High-resolution Electron Energy Loss Spectroscopy Research Articles

Embedded Hybrid-Dimensional Heterointerface for Filament Modulation in 2D Material-Based Artificial Nociceptor.

Nociceptors are key sensory receptors that transmit warning signals to the central nervous system in response to painful stimuli. This fundamental process is emulated in an electronic device by developing a novel artificial nociceptor with an ultrathin, nonstoichiometric gallium oxide (GaOx)-silicon oxide heterostructure. A large-area 2D-GaOx film is printed on a substrate through liquid metal printing to facilitate the production of conductive filaments. This nociceptive structure exhibits a unique short-term temporal response following stimulation, enabling a facile demonstration of threshold-switching physics. The developed heterointerface 2D-GaOx film enables the fabrication of fast-switching, low-energy, and compliance-free 2D-GaOx nociceptors, as confirmed through experiments. The accumulation and extrusion of Ag in the oxide matrix are significant for inducing plastic changes in artificial biological sensors. High-resolution transmission electron microscopy and electron energy loss spectroscopy demonstrate that Ag clusters in the material dispersed under electrical bias and regrouped spontaneously when the bias is removed owing to interfacial energy minimization. Moreover, 2D nociceptors are stable; thus, heterointerface engineering can enable effective control of charge transfer in 2D heterostructural devices. Furthermore, the diffusive 2D-GaOx device and its Ag dynamics enable the direct emulation of biological nociceptors, marking an advancement in the hardware implementation of artificial human sensory systems.

STEM Developments: A Versatile Light Injector/Collector, Fast 4D-STEM, and High Energy Resolution EELS without Compromising Beam Current

STEM Developments: A Versatile Light Injector/Collector, Fast 4D-STEM, and High Energy Resolution EELS without Compromising Beam Current

Tailoring Heterostructure Growth on Liquid Metal Nanodroplets through Interface Engineering.

Liquid metal (LM) nanodroplets possess intriguing surface properties, thus offering promising potential in chemical synthesis, catalysis, and biomedicine. However, the reaction kinetics and product growth at the surface of LM nanodroplets are significantly influenced by the interface involved, which has not been thoroughly explored and understood. Here, we propose an interface engineering strategy, taking a spontaneous galvanic reaction between Ga0 and AuCl4- ions as a representative example, to successfully modulate the growth of heterostructures on the surface of Ga-based LM nanodroplets by establishing a dielectric interface with a controllable thickness between LM and reactive surroundings. Combining high-resolution electron energy-loss spectroscopy (EELS) analysis and theoretical simulation, it was found that the induced charge distribution at the interface dominates the spatiotemporal distribution of the reaction sites. Employing tungsten oxide (WOx) with varying thicknesses as the demonstrated dielectric interface of LM, Ga@WOx@Au with distinct core-shell-satellite or dimer-like heterostructures has been achieved and exhibited different photoresponsive capabilities for photodetection. Understanding the kinetics of product growth and the regulatory strategy of the dielectric interface provides an experimental approach to controlling the structure and properties of products in LM nanodroplet-involved chemical processes.

Petrographic and chemical characterization and carbon and nitrogen isotopic compositions of cometary IDPs and their GEMS amorphous silicates

GEMS (glass with embedded metal and sulfides) are the dominant carrier of amorphous silicates in anhydrous interplanetary dust particles (IDPs) and one of the most suitable materials to study early solar system processes. Amorphous silicates in 105 GEMS from eight IDPs were analyzed regarding texture and chemical composition to reassess GEMS formation theories and genetic relationships to amorphous silicate material in meteorites. Petrography of bulk IDPs was investigated to understand GEMS’ relationships to other IDP components. Furthermore, carbon and nitrogen isotopic compositions were measured. Nearly all GEMS are aggregates of several subgrains with variable amount of nanophase inclusions and different Mg- and Si-contents, while single GEMS are rare. The subgrains within aggregates are typically surrounded by one or more carbon rims with high density. The chemical compositions of GEMS amorphous silicates are subsolar for all major element/Si ratios but exhibit wide heterogeneity. This is not influenced by silicon oil from the capturing process of IDPs as assumed before, as a penetration of the silicon oil is excluded by high resolution EELS (electron energy loss spectroscopy) areal density maps of silicon. Furthermore, low Fe-content in GEMS amorphous silicates shows that these are not altered by aqueous activity on the parent body as it is the case for amorphous silicate material in primitive meteorites. The subsolar element/Si ratios and the wide chemical heterogeneity point to a non-equilibrium fractional condensation origin either in the early solar nebula or in a circumstellar environment and are not in agreement with homogenization via sputtering in the ISM. The close association with carbon around GEMS subgrains and as double-rims around GEMS aggregates argue for a multi-step aggregation after formation of the smallest GEMS subgrains in the ISM or the early solar nebula. Carbon acting as matrix material connecting GEMS and other IDP components has lower areal density as seen from carbon EELS areal density maps and isotopic anomalies varying at the nanometer scale, pointing to different origins and processing of materials to varying extent or at changing temperatures.To balance GEMS’ subsolar element/Si ratios, a supersolar component in IDPs was assumed to account for the overall chondritic composition of bulk IDPs. Nevertheless, our bulk IDP analyses revealed subsolar, but variable, element/Si ratios for complete particles as well, depending on type and amount of mineral phases in each particle. Pyroxenes in the investigated particles can occur as elongated euhedral crystals, but are overall rare. The dominant crystalline fraction in the investigated IDP samples are equilibrated aggregates (EAs) that show the same chemical compositions as GEMS, indicating that the EAs are recrystallized GEMS grains and formed after GEMS formation as secondary phases.

