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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Chemical interaction and enhanced interfacial ion transport in a ceramic nanofiber–polymer composite electrolyte for all-solid-state lithium metal batteries

This article reports the synergy between ceramic nanofibers and a polymer, and the enhanced interfacial Li-ion transport along the nanofiber/polymer interface in a solid-state ceramic/polymer composite electrolyte, in which a three-dimensional (3D) electrospun aluminum-doped Li 0.33 La 0.557 TiO 3 (LLTO) nanofiber network is embedded in a polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) matrix. Strong chemical interaction occurs between the nanofibers and the polymer matrix. Addition of the ceramic nanofibers into the polymer matrix results in the dehydrofluorination of the PVDF chains, deprotonation of the –CH 2 moiety and amorphization of the polymer matrix. Solid-state nuclear magnetic resonance (NMR) spectra reveal that lithium ions transport via three pathways: (i) intra-polymer transport, (ii) intra-nanofiber transport, and (iii) interfacial polymer/nanofiber transport. In addition, lithium phosphate is coated on the LLTO nanofiber surface before the nanofibers are embedded into the polymer matrix. The presence of lithium phosphate at the LLTO/polymer interface further enhances the chemical interaction between the nanofibers and the polymer, which promotes the lithium ion transport along the polymer/nanofiber interface. This in turn improves the ionic conductivity and electrochemical cycling stability of the nanofiber/polymer composite. As a result, the flexible LLTO/Li 3 PO 4 /polymer composite electrolyte membrane exhibits an ionic conductivity of 5.1 × 10 -4 S cm -1 at room temperature and an electrochemical stability window of 5.0 V vs. Li/Li + . A symmetric Li|electrolyte|Li half-cell shows a low overpotential of 50 mV at a constant current density of 0.5 mA cm -2 for more than 800 h. In addition, a full cell is constructed by sandwiching the composite electrolyte between a lithium metal anode and a LiFePO 4 -based cathode. Such an all-solid-state lithium metal battery exhibits excellent cycling performance and rate capability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Revealing the complex chemistry of grain boundaries in K-doped BaFe 2 As 2 with atom probe tomography

Iron-based superconductors have attractive properties for high-field applications, but there is a lack of understanding of the effect of grain boundary chemistry on the in-field performance. The near atomic-scale resolution, ppm sensitivity and 3D analysis offered by atom probe tomography make it a powerful tool to investigate the nanoscale structure and chemistry of these defects in fine-grained K-doped BaFe 2 As 2 samples. A computational method to systematically extract and compare the Gibbsian interfacial excess of chemical species across grain boundaries has been explored in this work. The robustness of the method has been tested by evaluating the effects of selected variables on simulated APT datasets. The accuracy and precision of the calculated Gibbsian interfacial excess were found to be stable over a range of analysis conditions: varying grain boundary widths and detection efficiencies, spatial precisions below 1.5 nm, and bin widths between 1.2 and 1.6 nm. For the K-doped BaFe 2 As 2 samples studied, segregation of As, Ba, K and impurities of O, Na, and Sb were found at grain boundaries. The Gibbsian excess values were found to vary widely between different boundaries, showing the complexity of the grain boundary chemistry in this material. Possible links between the observed critical current density (Jc) of these samples and their nano- and micro-structure have also been investigated and discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Comparison of semi-doped PANI/DBSA complex achieved by thermal doping and roll-mill process: A new perspective for application

Conductive polymers have garnered extensive attention over the last few decades owing to their vast applications and relative ease of production. One such polymer is PANI; with versatile thermo-mechanical, chemical, and electrical properties, has been researched for varied applications in the field of electronics, electrodes and corrosion protection. In this study, we focus on an alternative route to process semi-doped PANI/DBSA complexes with special focus on material properties for improved processability. This study investigates the influence of two different material preparation techniques: roll-milling and thermal-doping, on the formability and processability of such polymer-complex systems. Results confirm similar doping levels achieved in both processes and shear-thinning behavior was only observed for roll-milled samples. These results underline the formability of roll-milled PANI/DBSA with thermosetting resins. It essentially explains the production route and offers a perspective for commercial manufacturing.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Chemical and Electrochemical O 2 Reduction on Earth-Abundant M-N-C Catalysts and Implications for Mediated Electrolysis

