Characterization of physical aging by time-resolved rheometry: fundamentals and application to bituminous binders

Physical aging is a ubiquitous phenomenon in glassy materials and it is reflected, for example, in the time evolution of rheological properties under isothermal conditions. In this paper, time-resolved rheometry (TRR) is used to characterize this time-dependent rheological behavior. The fundamentals of TRR are briefly reviewed, and its advantages over the traditional Struik’s physical aging test protocol are discussed. In the experimental section, the TRR technique is applied to study physical aging in bituminous binders. Small-diameter parallel plate (SDPP) rheometry is employed to perform cyclic frequency sweep (CFS) experiments over extended periods of time (from one to 8.6 days). The results verify that the mutation of rheological properties is relatively slow during physical aging (mutation number N′_mu?<<?1), thus allowing rheological measurements on a quasi-stable sample. The effects of temperature, crystallinity, and styrene-butadiene-styrene (SBS) polymer modification on the physical aging of bitumen are evaluated. The time-aging time superposition is found to be valid both for unmodified and for polymer-modified bitumen. Vertical shifts are necessary, in addition to horizontal time-aging time shifts, to generate smooth master curves for highly SBS-modified bitumen.     

Application of scaling transformation to characterizing complex rheological behaviors and fractal derivative modeling

It has been long observed that cumbersome parameters are required for the traditional viscoelastic models to describe complex rheological behaviors. Inspired by the relationship between normal and anomalous diffusions, this paper tentatively employs t ^α to replace t, called as the scaling transformation, in the traditional creep compliance and relaxation modulus. With this methodology, the relaxation modulus is found to agree with the well-known Kohlrausch-Williams-Watts (KWW) stretched exponential function. The fitting results confirm that the proposed models accurately characterize rheological behaviors only with one more parameter α. Moreover, it is noted that the present formulations are directly related to the fractal derivative viscoelastic models and the index α is actually the order of the fractal derivative.     

Rheology and structural changes of plasticized zeins in the molten state

Zeins, storage proteins from maize, are suitable for making biobased thermoplastic materials. The rheological behavior of a commercial zein plasticized with 20 w% glycerol was studied in the molten state by steady-state flow experiments in extrusion conditions and oscillatory rheometry. For low residence times, a shear-thinning viscoelastic behavior was observed, with G″ exceeding G′. After 300 s at 130 °C, the complex viscosity |η ^?|?=?7?×?10³ ω ^?0.46 was found to be similar to that of thermoplastic polymer melts used in fused deposition modeling. However, the ratio between the exponents of the power laws describing G′(ω) and G″(ω) did not meet the typical value of 2 for entangled polymer melts. Moreover, for longer residence times, the viscosity increased and a gelation phenomenon was observed with a crossing over of G′(ω) and G″(ω). Gel times ranged from 6000 s at 120 °C to 1700 s at 150 °C. The evolution of the macromolecular structure assessed by sodium dodecyl sulfate-polyacrylamide gel electrophoresis and high-performance size exclusion chromatography suggested that this gelation phenomenon involves various types of covalent and non-covalent cross-links. Disulfide bonds played a significant role in gelation kinetics despite a very low cysteine residue content in the protein primary structure (about 1 mol%). These results suggested that plasticized zeins initially behave like a low-viscosity non-entangled polymer melt, before cross-linking progressively led to a continuous network.     

Filling the gap between transient and steady shear rheology of aqueous graphene oxide dispersions

Even though the rheological behavior of aqueous graphene oxide (G-O) dispersions has been shown to be strongly time-dependent, only few transient measurements have been reported in the literature. In this work, we attempt to fill the gap between transient and steady shear rheological characterizations of aqueous G-O dispersions in the concentration range of 0.004 < ? <?3.5 wt%, by conducting comprehensive rheological measurements, including oscillatory shear flow, transient shear flow, and steady shear flow. Steady shear measurements have been performed after the evaluation of transient properties of the G-O dispersions, to assure steady-state conditions. We identify the critical concentration ? _c =?0.08 wt% (where G-O sheets start to interact) from oscillatory shear experiments. We find that the rheology of G-O dispersions strongly depends on the G-O concentration ?. Transient measurements of shear viscosity and first normal stress difference suggest that G-O dispersions behave like nematic polymeric liquid crystals at ?/? _c =?25, in agreement with other work reported in the literature. G-O dispersions also display a transition from negative to positive values of the first normal stress difference with increasing shear rates. Experimental findings of aqueous graphene oxide dispersions are compared and discussed with models and experiments reported for nematic polymeric liquid crystals, laponite, and organoclay dispersions.     

