Microscopic Mechanism Research Articles

Reactive molecular dynamics simulations of poly(vinyl alcohol) gasification in supercritical carbon dioxide

Supercritical fluid gasification technology, as an environmentally friendly technology, can convert organic components of plastic waste into fuels and chemical materials. Moreover, the utilization of CO2 as the gasification environment holds significant importance for reducing carbon emissions. To better comprehend the microscopic mechanism of plastic gasification in supercritical environment, this sthdy used the Reactive Force Field (ReaxFF) molecular dynamics method to study the gasification process of long-chain poly(vinyl alcohol) molecule in supercritical H2O/CO2 under different reaction conditions. The result illustrated that during the gasification process, poly(vinyl alcohol) initially depolymerized into multiple long carbon chain (C5+) molecular fragments. Subsequently, these fragments underwent cleavage into short carbon chains and various gaseous small molecules. In this reaction, O radicals generated by CO2 decomposition play a crucial role in promoting the cleavage of plastic C–C bonds. In addition, through the analysis of the products and chemical bonds, we found that increasing temperature and prolonging reaction time significantly enhance the gasification efficiency and hydrogen production of plastics. Conversely, exceedingly high pressure inhibits the gasification reaction.

The Influence and Mechanism of Curing Methods and Curing Age on the Mechanical Properties of Yellow River Sand Engineered Cementitious Composites.

This study investigates the potential use of Yellow River sand (YRS) sourced from the lower reaches of the Yellow River in China as a sustainable and cost-effective substitute for quartz sand in Engineered Cementitious Composites (ECC). With an annual accumulation of approximately 400 million tons in this region, YRS presents a substantial resource. ECC specimens with 100% YRS replacement with quartz sand were subjected to various curing methods: natural, steam, standard, and sprinkler. Extensive mechanical testing including flexural, compressive, uniaxial tensile, and four-point flexural tests was conducted. Additionally, Scanning Electron Microscope (SEM) and Mercury Intrusion Porosimetry (MIP) analyses investigated microscopic mechanisms influencing macroscopic mechanical properties. Finally, the mechanical properties of the YRS-ECC test block after 14 days of standard curing and the traditional sand ECC test block were compared and analyzed. The results indicate that ECC specimens with 100% YRS substitution under natural curing show an optimal ultimate tensile strain of more than 4%, providing the best resistance to the reduction in ultimate flexural load and deflection due to aging. Steam curing enhances flexural and compressive strength, achieving an ultimate flexural load of 5 kN and a maximum deflection of 4.42 mm at 90 days. SEM analysis revealed lower C-S-H gel density under natural curing and higher under steam curing, enhancing fiber pull-out in steam-cured specimens. The MIP tests demonstrated that natural curing had the highest porosity (32.86%) and average pore size (51.69 nm), whereas steam curing resulted in the smallest average pore size, with 44% of pores under 50 nm. Compared with traditional sand, it is found that the ultimate bending load and deflection of YRS-ECC are 5.7% and 9.4% higher than those of traditional sand ECC, respectively, and its ultimate tensile strength and strain are also improved. These findings highlight YRS as a sustainable alternative to natural sand in ECC, with natural curing proving the most effective for superior mechanical performance, including tensile strain, crack resistance, and durability.

Metagenomic analysis reveals enhanced sludge dewaterability through acidified sludge inoculation: Regulation of Fe (II) oxidation electron transport pathway

The bioleaching utilizing indigenous microbial inoculation can continuously improve the dewaterability of sludge. In this study, metagenomic analysis was innovative employed to identify the key microorganisms and functional genes that affect the dewatering performance of sludge in the bioleaching conditioning process. The results demonstrated that long-term repeated inoculation of acidified sludge resulted in increased abundance of many functional genes associated with the transport of carbohydrate and amino acid. Additionally, genes encoding key iron transport proteins (such as afuA, fhuC, and fhuD) and genes related to electron transfer carriers in ferrous iron oxidation process (such as rus and cyc2) were significantly enriched, thereby promoting the improvement of sludge dewatering performance through enhanced iron oxidation. Notably, Acidithiobacillus, Betaproteobacteria, and Hyphomicrobium were the major sources of functional genes. This study reveals the microscopic mechanisms underlying the improvement of sludge dewaterability through bioleaching based on mixed culture from a novel perspective of gene metabolism.

