Ab Initio Density Functional Theory Research Articles

Spin-orbit coupling and electronic properties in Pt2MnGa: an ab-initio study

The electronic and magnetic properties of full-Heusler alloy Pt2MnGa with and without the effect of spin–orbit coupling are studied. The calculations have been carried out using ab initio density functional theory. Both the magnetic spin orders of Pt2MnGa, ferromagnetic and antiferromagnetic, are considered. It is found that the ferromagnetic spin arrangement is the most stable spin order at the ground state, regardless of the incorporation of spin–orbit coupling. The density of states and band structure plots are used to validate the obtained ground state structure, which is further validated by the Bader charge analysis and the charge density distribution of the individual atoms. The obtained results of magnetocrystalline anisotropy energy, total magnetic moment, Curie temperature, and the spin-polarization hint at the possible application of this compound in spintronics devices such as bit-patterned media.

Direct Probing of Lattice-Strain-Induced Oxygen Release in LiCoO2 and Li2 MnO3 without Electrochemical Cycling.

Since the recognition of a significant oxygen-redox contribution to enhancing the capacity of Li transition-metal oxide cathodes, the oxygen release and subsequent structural variations together with capacity fading have been critical issues to achieve better electrochemical performance. As most previous reports dealt with the structural degradation of cathodes after electrochemical cycling, it has been fairly difficult to clarify how substantial the effect of lattice strain on the oxygen release would be while exclusively ruling out any electrochemical influences. By utilizing nanoindentation and mechanical surface polishing of single-crystal LiCoO2 and Li2 MnO3 , we scrutinize the local variations of both the atomic structure and oxygen content. Atomic-column-resolved imaging reveals that local Li-M (M = Co and Mn) disordering and further amorphization are induced by mechanical strain. Moreover, substantial oxygen deficiency in the regions with these structure changes is directly identified by spectroscopic analyses. Ab initio density functional theory calculations also demonstrate energetically favorable formation of oxygen vacancies under shear strain. Providing direct evidence of oxygen release as a consequence of lattice strain, the findings in this work suggest that efficient strain relaxation will be of great significance for longevity of the anion framework in layered oxide cathodes. This article is protected by copyright. All rights reserved.

Electrons Surf Phason Waves in Moiré Bilayers.

We investigate the effect of thermal fluctuations on the atomic and electronic structure of a twisted MoSe2/WSe2 heterobilayer using a combination of classical molecular dynamics and ab initio density functional theory calculations. Our calculations reveal that thermally excited phason modes give rise to an almost rigid motion of the moiré lattice. Electrons and holes in low-energy states are localized in specific stacking regions of the moiré unit cell and follow the thermal motion of these regions. In other words, charge carriers surf phason waves that are excited at finite temperatures. We also show that such surfing survives in the presence of a substrate and frozen potential. This effect has potential implications for the design of charge and exciton transport devices based on moiré materials.

Investigating the Increased CO2 Capture Performance of Amino Acid Functionalized Nanoporous Materials from First-Principles and Grand Canonical Monte Carlo Simulations

Nanoporous materials such as metal-organic frameworks (MOFs) and covalent-organic frameworks (COFs) have been identified as key candidates for environmental remediation through catalytic reduction and sequestration of pollutants. Given the prevalence of CO2 as a target molecule for capture, MOFs and COFs have seen a long history of application in the field. More recently, functionalized nanoporous materials have been demonstrated to improve performance metrics associated with the capture of CO2. We employ a multiscale computational approach including ab initio density functional theory (DFT) calculations and classical grand canonical Monte Carlo (GCMC) simulations, to investigate the impact of amino acid (AA) functionalization in three such nanoporous materials. Our results demonstrate a nearly universal improvement of CO2 uptake metrics such as adsorption capacity, accessible surface area, and CO2/N2 selectivity for six AAs. In this work, we elucidate the key geometric and electronic properties associated with improving the CO2 capture performance of functionalized nanoporous materials.