In situ measurement of localization error in particle tracking microrheology

A method is presented to estimate the static error ?? in a multiple particle tracking microrheology experiment. This in situ estimate of ?? is measured under the same conditions of the material under test, and without any additional experiments. The correction of the mean-squared displacement by the in situ method is potentially more reliable than methods that rely on characterizing ?? in a separate gel sample. With the true mean-squared displacements accessible at short lag times, experimental artifacts introduced by static error can be distinguished from true rheological properties, even in highly viscous (>10,000 mPa?s) samples.     

Experimental study on rheological and thermophysical properties of seawater with surfactant additive—part I: rheological properties

The rheological properties of seawater with the addition of surfactant additive (cetyltrimethyl ammonium chloride (CTAC)/sodium salicylate (NaSal)) are measured at different temperatures, including shear viscosity and first normal stress difference (N₁). The effects of the temperature, the salts, and CTAC/NaSal concentration on the rheological properties of test solutions are investigated, and the corresponding influence mechanisms are analyzed. It shows that the addition of salt can decrease the shear viscosities of the solutions, and also decrease N₁ and even eliminate the sharp augment of N₁ above a certain shear rate. The growing elasticity can be characterized by the increase of the initial shear rate for shear-thickening inception. High temperature can also remove the sharp increase of N₁ with salt. Nevertheless, the increase of CTAC/NaSal concentration can withstand the elimination of the sharp augment of N₁.     

An empirical constitutive model for complex glass-forming liquids using bitumen as a model material

While extensive research efforts have been devoted to understand the dynamics of chemically and structurally simple glass-forming liquids (SGFLs), the viscoelasticity of chemically and structurally complex glass-forming liquids (CGFLs) has received only little attention. This study explores the rheological properties of CGFLs in the vicinity of the glass transition. Bitumen is selected as the model material for CGFLs due to its extremely complex chemical composition and microstructure, fast physical aging and thermorheological simplicity, and abundant availability. A comprehensive rheological analysis reveals a significant broadening of the glass transition dynamics in bitumen as compared to SGFLs. In particular, the relaxation time spectrum of bitumen is characterized by a broad distribution of long relaxation modes. This observation leads to the development of a new constitutive equation, named the broadened power-law spectrum model. In this model, the wide distribution of long relaxation times is described by a power-law with positive exponent and a stretched exponential cut-off, with parameter β serving as a measure of the broadness of the distribution. This characteristic shape of the bitumen spectrum is attributed to the heterogeneous freezing of different molecular components of bitumen, i.e., to the coexistence of liquid and glassy micro-phases. Furthermore, as this type of heterogeneous glass transition behavior can be considered as a general feature of complex glass-forming systems, the broadened power-law spectrum model is expected to be valid for all types of CGFLs. Examples of the applicability of this model in various complex glass-forming systems are given.     

Large amplitude oscillatory shear rheology of three different shear-thickening particle dispersions

We present a large amplitude oscillatory shear rheology (LAOS) investigation of three different shear-thickening particle dispersions - fumed silica in polyethylene oxide (FLOC), fumed silica in polypropylene glycol (HydroC), and cornstarch in water (JAM). These systems shear-thicken by three different mechanisms - shear-induced formation of particle clusters flocculated by polymer bridging, hydrocluster formation, and jamming. The viscoelastic non-linearities of the three fluids were studied as a function of strain and strain-rate space through the use of Lissajous-Bowditch curves and local nonlinear viscoelastic moduli of an oscillatory shear cycle. The nonlinear behaviors of the three fluids were compared and contrasted to understand the nonlinear shear-thickening mechanism of each. Both HydroC and JAM dispersions were found to exhibit strong strain stiffening of the elastic moduli and strain thickening of the loss moduli behavior associated with possible hydrocluster formation and particle jamming. However, the FLOC dispersion, in contrast, showed strong strain softening and strain thinning behavior at large strain amplitudes associated with yielding of the microstructure. The expected thickening of the loss modulus of FLOC in LAOS with increasing strain was not observed even though viscosity of FLOC was found to shear-thicken in steady-shear measurements. This disagreement is likely due to very large strain amplitudes required for shear-thickening to occur by shear-induced polymer bridging mechanism. The hypothesis was confirmed through stress growth experiments. Conversely, the HydroC and JAM dispersions required relatively small applied strains for shear-thickening to occur by hydrocluster and jamming mechanism. The comparison of local intra-cycle nonlinearity through Lissajous-Bowditch plots and nonlinear viscoelastic parameters indicated that the elastic nonlinearities of all three systems are primarily driven by a strong dependence on the magnitude of the applied strain-rates within an oscillatory cycle rather than the amplitude of the applied strain. A close inspection of the LAOS data reveals strong differences in the viscoelastic nonlinearities of these three different shear-thickening dispersions which can be used to create a nonlinear rheological fingerprint for each and offers valuable new insights into the nonlinear dynamics associated with each of the shear-thickening mechanisms.     