Investigating the microscopic enhancement mechanisms of adsorption-based CO2 capture with Cu-loaded γ−Al2O3 using density functional theory

Transition-metal-loaded γ−alumina (Al2O3) is considered to be an effective adsorbent for CO2 capture, but its microscopic process and mechanisms of CO2 adsorption are not fully understood. To investigate the microscopic enhancement role of Cu atoms in CO2 adsorption, this work compares various adsorption configurations and parameters of CO2 on γ−Al2O3 (110) facets with or without Cu atoms and small Cu cluster loading (Cun (n=1,2,3)/γ−Al2O3) using the first-principles approach. According to the adsorption energy, charge transfer, difference charge density, and other parameters of different configurations, the γ−Al2O3 (110) slab loaded with the Cu atom is found to exhibit enhanced adsorption of CO2 molecules compared to that without Cu loading. Moreover, the surface stability increases with the number of loaded Cu atoms. However, the hydroxyl groups in the active sites partially undermine the adsorption effect during the CO2 adsorption process. The density of states indicates that the doping of Cu atoms in the system creates an orbital peak closer to the Fermi energy level. This facilitates the transfer of charge within the slab, making the activation of CO2 easier and promoting stable adsorption. Finally, the amount of crystal orbital overlap population and crystal orbital Hamilton population shows that the stability of adsorption is due to the formation of C-Cu and C-Al bonds. It is demonstrated that the Cun-loaded γ−Al2O3 (110) slab improves the adsorption performance and contributes to a better understanding of the effect of transition-state metal loaded γ−Al2O3 on CO2 adsorption.

Role of the structural order of the hydration layer in regulating the heterogeneous ice nucleation efficiency

Understanding the complex microscopic mechanisms of heterogeneous ice nucleation is crucial across diverse fields from cloud science to microbiology. In this work, we examined the ability of solid surfaces to promote ice nucleation as a function of the structural order of interfacial water, including the first and second hydration layers. Comprehensive all-atom molecular dynamics simulations using the TIP4P/ice water model were conducted on a water film atop a modeled surface inspired by the (0001) surface of AgI crystal, with varying surface charges. These simulations revealed non-monotonic nucleation rates. The first hydration layer formed a hexagonal hydrogen-bond network resembling ice structures, exhibiting low mobility essential for inducing ice nucleation. Notably, the second hydration layer, acting as a key-point bridge, displayed varying degrees of orientational preference facilitated by inter-layer hydrogen bonds. The calculation of fluctuation parameters indicated that the greater structural order of the second layer significantly enhances the surface’s ice-forming capabilities. Unlike previous studies that focused primarily on the role of the first layer of interfacial water, our findings demonstrate that the second layer provides a more accurate indicator of ice nucleation capabilities.

Tailorable piezoelectric and flexoelectric output of a polymer-particle composite

Materials with different combinations of piezoelectric and flexoelectric properties offer multifunctionality and versatility in terms of modes of operation in sensing, actuation, and energy harvesting. We explore a microscopic mechanism for tailoring the macroscopic quasi-static mechanoelectrical output of polymer-particle composites by taking advantage of heterogeneity-induced enhancement of the stress fields and strain gradient fields. The idea focuses on using microscopic inclusions, such as embedded particles and voids, to manipulate the activation and relative contributions of the piezoelectric and flexoelectric effects under different modes of mechanical excitation, such as uniaxial compression and flexural bending. The material system studied is a composite of poly(vinylidene fluoride-co-trifluoroethylene [P(VDF-TrFE)] polymer and nanoaluminum (nAl) particles, or P(VDF-TrFE)/nAl. This system is interesting because P(VDF-TrFE) exhibits both piezoelectric and flexoelectric behaviors and nAl particles have significantly higher elastic stiffness than the polymer. A range of piezoelectric and flexoelectric properties of P(VDF-TrFE) and the stiffness of the particles are considered. Significant microstructural effects are found to enable tailoring of the mechanoelectrical response through microstructure variation. The responses of the composite are quantified using the effective piezoelectric constant (d33,effo) and the effective flexoelectric coefficient (μTR,effo). It is found that the effective macroscopic piezoelectric and flexoelectric behaviors can be changed either independently or simultaneously through different combinations of microstructure attribute changes. The mechanism revealed points out avenues for developing materials with tunable mechanoelectrical behaviors and multifunctionality.

