lack of a detectable structural component in the peak.

cond-mat.str-el

Stripe Symmetry of Short-range Charge Density Waves in Cuprate Superconductors

The omnipresence of charge density waves (CDWs) across almost all cuprate families underpins a common organizing principle. However, a longstanding debate of whether its spatial symmetry is stripe or checkerboard remains unresolved. While CDWs in lanthanum- and yttrium-based cuprates possess a stripe symmetry, distinguishing these two scenarios has been challenging for the short-range CDW in bismuth-based cuprates. Here, we employed high-resolution resonant inelastic x-ray scattering to uncover the spatial symmetry of the CDW in Bi$_2$Sr$_{2-x}$La$_{x}$CuO$_{6+δ}$. Across a wide range of doping and temperature, anisotropic CDW peaks with elliptical shapes were found in reciprocal space. Based on Fourier transform analysis of real-space models, we interpret the results as evidence of unidirectional charge stripes, hosted by mutually 90$^\circ$-rotated anisotropic domains. Our work paves the way for a unified symmetry and microscopic description of CDW order in cuprates.

cond-mat.str-el

Charge density waves in infinite-layer NdNiO$_2$ nickelates

In materials science, much effort has been devoted to reproduce superconductivity in chemical compositions analogous to cuprate superconductors since their discovery over thirty years ago. This approach was recently successful in realising superconductivity in infinite-layer nickelates. Although differing from cuprates in electronic and magnetic properties, strong Coulomb interactions suggest infinite-layer nickelates have a propensity to various symmetry-breaking orders that populate the cuprates. Here we report the observation of charge density waves (CDWs) in infinite-layer NdNiO$_2$ films using Ni-$L_3$ resonant x-ray scattering. Remarkably, CDWs form in Nd 5$d$ and Ni 3$d$ orbitals at the same commensurate wavevector $(0.333, 0)\;r.l.u.$, with non-negligible out-of-plane dependence, and an in-plane correlation length up to $\sim$ 60 Angstrom. Spectroscopic studies reveal a strong connection between CDWs and the Nd 5$d$ - Ni 3$d$ orbital hybridisation. Upon entering the superconducting state at 20\% Sr doping, the CDWs disappear. Our work demonstrates the existence of CDWs in infinite-layer nickelates with a multi-orbital character distinct from cuprates, which establishes their low-energy physics.

cond-mat.supr-con