M-N-C catalysts, incorporating non-precious-metal ions (e.g. M = Fe, Co) within a nitrogen-doped carbon support, have been the focus of broad interest for electrochemical O 2 reduction and aerobic oxidation reactions. The present study explores the mechanistic relationship between the O 2 reduction mechanism under electrochemical and chemical conditions. In this work, chemical O 2 reduction is investigated via the aerobic oxidation of a hydroquinone, in which the O–H bonds supply the protons and electrons needed for O 2 reduction to water. Mechanistic studies have been conducted to elucidate whether the M-N-C catalyst couples two independent half-reactions (IHR), similar to electrode-mediated processes, or mediates a direct inner-sphere reaction (ISR) between O 2 and the organic molecule. Kinetic data support the latter ISR pathway. This conclusion is reinforced by rate/potential correlations that reveal significantly different Tafel slopes, implicating different mechanisms for chemical and electrochemical O 2 reduction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Thermal transport and mixed valence in ZrTe3 doped with Hf and Se

Two-dimensional transition metal trichalcogenides (TMTCs) feature covalently bonded metal-chalcogen layers separated by the van der Waals (vdW) gap. Similar to transition metal dichalcogenides (TMDCs), TMTCs often host charge density waves (CDWs) and superconductivity, but unlike TMDCs, atomic chains in the crystal structure give rise to quasi one-dimensional (quasi 1D) conduction. ZrTe3 features the CDW below TCDW = 63 K and filamentary superconductivity below 2 K that can be enhanced by pressure or chemical substitution. Here, we report the presence of mixed valent Zr2+ and Zr4+ atoms in ZrTe3 crystals that are reduced by doping in ZrTe3−xSex and Zr1−yHfyTe3. Superconductivity is enhanced via disorder in Te2-Te3 atomic chains that are associated with CDW formation. Hf substitution on the Zr atomic site enhances TCDW due to unperturbed Te2-Te3 chain periodicity and enhanced electron-phonon coupling. Weak electronic correlations in ZrTe3−xSex are likely governed by the lattice contraction effects.

Liu, Yu (ORCID:0000000188862876)↗
DOE OSTI2024

Catalysis of the Oxygen-Evolution Reaction in 1.0 M Sulfuric Acid by Manganese Antimonate Films Synthesized via Chemical Vapor Deposition

Manganese antimonate (Mn y Sb 1–y O x ) electrocatalysts for the oxygen-evolution reaction (OER) were synthesized via chemical vapor deposition. Mn-rich rutile Mn 0.63 Sb 0.37 O x catalysts on fluorine-doped tin oxide (FTO) supports drove the OER for 168 h (7 days) at 10 mA cm –2 with a time-averaged overpotential of 687 ± 9 mV and with >97% Faradaic efficiency. Time-dependent anolyte composition analysis revealed the steady dissolution of Mn and Sb. Extended durability analysis confirmed that Mn-rich Mn y Sb 1–y O x materials are more active but dissolve at a faster rate than previously reported Sb-rich Mn y Sb 1–y O x alloys.

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

Thiolate‐Protected Single‐Atom Alloy Nanoclusters: Correlation between Electronic Properties and Catalytic Activities

Abstract Due to their interesting chemical and optical properties, metal nanoclusters are used in various catalytic reactions and in energy conversion. By incorporating thiolate‐protecting ligands, their size and composition can be tuned. Doping these nanoclusters to form single‐atom alloy (SAA) nanoclusters is shown to further enhance these properties as a result from the synergy between the dopant and host atoms. In addition to their optical and chemical properties, SAA nanoclusters also have interesting electronic properties. However, these properties are often underdiscussed when studying SAA nanoclusters. This review provides an overview of representative studies done on the in‐depth understanding of the electronic properties and catalytic activities of Ag‐based and Au‐based thiolate‐protected SAA nanoclusters. The use of density functional theory (DFT), X‐ray absorption spectroscopy, and X‐ray photoelectron spectroscopy are employed to correlate the changes in charge states of thiolate‐protected SAA nanoclusters with their superior catalytic activity versus monometallic nanoclusters. DFT, UV–vis spectroscopy, and voltammetric methods link the changes in molecular energy levels of thiolate‐protected SAA nanoclusters to their enhanced catalytic performance over monometallic nanoclusters.

