skip to main content

Title: Properties of bulk scandium nitride crystals grown by physical vapor transport
In this study, the growth of scandium nitride (100) single crystals with high electron mobility and high thermal conductivity was demonstrated by physical vapor transport (PVT). Single crystals were grown in the temperature range of 1900 C–2140 C under a nitrogen pressure between 15 and 20 Torr. Single crystal tungsten (100) was used as a nearly lattice constant matched seed crystal. Growth for 20 days resulted in a 2mm thick crystal. Hall-effect measurements revealed that the layers were n-type with a 300 K electron concentration and a mobility of 2.17 x 1021 cm-3 and 73 cm2/V s, respectively. Consequently, this ScN crystal had a low electrical resistivity, 3.94 x 10- 5 Xcm. The thermal conductivity was in the range of 51–56W/mK, three times higher than those in previous reports for ScN thin films. This study demonstrates the viability of the PVT crystal growth method for producing high quality bulk scandium nitride single crystals.
Authors:
Award ID(s):
1800130
Publication Date:
NSF-PAR ID:
10165354
Journal Name:
Applied physics letters
Volume:
116
Page Range or eLocation-ID:
132103-132106
ISSN:
1077-3118
Sponsoring Org:
National Science Foundation
More Like this
  1. The success of graphene created a new era in materials science, especially for two-dimensional (2D) materials. 2D single-crystal carbon nitride (C 3 N) is the first and only crystalline, hole-free, single-layer carbon nitride and its controlled large-scale synthesis has recently attracted tremendous interest in thermal transport. Here, we performed a comparative study of thermal transport between monolayer C 3 N and the parent graphene, and focused on the effect of temperature and strain on the thermal conductivity ( κ ) of C 3 N, by solving the phonon Boltzmann transport equation (BTE) based on first-principles calculations. The κ of C 3 N shows an anomalous temperature dependence, and the κ of C 3 N at high temperatures is larger than the expected value following the common trend of κ ∼ 1/ T . Moreover, the κ of C 3 N is found to be increased by applying a bilateral tensile strain, despite its similar planar honeycomb structure to graphene. The underlying mechanism is revealed by providing direct evidence for the interaction between lone-pair N-s electrons and bonding electrons from C atoms in C 3 N based on the analysis of orbital-projected electronic structures and electron localization function (ELF). Our researchmore »not only conduct a comprehensive study on the thermal transport in graphene-like C 3 N, but also reveal the physical origin of its anomalous properties, which would have significant implications on the future studies of nanoscale thermal transport.« less
  2. A suite of hydrous orthoenstatite crystals were synthesized at 5–7 GPa and 1100–1300 °C, corresponding to the mid upper mantle conditions in continental regions. The synthetic crystals presented a clear, inclusion-free, and euhedral form with a size range from 100 to a few hundred microns. The Al- and water content of crystals were less than 2 wt. % and ranging from ~500 ppm to 1000 ppm, respectively, characterized by Raman and IR spectroscopy, electron microscopy, and SIMS. The analysis shows that the capability of water incorporation for this suite of hydrous orthoenstatite is correlated to the Al-content in the crystal structure. To understand how the detailed crystal structure reflects the influence of water and Al, single crystal X ray diffraction analysis was performed for this suite of hydrous orthoenstatite. By comparing the results obtained at ambient conditions, we find that for low-level of Al-content, <2 wt. %, the Al3+ cation tends to occupy one of tetrahedral sites (TB) only. Analysis of the X ray diffraction results under high pressure indicates that the elasticity of orthoenstatites is insensitive to the presence of low-level water and Al. We use this finding to evaluate the velocity profile at the mid upper mantle ofmore »continental regions to compare with seismic observation. The comparison indicates that the cause of the low velocity zone in continental regions originates from the geotherm profile rather than the effect of water on the elasticity of mantle phases.« less
  3. MXenes are a rapidly growing class of 2D transition metal carbides and nitrides, finding applications in fields ranging from energy storage to electromagnetic interference shielding and transparent conductive coatings. However, while more than 20 carbide MXenes have already been synthesized, Ti 4 N 3 and Ti 2 N are the only nitride MXenes reported so far. Here by ammoniation of Mo 2 CT x and V 2 CT x MXenes at 600 °C, we report on their transformation to 2D metal nitrides. Carbon atoms in the precursor MXenes are replaced with N atoms, resulting from the decomposition of ammonia molecules. The crystal structures of the resulting Mo 2 N and V 2 N were determined with transmission electron microscopy and X-ray pair distribution function analysis. Our results indicate that Mo 2 N retains the MXene structure and V 2 C transforms to a mixed layered structure of trigonal V 2 N and cubic VN. Temperature-dependent resistivity measurements of the nitrides reveal that they exhibit metallic conductivity, as opposed to semiconductor-like behavior of their parent carbides. As important, room-temperature electrical conductivity values of Mo 2 N and V 2 N are three and one order of magnitude larger than those ofmore »the Mo 2 CT x and V 2 CT x precursors, respectively. This study shows how gas treatment synthesis such as ammoniation can transform carbide MXenes into 2D nitrides with higher electrical conductivities and metallic behavior, opening a new avenue in 2D materials synthesis.« less
  4. Abstract

