SIMES Publications

Abstract

Although liquid-solid interfaces are foundational in broad areas of science, characterizing this delicate interface remains inherently difficult because of shortcomings in existing tools to access liquid and solid phases simultaneously at the nanoscale. This leads to substantial gaps in our understanding of the structure and chemistry of key interfaces in battery systems. We adopt and modify a thin film vitrification method to preserve the sensitive yet critical interfaces in batteries at native liquid electrolyte environments to enable cryo–electron microscopy and spectroscopy. We report substantial swelling of the solid-electrolyte interphase (SEI) on lithium metal anode in various electrolytes. The swelling behavior is dependent on electrolyte chemistry and is highly correlated to battery performance. Higher degrees of SEI swelling tend to exhibit poor electrochemical cycling.

Abstract

The elastocaloric effect (ECE) relates changes in entropy to changes in strain experienced by a material. As such, ECE measurements can provide valuable information about the entropy landscape proximate to strain-tuned phase transitions. For ordered states that break only point symmetries, bilinear coupling of the order parameter with strain implies that the ECE can also provide a window on fluctuations above the critical temperature and hence, in principle, can also provide a thermodynamic measure of the associated susceptibility. To demonstrate this, we use the ECE to sensitively reveal the presence of nematic fluctuations in the archetypal Fe-based superconductor Ba(Fe_1−xCo_x)₂As₂. By performing these measurements simultaneously with elastoresistivity in a multimodal fashion, we are able to make a direct and unambiguous comparison of these closely related thermodynamic and transport properties, both of which are sensitive to nematic fluctuations. As a result, we have uncovered an unanticipated doping dependence of the nemato-elastic coupling and of the magnitude of the scattering of low-energy quasi-particles by nematic fluctuations—while the former weakens, the latter increases dramatically with increasing doping.

Abstract

In the cuprates, one-dimensional (1D) chain compounds provide a distinctive opportunity to understand the microscopic physics, owing to the availability of reliable theories. However, progress has been limited by the challenge of controllably doping these materials. We report the synthesis and spectroscopic analysis of the 1D cuprate Ba_2-xSr_xCuO_3+δ over a wide range of hole doping. Our angle-resolved photoemission experiments reveal the doping evolution of the holon and spinon branches. We identify a prominent folding branch whose intensity fails to match predictions of the simple Hubbard model. An additional strong near-neighbor attraction, which may arise from coupling to phonons, quantitatively explains experiments for all accessible doping levels. Considering structural and quantum chemistry similarities among cuprates, this attraction may play a similarly important role in high-temperature cuprate superconductors.

Abstract

Graphene nanoribbons are of potential use in the development of electronic and optoelectronic devices. However, the preparation of narrow and long nanoribbons with smooth edges, sizeable bandgaps and high mobilities is challenging. Here we show that sub-10-nm-wide semiconducting graphene nanoribbons with atomically smooth closed edges can be produced by squashing carbon nanotubes using a high-pressure and thermal treatment. With this approach, nanoribbons as narrow as 1.4 nm can be created, and up to 54% of single- and double-walled nanotubes in a sample can be converted into edge-closed nanoribbons. We also fabricate edge-opened nanoribbons using nitric acid as the oxidant to selectively etch the edges of the squashed nanotubes under high pressure. A field-effect transistor fabricated using a 2.8-nm-wide edge-closed nanoribbon exhibits an on/off current ratio of more than 10⁴, from which a bandgap of around 494 meV is estimated. The device also exhibits a field-effect mobility of 2,443 cm² V⁻¹ s⁻¹ and an on-state channel conductivity of 7.42 mS.

Abstract

The stranglehold of low temperatures on fascinating quantum phenomena in one-dimensional quantum magnets has been challenged recently by the discovery of anomalous spin transport at high temperatures. Whereas both regimes have been investigated separately, no study has attempted to reconcile them. For instance, the paradigmatic quantum Heisenberg spin-$1/2$ chain falls at low temperature within the Tomonaga-Luttinger liquid framework, while its high-temperature dynamics is superdiffusive and relates to the Kardar-Parisi-Zhang universality class in $1+1$ dimensions. This Letter aims at reconciling the two regimes. Building on large-scale matrix product state simulations, we find that they are connected by a temperature-dependent spatiotemporal crossover. As the temperature $T$ is reduced, we show that the onset of superdiffusion takes place at longer length and timescales $\propto 1/T$. This prediction has direct consequences for experiments including nuclear magnetic resonance: it is consistent with earlier measurements on the nearly ideal Heisenberg $S=1/2$ chain compound ${\mathrm{Sr}}_2{\mathrm{CuO}}_3$, yet calls for new and dedicated experiments.