Eggshell-enhanced biochar with in-situ formed CaO/Ca(OH)2 for efficient removal of Pb2+ and Cd2+ from wastewater: Performance and mechanistic insights

This study proposes a green and simple strategy for efficiently removing heavy metals from wastewater by activating biochar with eggshell and in-situ generating CaO/Ca(OH)2. Characterization results revealed that the composite carbon material (BCEg15) successfully incorporated CaO/Ca(OH)2 active sites compared to the raw biochar (BC). Additionally, eggshell activation increased the specific surface area and pore volume of BCEg15 by 4.36 and 6.80 times, respectively, compared to BC. These structural enhancements increased the maximum adsorption capacity of BCEg15 for Pb2+ and Cd2+ by 20.68 and 42 times, respectively, compared to BC. Importantly, the loading of CaO and Ca(OH)2 significantly enhanced the ion exchange and mineral precipitation capacities of the biochar. For instance, compared to BC, the adsorption capacities of BCEg15 attributed to ion exchange (Qe) for Pb2+ and Cd2+ rose by 403.12 mg/g and 197.65 mg/g, respectively, while the adsorption capacities attributed to mineral precipitation (Qp) increased by 19.60 times and 45.20 times, respectively. BCEg15 demonstrated excellent reusability, maintaining adsorption capacities of 461.18 mg/g for Pb2+ and 265.26 mg/g for Cd2+ after five cycles. Additionally, BCEg15 outperformed commercial activated carbon in treating heavy metals from desulfurization wastewater from coal-fired power plants, achieving a removal efficiency of 99.98 % compared to 48.22 %. The primary mechanisms by which BCEg15 removes Pb2+ and Cd2+ were identified as ion exchange, mineral precipitation, complexation with oxygen-containing functional groups, and interactions with π electrons. Density functional theory (DFT) was utilized to delve deeper into the microscopic mechanisms of adsorption. The findings showed that the O-top site of CaO exhibited the greatest stability for heavy metal adsorption. Electron density difference maps and partial density of states (PDOS) results revealed a denser electron cloud and greater orbital overlap between CaO and Pb2+ compared to Cd2+, suggesting a higher affinity and adsorption capacity for Pb2+, consistent with the experimental findings. This study presents an effective method for preparing adsorbents capable of removing Pb2+ and Cd2+ from wastewater and offers theoretical insights into the adsorption mechanisms of metal oxide-incorporated biochar.

Molecular dynamics study of ionic liquid electrospray: Revealing the effect of types of electric fields

The microscopic behaviors and characteristics of BMIM+BF4− ionic liquid electrospray in the presence of the axial electric field and axial-radial electric field were investigated by molecular dynamics method. The formation and fragmentation of the jet, the structure characteristics of the ions, the interactions between the ions and the energy properties were analyzed. Since ionic liquid is commonly used in spacecraft thruster, their specific impulse and thrust are also evaluated. It was found that the occurrence of ionic liquid electrospray was determined by the axial voltage, not less than 0.8V/nm. The flow rate and radial voltage mainly affect the jet instability and the secondary disintegration. When the jet is broken, it is almost ejected in the form of (BMIM+BF4−)1(BMIM+) and BMIM+, but finally it presents four main clusters, including BF4−, BMIM+, (BMIM+BF4−)1 and (BMIM+BF4−)1(BMIM+). For the unbroken jet at the capillary outlet, BMIM+ is concentrated on the surface of the jet, and BF4− is concentrated inside. The number of clusters will occasionally decrease owing to coalesce. The internal bonds of BMIM+ and BF4− is likely to break, and the bond angle may also vary. In the presence of the axial-radial electric field with an axial electric field intensity of 1.2V/nm, the electrospray ionization effect is the best at the radial electric field intensity of 0.001V/nm, and the specific impulse and thrust can be obtained by adjusting the axial electric field intensity. This work provides a new insight into the microscopic mechanisms of BMIM+BF4− ionic liquid electrospray.

Understanding copper corrosion in bentonite-enriched environments: Insights from the point defect model

The study simulated copper corrosion in a bentonite/groundwater solution, analyzing the kinetics of metal passivation through potentiodynamic polarization, potentiostatic polarization, and electrochemical impedance spectroscopy experiments. Morphological characterization provided insights into corrosion development patterns, and the mechanisms by which bentonite affects copper corrosion were comprehensively elucidated based on the point defect model. The findings revealed that bentonite affects copper corrosion resistance through Donnan exclusion, cation adsorption, and hydrolysis salt effects. At lower potentials, bentonite aids in inhibiting anodic dissolution, reducing the polarization current by approximately 75 % under certain conditions. With increasing bentonite content, the induction time for stable pitting corrosion shortens significantly, down to 10 %, the current surge before breakdown intensifies, and the breakdown potential decreases. When the bentonite volume ratio exceeds 0.5/0.1, the breakdown potential of OFP-Cu/OF-Cu markedly decreases and stabilizes at 0.1/0 VSCE. The microscopic mechanism of pitting corrosion induced by bentonite hydrolysis salts was elucidated using the point defect model, calculating the polarizability of the passive layer/outer layer interface as α = 0.1. The reliability of the cation adsorption and adsorption-desorption mechanisms was confirmed through experimental data fitting, point defect model fitting, and theoretical analysis.

