arXiv subjects

Yury Gogotsi

Publications and source records attributed to Yury Gogotsi.

18 recordsLinked to original sources

arXiv2026

Operando imaging of intercalation memory in MXenes

Ion intercalation enables reversible control of charge, structure and function in layered solids. Yet layered materials contain nanosheets with different thicknesses and stacking, whose intercalation pathways are averaged out in ensemble measurements. This becomes critical under Angstrom-scale confinement, where ion transport couples to solvent reorganization and host deformation, leaving the origins of kinetics, reversibility and activation unresolved. Here we combine operando interferometric scattering and interference reflection microscopy to resolve proton-driven dynamics in individual single- and multilayer Ti3C2Tx MXene flakes and show that even a few stacked layers introduce a significant kinetic barrier. Cycling then separates nanosheets into three persistent behaviors: reversible monolayers, restacked multilayers with incomplete recovery and delayed deintercalation, and coherently stacked multilayers that self-stabilize through reversible folding. Operando synchrotron X-ray diffraction shows this memory at electrode scale, where the interlayer structure converges towards a reproducible state. Our findings reveal cycling-induced structural memory that governs subsequent intercalation in layered MXenes.

physics.chem-ph↗

arXiv2026

Large-scale Integration of Experimental and Computational Data for 2D Materials

The past decade has seen rapid growth in the number of experimentally realized two-dimensional (2D) materials with diverse chemical and physical properties. However, information on their crystal structure, synthesis routes, and measured or predicted properties, remains scattered across thousands of publications. Here we consolidate this fragmented knowledge by establishing X2DB - an open infrastructure that integrates experimental and computational data on 2D materials. Using extensive literature mining and direct community uploads, we identify 370 unique 2D materials that have been realized in monolayer or few-layer form, and link them to their digital counterparts in computational databases, enabling consistent ab initio characterization of their properties across monolayer, bilayer and bulk forms. We describe the structure and content of the database highlighting its support for community uploads, illustrate how it can be used to generate new scientific insight and introduce a hierarchical classification of the known set of 2D materials. Our work provides a foundation for the integration and cross-fertilization of experimental and theoretical knowledge, opening new avenues for data-driven, predictive synthesis of novel 2D materials.

cond-mat.mtrl-sci↗

arXiv2025

The 2D Materials Roadmap

Over the past two decades, 2D materials have rapidly evolved into a diverse and expanding family of material platforms. Many members of this materials class have demonstrated their potential to deliver transformative impact on fundamental research and technological applications across different fields. In this roadmap, we provide an overview of the key aspects of 2D material research and development, spanning synthesis, properties and commercial applications. We specifically present roadmaps for high impact 2D materials, including graphene and its derivatives, transition metal dichalcogenides, MXenes as well as their heterostructures and moiré systems. The discussions are organized into thematic sections covering emerging research areas (e.g., twisted electronics, moiré nano-optoelectronics, polaritronics, quantum photonics, and neuromorphic computing), breakthrough applications in key technologies (e.g., 2D transistors, energy storage, electrocatalysis, filtration and separation, thermal management, flexible electronics, sensing, electromagnetic interference shielding, and composites) and other important topics (computational discovery of novel materials, commercialization and standardization). This roadmap focuses on the current research landscape, future challenges and scientific and technological advances required to address, with the intent to provide useful references for promoting the development of 2D materials.

cond-mat.mtrl-sci↗

arXiv2025

Organometallic-Inorganic Hybrid MXenes with Tunable Superconductivity

Ti-based two-dimensional transition-metal carbides (MXenes) have attracted attention due to their superior properties and are being explored across various applications1,2. Despite their versatile properties, superconductivity has never been demonstrated, not even predicted, for this important group of 2D materials. In this work, we have introduced an electrochemical intercalation protocol to construct versatile organometallic-inorganic hybrid MXenes and achieved tunable superconductivity in the metallocene-modified layered crystals. Through structural editing of MXene matrix at atomic scale and meticulously modulated intercalation route, Ti3C2Tx intercalated with metallocene species exhibits a superconductive transition temperature (Tc) of 10.2 K. Guest intercalation induced electron filling and strain engineering are responsible for the emerging superconductivity in this intrinsically non-superconducting material. Theoretically, simulated electron-phonon interaction effects further elucidate the nature of the changes in Tc. Furthermore, the Tc of crafted artificial superlattices beyond Ti-based MXenes have been predicted, offering a general strategy for engineering superconductivity and magnetism in layered hybrid materials.