Walsh, Andrew G.↗
DOE OSTI2024

Optical properties of semiconductor nanoparticles doped with 3d and 4f block elements

Doped inorganic nanoparticles (NPs) have enabled researchers across multiple disciplines to create new materials with unique optical, electronic, magnetic, electrical, chemical, and/or compositional properties. In the quest for generating newer functional materials with controlled optical and electronic properties, the use of d- and f-block elements as dopants in the inorganic NPs remain at the forefront of research. This article summarizes experiments that identify the important control parameters, in the form of NP core and surface properties, for promoting host-sensitized dopant emission from d- and f-doped inorganic/semiconductor NPs. We conclude that energy offsets between the dopant and NP electronic levels and an understanding of the charge trapping mechanisms can be used to predict dopant luminescence, and we claim that these features can be used to choose NP host materials by design, rather than by trial and error.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Crystal structure, magnetism, and specific heat of lightly depleted layered honeycomb oxides, Na$_2$(Ni$_{2-x}$D$_x$)TeO$_6$ ($D$ = Mg, Ga, Co; 0.10 ≤ $x$ ≤ 0.25)

Layered oxides, in which transition metal atoms form a honeycomb lattice, are known for complex magnetic phase diagrams. In this work we study the doped compounds, Na$_2$(Ni$_{2-x}$D$_x$)TeO$_6$, $D$ = Mg, Ga, and Co (0.10 ≤ $x$ ≤ 0.25), to understand how chemical dilution at the nickel site influences the stability of magnetic exchanges within the honeycomb layer of the parent, Na$_2$ Ni$_2$ TeO$_6$. Here, the studied compounds were found to crystallize in $P6_3/mcm$ space group common to P2 type layered oxides. In general, the lattice parameters and the unit cell volume expanded with increased doping. The oxidation states determined from X-ray photoelectron spectroscopy were consistent with bond valence sum estimates, that confirmed the presence of Ni$^{2+}$, Mg$^{2+}$, Ga$^{3+}$, Co$^{2+}$ in our samples. Irrespective of magnetic or non-magnetic doping, the magnetic phase transition temperature ($T_N$) of the doped compounds were reduced from that of Na$_2$ Ni$_2$ TeO$_6$ or Na$_2$ Co$_2$ TeO$_6$, and lay between 21.7 K and 26.8 K. The effective paramagnetic moments extracted from Curie–Weiss analysis were in the range 3.17 μ B to 3.84 μ B and the Weiss temperatures were between $-15$ K and $-25$ K, suggesting antiferromagnetism. Mg- and Ga-doped compounds showed free spin formation, indicated by Curie–Weiss tails in their magnetic susceptibility. Our results suggest emergence of short-range magnetic correlations in Na$_2$(Ni$_{2-x}$D$_x$)TeO$_6$, enhanced due to the depletion of the Ni honeycomb lattice.

75 - CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY A↗
DOE OSTI2022

Deep level defects in low-pressure chemical vapor deposition grown (010) β-Ga 2 O 3

This study provides the full-bandgap evaluation of defect state distributions in beta phase gallium oxide (β-Ga 2 O 3 ) grown by low-pressure chemical vapor deposition (LPCVD) on (010) β-Ga 2 O 3 substrates at high growth of up to 20 µm/h. Deep-level optical spectroscopy and deep-level transient spectroscopy measurements applied to Ni/β-Ga 2 O 3 Schottky diodes revealed the presence of a previously unreported defect state at E C -3.6 eV, which dominated the overall trap distribution in LPCVD grown material. However, states at E C -0.8 eV, E C -2.0 eV, and E C -4.4. eV were also detected, similar to prior studies on β-Ga 2 O 3 grown by other methods, with similar or lower concentrations for the LPCVD samples. The E C -0.8 eV and E C -2.0 eV states were previously connected to residual Fe impurities and gallium vacancies, respectively. The total concentration of traps in the LPCVD material was on par with or lower than the state-of-the-art metal–organic chemical vapor deposition-grown materials despite the much higher growth rate, and the distribution of states showed negligible dependence on SiCl 4 flow rate and doping concentration. These results demonstrate that the high growth rate of LPCVD-grown β-Ga 2 O 3 is very promising for achieving thick, low defect density, and high-quality layers needed for multi-kV device applications.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Bandgap engineering of SrZrS 3 chalcogenide perovskite via substitutional doping for photovoltaic applications: a first-principles DFT study