Abstract

The kagome Heisenberg antiferromagnet formed by frustrated spins arranged in a lattice of corner-sharing triangles is a prime candidate for hosting a quantum spin liquid (QSL) ground state consisting of entangled spin singlets1. However, the existence of various competing states makes a convincing theoretical prediction of the QSL ground state difficult2, calling for experimental clues from model materials. The kagome lattice materials Zn-barlowite (ZnCu3(OD)6FBr)3,4,5 and herbertsmithite (ZnCu3(OD)6Cl2)6,7,8,9,10 do not exhibit long-range order and are considered the best realizations of the kagome Heisenberg antiferromagnet known so far. Here we use 63Cu nuclear quadrupole resonance combined with the inverse Laplace transform11,12,13 to locally probe the inhomogeneity of delicate quantum ground states affected by disorder14,15,16,17. We present direct evidence for the gradual emergence of spin singlets with spatially varying excitation gaps, but even at temperatures far below the super-exchange energy scale their fraction is limited to ~60% of the total spins. Theoretical models18,19 need to incorporate the role of disorder to account for the observed inhomogeneously gapped behaviour.

Abstract

On-chip dynamic strain engineering requires efficient micro-actuators that can generate large in-plane strains. Inorganic electrochemical actuators are unique in that they are driven by low voltages (≈1 V) and produce considerable strains (≈1%). However, actuation speed and efficiency are limited by mass transport of ions. Minimizing the number of ions required to actuate is thus key to enabling useful “straintronic” devices. Here, it is shown that the electrochemical intercalation of exceptionally few lithium ions into WTe2 causes large anisotropic in-plane strain: 5% in one in-plane direction and 0.1% in the other. This efficient stretching of the 2D WTe2 layers contrasts to intercalation-induced strains in related materials which are predominantly in the out-of-plane direction. The unusual actuation of LixWTe2 is linked to the formation of a newly discovered crystallographic phase, referred to as Td’, with an exotic atomic arrangement. On-chip low-voltage (<0.2 V) control is demonstrated over the transition to the novel phase and its composition. Within the Td’-Li0.5−δWTe2 phase, a uniaxial in-plane strain of 1.4% is achieved with a change of δ of only 0.075. This makes the in-plane chemical expansion coefficient of Td’-Li0.5−δWTe2 far greater than of any other single-phase material, enabling fast and efficient planar electrochemical actuation.

Abstract

Vanadium dioxide is known to have a coupled structural and electronic transition that can be accessed through light, thermal, or electrical excitation. Ultrafast optical studies of this insulator-to-metal transition indicate that it is mediated by the formation of a transient metallic phase that retains the structure of the original insulating phase. Sood et al. show that a similar sequence occurs when the material is electrically excited with a series of voltage pulses. Using ultrafast electron diffraction, the researchers monitored the structure of a vanadium dioxide sample after excitation and found evidence of a metastable metallic phase that appears during the transition.

Abstract

The discovery of superconductivity in infinite-layer nickelates brings us tantalizingly close to a material class that mirrors the cuprate superconductors. We measured the magnetic excitations in these nickelates using resonant inelastic x-ray scattering at the Ni L3-edge. Undoped NdNiO2 possesses a branch of dispersive excitations with a bandwidth of approximately 200 milli–electron volts, which is reminiscent of the spin wave of strongly coupled, antiferromagnetically aligned spins on a square lattice. The substantial damping of these modes indicates the importance of coupling to rare-earth itinerant electrons. Upon doping, the spectral weight and energy decrease slightly, whereas the modes become overdamped. Our results highlight the role of Mottness in infinite-layer nickelates.

Abstract

We study the effects of doping the Kitaev model on the honeycomb lattice where the spins interact via the bond-directional interaction J_K, which is known to have a quantum spin liquid as its exact ground state. The effect of hole doping is studied within the t-J_K model on a three-leg cylinder using density-matrix renormalization group. Upon light doping, we find that the ground state of the system has a dominant quasi-long-range charge-density-wave correlations but short-range single-particle correlations. In the pairing channel, the even-parity superconducting correlation is dominant with d-wave-like symmetry, which oscillates in sign as a function of separation with a period equal to that of the spin-density wave and two times the charge-density wave. Although these correlations fall rapidly (possibly exponentially) at long distances, this is never-the-less the example where a pair-density wave is the leading instability in the pairing channel on the honeycomb lattice.