cond-mat.supr-con↗

arXiv2025

A Panoramic View of MXenes via a New Design Strategy

Two-dimensional (2D) transition metal carbides and nitrides, known as MXenes, possess unique physical and chemical properties, enabling diverse applications in fields ranging from energy storage to communication, catalysis, sensing, healthcare, and beyond. The transition metal and nonmetallic atoms in MXenes can exhibit distinct coordination environments, potentially leading to a wide variety of 2D phases. Despite extensive research and significant advancements, a fundamental understanding of MXenes' phase diversity and its relationship with their hierarchical precursors, including intermediate MAX phases and parent bulk phases, remains limited. Using high-throughput modeling based on first-principles density functional theory, we unveil a wide range of MXenes and comprehensively evaluate their relative stabilities across a large chemical space. The key lies in considering both octahedral and trigonal prismatic coordination environments characteristic of various bulk phases. Through this comprehensive structural library of MXenes, we uncover a close alignment between the phase stability of MXenes and that of their hierarchical 3D counterparts. Building on this, we demonstrate a new design strategy where the atomic coordination environments in parent bulk phases can serve as reliable predictors for the design of MXenes, reducing reliance on intermediate MAX phases. Our study significantly expands the landscape of MXenes, at least doubling the number of possible structures.

cond-mat.mtrl-sci↗

arXiv2024

Emerging Ta$_{4}$C$_{3}$ and Mo$_{2}$Ti$_{2}$C$_{3}$ MXene Nanosheets for Ultrafast Photonics

Ultrafast nonlinear optical (NLO) response, fast carrier recovery, broadband absorption, and resistance to radiation and heat make 2D materials promising for photonic technologies. However, low electronic conductivity and carrier concentration limit the performance of semiconducting or semimetallic materials. This work investigates the ultrafast NLO properties and carrier dynamics of Ta$_{4}$C$_{3}$T$_{x}$ and out-of-plane ordered Mo$_{2}$Ti$_{2}$C$_{3}$T$_{x}$ MXenes using Z-scan and pump-probe optical Kerr effect techniques under visible and infrared femtosecond laser pulses. Their NLO response surpasses all previously studied MXenes and most other 2D nanomaterials, attaining exceptionally high third-order susceptibility (\c{hi}(3)) values on the order of 10^{-13} esu. Mo$_{2}$Ti$_{2}$C$_{3}$T$_{x}$ exhibits the strongest NLO response under both excitation regimes, attributed to charge transfer between Mo and Ti layers in the MXene structure. Under visible excitation, the studied MXenes display pronounced saturable absorption, while under infrared excitation, they exhibit strong reverse saturable absorption, resulting in efficient optical limiting. Additionally, pump-probe experiments identify two distinct relaxation processes: a fast one on the sub-picosecond timescale and a slower one a few picoseconds after photoexcitation. Our results indicate that these MXenes are among the strongest NLO materials. They show their great potential for advanced photonic and optoelectronic applications in laser technologies, optical protection, telecommunications, and optical/quantum computing.

physics.optics↗

arXiv2024

Violation of the Wiedemann-Franz law and ultra-low thermal conductivity of Ti$_3$C$_2$T$_x$ MXene

The high electrical conductivity and good chemical stability of MXenes offer hopes for their use in many applications, such as wearable electronics, energy storage, or electromagnetic interference shielding. While their optical, electronic and electrochemical properties have been widely studied, the information on thermal properties of MXenes is scarce. In this study, we investigate the heat transport properties of Ti$_3$C$_2$T$_x$ MXene single flakes using scanning thermal microscopy and find exceptionally low anisotropic thermal conductivities within the Ti$_3$C$_2$T$_x$ flakes, leading to an effective thermal conductivity of 0.78$\pm$0.21 W m$^{-1}$ K$^{-1}$. This observation is in stark contrast to the predictions of the Wiedemann-Franz law, as the estimated Lorenz number is only 0.25 of the classical value. Due to the combination of low thermal conductivity and low emissivity of Ti$_3$C$_2$T$_x$, the heat loss from it is two orders of magnitude smaller than that from common metals. Our study explores the heat transport mechanisms of MXenes and highlights a promising approach for developing thermal insulation, two-dimensional thermoelectric, or infrared stealth materials.