N‐Heterocyclic Olefins on a Metallic Surface – Adsorption, Orientation, and Electronic Influence

AbstractN‐Heterocyclic olefins (NHOs), possessing highly polarizable and remarkably electron‐rich double bonds, have been effectively utilized as exceptional anchors for surface modifications. Herein, the adsorption, orientation, and electronic properties of NHOs on a metal surface are investigated. On Cu(111), the sterically low‐demanding IMe‐NHO is compared to its analogous IMe‐NHC counterpart. High‐resolution electron energy‐loss spectroscopy (HREELS) measurements show for both molecules a flat‐lying ring adsorption configuration. While the NHC adopts a dimer configuration including a Cu adatom, the NHO chemisorbs over a C–Cu bond perpendicular to the surface. This distinct difference leads for the IMe‐NHOs to have a higher thermal stability on the surface. Moreover, IMe‐NHOs introduce a higher net electron transfer to the surface compared to the IMe‐NHCs, which results in a stronger effect on the work function. These results highlight the role of NHOs in surface science as they extend the functionalization capabilities of NHCs into stronger electronic modification.

Fabrication of monolayer h-BN/LaB6 heterostructure thin film with low work function and high chemical stability

To expand the applications of low work function materials, high chemical stability is necessary to prevent the surface from unfavorable reactions. We developed a 20-nm-thick lanthanum hexaboride (LaB6) thin film covered by a monolayer hexagonal boron nitride (h-BN), which exhibits not only low work function but also high chemical stability. Results demonstrated that the h-BN/LaB6 heterostructure can be formed by vacuum annealing a nitrogen-doped LaB6 thin film. The formation process was investigated using Auger electron spectroscopy (AES), high-resolution electron energy loss spectroscopy (HREELS), and X-ray absorption near edge structure (XANES) spectroscopy. We have elucidated that the doped nitrogen atoms and boron atoms in the film thermally diffuse into the surface during annealing, thereby forming the monolayer h-BN on the surface. Work function was measured using scanning tunneling microscopy (STM). From a practical perspective, chemical stability was evaluated with a heating temperature necessary for restoring the low work function state after air exposure. The work function was comparable to that of the clean LaB6(100) surface. Moreover, it recovered at a much lower temperature than the cleaning temperature of the LaB6(100) surface. We anticipate that this material development will facilitate implementation of the low work function material.

Unveiling Enhanced PEC Water Oxidation: Morphology Tuning and Interfacial Phase Change in α-Fe2O3@K-OMS-2 Branched Core-Shell Nanoarrays.