Effect of Moisture Content on High Strain Rate Compressibility and Particle Breakage in Loose Sand

Soil-filled gabion structures are widely used to protect against the effects of blast and fragmentation. It is known that moisture content significantly affects the capability of such structures, but the behaviour of partially-saturated soils is not well characterised at the strain rates and stresses experienced in these events. In particular, little data is available for loose soils, whose compaction behaviour can have a substantial impact on structural stability and ballistic performance. This paper describes the use of split Hopkinson pressure bar experiments to characterise the pre- and post-saturation compressibility of a loose quartz sand at moisture contents of up to 15.0%. In contrast to dense soils, increases in moisture content between 0.0% and 7.5% led to a decrease in the stiffness of the sand. Above 7.5% moisture content, specimens reached full saturation during the experiment: the additional water had no further effect on the pre-saturation stiffness, but post-saturation behaviour was dominated by the stiffness of the pore water. Full saturation occurred at lower dry densities as moisture content increased, leading to a decrease in particle breakage.     

An iterative updating method for undamped structural systems

Finite element model updating is a procedure to minimize the differences between analytical and experimental results and can be mathematically reduced to solving the following problem. Problem P: Let M _a ∈SR ^n×n and K _a ∈SR ^n×n be the analytical mass and stiffness matrices and Λ=diag{λ ₁,…,λ _p }∈R ^p×p and X=[x ₁,…,x _p ]∈R ^n×p be the measured eigenvalue and eigenvector matrices, respectively. Find \((\hat{M}, \hat{K}) \in \mathcal{S}_{MK}\) such that \(\| \hat{M}-M_{a} \|^{2}+\| \hat{K}-K_{a}\|^{2}= \min_{(M,K) \in {\mathcal{S}}_{MK}} (\| M-M_{a} \|^{2}+\|K-K_{a}\|^{2})\), where \(\mathcal{S}_{MK}=\{(M,K)| X^{T}MX=I_{p}, MX \varLambda=K X \}\) and ∥?∥ is the Frobenius norm. This paper presents an iterative method to solve Problem P. By the method, the optimal approximation solution \((\hat{M}, \hat{K})\) of Problem P can be obtained within finite iteration steps in the absence of roundoff errors by choosing a special kind of initial matrix pair. A numerical example shows that the introduced iterative algorithm is quite efficient.     

Miscible Thermo-Viscous Fingering Instability in Porous Media. Part 1: Linear Stability Analysis

The development of the thermo-viscous fingering instability of miscible displacements in homogeneous porous media is examined. In this first part of the study dealing with stability analysis, the basic equations and the parameters governing the problem in a rectilinear geometry are developed. An exponential dependence of viscosity on temperature and concentration is represented by two parameters, thermal mobility ratio β _T and a solutal mobility ratio β _C , respectively. Other parameters involved are the Lewis number Le and a thermal-lag coefficient λ. The governing equations are linearized and solved to obtain instability characteristics using either a quasi-steady-state approximation (QSSA) or initial value calculations (IVC). Exact analytical solutions are also obtained for very weakly diffusing systems. Using the QSSA approach, it was found that an increase in thermal mobility ratio β _T is seen to enhance the instability for fixed β _C , Le and λ. For fixed β _C and β _T , a decrease in the thermal-lag coefficient and/or an increase in the Lewis number always decrease the instability. Moreover, strong thermal diffusion at large Le as well as enhanced redistribution of heat between the solid and fluid phases at small λ is seen to alleviate the destabilizing effects of positive β _T . Consequently, the instability gets strictly dominated by the solutal front. The linear stability analysis using IVC approach leads to conclusions similar to the QSSA approach except for the case of large Le and unity λ flow where the instability is seen to get even less pronounced than in the case of a reference isothermal flow of the same β _C , but β _T  = 0. At practically, small value of λ, however, the instability ultimately approaches that due to β _C only.     

