Nucleation Free Energy Barrier Research Articles

Insights into the crystallization behavior of structurally and spatially doubly confined polymer systems studied by molecular simulation

The impact of grafting density and polymer-substrate interactions on the crystallization behavior of structurally and spatially doubly confined polymer systems was studied using Monte Carlo simulation methods. In the confined polymer system with low grafting density, as the polymer-substrate interactions increase, the nucleation mode shifts from homogeneous nucleation to heterogeneous nucleation. The melting temperature and undercooling increase, while the critical nucleation free energy barrier decreases, favoring the crystallization process. Nevertheless, significant polymer-substrate interactions can lead to a decrease in the mobility of polymer chains, thereby inhibiting the crystallization process. In highly grafted polymer systems, homogeneous nucleation controls the entire crystallization process and the crystallization rate and final degree of crystallinity are almost unaffected by polymer-substrate interactions. Grafting density and polymer-substrate interactions play a dual role, acting as a “double-edged sword” in the crystallization process of doubly confined polymer systems. An appropriate grafting density and polymer-substrate interactions facilitate the nucleation ability, thereby promoting the crystallization capability of polymer systems. Conversely, excessive interactions can weaken nucleation ability and suppress crystal growth.

Cryopreservation of human semen by inherently-controlled icing probability: Or how the surface profile of superhydrophobic carbon soot coatings and the sperm volume affect the outcome of slow freezing?

The restoration of initial functionality of human spermatozoa subjected to cryopreservation is challenging, because the deleterious intracellular icing and the occurrence of osmotic shocks due to prolonged exposure to increased concentrations of intracellular solutes are oppositely dependent on the cooling rate. This longstanding problem could be overcome if using superhydrophobic soot coatings delaying the heat transfer rate, reducing the ice formation probability and triggering balanced and timely dehydration of the cells, but the effect of their surface profile and sperm volume on the success rate of slow freezing is unclear. Here, we show for the first time that the two-factor freezing injury is entirely avoidable by tailoring the solid-to-gas voids (pores) fraction in the soot, leading to increased nucleation free energy barrier, presumable incipiency of ice crystals with controllable shape and size and hence, fully (100 %) recovered post-thaw sperm motility. It is demonstrated that the reason for such a unique scientific result is the selection of soot coatings with appropriate morphochemical features, hypothetically (not directly proven yet) inducing equilibrium among the solution composition and ice crystals formation, retarding the undesirable compression of liquid-filled “slush ice” channels surrounding the cytoplasm and impeding the ice recrystallization. The novel insights introduced in this article open endless horizon for customizing and revolutionizing the technical protocols in cryobiology.

A first-principles machine-learning force field for heterogeneous ice nucleation on microcline feldspar.

The formation of ice in the atmosphere affects precipitation and cloud properties, and plays a key role in the climate of our planet. Although ice can form directly from liquid water under deeply supercooled conditions, the presence of foreign particles can aid ice formation at much warmer temperatures. Over the past decade, experiments have highlighted the remarkable efficiency of feldspar minerals as ice nuclei compared to other particles present in the atmosphere. However, the exact mechanism of ice formation on feldspar surfaces has yet to be fully understood. Here, we develop a first-principles machine-learning model for the potential energy surface aimed at studying ice nucleation at microcline feldspar surfaces. The model is able to reproduce with high-fidelity the energies and forces derived from density-functional theory (DFT) based on the SCAN exchange and correlation functional. Our training set includes configurations of bulk supercooled water, hexagonal and cubic ice, microcline, and fully-hydroxylated feldspar surfaces exposed to a vacuum, liquid water, and ice. We apply the machine-learning force field to study different fully-hydroxylated terminations of the (100), (010), and (001) surfaces of microcline exposed to a vacuum. Our calculations suggest that terminations that do not minimize the number of broken bonds are preferred in a vacuum. We also study the structure of supercooled liquid water in contact with microcline surfaces, and find that water density correlations extend up to around 10 Å from the surfaces. Finally, we show that the force field maintains a high accuracy during the simulation of ice formation at microcline surfaces, even for large systems of around 30 000 atoms. Future work will be directed towards the calculation of nucleation free-energy barriers and rates using the force field developed herein, and understanding the role of different microcline surfaces in ice nucleation.