Engineering 2D MoS2 for Enhanced Selectivity and Sensitivity of Selected Green House Gases (CO2, CH4 and N2O): An ab initio Study

2D MoS2 has been identified as a potential material for greenhouse gas (CO2, N2O, and CH4) sensing, however, the underlying principles are not well understood yet such knowledge may offer optimization opportunities for the development of superior devices. Using ab initio Density Functional Theory approach, selected dopants X (X= Cl, O, P, and Se) were judiciously introduced on 2D MoS2 and the response of the modified monolayer to the various greenhouse gases analyzed. The results showed that when the gas molecules are introduced within the periphery of the dopant site, the gases become adsorbed on the dopant with interactions that are characteristic of physisorption due to moderate adsorption energies. Based on the magnitude of adsorption energies, Cl, P, and O doped 2D MoS2 were found to be sensitive and selective to CO2, N2O and CH4 gas molecules respectively. Further, charge transfer analysis of CO2, and N2O adsorbed on Cl and P doped 2D MoS2 monolayer respectively, showed that these gas molecules gain electrons from the doped 2D MoS2 monolayer during adsorption, while CH4 molecule loses electrons to O doped 2D MoS2 surface. In addition, CO2, N2O, and CH4 gas molecules are desorbed from the surfaces of Cl, P, and O doped 2D MoS2 at 432 K, 438 K and 298 K respectively, thus rendering the modified monolayer re-usable detection of greenhouse gases. Cl doped 2D MoS2 monolayer showed superior performance in CO2 detection due to its fast recovery time and moderate thermal treatment temperature.Our results reveal that the competitive adsorption at the X doped 2D MoS2 surfaces between the analyte and the greenhouse gas present in the atmosphere induces a switching in surface conductance that can be related to the greenhouse gases concentration and can be detected electronically, thus disclosing the sensing mechanism and optimization route that can guide future experimental studies.

Formation mechanism of mirror twin grain boundaries in molecular beam epitaxy grown monolayer WSe2–MoSe2 lateral heterojunctions

Mirror twin grain boundary (MTB) defects, being a special type of high-symmetry one-dimensional (1D) defects in two-dimensional atomically thin transition metal dichalcogenides (TMDCs), have received considerable interest due to their unique structures and intriguing 1D properties. However, formation and distribution of MTBs in hybrid TMDC materials such as heterojunction remain scarcely studied. Herein, we investigate the spatial distribution, lattice registry and formation mechanism of MTBs in molecular beam epitaxy grown monolayer WSe2–MoSe2 lateral heterojunctions using atomic-resolution annular dark-field scanning transmission electron microscopy (ADF-STEM). MTBs manifest a much higher density in MoSe2 than in WSe2 domains with a few of them spanning coherently across the domain interface. Compositionally, a Mo-dominant rather than W-dominant configuration was observed in those MTBs located in WSe2 domains and its origin can be attributed to the preferable Mo substitution to W along the MTBs occurring at the later MoSe2 growth period. This proposed mechanism is supported by ab-initio density functional theory calculations and substitution dynamics captured by in-situ ADF-STEM. The present study deepens our understanding of MTBs in heterostructured TMDCs, which may also serve as an excellent platform for the exploration of intriguing 1D physics.

A comparative investigation for identification of N-(4-dimethylamino 3,5-dinitrophenyl)maleimide

This study has identified the characteristic behaviors of N-(4-dimethylamino 3,5-dinitrophenyl)maleimide molecule using ab initio Hartree-Fock (HF) and density functional theory (DFT) based on Becke’s three-parameter hybrid exchange functional combined with Lee-Yang-Parr non-local correlation function (HF/B3LYP and DFT/B3LYP) at 6-311G++(d,p) level of theory for the first time. On this basis, the optimized molecular structures, some thermodynamic features at 300 K, function groups of structures, charge distributions-dipole moments, molecular charge transfer regions, spectroscopic characteristic properties, vibrational frequencies, nuclear magnetic resonance chemical shifts of 13C-NMR and 1H-NMR spectra, and corresponding vibrational assignments have been investigated in detail. Comparisons between some experimental findings and theoretical results are performed to test the reliability of the calculation method preferred in the study. The comparison results in high correlation parameters such as R2 =0.976 and R2 =0.985 for the molecular structures and vibrational frequencies in the DFT and HF calculation levels, respectively. Moreover, the obtained vibrational frequencies and calculated results are in good agreement with the experimental data. Additionally, the simulations of highest/lowest occupied/unoccupied molecular orbital (HOMO and LUMO), molecular electrostatic potential (MEP), and electrostatic potential (ESP) maps have shown that there appear strong non-uniform intra-molecular charge distributions (ICT), electron engagements, lone pairs of electrons, π-π* conjugative effects based on the bond weakening, and intermolecular hydrogen bonding in the compound. Correspondingly, the molecule with the electrophilic reactive and nucleophilic regions has been noted to exhibit kinetical chemical stability. All the discussions have been confirmed by means of the findings of optimized molecular structures and vibrational frequencies belonging to the molecule.