Suspensions of titania nanoparticle networks in nematic liquid crystals: rheology and microstructure

We study the influence of confinement on the rheology and structure of nematic liquid crystals (NLCs). NLCs get confined in networks of titania (TiO₂, primary particle size = 21 nm) nanoparticles in suspensions of TiO₂ and NLC, N-(4-methoxybenzylidene)-4-butylaniline (MBBA). Suspensions with TiO₂ nanoparticle volume fraction (?) of 0.006–0.017, form viscoelastic solids with low elastic modulus (G′) of 10¹ Pa–10² Pa and short relaxation times. Increase in TiO₂ nanoparticle ? leads to a rise in G′ with TiO₂ nanoparticles forming a percolating network at a critical volume fraction (? _c) = 0.023, and G′ of ~10³ Pa. TiO₂/MBBA NLC suspensions at and above ? _c = 0.023 show G′ ~ ω ^x?1 scaling, where ω is the angular frequency and the minimum in loss modulus (G′′) with ω. The effective noise temperature, x decreases and approaches 1 with the increase in the TiO₂ nanoparticle ? from 0.023–0.035, is indicative of an increase in the glassy dynamics. Through the polarized light microscopy and differential scanning calorimetry experiments, we propose that the progressive addition of TiO₂ nanoparticles introduces a quenched random disorder (QRD) in the NLC medium which disturbs the nematic order. This results in metastable TiO₂/MBBA NLC suspensions in which NLC domains get confined in the network of flocs of TiO₂ nanoparticles. We also show that the salient rheological signatures of soft glassy rheology develop only in the presence of NLC MBBA and are absent in the isotropic phase of MBBA.     

Operator method for solving the plane elasticity problem for a strip with periodic cuts

In the present paper, we use the conformal mapping z/c = ζ?2a sin ζ (a, c?const, ζ = u + iv) of the strip {|v| ≤ v ₀, |u| < ∞} onto the domain D, which is a strip with symmetric periodic cuts. For the domain D, in the orthogonal system of isometric coordinates u, v, we solve the plane elasticity problem. We seek the biharmonic function in the form F = C ψ ₀ + S ψ*₀ + x(C ψ ₁ ? S ψ ₂) + y(C ψ ₂ + S ψ ₁), where C(v) and S(v) are the operator functions described in [1] and ψ ₀(u), …, ψ ₂(u) are the desired functions. The boundary conditions for the function F posed for v = ±v ₀ are equivalent to two operator equations for ψ ₁(u) and ψ ₂(u) and to two ordinary differential equations of first order for ψ ₀(u) and ψ*₀(u) [2]. By finding the functions ψ _j (u) in the form of trigonometric series with indeterminate coefficients and by solving the operator equations, we obtain infinite systems of linear equations for the unknown coefficients. We present an efficient method for solving these systems, which is based on studying stable recursive relations. In the present paper, we give an example of analysis of a specific strip (a = 1/4, v ₀ = 1) loaded on the boundary v = v ₀ by a normal load of intensity p. We find the particular solutions corresponding to the extension of the strip by the longitudinal force X ^∞ and to the transverse and pure bending of the strip due to the transverse force Y ^∞ and the constant moment M ^∞, respectively. We also present the graphs of normal and tangential stresses in the transverse cross-section x = 0 and study the stress concentration effect near the cut bottom.     

Wave reflection at a free interface in an anisotropic pyroelectric medium with nonclassical thermoelasticity

In this paper, the well-established two-dimensional mathematical model for linear pyroelectric materials is employed to investigate the reflection of waves at the boundary between a vacuum and an elastic, transversely isotropic, pyroelectric material. A comparative study between the solutions of (a) classical thermoelasticity, (b) Cattaneo–Lord–Shulman theory and (c) Green–Lindsay theory equations, characterised by none, one and two relaxation times, respectively, is presented. Suitable boundary conditions are considered in order to determine the reflection coefficients when incident elasto–electro–thermal waves impinge the free interface. It is established that, in the quasi-electrostatic approximation, three different classes of waves: (1) two principally elastic waves, namely a quasi-longitudinal Primary (qP) wave and a quasi-transverse Secondary (qS) wave; and (2) a mainly thermal (qT) wave. The observed electrical effects are, on the other hand, a direct consequence of mechanical and thermal phenomena due to pyroelectric coupling. The computed reflection coefficients of plane qP waves are found to depend upon the angle of incidence, the elastic, electric and thermal parameters of the medium, as well as the thermal relaxation times. The special cases of normal and grazing incidence are also derived and discussed. Finally, the reflection coefficients are computed for cadmium selenide observing the influence of (1) the anisotropy of the material, (2) the electrical potential and (3) temperature variations and (4) the thermal relaxation times on the reflection coefficients.     