Convective Instability Driven by Diffusiophoresis of Colloids in Binary Liquid Mixtures.

In a binary fluid mixture, the concentration gradient of a heavier molecular solute leads to a diffusive flux of solvent and solute to achieve thermodynamic equilibrium. If the solute concentration decreases with height, the system is always in a condition of stable mechanical equilibrium against gravity. We show experimentally that this mechanical equilibrium becomes unstable in case colloidal particles are dispersed uniformly within the mixture and that the resulting colloidal suspension undergoes a transient convective instability with the onset of convection patterns. By means of a numerical analysis, we clarify the microscopic mechanism from which the observed destabilization process originates. The solute concentration gradient drives an upward diffusiophoretic migration of colloids, in turn causing the development of a mechanically unstable layer within the sample, where the density of the suspension increases with height. Convective motions arise to minimize this localized rise in gravitational potential energy.

Investigating the internal erosion behavior and microscopic mechanisms of chemically stabilized soil: an experimental study

IntroductionInternal erosion triggered by water pipeline leaks seriously threatens the stability of the urban ground. Hangzhou, a city in Zhejiang Province, China, is facing critical challenges due to urban ground collapse (UGC) caused by internal erosion. However, there is a lack of research on the prevention of UGC by improving the internal erodibility of underground soil. Addressing this issue is of utmost importance to ensure the city’s stability and safety. This paper proposes to improve the internal erodibility of typical sandy silt soils with chemical stabilisers.MethodsThe effects of three chemical stabilisers, lignosulphonate (LS), lime (LI), and lignin fibre (LF), on the critical shear stress (τc) and erosion coefficient (kd) of sandy silt soils were investigated, which from Hangzhou, Zhejiang, China, by the hole erosion test (HET) at different mixing amounts and at different conservation times.ResultsThe findings indicate that LF mainly improves the erosion resistance of sandy silt by increasing τc, and the maximum increase is 2.38 times; LI mainly improves the erosion resistance by decreasing kd, and the maximum decrease is 2.18 times. After adding LS, τc and kd did not change significantly. The scanning electron microscope (SEM) test revealed that the inclusion of LF led to the formation of larger agglomerates in the sandy silt soil. The microstructure of sandy silt soil remained dispersed even after adding LS. Various chemical stabilisers used to improve sandy silt soils exhibited distinct erosion mechanisms. Sandy silt soils improved with LF exfoliated into agglomerates, displaying high resistance to erosion. On the other hand, the sandy silt treated with LF still lacks a protective layer and shows minimal improvements in its ability to withstand erosion. In contrast, the LS-amended sandy silt remains stripped with individual soil particles with insignificant changes in erosion resistance.DiscussionThis study can provide a conceptual framework for choosing foundation treatment techniques in future urban development projects.

Study of microscopic mechanisms in HAT-CN/NPB interface devices under consideration of trap action

Traps within semiconductor devices are crucial in determining the device performance. Identifying the root cause of trap generation necessitates a thorough investigation of the underlying micro-mechanisms. This study presents the current density–voltage (J-V) characteristic curves for devices employing HAT-CN/NPB as the interface material. The presence of traps in the devices is confirmed by fitting the power-law relationship J∝(V−Vi)m+1. Subsequent investigation employs the magnetic effect as a diagnostic tool, uncovering that the TPI process generates distinct substates, which markedly influence the device performance. The interaction between a trap-bound triplet exciton and a free polariton leads to the formation of double-state trions, thereby enhancing device luminous intensity. In contrast, the interaction of a free triplet exciton with a bound polariton yields quartet trions, which impede charge transport, as demonstrated by the analysis of magneto-conductance amplitude and positive and negative in this study. This manuscript integrates findings from the TPI process, photoelectric data, and magnetic effect data to elucidate the device response to traps.