First principle calculations: The electronic, optical, mechanical, and vibrational properties of TiS3

The computational predictions of transition-metal tri-chalcogenide (TMTCs) were performed using ab initio density functional theory (DFT) to investigate the electronic band structure, the partial density of states (PDOS), optical absorptions, dielectric functions, complex conductivity, reflectivity, refractive index, electron loss, the Poisson’s ratio, Young’s modulus, bulk-to-shear ratio, and phonon dispersion. The bandgap is measured from the valence band maximum (VBM) to the conduction band minimum (CBM) with the G–Z transitions. This suggests that the material is an indirect bandgap semiconductor. The electronic bandgap ([Formula: see text] is significantly improved with nonlocal hybrid functionals, especially in HSE0s, with [Formula: see text] of 1.0[Formula: see text]eV, which is in excellent agreement with the experimental data. However, our data shows that the HF-LDA exchange correlations significantly overestimate the [Formula: see text] with 7.33[Formula: see text]eV. Also, our optical absorption data indicates a high absorption coefficient of about [Formula: see text][Formula: see text]cm[Formula: see text]. The absorption peak of 7.4[Formula: see text]eV indicates TiS3 can be applied in vacuum ultra-violet (VUV) applications. The reflectivity is also shown to be high, with over 90% of light being reflected. The mechanical stability of the monoclinic system can be testified by our elastic coefficients and the phonon dispersions.

Unraveling the atomic and electronic structure of nanocrystals on superconducting Nb(110): Impact of the oxygen monolayer

The niobium surface is almost always covered by a native oxide layer which greatly influences the performance of superconducting devices. Here we investigate the highly stable niobium oxide overlayer of Nb(110), which is characterized by its distinctive nanocrystal structure as observed by scanning tunneling microscopy (STM). Our ab initio density functional theory (DFT) calculations show that a subtle reconstruction in the surface niobium atoms gives rise to rows of fourfold coordinated oxygen separated by regions of threefold coordinated oxygen. The fourfold oxygen rows are determined to be the source of the nanocrystal pattern observed in STM and the two chemical states of oxygen observed in core-level x-ray photoelectron spectroscopy (XPS) are ascribed to the threefold and fourfold oxygens. Furthermore, we find excellent agreement between the DFT calculated electronic structure with scanning tunneling spectroscopy and valence XPS measurements.

Competing Magnetic Interactions and the Role of Unpaired 4f Electrons in Oxygen-Deficient Perovskites Ba3RFe2O7.5 (R = Y, Dy)

Oxygen-deficient perovskite compounds with the general formula Ba3RFe2O7.5 present a good opportunity to study competing magnetic interactions between Fe3+ 3d cations with and without the involvement of unpaired 4f electrons on R3+ cations. From analysis of neutron powder diffraction data, complemented by ab initio density functional theory calculations, we determined the magnetic ground states when R3+ = Y3+ (non-magnetic) and Dy3+ (4f9). They both adopt complex long-range ordered antiferromagnetic structures below TN = 6.6 and 14.5 K, respectively, with the same magnetic space group Ca2/c (BNS #15.91). However, the dominant influence of f-electron magnetism is clear in temperature dependence and differences between the size of the ordered moments on the two crystallographically independent Fe sites, one of which is enhanced by R-O-Fe superexchange in the Dy compound, while the other is frustrated by it. The Dy compound also shows evidence for temperature- and field-dependent transitions with hysteresis, indicating a field-induced ferromagnetic component below TN.