Inviscid Models Generalizing the Two-dimensional Euler and the Surface Quasi-geostrophic Equations

Any classical solution of the two-dimensional incompressible Euler equation is global in time. However, it remains an outstanding open problem whether classical solutions of the surface quasi-geostrophic (SQG) equation preserve their regularity for all time. This paper studies solutions of a family of active scalar equations in which each component u _j of the velocity field u is determined by the scalar θ through \({u_j =\mathcal{R}\Lambda^{-1}P(\Lambda) \theta}\) , where \({\mathcal{R}}\) is a Riesz transform and Λ = (?Δ)^1/2. The two-dimensional Euler vorticity equation corresponds to the special case P(Λ) = I while the SQG equation corresponds to the case P(Λ) = Λ. We develop tools to bound \({\|\nabla u||_{L^\infty}}\) for a general class of operators P and establish the global regularity for the Loglog-Euler equation for which P(Λ) = (log(I + log(I ? Δ))) ^γ with 0 ≦ γ ≦ 1. In addition, a regularity criterion for the model corresponding to P(Λ) = Λ ^β with 0 ≦ β ≦ 1 is also obtained.     

Consequences of the Translation Invariance on the Darcy Free Convection Flow Past a Vertical Surface

It is shown that the governing equation for the stream function of the Darcy free convection boundary layer flows past a vertical surface is invariant under arbitrary translations of the transverse coordinate y. The consequences of this basic symmetry property on the solutions corresponding to a prescribed surface temperature distribution T _w (x) are investigated. It is found that starting with a “primary solution” which describes the temperature boundary layer on an impermeable surface, infinitely many “translated solutions” can be generated which form a continuous group, the “translation group” of the given primary solution. The elements of this group describe free convection boundary layer flows from permeable counterparts of the original surface with a transformed temperature distribution \({\tilde {T}_w \left( x \right)}\), when simultaneously a suitable lateral suction/injection of the fluid is applied. It turns out in this way that several exact solutions discovered during the latter few decades are in fact not basically new solutions, but translated counterparts of some formerly reported primary solutions. A few specific examples are discussed in detail.     

Effects of Fuel Lewis Number on Localised Forced Ignition of Globally Stoichiometric Stratified Mixtures: a Numerical Investigation

The influences of fuel Lewis number Le_F on localised forced ignition of globally stoichiometric stratified mixtures have been analysed using three-dimensional compressible Direct Numerical Simulations (DNS) for cases with Le_F ranging from 0.8 to 1.2. The globally stoichiometric stratified mixtures with different values of root-mean-square (rms) equivalence ratio fluctuation (i.e. ?^′= 0.2, 0.4 and 0.6) and the Taylor micro-scale l_? of equivalence ratio ? variation (i.e. l_?/l_f= 2.1, 5.5 and 8.3 with l_f being the Zel’dovich flame thickness of the stoichiometric laminar premixed flame) have been considered for different initial rms values of turbulent velocity u^′. A pseudo-spectral method is used to initialise the equivalence ratio variation following a presumed bi-modal distribution for prescribed values of ?^′ and l_?/l_f for global mean equivalence ratio 〈?〉=1.0. The localised ignition is accounted for by a source term in the energy transport equation that deposits energy for a stipulated time interval. It has been observed that the maximum values of temperature and the fuel reaction rate magnitude increase with decreasing Le_F during the period of external energy deposition. The initial values of Le_F, u^′/S_b(?=1), ?^′ and l_?/l_f have been found to have significant effects on the extent of burning of the stratified mixtures following localised ignition. For a given value of u^′/S_b(?=1), the extent of burning decreases with increasing Le_F. An increase in u^′ leads to a monotonic reduction in the burned gas mass for all values of Le_F in all stratified mixture cases but an opposite trend is observed for the Le_F=0.8 homogeneous mixture. It has been found that an increase in ?^′ has adverse effects on the burned gas mass, whereas the effects of l_?/l_f on the extent of burning are non-monotonic and dependent on ?^′ and Le_F. Detailed physical explanations have been provided for the observed Le_F, u^′/S_b(?=1), ?^′ and l_?/l_f dependences.     