cond-mat.mtrl-sci↗

arXiv2023

Multi-year Study of Environmental Stability of Ti$_3$C$_2$T$_x$ MXene Films

MXenes are a family of two-dimensional (2D) carbides and nitrides that display extraordinary electrical, optical, chemical, and electrochemical properties. There is a perception that MXenes are unstable and degrade quickly, limiting potential applications and requiring specific storage conditions to last for a long time. This was true for delaminated MXenes flakes in dilute dispersions prepared from defective precursors when MXene research was in its infancy. Since then, significant developments in MXene synthesis, processing, and understanding of its chemistry led to dramatic increases in environmental stability. Herein, we analyze Ti$_3$C$_2$T$_x$ free-standing films aged from 4 to 9 years through structural and morphological characterization along with electrical conductivity measurements to reveal the effect, or lack thereof, of prolonged storage under ambient conditions. Further, we show that the decrease in electronic conductivity over time is largely caused by the uptake of water by the hydrophilic surface chemistry of MXenes, which can be easily removed and its effect reversed by vacuum annealing.

physics.app-ph↗

arXiv2023

Direct Fabrication of Atomically Defined Pores in MXenes

Controlled fabrication of nanopores in atomically thin two-dimensional material offers the means to create robust membranes needed for ion transport, nanofiltration, and DNA sensing. Techniques for creating nanopores have relied upon either plasma etching or direct irradiation using electrons or ions; however, aberration-corrected scanning transmission electron microscopy (STEM) offers the advantage of combining a highly energetic, sub-angstrom sized electron beam for atomic manipulation along with atomic resolution imaging. Here, we utilize a method for automated nanopore fabrication with real-time atomic visualization to enhance our mechanistic understanding of beam-induced transformations. Additionally, an electron beam simulation technique, Electron-Beam Simulator (E-BeamSim) was developed to observe the atomic movements and interactions resulting from electron beam irradiation. Using the 2D MXene Ti3C2Tx, we explore the influence of temperature on nanopore fabrication by tracking atomic transformation pathways and find that at room temperature, electron beam irradiation induces random displacement of atoms and results in a pileup of titanium atoms at the nanopore edge. This pileup was confirmed and demonstrated in E-BeamSim simulations around the small, milled area in the MXene monolayer. At elevated temperatures, the surface functional groups on MXene are effectively removed, and the mobility of atoms increases, which results in atomic transformations that lead to the selective removal of atoms layer by layer. Through controllable manufacture using e-beam milling fabrication, the production and then characterization of the fabricated defects can be better understood for future work. This work can lead to the development of defect engineering techniques within functionalized MXene layers.

cond-mat.mtrl-sci↗

arXiv2022

Chemical-scissor-mediated structural editing of layered transition metal carbides

Intercalation of non-van der Waals (vdW) layered materials can produce new 2D and 3D materials with unique properties, but it is difficult to achieve. Here, we describe a structural editing protocol for 3D non-vdW layered ternary carbides and nitrides (MAX phases) and their 2D vdW derivatives (MXenes). Gap-opening and species-intercalating stages were mediated by chemical scissors and guest intercalants, creating a large family of layered materials with unconventional elements and structures in MAX phases, as well as MXenes with versatile termination species. Removal of surface terminations by metal scissors and stitching of carbide layers by metal atoms leads to a reverse transformation from MXenes to MAX phases, and metal-intercalated 2D carbides. This scissor-mediated structural editing may enable structural and chemical tailoring of other layered ceramics.

cond-mat.mtrl-sci↗

arXiv2022

Removal and Recovery of Ammonia from Wastewater using Ti$_3$C$_2$T$_x$ MXenes in Flow Electrode Capacitive Deionization

Flowing electrode capacitive deionization systems (FE-CDI) have recently garnered attention because of their ability to prevent cross contamination and operate in uninterrupted cycles ad infinitum. Typically, FE-CDI electrodes suffer from low conductivity, reducing deionization performance. Utilization of higher mass loadings to combat this leads to poor rheological properties. Herein, Ti$_3$C$_2$T$_x$ MXene was introduced as 1 mg/mL slurry electrodes in an FE-CDI system for the removal and recovery of ammonia from simulated agricultural wastewater. The electrode performance was evaluated by operating the FE-CDI system with a feed solution of 500 mg/L NH$_4$Cl running in batch mode at a constant voltage of 1.20 V and -1.20 V in charging and discharging modes, respectively. Despite the low loading, Ti$_3$C$_2$T$_x$ flowing electrodes showed markedly improved performance, achieving 60% ion removal efficiency in a saturation time of 115 minutes with an adsorption capacity of 460 mg/g. To understand the high adsorption performance of the electrodes, physiochemical and structural analysis was done via a variety of characterization techniques such as SEM, TEM, XRD, DLS, and Raman Spectroscopy. Cyclic Voltammetry and Galvanostatic charge/discharge profiles were obtained to evaluate the electrochemical properties of the electrodes. The system proved to be an energy-saving technology by exhibiting a charge efficiency of 58-70% while operating at an energy consumption of 0.45 kWh/kg. A 92% regeneration efficiency showed that the electrodes were stable and suitable for long term and scalable usage. The results demonstrate that MXenes have the potential to improve the FE-CDI process for energy-efficient removal and recovery of ammonia.