Enhanced nucleation of bimodal molecular weight distribution polymers: A molecular dynamics study

We perform coarse-grained molecular dynamics (CGMD) simulations to study the homogeneous nucleation of bimodal and unimodal molecular weight distribution polymers with equivalent average molecular weight. First, a statistical method is proposed to determine the critical nuclei and thus calculate the free energy barrier of nucleation. From the temperature dependence of diffusion coefficient, we also determine the activation energy of diffusion. Then we calculate the nucleation rate and find that it is consistent with the classical nucleation theory for homogeneous nucleation in semi-crystalline polymers. Compared with unimodal system, the bimodal system exhibits lower interfacial free energy and consequently lower free energy barrier for nucleation, while the two systems have similar activation energy for diffusion. This suggests that the promoted nucleation rate of bimodal molecular weight distribution polymer is a result of the reduction of interfacial free energy, which is eventually a consequence of chain-folding nucleation of long chain component.

Room-temperature growth of perovskite single crystals via antisolvent-assisted confinement for high-performance electroluminescent devices

Organic-inorganic halide perovskite single crystals (OIHP-SCs) are promising light-emitting materials for bright electroluminescence (EL) devices due to their superior optoelectronic properties and excellent stability. However, the conventional high-temperature growth methods will inevitably disturb the ordered growth and introduce massive defects in OIHP-SCs, leading to the degradation of device performance. The preparation of thin OIHP-SCs with low trap-state densities for high-performance EL devices remains a formidable challenge. Here, we develop an efficient antisolvent-assisted confined growth (AACG) method for the room-temperature growth of formamidinium lead bromide (FAPbBr3) perovskite SCs. An antisolvent vapour environment is intentionally introduced in the spatially confined growth process to lower the free energy barrier for nucleation, enabling the growth of high-quality FAPbBr3 SCs at room temperature. Consequently, FAPbBr3 SCs with ultralow trap-state density of 2.15 × 109 cm−3 and amplified spontaneous emission (ASE) threshold of 7.1 µJ cm−2 could be achieved, representing the best results ever reported for FAPbBr3 SCs. By leveraging the high crystal quality of FAPbBr3 SCs, SC-based perovskite light-emitting diodes (PeLEDs) with a high luminance of over 26,000 cd m−2 and a peak current efficiency (CE) of 13.02 cd A−1 are demonstrated. Our work opens up new opportunities for the development of high-performance EL devices based on OIHP-SCs.

Are Neural Network Potentials Trained on Liquid States Transferable to Crystal Nucleation? A Test on Ice Nucleation in the mW Water Model.

Neural network potentials (NNPs) are increasingly being used to study processes that happen on long time scales. A typical example is crystal nucleation, which rate is controlled by the occurrence of a rare fluctuation, i.e., the appearance of the critical nucleus. Because the properties of this nucleus are far from those of the bulk crystal, it is yet unclear whether NN potentials trained on equilibrium liquid states can accurately describe nucleation processes. So far, nucleation studies on NNPs have been limited to ab initio models whose nucleation properties are unknown, preventing an accurate comparison. Here we train a NN potential on the mW model of water─a classical three-body potential whose nucleation time scale is accessible in standard simulations. We show that a NNP trained only on a small number of liquid state points can reproduce with great accuracy the nucleation rates and free energy barriers of the original model, computed from both spontaneous and biased trajectories, strongly supporting the use of NNPs to study nucleation events.

Nucleation of Biomolecular Condensates from Finite-Sized Simulations.