Strontium zirconium sulfide (SrZrS 3 ) has garnered significant attention for photovoltaic (PV) applications due to its excellent optoelectronic properties, high chemical and moisture stability, and non-toxicity. However, the bandgaps of both the α- and β-phases lie outside the optimum ranges for both single-junction solar cells (SJSCs) and tandem solar cells (TSCs), thereby limiting their applications in PV technologies. In this study, we employed hybrid density functional theory to engineer the band gaps of α- and β-SrZrS 3 through substitutional doping. We considered three dopants (Hf, Sn, and Ti) at the Zr site of SrZrS 3 with varying doping concentrations and investigated their effects on the structural, electronic, and optical properties of the materials. We found that Sn and Ti doping effectively lowers the band gaps of both α- and β-SrZrS 3 , whereas Hf doping increases them. For x values up to 0.25, the band gaps of the α-SrZr 1−x Sn x S 3 and α-SrZr 1−x Ti x S 3 are within the optimum range for SJSCs, and those of β-SrZr 1−x Sn x S 3 and β-SrZr 1−x Ti x S 3 lie within the optimum range for Si/perovskite as well as perovskite/perovskite TSCs. The three dopants exhibited significant effects on the optical properties of both α- and β-SrZrS 3 , including the absorption coefficient, energy-loss functions, reflectivity, and refractivity spectra. Thermodynamic stability analysis revealed that for both phases, SrZr 1−x Hf x S 3 can be synthesized via exothermic processes, whereas the formation of SrZr 1−x Ti x S 3 and SrZr1−xSn x S 3 is endothermic and hence, not thermodynamically favorable. Further analysis showed that SrZr 1−x Ti x S 3 in both α- and β-phases are stable under thermodynamic equilibrium conditions, whereas SrZr 1−x Sn x S 3 is prone to dissociation into ternary phases (SrZrS 3 and SrSnS 3 ), especially at higher doping concentrations. These results show that Ti doping is effective in tuning the band gaps of α- and β-SrZrS 3 toward the optimal values for PV applications.

14 SOLAR ENERGY↗
DOE OSTI2020

In-situ resonant band engineering of solution-processed semiconductors generates high performance n-type thermoelectric nano-inks

Thermoelectric devices possess enormous potential to reshape the global energy landscape by converting waste heat into electricity, yet their commercial implementation has been limited by their high cost to output power ratio. No single “champion” thermoelectric material exists due to a broad range of material-dependent thermal and electrical property optimization challenges. While the advent of nanostructuring provided a general design paradigm for reducing material thermal conductivities, there exists no analogous strategy for homogeneous, precise doping of materials. Here, we demonstrate a nanoscale interface-engineering approach that harnesses the large chemically accessible surface areas of nanomaterials to yield massive, finely-controlled, and stable changes in the Seebeck coefficient, switching a poor nonconventional p- type thermoelectric material, tellurium, into a robust n -type material exhibiting stable properties over months of testing. These remodeled, n -type nanowires display extremely high power factors (~500 µW m -1 K -2 ) that are orders of magnitude higher than their bulk p -type counterparts.