physics.app-ph↗

arXiv2021

Ti$_3$C$_2$T$_x$ MXene Enabled All-Optical Nonlinear Activation Function for On-Chip Photonic Deep Neural Networks

Neural networks are one of the first major milestones in developing artificial intelligence systems. The utilisation of integrated photonics in neural networks offers a promising alternative approach to microelectronic and hybrid optical-electronic implementations due to improvements in computational speed and low energy consumption in machine-learning tasks. However, at present, most of the neural network hardware systems are still electronic-based due to a lack of optical realisation of the nonlinear activation function. Here, we experimentally demonstrate two novel approaches for implementing an all-optical neural nonlinear activation function based on utilising unique light-matter interactions in 2D Ti$_3$C$_2$T$_x$ (MXene) in the infrared (IR) range in two configurations: 1) a saturable absorber made of MXene thin film, and 2) a silicon waveguide with MXene flakes overlayer. These configurations may serve as nonlinear units in photonic neural networks, while their nonlinear transfer function can be flexibly designed to optimise the performance of different neuromorphic tasks, depending on the operating wavelength. The proposed configurations are reconfigurable and can therefore be adjusted for various applications without the need to modify the physical structure. We confirm the capability and feasibility of the obtained results in machine-learning applications via an Modified National Institute of Standards and Technology (MNIST) handwritten digit classifications task, with near 99% accuracy. Our developed concept for an all-optical neuron is expected to constitute a major step towards the realization of all-optically implemented deep neural networks.

physics.optics↗

arXiv2021

Ultralow and Selective Infrared Emission from MXenes

Low and selective infrared emission materials are necessary for next generation thermal technologies, including passive heating, infrared identification, and photothermal conversion. Here, we report on the intrinsic infrared radiation properties of three MXenes: Ti3C2Tx, Ti3CNTx, and V4C3Tx. The infrared emissivity of 200 nm thick Ti3C2Tx coating is lower than 0.06 between wavelengths of 3-27 μm, while Ti3CNTx and V4C3Tx have values of 0.13 and 0.26, respectively. Investigation using a laboratory-based passive heating process showed that MXene coatings suppress the thermal radiation. The infrared identification capability was also validated using a patterned MXene fabric. This work paves the way for developing MXene-based smart wearable devices and garments capable of selective and localized thermal management.

physics.app-ph↗

arXiv2021

High-speed ionic synaptic memory based on two-dimensional titanium carbide MXene

Synaptic devices with linear high-speed switching can accelerate learning in artificial neural networks (ANNs) embodied in hardware. Conventional resistive memories however suffer from high write noise and asymmetric conductance tuning, preventing parallel programming of ANN arrays as needed to surpass conventional computing efficiency. Electrochemical random-access memories (ECRAMs), where resistive switching occurs by ion insertion into a redox-active channel address these challenges due to their linear switching and low noise. ECRAMs using two-dimensional (2D) materials and metal oxides suffer from slow ion kinetics, whereas organic ECRAMs enable high-speed operation but face significant challenges towards on-chip integration due to poor temperature stability of polymers. Here, we demonstrate ECRAMs using 2D titanium carbide (Ti3C2Tx) MXene that combines the high speed of organics and the integration compatibility of inorganic materials in a single high-performance device. Our ECRAMs combine the speed, linearity, write noise, switching energy and endurance metrics essential for parallel acceleration of ANNs, and importantly, they are stable after heat treatment needed for back-end-of-line integration with Si electronics. The high speed and performance of these ECRAMs introduces MXenes, a large family of 2D carbides and nitrides with more than 30 compositions synthesized to date, as very promising candidates for devices operating at the nexus of electrochemistry and electronics.