Effect of tube diameter and capillary number on platelet margination and near-wall dynamics

I investigate the effect of tube diameter D and red blood cell capillary number Ca (i.e. the ratio of viscous to elastic forces) on platelet margination in blood flow at ≈37 % tube haematocrit. The system is modelled as three-dimensional suspension of deformable red blood cells and nearly rigid platelets using a combination of the lattice-Boltzmann, immersed boundary and finite element methods. Results of simulations during the dynamics before the steady state has been reached show that a non-diffusive radial platelet transport facilitates margination. This non-diffusive effect is important near the edge of the cell-free layer, but only for Ca > 0.2, when red blood cells are tank-treading. I also show that platelet trapping in the cell-free layer is reversible for Ca ≤ 0.2. Margination is essentially independent of Ca only for the smallest investigated tube diameter (D = 10 μm). Once platelets have reached the cell-free layer, they tend to slide rather than tumble. The tumbling rate is essentially independent of Ca but increases with D. Strong confinement suppresses tumbling due to the relatively small cell-free layer thickness at ≈ 37 % tube haematocrit.     

Regularity and Singularities of Optimal Convex Shapes in the Plane

We focus here on the analysis of the regularity or singularity of solutions Ω ₀ to shape optimization problems among convex planar sets, namely:

$J(\Omega_{0})={\rm min} \{J(\Omega), \Omega \quad {\rm convex},\Omega \in \mathcal{S}_{\rm ad}\},$

where \({\mathcal{S}_{\rm ad}}\) is a set of 2-dimensional admissible shapes and \({J:\mathcal{S}_{\rm ad}\rightarrow\mathbb{R}}\) is a shape functional. Our main goal is to obtain qualitative properties of these optimal shapes by using first and second order optimality conditions, including the infinite dimensional Lagrange multiplier due to the convexity constraint. We prove two types of results:

1. i)
   under a suitable convexity property of the functional J, we prove that Ω ₀ is a W ^2,p -set, \({p\in[1, \infty]}\). This result applies, for instance, with p = ∞ when the shape functional can be written as J(Ω) = R(Ω) + P(Ω), where R(Ω) = F(|Ω|, E _f (Ω), λ₁(Ω)) involves the area |Ω|, the Dirichlet energy E _f (Ω) or the first eigenvalue of the Laplace–Dirichlet operator λ₁(Ω), and P(Ω) is the perimeter of Ω;
    

1. ii)
   under a suitable concavity assumption on the functional J, we prove that Ω ₀ is a polygon. This result applies, for instance, when the functional is now written as J(Ω) = R(Ω) ? P(Ω), with the same notations as above.
    

     

Effects of Fuel Lewis Number on Localised Forced Ignition of Turbulent Mixing Layers

The influences of fuel Lewis number Le _F on localised forced ignition of inhomogeneous mixtures are analysed using three-dimensional compressible Direct Numerical Simulations (DNS) of turbulent mixing layers for Le _F  = 0.8, 1.0 and 1.2 and a range of different root-mean-square turbulent velocity fluctuation u′ values. For all Le _F cases a tribrachial flame has been observed in case of successful ignition. However, the lean premixed branch tends to merge with the diffusion flame on the stoichiometric mixture fraction isosurface at later stages of the flame evolution. It has been observed that the maximum values of temperature and reaction rate increase with decreasing Le _F during the period of external energy addition. Moreover, Le _F is found to have a significant effect on the behaviours of mean temperature and fuel reaction rate magnitude conditional on mixture fraction values. It is also found that reaction rate and mixture fraction gradient magnitude \(\vert \nabla \xi \vert \) are negatively correlated at the most reactive region for all values of Le _F explored. The probability of finding high values of \(\vert \nabla \xi \vert \) increases with increasing Le _F . For a given value of u′, the extent of burning decreases with increasing Le _F . A moderate increase in u′ gives rise to an increase in the extent of burning for Le _F  = 0.8 and 1.0, which starts to decrease with further increases in u′. For Le _F  = 1.2, the extent of burning decreases monotonically with increasing u′. The extent of edge flame propagation on the stoichiometric mixture fraction ξ = ξ _st isosurface is characterised by the probability of finding burned gas on this isosurface, which decreases with increasing u′ and Le _F . It has been found that it is easier to obtain self-sustained combustion following localised forced ignition in case of inhomogeneous mixtures than that in the case of homogeneous mixtures with the same energy input, energy deposition duration when the ignition centre is placed at the stoichiometric mixture. The difficultly to sustain combustion unaided by external energy addition in homogeneous mixture is particularly prevalent in the case of Le _F  = 1.2.