A simple fabrication method that involves two steps of hydrothermal reaction has been demonstrated for the growth of α-Fe2O3@K-OMS-2 branched core-shell nanoarrays. Different reactant concentrations in the shell-forming step led to different morphologies in the resultant composites, denoted as 0.25 OC, 0.5 OC, and 1.0 OC. Both 0.25 OC and 0.5 OC formed perfect branched core-shell structures, with 0.5 OC possessing longer branches, which were observed by SEM and TEM. The core K-OMS-2 and shell α-Fe2O3 were confirmed by grazing incidence X-ray diffraction (GIXRD), EDS mapping, and atomic alignment from high-resolution STEM images. Further investigation with high-resolution HAADF-STEM, EELS, and XPS indicated the existence of an ultrathin layer of Mn3O4 sandwiched at the interface. All composite materials offered greatly enhanced photocurrent density at 1.23 VRHE, compared to the pristine Fe2O3 photoanode (0.33 mA/cm2), and sample 0.5 OC showed the highest photocurrent density of 2.81 mA/cm2. Photoelectrochemical (PEC) performance was evaluated for the samples by conducting linear sweep voltammetry (LSV), applied bias photo-to-current efficiency (ABPE), electrochemical impedance spectroscopy (EIS), incident-photo-to-current efficiency (IPCE), transient photocurrent responses, and stability tests. The charge separation and transfer efficiencies, together with the electrochemically active surface area, were also investigated. The significant enhancement in sample 0.5 OC is ascribed to the synergetic effect brought by the longer branches in the core-shell structure, the conductive K-OMS-2 core, and the formation of the Mn3O4 thin layer formed between the core and shell.

4H-SiC/SiO2 Interface Degradation in 1.2 kV 4H-SiC MOSFETs due to Power Cycling Tests

Power cycling tests (PCTs) assess the reliability of power devices by closely simulating their operating conditions. A PCT was performed on commercially available 1.2 kV 4H-SiC power metal–oxide–semiconductor field-effect transistors to observe its impact on the 4H-SiC/SiO2 interface. High-resolution transmission electron microscopy and electron energy loss spectroscopy measurements showed variations in the length of the 4H-SiC/SiO2 transition layer, depending on whether the device was power cycled. Moreover, the total resistance at Vg >> Vt in Rtot − (Vg-Vt)−1 graph increased to 16.5%, while it changed more radically to 47.3% at Vg ≈ Vt. The threshold voltage shifted negatively. These variations cannot be expected solely through the wearout of the package.

Oxygen Transport through Amorphous Cathode Coatings in Solid-State Batteries.

All solid-state batteries (SSBs) are considered the most promising path to enabling higher energy-density portable energy, while concurrently improving safety as compared to current liquid electrolyte solutions. However, the desire for high energy necessitates the choice of high-voltage cathodes, such as nickel-rich layered oxides, where degradation phenomena related to oxygen loss and structural densification at the cathode surface are known to significantly compromise the cycle and thermal stability. In this work, we show, for the first time, that even in an SSB, and when protected by an intact amorphous coating, the LiNi0.5Mn0.3Co0.2O2 (NMC532) surface transforms from a layered structure into a rocksalt-like structure after electrochemical cycling. The transformation of the surface structure of the Li3B11O18 (LBO)-coated NMC532 cathode in a thiophosphate-based solid-state cell is characterized by high-resolution complementary electron microscopy techniques and electron energy loss spectroscopy. Ab initio molecular dynamics corroborate facile transport of O2- in the LBO coating and in other typical coating materials. This work identifies that oxygen loss remains a formidable challenge and barrier to long-cycle life high-energy storage, even in SSBs with durable, amorphous cathode coatings, and directs attention to considering oxygen permeability as an important new design criteria for coating materials.

On the origin of epitaxial rhombohedral-B4C growth by CVD on 4H-SiC.

Rhombohedral boron carbide, often referred to as r-B4C, is a potential material for applications in optoelectronic and thermoelectric devices. From fundamental thin film growth and characterization, we investigate the film-substrate interface between the r-B4C films grown on 4H-SiC (0001̄) (C-face) and 4H-SiC (0001) (Si-face) during chemical vapor deposition (CVD) to find the origin for epitaxial growth solely observed on the C-face. We used high-resolution (scanning) transmission electron microscopy and electron energy loss spectroscopy to show that there is no surface roughness or additional carbon-based interlayer formation for either substrate. Based on Raman spectroscopy analysis, we also argue that carbon accumulation on the surface hinders the growth of continued epitaxial r-B4C in CVD.

Metal Core-Shell Nanoparticle Supercrystals: From Photoactivation of Hydrogen Evolution to Photocorrosion.

