SearcharxivSearch

arXiv subjects

Shin Muramoto

Publications and source records attributed to Shin Muramoto.

4 recordsLinked to original sources

Evaluation of carbon incorporation in sulfide thin films grown by hybrid pulsed laser deposition

Vapor-pressure-mismatched materials, such as transition metal chalcogenides, have emerged as key electronic, photonic, and quantum materials. Hybrid pulsed laser deposition (hPLD) has become a preferred method for epitaxial or textured growth of these materials; however, unintentional carbon (C) incorporation remains a persistent concern, particularly when using organic chalcogen precursors as safer alternatives to toxic hydrides. The mechanisms governing C incorporation and its impact on film growth and properties in hPLD remain poorly understood. Here, we investigate the influence of C-containing side products generated from organosulfur precursor pyrolysis on ZnS, BaTiS$_3$, and TiS$_2$ thin films grown by hPLD using tert-butyl disulfide (TBDS). Structural characterization via X-ray diffraction and atomic force microscopy, combined with secondary ion mass spectrometry, is used to systematically examine the effects of growth temperature and TBDS partial pressure on film morphology, crystallinity, and C incorporation. Optimal growth temperatures of 400{\deg}C, 500{\deg}C, and 700{\deg}C are identified for ZnS, TiS$_2$, and BaTiS$_3$, respectively. Growth above or below these temperatures leads to increased C incorporation at both the interface and within the film, correlating with degraded texture. In contrast, highly textured films exhibit minimal C content, comparable to films grown without TBDS. For TiS$_2$, C incorporation depends strongly on TBDS pressure, with 10$^{-1}$ Pa identified as the optimal pressure for minimizing contamination. At higher pressures, loss of preferential texture is observed, likely due to C graphitization poisoning the interface and bulk. These results provide new insight into process-induced C impurities in hPLD-grown chalcogenide thin films and have important implications for sulfide-based thin film technologies.

cond-mat.mtrl-sci

Topotactic oxidation of Ruddlesden-Popper nickelates reveals new structural family: oxygen-intercalated layered perovskites

Layered perovskites such as the Dion-Jacobson, Ruddlesden-Popper, and Aurivillius families host a wide range of correlated electron phenomena, from high-temperature superconductivity to multiferroicity. Here we report a new family of layered perovskites, realized through topotactic oxygen intercalation of La_{n+1}Ni_{n}O_{3n+1} (n=1-4) Ruddlesden-Popper nickelate thin films grown by ozone-assisted molecular-beam epitaxy. Post-growth ozone annealing induces a large c-axis expansion - 17.8% for La_{2}NiO_{4} (n=1) - that monotonically decreases with increasing n. Surface X-ray diffraction coupled with Coherent Bragg Rod Analysis reveals that this structural expansion arises from the intercalation of approximately 0.7 oxygen atoms per formula unit into interstitial sites within the rock salt spacer layers. The resulting structures exhibit a spacer layer composition intermediate between that of the Ruddlesden-Popper and Aurivillius phases, defining a new class of layered perovskites. Oxygen-intercalated nickelates exhibit metallicity and significantly enhanced nickel-oxygen hybridization, a feature linked to high-temperature superconductivity. Our work establishes topotactic oxidation as a powerful synthetic approach to accessing highly oxidized, metastable phases across a broad range of layered oxide systems, offering new platforms to tune properties via spacer-layer chemistry.

cond-mat.mtrl-sci

Primary activity measurement of an Am-241 solution using microgram inkjet gravimetry and decay energy spectrometry

We demonstrate a method for radionuclide assay that is spectroscopic with 100 % counting efficiency for alpha decay. Advancing both cryogenic decay energy spectrometry (DES) and drop-on-demand inkjet metrology, a solution of Am-241 was assayed for massic activity (of order 100 kBq/g) with a relative combined standard uncertainty less than 1 %. We implement live-timed counting, spectroscopic analysis, validation by liquid scintillation (LS) counting, and confirmation of quantitative solution transfer. Experimental DES spectra are well modeled with a Monte Carlo simulation. The model was further used to simulate Pu-238 and Pu-240 impurities, calculate detection limits, and demonstrate the potential for tracer-free multi-nuclide analysis, which will be valuable for new cancer therapeutics based on decay chains, Standard Reference Materials (SRMs) containing impurities, and more widely in nuclear energy, environmental monitoring, security, and forensics.

physics.ins-det

Hydrogen is not necessary for superconductivity in topotactically reduced nickelates

A key open question in the study of layered superconducting nickelate films is the role that hydrogen incorporation into the lattice plays in the appearance of the superconducting state. Due to the challenges of stabilizing highly crystalline square planar nickelate films, films are prepared by the deposition of a more stable parent compound which is then transformed into the target phase via a topotactic reaction with a strongly reducing agent such as CaH$_2$. Recent studies, both experimental and theoretical, have introduced the possibility that the incorporation of hydrogen from the reducing agent into the nickelate lattice may be critical for the superconductivity. In this work, we use secondary ion mass spectrometry to examine superconducting La$_{1-x}$X$_x$NiO$_2$ / SrTiO$_3$ (X = Ca and Sr) and Nd$_6$Ni$_5$O$_{12}$ / NdGaO$_3$ films, along with non-superconducting NdNiO$_2$ / SrTiO$_3$ and (Nd,Sr)NiO$_2$ / SrTiO$_3$. We find no evidence for extensive hydrogen incorporation across a broad range of samples, including both superconducting and non-superconducting films. Theoretical calculations indicate that hydrogen incorporation is broadly energetically unfavorable in these systems, supporting our conclusion that hydrogen incorporation is not generally required to achieve a superconducting state in layered square-planar nickelates.

cond-mat.supr-con