Cryogenic damage behavior of carbon fiber reinforced polymer composite laminates via fiber-optic acoustic emission

Cryogenic temperatures cause significant changes in the mechanical response and microscopic failure mechanisms of carbon fiber reinforced polymer (CFRP) composites. However, the mechanisms by which cryogenic temperatures affect composites are not yet fully understood due to a lack of adequate in-situ characterization techniques. Herein, the cryogenic damage evolution process of CFRP composites was investigated by constructed fiber-optic acoustic emission (AE) detection system. Tensile damage behavior of woven CFRP composites at 300 K, 153 K and 77 K was evaluated by AE characteristic response and cluster analysis combined with scanning electron microscopy. According to the results, increased damage activity within the composites at cryogenic condition promoted the release of mechanical energy, as well as an increase in the contribution of fiber damage to overall damage, which are the dominant micro-strengthening mechanisms of composite laminates under cryogenic conditions. This study provides a novel explanation for understanding the cryogenic damage behavior of composites.

Femtosecond Terahertz Pulse Propagation Measurements and Simulations of Dewetting Kinetics in Real Time.

We report a terahertz time-domain study of dewetting kinetics on two time scales: femtoseconds and in real time (on the order of minutes). We recorded full electric field terahertz time domain signals with femtosecond time resolution during dewetting of water in cellulose. The femtosecond time-domain signals were analyzed with respect to the amplitude and signal emission times and how these two quantities changed over the course of dewetting kinetics. The femtosecond time-domain signals were modeled by a combination of finite-difference time-domain electromagnetic simulations of linear terahertz pulse propagation and an effective medium description of the dielectric permittivity. A logistic regression mechanism was incorporated into the electrodynamics simulations to account for the observed kinetics. In addition, analysis of the area-normalized, real-time time-dependent terahertz spectra was used to identify broad regions in the terahertz spectral range that correlated with the kinetic process. Real-time two-dimensional terahertz correlation maps were used to identify the pure rotational spectrum of water vapor, thus characterizing the evaporation part of the dewetting kinetics problem. We conclude with a kinetic model that accounts for our observations through a microscopic mechanism involving the interconversion among bulk water, water clusters, and individual water molecules in the gas phase. Overall, the approach presented here illustrates an application of femtosecond time-resolved experiments in the terahertz spectral range to the study of kinetic processes.

Finite element simulation and experimental verification of laser machining of nitinol tubes

Nitinol tubes are widely used to cut various biological stents, especially cardiovascular stents. However, stent fabrication defects, such as residual stress, microcracks, and heat-affected zones (HAZs) from the laser cutting, can lead to severe clinical complications. In this study, a multiphase flow coupling model for fiber laser cutting simulation is established by considering surface tension, gravity, and recoil pressure and combining the characteristics of fluid heat transfer with phase transition dynamics. The accuracy of the model is verified through the fiber laser cutting experiments. The simulation model is used to explore the influence of the key process parameters of laser cutting on the kerf width, stress, temperature distribution, and the HAZ. The microscopic removal mechanism of the material during the laser cutting is revealed, thus minimizing the problems generated during stent forming. The simulation model can provide an optimized process plan for fiber laser cutting.

Effects of Particle Migration on the Relaxation of Shock Wave Collisions.

The non-equilibrium characteristics during the shock relaxation process hold a foundational position in various fields. In contrast to the propagation of a single shock wave, the collision process of two shock waves exhibits distinct non-equilibrium features. Employing non-equilibrium molecular dynamics, we simulated the collision of ultra-strong shock waves in a classical gas system, investigating the relationship between equilibrium relaxation time and shock intensity. Tracking the spatial migration of microscopic particles in the shock collision region during the relaxation process, we observed a significant contribution of particle migration to the average energy changes during relaxation. The discussion on particle migration provides a valuable new perspective for understanding the microscopic mechanisms of the relaxation process.

Mechanism study of replacing adsorbed O2 molecules in different pore sizes under different CO2/N2 inert gas conditions