Effects of Alloying Elements on the Solution and Diffusion of Oxygen at Iron Grain Boundary Investigated by First-Principles Study

The effects of alloying elements (Si, Cr, Mo) on the solution and diffusion of oxygen (O) atoms at the grain boundary of iron (Fe) Σ5(310)/[001] are investigated by the simulations of ab initio density functional theory (DFT). It is found that Si, Mo and Cr prefer to segregate to the grain boundary, and further affect the solution and diffusion of O atoms at Fe grain boundaries. The segregated Cr promotes the solution of O, while Si and Mo inhibit the solution of O at the grain boundary. Meanwhile, Cr and Si accelerate the diffusion of O, and Mo retards the diffusion of O in the grain boundary. Further analysis indicates that the effects are closely related to the interactions between the alloying elements and O atoms, which are determined by the competition between the distortion of local structure and the charge transfer between local atoms. Finally, the effects of alloying elements on the O concentration distribution near the grain boundary are explored by employing the Langmuir–McLean models. This work not only provides insights into the effects of alloying elements on the solution and diffusion of O at grain boundaries, but also provides parameters of the atomic interactions for the initial oxidation simulation on a large scale, which relates to the growth of oxide in polycrystalline systems with various grain sizes at experimental temperatures.

Investigation of the electronic, optical, elastic, mechanical and vibrational properties of CuI using HSE03

Ab Initio density functional theory (DFT) simulations have been employed to systematically explore the electronic, optical, elastic, mechanical and vibrational properties. In this study, we revealed that [Formula: see text]-CuI has a wide direct bandgap energy of 3.21 eV, is pure covalent and brittle. We also found that the core level is made up of I s electron orbitals, the valence band is constructed with I p orbitals, and the Cu s orbital states mainly contribute to the conduction band minimum (CBM). The reflectivity of CuI is reported to be low (35.9% for the light reflected), showing high material absorption. A high absorption coefficient of [Formula: see text] is also reported. The elastic and mechanical properties can further confirm the mechanical stability of the CuI system, derived from DFT-calculated elastic constants and phonon dispersion from density functional perturbation theory (DFPT) calculations.

Comprehensive ab initio study of effects of alloying elements on generalized stacking fault energies of Ni and Ni3Al

Excellent high-temperature mechanical properties of Ni-based single-crystal superalloys (NSCSs) are attributed to the yield strength anomaly of ${\mathrm{Ni}}_{3}\mathrm{Al}$ that is intimately related to generalized stacking fault energies (GSFEs). Therefore, clarifying the effects of alloying elements on the GSFEs is of great significance for alloys design. Here, by means of ab initio density functional theory calculations, we systematically calculated the GSFEs of different slip systems of Ni and ${\mathrm{Ni}}_{3}\mathrm{Al}$ without and with alloying elements using the alias shear method. We obtained that for Ni, except for magnetic elements Mn, Fe, and Co, most of the alloying elements decrease the unstable stacking fault energy (${\ensuremath{\gamma}}_{\text{USF}}$) of the $[01\overline{1}](111)$ and $[11\overline{2}](111)$ slip systems and also decrease the stable stacking fault energy (${\ensuremath{\gamma}}_{\text{SF}}$) of the $[11\overline{2}](111)$ slip system. Interestingly, the reduction effects exhibit a strong correlation with the inverse of atom radii. For ${\mathrm{Ni}}_{3}\mathrm{Al}$, most of the alloying elements in groups IIIB--VIIB show a strong Al site preference. Except for Mn and Fe, the elements in groups VB--VIIB and the first column of group VIII increase the values of ${\ensuremath{\gamma}}_{\text{USF}}$ of different slip systems of ${\mathrm{Ni}}_{3}\mathrm{Al}$, which makes the slip deformation and dislocation emits difficult. On the other hand, the elements in groups IIIB--VIIB also increase the value of ${\ensuremath{\gamma}}_{\text{SF}}$, and thus reduce the stability of the antiphase boundary, complex stacking fault, and superlattice intrinsic stacking fault of ${\mathrm{Ni}}_{3}\mathrm{Al}$. We found that Re is an excellent strengthening alloying element that significantly increases the slip barrier of the tailing slip process for Ni, and also enhances the slip barrier of the leading slip process of three slip systems for ${\mathrm{Ni}}_{3}\mathrm{Al}$. W and Mo exhibit similar effects as Re. We predicted that Os, Ru, and Ir are good strengthening alloying elements as well, since they show the strengthening effects on both the leading and the tailing slip process for Ni and ${\mathrm{Ni}}_{3}\mathrm{Al}$. This work established an exhaustive dictionary of the effects of various alloying elements on the GSFEs of both Ni and ${\mathrm{Ni}}_{3}\mathrm{Al}$ phases, which would help to guide the design of next-generation high-performance NSCSs.