42 ENGINEERING↗
DOE OSTI2022

Prediction of orbital-selective Mott phases and block magnetic states in the quasi-one-dimensional iron chain Ce 2 O 2 FeSe 2 under hole and electron doping

The recent detailed study of quasi-one-dimensional iron-based ladders, with the 3d iron electronic density n=6, has unveiled surprises, such as orbital-selective phases. However, similar studies for n=6 iron chains are still rare. Here a three-orbital electronic Hubbard model was constructed to study the magnetic and electronic properties of the quasi-one-dimensional n=6 iron chain Ce 2 O 2 FeSe 2 , with focus on the effect of doping. Specifically, introducing the Hubbard U and Hund J H couplings and studying the model via the density matrix renormalization group, we report the ground-state phase diagram varying the electronic density away from n=6. For the realistic Hund coupling J H /U=1/4, several electronic phases were obtained, including a metal, orbital-selective Mott, and Mott insulating phases. Doping away from the parent phase, the competition of many tendencies leads to a variety of magnetic states, such as ferromagnetism, as well as several antiferromagnetic and magnetic “block” phases. In the hole-doping region, two different interesting orbital-selective Mott phases were found: OSMP1 (with one localized orbital and two itinerant orbitals) and OSMP2 (with two localized orbitals and one itinerant orbital). Moreover, charge disproportionation phenomena were found in special doping regions. We argue that our predictions can be tested by simple modifications in the original chemical formula of Ce 2 O 2 FeSe 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Neutral Silicon Vacancy Centers in Undoped Diamond via Surface Control

Neutral silicon vacancy centers (SiV 0 ) in diamond are promising candidates for quantum applications; however, stabilizing SiV 0 requires high-purity, boron-doped diamond, which is not a readily available material. Here, we demonstrate an alternative approach via chemical control of the diamond surface. We use low-damage chemical processing and annealing in a hydrogen environment to realize reversible and highly stable charge state tuning in undoped diamond. The resulting SiV 0 centers display optically detected magnetic resonance and bulklike optical properties. Controlling the charge state tuning via surface termination offers a route for scalable technologies based on SiV 0 centers, as well as charge state engineering of other defects.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Conduction via surface states in antiferromagnetic Mott-insulating Ni S 2 single crystals

Pyrite structure transition-metal disulfides exhibit diverse ground states vs d-band filling, spanning diamagnetic semiconducting, ferromagnetic metallic, antiferromagnetic Mott insulating, and superconducting in FeS 2 , CoS 2 , NiS 2 , and CuS 2 . NiS is particularly interesting and poorly understood as its Mott insulating behavior is accompanied by complex antiferromagnetic ordering below ~38 K and perplexing weak ferromagnetism below ~30 K. Temperature-, pressure-, and composition-dependent insulator-metal transitions also occur, particularly in bandwidth-controlled NiS 2–x Se x , hole-doped Ni 1–x Co x S 2 , etc. Here, we use high-quality chemical-vapor-transport-grown NiS 2 single crystals characterized by x-ray diffraction, energy-dispersive x-ray spectroscopy, magnetometry, and extensive transport and magnetotransport measurements, to generate new insight into this system. In particular, resistivity, magnetoresistance, and Hall effect analyses vs temperature, thickness, and surface preparation, provide unequivocal evidence of surface conduction, where the more conductive surface shunts essentially all current at low temperatures. The surface transport changes from two dimensional and insulating to three dimensional and metallic as the surface preparation is varied (also displaying intriguing sensitivity to magnetic ordering), significantly clarifying literature ambiguities with respect to the electronic ground state. These results have immediate implications. First, the temperature-, pressure-, and composition-dependent insulator-metal transitions deduced in the extensive prior work on NiS 2-x Se x , Ni 1–x Co x S 2 , etc., must clearly be reexamined in light of rife metallic surface conduction, not previously taken into account. Second, NiS 2 now joins FeS 2 and CoS 2 as systems in which bulk and surface electronic behaviors are strikingly different, suggesting that metallic surface states could be a universal feature of pyrite structure transition-metal disulfides.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Sorption-enhanced steam reforming of toluene using multifunctional perovskite phase transition sorbents in a chemical looping scheme

