arXiv subjects

Zihua Zhu

Publications and source records attributed to Zihua Zhu.

8 recordsLinked to original sources

arXiv2026

Effect of Buried-Interface Preparation for Nb Superconducting Resonators on InP

Substrate surface preparation is a key step in the fabrication of electronic devices. In III--V semiconductor platforms, e.g. used in HEMTs and lasers, removal of the native substrate oxide is extremely important, where improper removal will negatively affect end-of-line device performance. However, the impact of substrate preparation in hybrid superconductor--semiconductor (S--Sm) systems relevant to quantum information applications remains poorly understood. This study compares three surface preparations for the deposition of sputtered Nb films on InP: (i) no intentional oxide removal (control), (ii) \textit{in-situ} $\mathrm{Ar}^{+}$ milling, and (iii) S-passivation. \textit{In-situ} $\mathrm{Ar}^{+}$ milling reduces the O concentration at the metal--substrate (MS) interface, but also roughens the InP surface, increasing the effective thickness of the Nb--InP interface and promoting O incorporation through extended defects in the Nb film. S-passivation suppresses interfacial O more effectively while preserving a sharper and smoother buried interface. It also yields Nb films with higher superconducting transition temperatures and less structural damage than the $\mathrm{Ar}^{+}$-milled samples. Despite these materials improvements, the microwave response is comparable across the three preparations. At single photon powers, the highest internal quality factors, $Q_i$, are approximately $1.30\times10^{5}$ ($130\mathrm{k}$) for the control resonators, $9.7\times10^{4}$ ($97\mathrm{k}$) for the S-passivated resonators, and $8.4\times10^{4}$ ($84\mathrm{k}$) for the $\mathrm{Ar}^{+}$-milled resonators. These results suggest that the present devices are not primarily limited by dielectric loss at the buried Nb--InP interface.

cond-mat.mes-hall↗

arXiv2026

Isotopically enriched epitaxial CaWO$_{4}$ thin films for Er$^{3+}$ spin-photon quantum interfaces

Rare earth ion (REI)-doped oxide thin films are attractive for the application of quantum interconnects due to their stable optical levels and scalability$^{1-3}$. Among them, Er$^{3+}$ doped CaWO$_{4}$ is promising because it possesses narrow optical linewidth transitions and a long spin coherence time$^{4-6}$. The electron spin coherence is limited at high temperatures by paramagnetic impurities and by the presence of the 14.3% $^{183}$W nuclear spin. To further increase the spin coherence time at millikelvin temperatures, where the paramagnetic impurities are frozen out, our approach is to synthesize chemically and isotopically purified thin films as a host material. We first grow non-isotopically enriched Er$^{3+}$ doped CaWO$_{4}$ thin films, which exhibit a 214(13) MHz photoluminescence (PL) inhomogeneous linewidth, indicating the thin film has high crystalline quality. We then grow isotopically enriched CaWO$_{4}$ thin films using an isotopically purified $^{186}$WO$_{3}$ source. Time of flight secondary ion mass spectrometry (ToF-SIMS) was used to measure the relative concentration of W isotopes. $^{183}$W, the only W isotope that has a net nuclear spin and is the major cause of spin decoherence, was at a relative abundance of 1.2%, a factor of 10 lower than natural abundance. We also observed PL emission from single ions after integrating nano-photonic devices with the thin film. These results establish isotopically engineered CaWO$_{4}$ thin films as a promising platform for future studies of nuclear-spin-limited coherence and for scalable rare-earth-ion-based quantum nanophotonic devices.

quant-ph↗

arXiv2025

Selective Oxidation and Cr Segregation in High-Entropy Oxide Thin Films

High-entropy oxides (HEOs) offer exceptional compositional flexibility and structural stability, making them promising materials for energy and catalytic applications. Here, we investigate Sr doping effects on B-site cation oxidation states, local composition, and structure in epitaxial La1-xSrx(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 thin films. X-ray spectroscopies reveal that Sr doping preferentially promotes Cr oxidation from Cr3+ to Cr6+, partially oxidizes Co and Ni, while leaving Mn4+ and Fe3+ unchanged. Atomic-resolution scanning transmission electron microscopy with energy-dispersive X-ray spectroscopy shows pronounced Cr segregation, with Cr exhibiting depletion at the film-substrate interface and enrichment at the film surface, along with the formation of a partially amorphous phase in heavily Sr-doped samples. This segregation is likely driven by oxidation-induced migration of smaller, high-valence Cr cations during the growth. These findings underscore the critical interplay between charge transfer, local strain, and compositional fluctuations, providing strategies to control surface composition and electronic structure in HEOs for more robust electrocatalyst design.

cond-mat.mtrl-sci↗

arXiv2025

Molecular Insights into Yb(III) Speciation in Sulfate-Bearing Hydrothermal Fluids from X-ray Absorption Spectra Informed by ab initio Molecular Dynamics