Bulk Modulus, Elastic Constants, and Force Constants of Interatomic Bonds of II–III2–VI4 Compounds

Ab initio density functional perturbation theory is used to calculate the elastic constants of CdGa2S4, CdGa2Se4, CdGa2Te4, and ZnGa2Se4 thiogallates. The values of the bulk modulus, shear modulus, Young's modulus, and Poisson's ratio are determined. The force constants of interatomic bonds in CdGa2Te4 and ZnGa2Se4 compounds are calculated. Regularities in the dependence of the frequencies of Raman‐active phonons on the atomic masses are established.

Control of magnetic states and spin interactions in bilayer CrCl3 with strain and electric fields: an ab initio study

Using ab initio density functional theory, we demonstrated the possibility of controlling the magnetic ground-state properties of bilayer CrCl_{3} by means of mechanical strains and electric fields. In principle, we investigated the influence of these two fields on parameters describing the spin Hamiltonian of the system. The obtained results show that biaxial strains change the magnetic ground state between ferromagnetic and antiferromagnetic phases. The mechanical strain also affects the direction and amplitude of the magnetic anisotropy energy (MAE). Importantly, the direction and amplitude of the Dzyaloshinskii–Moriya vectors are also highly tunable under external strain and electric fields. The competition between nearest-neighbor exchange interactions, MAE, and Dzyaloshinskii–Moriya interactions can lead to the stabilization of various exotic spin textures and novel magnetic excitations. The high tunability of magnetic properties by external fields makes bilayer CrCl_{3} a promising candidate for application in the emerging field of two-dimensional quantum spintronics and magnonics.

Ab Initio Computational Screening and Performance Assessment of van der Waals and Semimetallic Contacts to Monolayer WSe2P-Type Field-Effect Transistors

Recent technology development of logic devices based on 2-D semiconductors such as MoS2, WS2, and WSe2 has triggered great excitement, paving the way to practical applications. Making low-resistance p-type contacts to 2-D semiconductors remains a critical challenge. The key to addressing this challenge is to find high-work function metallic materials which also introduce minimal metal-induced gap states (MIGSs) at the metal/semiconductor interface. In this work, we perform a systematic computational screening of novel metallic materials and their heterojunctions with monolayer WSe2 based on ab initio density functional theory and quantum device simulations. Two contact strategies, van der Waals (vdW) metallic contact and bulk semimetallic contact, are identified as promising solutions to achieving Schottky-barrier-free and low-contact-resistance p-type contacts for WSe2 p-type field-effect transistor (pFETs). Good candidates of p-type contact materials are found based on our screening criteria, including 1H-NbS2, 1H-TaS2, and 1T-TiS2 in the vdW metal category, as well as Co3Sn2S2 and TaP in the bulk semimetal category. Simulations of these new p-type contact materials suggest reduced MIGS, less Fermi-level pinning effect, negligible Schottky barrier height and small contact resistance (down to <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$20~\Omega \mu \text{m}$ </tex-math></inline-formula> ).

Effects of Anions and Protein Structures on Protein‐Based Solid Electrolytes

AbstractLow ionic conductivity is one of the main hurdles for the practical application of advanced all‐solid‐state lithium‐ion batteries. Protein‐based solid electrolytes are recently proposed and can potentially provide both high ionic conductivity and high mechanical properties due to the decoupled ion transport mechanism. In this work, the effects of lithium salts and protein structures on the performance of protein‐based electrolytes through both ab initio density functional theory calculations and experiments are systematically investigated. The results show that the anions can be strongly locked by the charged amino acids, thus providing intermediate hopping sites for lithium‐ion, reducing energy barrier for lithium‐ion transport, and then enhancing the ionic conductivity. These calculations also demonstrate that need to be locked at appropriate positions by properly controlling the protein structures in order to provide bridging effects and facilitate lithium‐ion transport. The findings are consistent with the experimental observations and can provide guidance for design and optimization of protein‐based solid electrolytes.

Influence of Capping Ligands, Solvent, and Thermal Effects on CdSe Quantum Dot Optical Properties by DFT Calculations.