Injecting inert gases into the goaf is a crucial method for inhibiting coal spontaneous combustion. Research has verified that the co-injection of CO2 and N2 provides a more effective control measure compared to a single gas, but the microscopic mechanism underlying the synergistic displacement of O2 by CO2 and N2 remains unclear. Injecting inert gases into the goaf is a crucial method for inhibiting coal spontaneous combustion. Research has verified that the co-injection of CO2 and N2 provides a more effective control measure compared to a single gas, but the microscopic mechanism underlying the synergistic displacement of O2 by CO2 and N2 remains unclear. Here, for the constructed multi-scale aperture slit model, the Grand Canonical Monte Carlo simulation (GCMC) and Molecular Dynamics (MD) simulation are used to investigate the mechanism of displacing adsorbed O2 molecules under different CO2/N2 inert gas conditions. The results indicate that CO2 and N2 aggregated on opposing sides of the coal molecules and dispersed within the slit layer, respectively. At 1 nm pore size, the relative concentration of O2 for optimal displacement was 1.054. The absolute value of the average binding energy is small when the CO2:N2 gas ratio is 80:20 and 40:60 at 2 nm and 4 nm apertures, respectively. This suggests that as the aperture size increases, the displacement effect on O2 shifts towards a higher proportion of N2, with a more conspicuous replacement effect as the aperture widens. The smaller pores ranging from 1-2 nm predominantly feature CO2 displacing adsorbed state O2, while larger pores exceeding 2 nm primarily N2 facilitate the transportation of free state O2.

Symbolic transform optimized convolutional neural network model for high-performance prediction and analysis of MXenes hydrogen evolution reaction catalysts

Two-dimensional MXenes materials are expected to be cost-effective and efficient catalysts for hydrogen evolution reaction (HER) due to their tunable surface electronic structure. To optimize its catalytic activity, this study proposes a data-driven framework (CROSST) to generate descriptors through feature engineering and integrate them into a convolutional neural network to predict the HER performance of transition-metal (TM) anchored bis-transition-metal carbon-nitride (TM-M′2M′′CNO2) catalysts. The STCNN model achieves a coefficient of determination of more than 0.93, showing the ability to predict the Gibbs free energy of hydrogen adsorption (ΔGH) with high accuracy. We explored the microscopic mechanisms of HER activity through density functional theory and machine learning analysis. It was found that TM anchoring altered the charge distribution of the MXenes material, elevated the atomic orbital occupancy of neighboring O sites, and weakened the O adsorption of H, thus affecting the HER activity. These results provide a theoretical basis for the design of high-performance MXenes HER catalysts and contribute new research perspectives.

Using the space-time evolution spectrum to investigate the transmission characteristics of lightning return stroke current

Exploring the physical characteristics of lightning discharge channels based on spectrum can help to reveal the microscopic mechanism of the discharge process and provide a theoretical basis for lightning protection research. According to the spectra of six cloud-to-ground lightning return stroke processes and plasma conduction theory, we investigated the evolution of the total intensity of ionic and atomic lines in the spectra, conductivity, and other parameters along the discharge channel at different stages of the return stroke. The results show that the intensity of ionic lines in the spectrum present an obvious decaying trend with increasing height along the channel during the initial current-rise phase of the return stroke. In the later stages, the decay of ionic line intensity along the channel height slowed down. The intensity of the atomic lines varied slightly with increasing height along the channel during the entire return stroke process. The different space-time evolution characteristics of the spectral line intensity with different excitation energies reflect the differences in the mechanism of light radiation in the core current-carrying and surrounding thermal channels. The spectral characteristics further confirm that the ionic line with higher excitation energy directly relates to the physical process in the core current-carrying channel, and its intensity can roughly reflect the change in current along the channel. The attenuation of the return stroke current along the channel was mainly manifested in the initial stage of the return stroke. The decay rate of conductivity along the channel height is slower than that of the ionic line intensity throughout the return stroke stage, which is related to the channel diameter, it is another key parameter affecting the current transmission in the discharge channel.

Unveiling the Mechanism of Phonon-Polariton Damping in α-MoO3.

Phonon polaritons (PhPs), light coupled to lattice vibrations, in the highly anisotropic polar layered material molybdenum trioxide (α-MoO3) are currently the focus of intense research efforts due to their extreme subwavelength field confinement, directional propagation, and unprecedented low losses. Nevertheless, prior research has primarily concentrated on exploiting the squeezing and steering capabilities of α-MoO3 PhPs, without inquiring much into the dominant microscopic mechanism that determines their long lifetimes, which is key for their implementation in nanophotonic applications. This study delves into the fundamental processes that govern PhP damping in α-MoO3 by combining ab initio calculations with scattering-type scanning near-field optical microscopy (s-SNOM) and Fourier transform infrared (FTIR) spectroscopy measurements across a broad temperature range (8-300 K). The remarkable agreement between our theoretical predictions and experimental observations allows us to identify third-order anharmonic phonon-phonon scattering as the main damping mechanism of α-MoO3 PhPs. These findings shed light on the fundamental limits of low-loss PhPs, which is a crucial factor for assessing their implementation into nanophotonic devices.