Gas nanobubbles are directly linked to many important chemical reactions. While they can be detrimental to operational devices, they also reflect the local activity at the nanoscale. Here, supercrystals made of highly monodisperse Ag@Pt core-shell nanoparticles are first grown onto a solid support and fully characterized by electron microscopies and X-ray scattering. Supercrystals are then used as a plasmonic photocatalytic platform for triggering the hydrogen evolution reaction. The catalytic activity is measured operando at the single supercrystal level by high-resolution optical microscopy, which allows gas nanobubble nucleation to be probed at the early stage with high temporal resolution and the amount of gas molecules trapped inside them to be quantified. Finally, a correlative microscopy approach and high-resolution electron energy loss spectroscopy help to decipher the mechanisms at the origin of the local degradation of the supercrystals during catalysis, namely nanoscale erosion and corrosion.

Chemical and topological disordering in M23C6 due to irradiation: An atomic-scale observation

To clarify the stability of M23C6 precipitate in steels under irradiation, the chemical and topological disordering behaviors in M23C6 subjected to ion irradiation at elevated temperatures were investigated with the combined application of high-resolution electron microscopy (HREM) and electron energy-loss spectroscopy (EELS). Results show that the duplex structured M23C6 which is the core-crystalline and shell-amorphous was observed in the specimen irradiated at 623 K, nevertheless, no amorphous phase was observed in the specimen irradiated at 673 K. HREM observation confirmed the occurrence of the chemical disordering in irradiated M23C6, and the disordering of W atoms in the M23C6 unit cell was clarified by the peak intensity profile of the atomic column from the HREM image. EELS analyses indicate that no obvious chemical shift was observed by the core-loss spectrum, however, the change in the electron mean free path (λ) due to irradiation was confirmed by the low-loss spectrum, which is related to the formation of both irradiation defects and amorphous phase. It is proposed that the decreased material density upon irradiation is ascribed to the formation of W-vacancy-dominated defect clusters. An obvious change in interatomic distance was not observed in the irradiated M23C6 based on the radical distribution function analysis by extended energy-loss fine structure spectrum. However, the peak intensity decreased by irradiation, confirming the occurrence of chemical and topological disordering, regardless of the carbide being crystalline or amorphous.

Direct Observation of Topological Phonons in Graphene.

Phonons, as the most fundamental emergent bosons in condensed matter systems, play an essential role in the thermal, mechanical, and electronic properties of crystalline materials. Recently, the concept of topology has been introduced to phonon systems, and the nontrivial topological states also exist in phonons due to the constraint by the crystal symmetry of the space group. Although the classification of various topological phonons has been enriched theoretically, experimental studies were limited to several three-dimensional (3D) single crystals with inelastic x-ray or neutron scatterings. The experimental evidence of topological phonons in two-dimensional (2D) materials is absent. Here, using high-resolution electron energy loss spectroscopy following our theoretical predictions, we directly map out the phonon spectra of the atomically thin graphene in the entire 2D Brillouin zone, and observe two nodal-ring phonons and four Dirac phonons. The closed loops of nodal-ring phonons and the conical structure of Dirac phonons in 2D momentum space are clearly revealed by our measurements, in nice agreement with our theoretical calculations. The ability of 3D mapping (2D momentum space and energy space) of phonon spectra opens up a new avenue to the systematic identification of the topological phononic states. Our work lays a solid foundation for potential applications of topological phonons in superconductivity, dynamic instability, and phonon diode.

Using electron energy-loss spectroscopy to measure nanoscale electronic and vibrational dynamics in a TEM.

Electron energy-loss spectroscopy (EELS) can measure similar information to x-ray, UV-Vis, and IR spectroscopies but with atomic resolution and increased scattering cross-sections. Recent advances in electron monochromators have expanded EELS capabilities from chemical identification to the realms of synchrotron-level core-loss measurements and to low-loss, 10-100meV excitations, such as phonons, excitons, and valence structures. EELS measurements are easily correlated with electron diffraction and atomic-scale real-space imaging in a transmission electron microscope (TEM) to provide detailed local pictures of quasiparticle and bonding states. This perspective provides an overview of existing high-resolution EELS (HR-EELS) capabilities while also motivating the powerful next step in the field-ultrafast EELS in a TEM. Ultrafast EELS aims to combine atomic-level, element-specific, and correlated temporal measurements to better understand spatially specific excited-state phenomena. Ultrafast EELS measurements also add to the abilities of steady-state HR-EELS by being able to image the electromagnetic field and use electrons to excite photon-forbidden and momentum-specific transitions. We discuss the technical challenges ultrafast HR-EELS currently faces, as well as how integration with in situ and cryo measurements could expand the technique to new systems of interest, especially molecular and biological samples.

