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  1. A mixture ofN,N,N′-trisubstituted thiourea and cyclicN,N,N′,N′-tetrasubstituted selenourea precursors were used to synthesize three monolayer thick CdS1−xSexnanoplatelets in a single synthetic step.

     
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    Free, publicly-accessible full text available November 8, 2024
  2. Abstract The layered square-planar nickelates, Nd n +1 Ni n O 2 n +2 , are an appealing system to tune the electronic properties of square-planar nickelates via dimensionality; indeed, superconductivity was recently observed in Nd 6 Ni 5 O 12 thin films. Here, we investigate the role of epitaxial strain in the competing requirements for the synthesis of the n  = 3 Ruddlesden-Popper compound, Nd 4 Ni 3 O 10 , and subsequent reduction to the square-planar phase, Nd 4 Ni 3 O 8 . We synthesize our highest quality Nd 4 Ni 3 O 10 films under compressive strain on LaAlO 3 (001), while Nd 4 Ni 3 O 10 on NdGaO 3 (110) exhibits tensile strain-induced rock salt faults but retains bulk-like transport properties. A high density of extended defects forms in Nd 4 Ni 3 O 10 on SrTiO 3 (001). Films reduced on LaAlO 3 become insulating and form compressive strain-induced c -axis canting defects, while Nd 4 Ni 3 O 8 films on NdGaO 3 are metallic. This work provides a pathway to the synthesis of Nd n +1 Ni n O 2 n +2 thin films and sets limits on the ability to strain engineer these compounds via epitaxy. 
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    Free, publicly-accessible full text available December 1, 2024
  3. Free, publicly-accessible full text available April 1, 2024
  4. The growing demands for high-energy density electrical energy storage devices stimulate the coupling of conversion-type cathodes and lithium (Li) metal anodes. While promising, the use of these “Li-free” cathodes brings new challenges to the Li anode interface, as Li needs to be dissolved first during cell operation. In this study, we have achieved a direct visualization and comprehensive analysis of the dynamic evolution of the Li interface. The critical metrics of the interfacial resistance, Li growth, and solid electrolyte interface (SEI) distribution during the initial dissolution/deposition processes were systematically investigated by employing multidimensional analysis methods. They include three-electrode impedance tests, in situ atomic force microscopy, scanning electrochemical microscopy, and cryogenic scanning transmission electron microscopy. The high-resolution imaging and real-time observations show that a loose, diffuse, and unevenly distributed SEI is formed during the initial dissolution process. This leads to the dramatically fast growth of Li during the subsequent deposition, deviating from Fick’s law, which exacerbates the interfacial impedance. The compactness of the interfacial structure and enrichment of electrolyte species at the surface during the initial deposition play critical roles in the long-term stability of Li anodes, as revealed by operando confocal Raman spectroscopic mapping. Our observations relate to ion transfer, morphological and structural evolution, and Li (de)solvation at Li interfaces, revealing the underlying pathways influenced by the initial dissolution process, which promotes a reconsideration of anode investigations and effective protection strategies. 
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    Free, publicly-accessible full text available February 14, 2024
  5. Free, publicly-accessible full text available March 1, 2024
  6. Abstract This work describes cryogenic ex situ lift out (cryo-EXLO) of cryogenic focused ion beam (cryo-FIB) thinned specimens for analysis by cryogenic transmission electron microscopy (cryo-TEM). The steps and apparatus necessary for cryo-EXLO are described. Methods designed to limit ice contamination include use of an anti-frost lid, a vacuum transfer assembly, and a cryostat. Cryo-EXLO is performed in a cryostat with the cryo-shuttle holder positioned in the cryogenic vapor phase above the surface of liquid N2 (LN2) using an EXLO manipulation station installed inside a glove box maintained at < 10% relative humidity and inert (e.g., N2 gas) conditions. Thermal modeling shows that a cryo-EXLO specimen will remain vitreous within its FIB trench indefinitely while LN2 is continuously supplied. Once the LN2 is cut off, modeling shows that the EXLO specimen will remain vitreous for over 4 min, allowing sufficient time for the cryo-transfer steps which take only seconds to perform. Cryo-EXLO was applied successfully to cryo-FIB-milled specimen preparation of a polymer sample and plunge-frozen yeast cells. Cryo-TEM of both the polymer and the yeast shows minimal ice contamination with the yeast specimen maintaining its vitreous phase, illustrating the potential of cryo-EXLO for cryo-FIB-TEM of beam-sensitive, liquid, or biological materials. 
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    Free, publicly-accessible full text available January 9, 2024
  7. We demonstrate the epitaxial growth of the first two members, and the [Formula: see text] member of the homologous Ruddlesden–Popper series of [Formula: see text] of which the [Formula: see text] member was previously unknown. The films were grown by suboxide molecular-beam epitaxy where the indium is provided by a molecular beam of indium-suboxide [[Formula: see text]O (g)]. To facilitate ex situ characterization of the highly hygroscopic barium indate films, a capping layer of amorphous [Formula: see text] was deposited prior to air exposure. The structural quality of the films was assessed by x-ray diffraction, reflective high-energy electron diffraction, and scanning transmission electron microscopy. 
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  8. Free, publicly-accessible full text available March 9, 2024
  9. Abstract: This article introduces a training simulator for electron beam alignment using Ronchigrams. The interactive web application, www.ronchigram.com, is an advanced educational tool aimed at making scanning transmission electron microscopy (STEM) more accessible and open. For experienced microscopists, the tool offers on-hand quantification of simulated Ronchigrams and their resolution limits. 
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