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Maleski, Kathleen

Publications and source records attributed to Maleski, Kathleen.

6 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Shifts in valence states in bimetallic MXenes revealed by electron energy-loss spectroscopy (EELS)

MXenes are an emergent class of two-dimensional materials with a very wide spectrum of promising applications. The synthesis of multiple MXenes, specifically solid-solution MXenes, allows fine tuning of their properties, expands their range of applications, and leads to enhanced performance. The functionality of solid-solution MXenes is closely related to the valence state of their constituents: transition metals, oxygen, carbon, and nitrogen. However, the impact of changes in the oxidation state of elements in MXenes is not well understood. In this work, three interrelated solid-solution MXene systems (Ti$_{2–y}$Nb$_y$CT$_x$, Nb$_{2–y}$V$_y$CT$_x$, and Ti$_{2–y}$V$_y$CT$_x$) were investigated with scanning transmission electron microscopy and electron energy-loss spectroscopy to determine the localized valence states of metals at the nanoscale. The analysis demonstrates changes in the electronic configuration of V upon modification of the overall composition and within individual MXene flakes. These shifts of oxidation state can explain the nonlinear optical and electronic features of solid-solution MXenes. Vanadium appears to be particularly sensitive to modification of the valence state, while titanium maintains the same oxidation state in Ti–Nb and Ti–V MXenes, regardless of stoichiometry. Here, the study also explains Nb's influential role in the previously observed electronic properties in the Nb–V and Nb–Ti systems.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Intercalation-Induced Reversible Electrochromic Behavior of Two-Dimensional Ti 3 C 2 T x MXene in Organic Electrolytes

MXenes, a large family of two-dimensional materials, have attracted tremendous attention due to their unique physical and chemical properties. Reversible ion intercalation between MXene layers allows modification of the optical, thermal, magnetic, and chemical properties. The electrochemical charge/discharge of MXenes in aqueous electrolytes was reported to lead to reversible electrochromic behavior. In this work, the electrochromic effect of semitransparent Ti 3 C 2 T x MXene film was probed by electrochemical intercalation of Li ions. Correspondingly, a peak shift of 100 nm was observed in the UV-vis spectrum. By combining in-situ Raman spectroscopy, in-situ X-ray diffraction, and density functional theory calculations, we show that the electrochromic shift is primarily due to the formation of robust O-Li bonds and the emerging bands induced changes of inter-band excitations. Finally, understanding the mechanism of electrochromic behavior in Ti 3 C 2 T x lays the foundations of designating 2D materials with durable, controllable, and efficient intercalation-induced electrochromic behaviors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Dynamically controlled random lasing with colloidal titanium carbide MXene

Control of lasing properties through tailorable and dynamically tunable materials and reconfigurable compositions can augment the performance of random lasers for a wide range of applications. Here, a colloid of randomly dispersed weakly scattering single-layer titanium carbide (Ti 3 C 2 T x ) MXene flakes embedded within rhodamine 101 gain medium is experimentally shown to provide feedback for random lasing. Additionally, in contrast to previously reported random laser systems where the optical properties of scatterers are static, the relative permittivity of Ti 3 C 2 T x MXene flakes can be varied under optical pumping due to the saturable absorption properties. Numerical simulations indicate that the observed nonlinear response of Ti 3 C 2 T x MXene flakes enables dynamically tunable random lasing. Thus, pumping the Ti 3 C 2 T x MXene flakes with a second optical source decreases the gain threshold required to obtain random lasing. Also, using numerical simulations, it is shown that the control over the intensity of the second pump enables tuning the field distribution of the random lasing modes. Considering the diversity of the MXenes family, the proposed MXene colloidal metamaterial design opens up a new avenue to advanced control of lasing properties for photonic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Tunable electrochromic behavior of titanium-based MXenes

Two-dimensional transition metal carbides, nitrides and carbonitrides, popular by the name MXenes, are a promising class of materials as they exhibit intriguing optical, optoelectronic and electrochemical properties. Taking advantage of their metallic conductivity and hydrophilicity, titanium carbide MXenes (Ti 3 C 2 T x and others) are used to fabricate solution processable transparent conducting electrodes (TCEs) for the design of three-electrode electrochromic cells. However, the tunable electrochromic behavior of various titanium-based MXene compositions across the entire visible spectrum has not yet been demonstrated. Here, we investigate the intrinsic electrochromic properties of titanium-based MXenes, Ti 3 C 2 T x , Ti 3 CNT x , Ti 2 CT x , and Ti 1.6 Nb 0.4 CT x , where individual MXenes serve as a transparent conducting, electrochromic, and plasmonic material layer. Plasmonic extinction bands for Ti 3 C 2 T x , Ti 2 CT x and Ti 1.6 Nb 0.4 CT x are centered at 800, 550 and 480 nm, which are electrochemically tunable to 630, 470 and 410 nm, respectively, whereas Ti 3 CNT x shows a reversible change in transmittance in the wide visible range. Additionally, the switching rates of MXene electrodes with no additional transparent conductor electrodes are estimated and correlated with the respective electrical figure of merit values. This work demonstrates that MXene-based electrochromic cells are tunable in the entire visible spectrum and suggests the potential of the MXene family of materials in optoelectronic, plasmonic, and photonic applications, such as tunable visible optical filters and modulators, to name a few.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