Characterization of Cu-Cu direct bonding in ambient atmosphere enabled using (111)-oriented nanotwinned-copper

The copper-copper (Cu-Cu) direct bonding technology was proposed in recent years in order to realize precise preparation and reliable service under high current density for three-dimension (3D) packaging in the post-Moore-era. In this study, Cu-Cu direct bonding was achieved in the ambient atmosphere by utilizing highly (111) oriented copper with nanotwin structure (called (111) nt-Cu). The thermal compression with a pressure of 30 MPa was conducted on a couple of Cu films at 300 and 400 °C in air. The Cu-Cu joints after bonding were further investigated by scanning electron microscopy (SEM), electron back-scattered diffraction (EBSD) and transmission electron microscopy (TEM). Different from the polycrystalline copper, perfect bonding was achieved as confirmed by high-resolution transmission electron microscopy (HRTEM) and electron energy loss spectroscopy (EELS). The shear strength after air bonding was measured as 96.04 ± 5.67 MPa on average, which demonstrated relatively high performance in traditional Cu-Cu bonding. The excellent resistance to oxidation and fast Cu(111) surface diffusivity of (111) nt-Cu guaranteed the bonding process. Above all, the achievement of (111) nt-Cu high performance bonding in the ambient atmosphere should give an insight into developing new interconnected technology.

Mechanistic Understanding of Ring-Opening of Tetrahydrofurfuryl Alcohol over WOx-Modified Pt Model Surfaces and Powder Catalysts

The upgrading of heterocyclic biomass-derived oxygenates such as tetrahydrofurfuryl alcohol (THFA) via ring-opening is a promising pathway to produce value-added diol molecules using renewable carbon sources. This study combines model surface experiments, first-principles calculations, and powder catalyst characterization and activity evaluation to unravel the nature of the Pt and WOx active sites and the reaction mechanism of the THFA ring-opening reaction on a WOx/Pt inverse oxide catalyst. Temperature-programmed desorption (TPD) and high-resolution electron energy loss spectroscopy (HREELS) measurements on model surfaces demonstrated that THFA ring opened on Pt(111) but underwent further decomposition due to its strong bonding with the surface. However, WOx deposited on Pt(111) altered the interaction strength between the ring-opened intermediate and the surface to a proper extent to facilitate the facile desorption of the desired 1,5-pentanediol (1,5-PeD) product. Density functional theory (DFT) calculations showed that WOx/Pt(111) could promote ring opening of THFA via an oxocarbenium ion-like transition state, which was stabilized by hydrogen bonding with the hydroxyl groups of WOx. The hydrogenation of the ring-opened 5-hydroxyvaleraldehyde intermediate to 1,5-PeD was then feasible via Brønsted acid sites present on WOx. Steady-state activity studies on the corresponding powder catalysts showed that the 1,5-PeD selectivity increased from 20% on Pt/SiO2 to 65% on WOx/Pt/SiO2 with 1 wt % WOx loading, consistent with model surface experiments and DFT calculations. This study demonstrates the feasibility of using model surface experiments and first-principles calculations to guide practical catalyst design, and provides a design strategy that can be applied to the selective ring-opening of relevant heterocyclic biomass-derived oxygenates.

How positioning of a hard ceramic TiB2 layer in Al/CuO multilayers can regulate the overall energy release behavior

This study reports on a new ternary thermite comprising of Al-TiB2/CuO multilayers, designed to take the advantage of high ignitability of titanium (Ti), high volumetric density of boron (B), and low melting point of aluminum (Al). Results demonstrate synergetic effects leading to an energetic layer outperforming its single fuel counterparts, Al/CuO or TiB2/CuO, while being safe to handle. The additive TiB2 not only lowers the ignition energy by 100%, but also enhances the burn rate by more than a factor of two compared to the single fuel samples (Al/CuO and TiB2/CuO). The thermite reaction sequences and synergy of Ti, B and Al oxidation, examined by thermo-analytical analyses coupled with X-ray spectroscopy and high-resolution electron energy loss spectroscopy, demonstrate the strong affinity of TiB2 to oxygen that catalyzes CuO decomposition at temperatures as low as 380 °C; followed by a dual-step TiB2 oxidation: first to TiO, and then to TiO2 led by a reaction limiting step of oxidizer availability. Finally, Al undergoes oxidation via liquid boron oxide as well as gaseous oxygen. This study also underlines the crucial effect of the nanolayer morphology in the thin-film technology: when Al is sputter-deposited onto the TiB2 layer, Al ions penetrate into the grain boundaries penalizing TiB2 reactivity. The results demonstrate the advantages of using TiB2 fuel to improve the ignitability and the combustion performance of Al based thermite and offer some means to finely tune the energetic properties.