physics.app-ph↗

arXiv2021

Multi-modal Spectroscopic Study of Surface Termination Evolution in Cr2TiC2Tx MXene

Control of surface functionalization of MXenes holds great potential, and in particular, may lead to tuning of magnetic and electronic order in the recently reported magnetic Cr2TiC2Tx. Here, vacuum annealing experiments of Cr2TiC2Tx are reported with in situ electron energy loss spectroscopy and novel in situ Cr K-edge extended energy loss fine structure analysis, which directly tracks the evolution of the MXene surface coordination environment. These in situ probes are accompanied by benchmarking synchrotron X-ray absorption fine structure measurements and density functional theory calculations. With the etching method used here, the MXene has an initial termination chemistry of Cr2TiC2O1.3F0.8. Annealing to 600 C results in the complete loss of -F, but -O termination is thermally stable up to (at least) 700 C. These findings demonstrate thermal control of -F termination in Cr2TiC2Tx and offer a first step towards termination engineering this MXene for magnetic applications. Moreover, this work demonstrates high energy electron spectroscopy as a powerful approach for surface characterization in 2D materials.

cond-mat.mtrl-sci↗

arXiv2014

Interfacial Ionic Liquids: Connecting Static and Dynamic Structures

It is well-known that room temperature ionic liquids (RTILs) often adopt a charge-separated layered structure, i.e., with alternating cation- and anion-rich layers, at electrified interfaces. However, the dynamic response of the layered structure to temporal variations in applied potential is not well understood. We used in situ, real-time X-ray reflectivity (XR) to study the potential-dependent electric double layer (EDL) structure of an imidazolium-based RTIL on charged epitaxial graphene during potential cycling as a function of temperature. The results suggest that the graphene-RTIL interfacial structure is bistable in which the EDL structure at any intermediate potential can be described by the combination of two extreme-potential structures whose proportions vary depending on the polarity and magnitude of the applied potential. This picture is supported by the EDL structures obtained by fully atomistic molecular dynamics (MD) simulations at various static potentials. The potential-driven transition between the two structures is characterized by an increasing width but with an approximately fixed hysteresis magnitude as a function of temperature. The results are consistent with the coexistence of distinct anion and cation adsorbed structures separated by an energy barrier (~0.15 eV).

cond-mat.soft↗

arXiv2014

MXenes as High Capacity Electrode Materials for Metal (Li, Na, K, Ca)-ion batteries

Two-dimensional (2D) materials can have an excellent capability to handle high rates of charge in ion batteries since metal ions need not diffuse in a 3D lattice structure. However graphene, which is the most important 2D material, is known to have no Li capacity. Herein, adsorption of Li, as well as Na, K, and Ca on Ti$_3$C$_2$, one representative MXene, is predicted by first-principles density functional calculations. In our study, we observed that these alkali ions exhibit different adsorption energy depending on the coverage. The adsorption energies of Na, K and Ca decrease as coverage increases, while Li shows little sensitivity to variance in coverage. This observed relationship between adsorption energies and coverage of alkali ions on Ti$_3$C$_2$ can be explained by their effective ionic radii. A larger effective ionic radius increases interaction between alkali atoms, thus lower capacity and coverage are obtained. Our calculated capacity values for Li, Na, K and Ca on Ti$_3$C$_2$ are 639.5, 319.8, 191.8 and 159.9 mAh g$^{-1}$, respectively. Compared to materials currently used in Li ion battery anodes, MXene shows great promise in increasing overall battery performance.

cond-mat.mtrl-sci↗

arXiv2012

Understanding Controls on Interfacial Wetting at Epitaxial Graphene: Experiment and Theory

The interaction of interfacial water with graphitic carbon at the atomic scale is studied as a function of the hydrophobicity of epitaxial graphene. High resolution X-ray reflectivity shows that the graphene-water contact angle is controlled by the average graphene thickness, due to the fraction of the film surface expressed as the epitaxial buffer layer whose contact angle (contact angle θ_c = 73°) is substantially smaller than that of multilayer graphene (θ_c = 93°). Classical and ab initio molecular dynamics simulations show that the reduced contact angle of the buffer layer is due to both its epitaxy with the SiC substrate and the presence of interfacial defects. This insight clarifies the relationship between interfacial water structure and hydrophobicity, in general, and suggests new routes to control interface properties of epitaxial graphene.

cond-mat.mtrl-sci↗