Rare earth elements (REEs) are critical for advanced technologies, yet in hydrothermal aqueous solutions the molecular level details of their interaction with ligands that control their geochemical transport and deposition remain poorly understood. This study elucidates the coordination behavior of Yb(III) in sulfate-rich hydrothermal fluids using in situ extended X-ray absorption fine structure (EXAFS) spectroscopy and ab initio molecular dynamics (AIMD) simulations. By integrating multi-angle EXAFS with AIMD-derived constraints, we precisely resolve Yb(III) coordination structures and ligand interactions under hydrothermal conditions. At room temperature, Yb (III) is coordinated by five water molecules and two sulfate ligands (coordination number, CN = 8), forming a distorted square antiprism geometry. Increasing temperature induces progressive dehydration, reducing the hydration shell and favoring stronger sulfate complexation. At 200 Celsius, sulfate ligands reorganize around Yb(III), shifting its geometry to a capped dodecahedron (CN = 7). At 300 Celsius, sulfate binding dominates, leading to structural reorganization that parallels the onset of sulfate mineral precipitation, consistent with the retrograde solubility of REE sulfates. These findings provide direct molecular-scale evidence that sulfate acts as both a transport and deposition ligand, critically influencing REE mobility in geochemical environments. Our results can also help to refine thermodynamic models of REE speciation in high-temperature hydrothermal fluids and improve our understanding of REE ore formation processes in nature.

physics.chem-ph↗

arXiv2023

Metal-to-insulator transition in oxide semimetals by anion doping

Oxide semimetals exhibiting both nontrivial topological characteristics stand as exemplary parent compounds and multiple degrees of freedom, offering great promise for the realization of novel electronic states. In this study, we present compelling evidence of profound structural and transport phase shifts in a recently uncovered oxide semimetal, SrNbO3, achieved through effective in-situ anion doping. Notably, a remarkable increase in resistivity of more than three orders of magnitude at room temperature is observed upon nitrogen-doping. The extent of electronic modulation in SrNbO3 is strongly correlated with the misfit strain, underscoring its phase instability to both chemical doping and crystallographic symmetry variations. Using first-principles calculations, we discern that elevating the level of nitrogen doping induces an upward shift in the conductive bands of SrNbO3-dNd. Consequently, a transition from a metallic state to an insulating state becomes apparent as the nitrogen concentration reaches a threshold of 1/3. This investigation sheds light on the potential of anion engineering in oxide semimetals, offering pathways for manipulating their physical properties. These insights hold promise for future applications that harness these materials for tailored functionalities.

cond-mat.mtrl-sci↗

arXiv2023

Direct and in situ examination of Li+ transport kinetics in isotope labelled solid electrolyte interphase

Here, using unique in-situ liquid secondary ion mass spectroscopy on isotope-labelled solid-electrolyte-interphase (SEI), assisted by cryogenic transmission electron microscopy and constrained ab initio molecular dynamics simulation, for the first time we answer the question regarding Li+ transport mechanism across SEI, and quantitatively determine the Li+-mobility therein. We unequivocally unveil that Li+ transport in SEI follows a mechanism of successive displacement, rather than "direct-hopping". We further reveal, in accordance with spatial-dependence of SEI structure across the thickness, the apparent Li+ self-diffusivity varies from 6.7*10-19 m2/s to 1.0*10-20 m2/s, setting a quantitative gauging of ionic transport behavior of SEI layer against the underlining electrode as well as the rate limiting step of battery operation. This direct study on Li+ kinetics in SEI fills part of the decade-long knowledge gap about the most important component in advanced batteries and provides more precise guidelines to the tailoring of interphasial chemistries for future battery chemistries.

cond-mat.mtrl-sci↗

arXiv2018

Charge transfer and tunable built-in electric fields across semiconductor-crystalline oxide interfaces

Built-in electric fields across heterojunctions between semiconducting materials underpin the functionality of modern device technologies. Heterojunctions between semiconductors and epitaxially grown crystalline oxides provide a rich setting in which built-in fields can be explored. Here, we present an electrical transport and hard X-ray photoelectron spectroscopy study of epitaxial SrNbxTi1-xO3-δ / Si heterojunctions. A non-monotonic anomaly in the sheet resistance is observed near room temperature, which is accompanied by a crossover in sign of the Hall resistance. The crossover is consistent with the formation of a hole gas in the Si and the presence of a built-in field. Hard X-ray photoelectron spectroscopy measurements reveal pronounced asymmetric features in both the SrNbxTi1-xO3-δ and Si core-level spectra that we show arise from built-in fields. The extended probe depth of hard X-ray photoelectron spectroscopy enables band bending across the SrNbxTi1-xO3-δ / Si heterojunction to be spatially mapped. Band alignment at the interface and surface depletion in SrNbxTi1-xO3-δ are implicated in the formation of the hole gas and built-in fields. Control of charge transfer and built-in electric fields across semiconductor-crystalline oxide interfaces opens a pathway to novel functional heterojunctions.

cond-mat.mtrl-sci↗

arXiv2016

Real-space characterization of reactivity towards water at Bi2Te3(111) surface

Surface reactivity is important in modifying the physical and chemical properties of surface sensitive materials, such as the topological insulators (TIs). Even though many studies addressing the reactivity of TIs towards external gases have been reported, it is still under heavy debate whether and how the topological insulators react with H$_2$O. Here, we employ scanning tunneling microscopy (STM) to directly probe the surface reaction of Bi$_2$Te$_3$ towards H$_2$O. Surprisingly, it is found that only the top quintuple layer is reactive to H$_2$O, resulting in a hydrated Bi bilayer as well as some Bi islands, which passivate the surface and prevent from the subsequent reaction. A reaction mechanism is proposed with H$_2$Te and hydrated Bi as the products. Unexpectedly, our study indicates the reaction with water is intrinsic and not dependent on any surface defects. Since water inevitably exists, these findings provide key information when considering the reactions of Bi$_2$Te$_3$ with residual gases or atmosphere.

cond-mat.mtrl-sci↗