Cadmium selenide nanomaterials are very important materials in photonics, catalysis, and biomedical applications due to their optical properties that can be tuned through size, shape, and surface passivation. In this report, static and ab initio molecular dynamics density functional theory (DFT) simulations are used to characterize the effect of ligand adsorption on the electronic properties of the (110) surface of zinc blende and wurtzite CdSe and a (CdSe)33 nanoparticle. Adsorption energies depend on ligand surface coverage and result from a balance between chemical affinity and ligand-surface and ligand-ligand dispersive interactions. In addition, while little structural reorganization occurs upon slab formation, Cd···Cd distances become shorter and the Se-Cd-Se angles become smaller in the bare nanoparticle model. This originates mid-gap states that strongly influence the absorption optical spectra of nonpassivated (CdSe)33. Ligand passivation on both zinc blende and wurtzite surfaces does not induce a surface reorganization, and thus, the band gap remains nonaffected with respect to bare surfaces. In contrast, structural reconstruction is more apparent for the nanoparticle, which significantly increases its highest occupied molecular orbital (HOMO)-lowest unoccupied molecular orbital (LUMO) gap upon passivation. Solvent effects decrease the band gap difference between the passivated and nonpassivated nanoparticles, the maximum of the absorption spectra being blue-shifted around 20 nm by the effect of the ligands. Overall, calculations show that flexible surface cadmium sites are responsible for the appearance of mid-gap states that are partially localized on the most reconstructed regions of the nanoparticle that can be controlled through appropriate ligand adsorption.

Isotopic Constraints on the Nature of Primary Precipitates in Archean–Early Paleoproterozoic Iron Formations from Determinations of the Iron Phonon Density of States of Greenalite and 2L- and 6L-Ferrihydrite

Iron formations (IFs) are chemical sedimentary rocks that were widely deposited before the Great Oxidation Event (GOE) around 2.4–2.2 Ga. It is generally thought that IFs precipitated as hydrated Fe3+ oxides (HFOs) such as ferrihydrite following surface oxidation of Fe2+-rich, anoxic deep waters. This model often implicates biological oxidation and underpins reconstructions of marine nutrient concentrations. However, nanoscale petrography indicates that an Fe2+ silicate, greenalite, is a common primary mineral in well-preserved IFs, motivating an alternative depositional model of anoxic ferrous silicate precipitation. It is unclear, however, if Fe2+-rich silicates can produce the Fe isotopic variations in IFs that are well explained by Fe2+ oxidation. To address this question, we constrain the equilibrium Fe isotopic (56Fe/54Fe) fractionation of greenalite and ferrihydrite by determining the iron phonon densities of states for those minerals. We use ab initio density functional theory (DFT + U) calculations and nuclear resonant inelastic X-ray scattering spectroscopy to show that ferrous greenalite should be isotopically lighter than ferrihydrite by ∼1–1.2‰ at equilibrium, and fractionation should scale linearly with increasing Fe3+ content in greenalite. By anchoring ferrihydrite–greenalite mineral pair fractionations to published experimental Fe isotopic fractionations between HFOs and aqueous Fe2+, we show that ferrous greenalite may produce all but the heaviest pre-GOE Fe isotopic compositions and mixed valence greenalites can produce the entire record. Our results suggest that heavy Fe isotope enrichments alone are not diagnostic of primary IF mineralogies, and ferrihydrite and partially oxidized or even purely ferrous greenalite are all viable primary IF mineralogies.

Quantifying symmetric exchange in ultrathin ferromagnetic films with chirality

The symmetric (Heisenberg) exchange interaction is fundamental to magnetism and assumes critical importance in designing magnetic materials for novel emergent phenomena and device applications. However, quantifying exchange is extremely challenging for ultrathin magnetic films, as techniques and approximations reliably used for bulk materials are largely inapplicable in the two-dimensional limit. Here we present and contrast the measurement of exchange stiffness $A$ by several methods on a series of five Co/Pt-based ultrathin ($1--2$ nm) films. We compare results from (a) spin-wave spectroscopy by Brillouin light scattering, (b) three analytical models describing the temperature dependence of magnetization obtained by magnetometry, (c) microscopic domain periodicity measurements and simulations, and (d) ab initio density functional theory calculations. While different methods present some qualitatively consistent trends across samples, we note, for any given sample, considerable differences (up to $5\ifmmode\times\else\texttimes\fi{})$ in the absolute values of $A$ across the techniques, consistent with discrepancies of $A$ reported in literature for nominally similar samples. We analyze possible sources of the discrepancies across various methods, notably including their relationship to the spin-wave dispersion, and the wave-vector ranges probed. We compare the strengths and limitations of the techniques, and outline directions for their future use in characterizing exchange interactions in ultrathin films.