    Understanding the thermal stability of metallic glasses is critical to determining their safe temperatures of service. In this paper, the crystallization mechanism in spark plasma sintered Fe48Cr15Mo14Y2C15B6metallic glass is established by analyzing the crystal size distribution using x-ray diffraction, transmission electron microscopy andin-situsmall angle neutron scattering. Isothermal annealing at 700 °C and 725 °C for 100 min resulted in the formation of (Fe,Cr)23C6crystals, measured from transmission electron micrographs, to be from 10 to 30 nm. The small angle neutron scattering intensity measuredin-situ, over a Q-range of 0.02 to 0.3 Å−1, during isothermal annealing of the sintered samples, confirmed the presence of (Fe,Cr)23C6crystals. The measured scattering intensity, fitted by the maximum entropy model, over the Q-range of 0.02 to 0.06 Å−1, revealed that the crystals had radii ranging from 3 to 18 nm. The total volume fraction of crystals were estimated to be 0.13 and 0.22 upon isothermal annealing at 700 °C and 725 °C for 100 min respectively. The mechanism of crystallization in this spark plasma sintered iron based metallic glass was established to be from pre-existing nuclei as confirmed by Avrami exponents of 0.25 ± 0.01 and 0.39 ± 0.01 at the aforesaid temperatures.

  5. All-solid-state batteries (ASSBs) have garnered increasing attention due to the enhanced safety, featuring nonflammable solid electrolytes as well as the potential to achieve high energy density. 1 The advancement of the ASSBs is expected to provide, arguably, the most straightforward path towards practical, high-energy, and rechargeable batteries based on metallic anodes. 1 However, the sluggish ion transmission at the cathode-electrolyte (solid/solid) interface would result in the high resistant at the contact and limit the practical implementation of these all solid-state materials in real world batteries. 2 Several methods were suggested to enhance the kinetic condition of the ion migration between the cathode and the solid electrolyte (SE). 3 A composite strategy that mixes active materials and SEs for the cathode is a general way to decrease the ion transmission barrier at the cathode-electrolyte interface. 3 The active material concentration in the cathode is reduced as much as the SE portion increases by which the energy density of the ASSB is restricted. In addition, the mixing approach generally accompanies lattice mismatches between the cathode active materials and the SE, thus providing only limited improvements, which is imputed by random contacts between the cathode active materials and the SE during the mixingmore »process. Implementing high-pressure for the electrode and electrolyte of ASSB in the assembling process has been verified is a but effective way to boost the ion transmission ability between the cathode active materials and the SE by decreasing the grain boundary impedance. Whereas the short-circuit of the battery would be induced by the mechanical deformation of the electrolyte under high pressure. 4 Herein, we demonstrate a novel way to address the ion transmission problem at the cathode-electrolyte interface in ASSBs. Starting from the cathode configuration, the finite element method (FEM) was employed to evaluate the current concentration and the distribution of the space charge layer at the cathode-electrolyte interface. Hierarchical three-dimensional (HTD) structures are found to have a higher Li + transfer number (t Li+ ), fewer free anions, and the weaker space-charge layer at the cathode-electrolyte interface in the resulting FEM simulation. To take advantage of the HTD structure, stereolithography is adopted as a manufacturing technique and single-crystalline Ni-rich (SCN) materials are selected as the active materials. Next, the manufactured HTD cathode is sintered at 600 °C in an N 2 atmosphere for the carbonization of the resin, which induces sufficient electronic conductivity for the cathode. Then, the gel-like Li 1.4 Al 0.4 Ti 1.6 (PO 4 ) 3 (LATP) precursor is synthesized and filled into the voids of the HTD structure cathode sufficiently. And the filled HTD structure cathodes are sintered at 900 °C to achieve the crystallization of the LATP gel. Scanning transmission electron microscopy (STEM) is used to unveil the morphology of the cathode-electrolyte interface between the sintered HTD cathode and the in-situ generated electrolyte (LATP). A transient phase has been found generated at the interface and matched with both lattices of the SCN and the SE, accelerating the transmission of the Li-ions, which is further verified by density functional theory calculations. In addition, Electron Energy Loss Spectroscopy demonstrates the preserved interface between HTD cathode and SEs. Atomic force microscopy is employed to measure the potential image of the cross-sectional interface by the peak force tapping mode. The average potential of modified samples is lower than the sample that mix SCN and SEs simply in the 2D planar structure, which confirms a weakened space charge layer by the enhanced contact capability as well as the ion transmission ability. To see if the demonstrated method is universally applicable, LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) is selected as the cathode active material and manufactured in the same way as the SCN. The HTD cathode based on NCM811 exhibits higher electrochemical performance compared with the reference sample based on the 2D planar mixing-type cathode. We believe such a demonstrated universal strategy provides a new guideline to engineer the cathode/electrolyte interface by revolutionizing electrode structures that can be applicable to all-solid-state batteries. Figure 1. Schematic of comparing of traditional 2D planar cathode and HTD cathode in ASSB Tikekar, M. D. , et al. , Nature Energy (2016) 1 (9), 16114 Banerjee, A. , et al. , Chem Rev (2020) 120 (14), 6878 Chen, R. , et al. , Chem Rev (2020) 120 (14), 6820 Cheng, X. , et al. , Advanced Energy Materials (2018) 8 (7) Figure 1« less