Abstract Sorption-enhanced steam reforming (SESR) of toluene (SESRT) using catalytic CO 2 sorbents is a promising route to convert the aromatic tar byproducts formed in lignocellulosic biomass gasification into hydrogen (H 2 ) or H 2 -rich syngas. Commonly used sorbents such as CaO are effective in capturing CO 2 initially but are prone to lose their sorption capacity over repeated cycles due to sintering at high temperatures. Herein, we present a demonstration of SESRT using A- and B-site doped Sr 1− x A’ x Fe 1− y B’ y O 3− δ (A’ = Ba, Ca; B’ = Co) perovskites in a chemical looping scheme. We found that surface impregnation of 5–10 mol% Ni on the perovskite was effective in improving toluene conversion. However, upon cycling, the impregnated Ni tends to migrate into the bulk and lose activity. This prompted the adoption of a dual bed configuration using a pre-bed of NiO/ γ –Al 2 O 3 catalyst upstream of the sorbent. A comparison is made between isothermal operation and a more traditional temperature-swing mode, where for the latter, an average sorption capacity of ∼38% was witnessed over five SESR cycles with H 2 -rich product syngas evidenced by a ratio of H 2 : CO x > 4.0. XRD analysis of fresh and cycled samples of Sr 0.25 Ba 0.75 Fe 0.375 Co 0.625 O 3- δ reveal that this material is an effective phase transition sorbent—capable of cyclically capturing and releasing CO 2 without irreversible phase changes occurring.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Effects of heteroatom doping on hydrogen uptake in tungsten oxide

Redox-active transition metal oxides (TMOs) that can undergo proton-insertion coupled electron transfer (PICET) are promising candidates for catalyzing molecular conversion reactions which require the transfer of hydrogen atoms (or the thermochemical equivalent, H + , e − ). Herein, we studied the effects of isovalent (Mo 6+ ) and aliovalent (V 5+ and Nb 5+ ) heteroatom doping on the electrochemical PICET behavior of monoclinic tungsten oxide (WO 3 ). Cyclic voltammetry in aqueous acidic electrolytes shows that the addition of redox-active heteroatoms (Mo 6+ and V 5+ ) leads to systematic shifts in redox couple half-wave potentials (E 1/2 ), broadening, and an overall decrease in the current response. Conversely, the non-redox active heteroatom (Nb 5+ ) only reduces the current response with no observable peak-current broadening. This broadening is attributed to changes in the proton binding affinities of oxygen in different chemical environments, i.e., bridging different pairs of redox-active transition metal cations. We determined the hydrogen bond dissociation free energy (H BDFE) values to elucidate the thermodynamic effect of heteroatom substitution. Density functional theory calculations reveal a differentiation in the hydrogen binding and oxygen vacancy formation energies between heteroatom doped structures. The PICET-induced structural phase transitions of the pristine and doped samples were further probed with operando electrochemical X-ray diffraction (EC-XRD) and with ex situ chemical reduction. The broadening of the potential-dependent current response with increased heteroatom doping manifests in the operando EC-XRD results as prolonged structural regions where multiple hydrogen bronze phases exist and the appearance of cubic bronze phases at lower degrees of reduction compared to pristine WO 3 .

Holzapfel, Noah P. [North Carolina State Universit↗
DOE OSTI2023

Magnetic properties of intercalated quasi-2D Fe 3-x GeTe 2 van der Waals magnet

Among several well-known transition metal-based compounds, cleavable van der Waals (vdW) Fe 3-x GeTe 2 (FGT) magnet is a strong candidate for use in two-dimensional (2D) magnetic devices due to its strong perpendicular magnetic anisotropy, sizeable Curie temperature (T C ~154 K), and versatile magnetic character that is retained in the low-dimensional limit. While the T C remains far too low for practical applications, there has been a successful push toward improving it via external driving forces such as pressure, irradiation, and doping. Here we present experimental evidence of a room temperature (RT) ferromagnetic phase induced by the electrochemical intercalation of common tetrabutylammonium cations (TBA+) into quasi-2D FGT. We obtained Curie temperatures as high as 350 K with chemical and physical stability of the intercalated compound. The temperature-dependent Raman measurements, in combination with vdW-corrected ab initio calculations, suggest that charge transfer (electron doping) upon intercalation could lead to the observation of RT ferromagnetism. This work demonstrates that molecular intercalation is a viable route in realizing high-temperature vdW magnets in an inexpensive and reliable manner and has the potential to be extended to bilayer and few-layer vdW magnets.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