Nodal-line plasmons in ZrSiX ( X=S,Se,Te ) and their temperature dependence

Topological nodal-line semimetals gain extensive attention for their peculiar linear band crossings along closed lines in the Brillouin zone leading to various interesting properties. Here, we systematically study the nodal-line plasmons of prototypical nodal-line semimetals $\mathrm{ZrSi}X$ ($X=\mathrm{S},\mathrm{Se},\mathrm{Te}$) by high-resolution electron energy loss spectroscopy, and first-principles calculations. In energy range from near- to mid-infrared frequencies, plasmons induced by the intraband correlations ($\ensuremath{\sim}0.8$ eV) and the interband correlations ($\ensuremath{\sim}0.3$ eV) of surface states related to the nodal-line electrons are universally observed in all the $\mathrm{ZrSi}X$ family. The bulk plasmon ($\ensuremath{\sim}0.6$ eV) is observed in ZrSiS but is indiscernible in both ZrSiSe and ZrSiTe owing to their stronger screening effect from the surface states and large interlayer distance. Although the plasmons in ZrSiS seem to be temperature independent, the frequencies of the intraband plasmons in ZrSiSe and ZrSiTe show large redshifts ($\ensuremath{\sim}10%$) with temperature increasing from 30 K to room temperature, which can be ascribed to the prominent thermal occupation effect of nodal-line electrons when the Fermi level is close to the nodal line.

Formation of Graphene on Gold–Nickel Surface Alloys

Nickel (Ni)-catalyzed growth of a single- or rotated-graphene layer is a well-established process above 800 K. In this report, a Au-catalyzed, low-temperature, and facile route at 500 K for graphene formation is described. The substantially lower temperature is enabled by the presence of a surface alloy of Au atoms embedded within Ni(111), which catalyzes the outward segregation of carbon atoms buried in the Ni bulk at temperatures as low as 400-450 K. The resulting surface-bound carbon in turn coalesces into graphene above 450-500 K. Control experiments on a Ni(111) surface show no evidence of carbon segregation or graphene formation at these temperatures. Graphene is identified by its out-of-plane optical phonon mode at 750 cm-1 and its longitudinal/transverse optical phonon modes at 1470 cm-1 while surface carbon is identified by its C-Ni stretch mode at 540 cm-1, as probed by high-resolution electron energy-loss spectroscopy. Dispersion measurements of the phonon modes confirm the presence of graphene. Graphene formation is observed to be maximum at 0.4 ML Au coverage. The results of these systematic molecular-level investigations open the door to graphene synthesis at the low temperatures required for integration with complementary metal-oxide-semiconductor processes.

The effect of ammonia addition on soot nanostructure and composition in ethylene laminar flames

The formation of soot in ammonia (NH3) combustion with a hydrocarbon such as ethylene (C2H4) is investigated using the analysis of particles’ nanostructure and surface chemical composition to identify the mechanisms by which NH3 suppresses soot growth. Young and mature soot particles were extracted from laminar diffusion co-flow flames of NH3C2H4 blends up to 50% NH3. The soot nanostructure is examined using lattice fringe analysis of high-resolution transmission electron microscopy (HRTEM) images, Raman Spectroscopy, and Electron Energy Loss Spectroscopy (EELS). The chemical composition of the soot surface is analyzed using X-ray Photoelectron Spectroscopy (XPS). With increasing NH3 addition, reduced planar growth of the soot graphitic layers is observed through the analysis of the soot nanostructure which indicates the suppression of carbon addition at the edge sites of the layer planes. It is also found that the carbon sp2/sp3 bonding ratio increases which shows a nanostructure with less carbon sp3 bonding at defect sites. By exploring the chemical composition, the nitrogen content of the soot surface increases with NH3 addition which is caused by the bonding of nitrogenated species with carbon at defect and edge sites of the carbon layer, reducing the potential for carbon addition, and thus soot growth. The results also show an increased risk of formation of nitrogenated polyaromatic hydrocarbons (N-PAHs) on the soot surface by NH3 addition. The study presents a novel investigation of the impact of NH3 on the soot surface chemistry and particles nanostructure which explains the role of NH3 in suppressing soot growth and reveals the potential for new toxic characteristics for the soot emissions formed in NH3-hydrocarbon cofired systems.