The nucleation of protein condensates is a concentration-driven process of assembly. When modeled in the canonical ensemble, condensation is affected by finite-size effects. Here, we present a general and efficient route for obtaining ensemble properties of protein condensates in the macroscopic limit from finite-sized nucleation simulations. The approach is based on a theoretical description of droplet nucleation in the canonical ensemble and enables estimation of thermodynamic and kinetic parameters, such as the macroscopic equilibrium density of the dilute protein phase, the surface tension of the condensates, and nucleation free energy barriers. We apply the method to coarse-grained simulations of NDDX4 and FUS-LC, two phase-separating disordered proteins with different physicochemical characteristics. Our results show that NDDX4 condensate droplets, characterized by lower surface tension, higher solubility, and faster monomer exchange dynamics compared to those of FUS-LC, form with negligible nucleation barriers. In contrast, FUS-LC condensates form via an activated process over a wide range of concentrations.

Effect of particle anisotropy on the thermodynamics and kinetics of ordering transitions in hard faceted particles.

Monte Carlo simulations were used to study the influence of particle aspect ratio on the kinetics and phase behavior of hard gyrobifastigia (GBF). First, the formation of a highly anisotropic nucleus shape in the isotropic-to-crystal transition in regular GBF is explained by the differences in interfacial free energies of various crystal planes and the nucleus geometry predicted by the Wulff construction. GBF-related shapes with various aspect ratios were then studied, mapping their equations of state, determining phase coexistence conditions via interfacial pinning, and computing nucleation free-energy barriers via umbrella sampling using suitable order parameters. Our simulations reveal a reduction of the kinetic barrier for isotropic-crystal transition upon an increase in aspect ratio, and that for highly oblate and prolate aspect ratios, an intermediate nematic phase is stabilized. Our results and observations also support two conjectures for the formation of the crystalline state from the isotropic phase: that low phase free energies at the ordering phase transition correlate with low transition barriers and that the emergence of a mesophase provides a steppingstone that expedites crystallization.

Nucleation and crystallization mechanism of heavy hydrocarbons in natural gas under flow field

The understanding of the crystallization mechanism of heavy hydrocarbons in natural gas directly determines the modification of nucleation theory and the development of new liquefaction processes. However, the mechanism of heavy hydrocarbon crystallization in the flow field is still not well understood. In this paper, molecular dynamics (MD) simulations were adopted to investigate heavy hydrocarbon crystallization under shear flow, and the nucleation pathway related to crystallization kinetics was explored. The results show that shear rates less than 1 × 108 s−1 promote the rapid growth of heavy hydrocarbon crystals with high final crystallinity, whereas higher shear rates cause crystals to grow slowly ending up with lower crystallinity. Compared with quiescent nucleation, the presence of a shear flow promotes the heavy hydrocarbon stretching and consequently accelerates the kinetic process of phase transition. In addition, molecular orientation fluctuations arising from the flow field are accompanied by the elastic deformation of solid nucleus, increasing the nucleation free energy barrier. Therefore, the nucleation rate of heavy hydrocarbon liquids peaks at the optimal shear rate 1 × 107 s−1. Moreover, a unified pathway for heavy hydrocarbon nucleation under shear flow was proposed.

Can solid surface energy be a predictor of ice nucleation ability?

Surface energy is one of the most important properties of materials that dictate many behaviors such as the spreading of water and ice nucleation. It is commonly thought that low surface energy leads to hydrophobicity and delays ice formation. Conventional studies mainly focus on rough surfaces where surface energy is amplified/reduced accordingly and it remains elusive to clearly decouple the effect of surface energy on ice nucleation. Here we experimentally construct the atomically smooth surfaces of halogen chemistry by varying silane self-assembled monolayers with exactly the same aliphatic chain but varied end groups of F, Cl, Br and I. By analyzing ice nucleation rate and free energy barrier based on the measured freezing temperature/delay time and the classical nucleation theory, we demonstrate that the ice nucleation efficiencies of various halogen chemistry surfaces increase in the order of Br, F, I and Cl, which is inconsistent with the surface energy sequence. The results indicate that solid surface energy is not a secure predictor of ice nucleation ability. By further analyzing the surface potentials of different halogen chemistry surfaces, we find that surface polarity plays a key role in ice nucleation maybe through impacting the orientation of interfacial water.

Nucleation in supercooled water triggered by mechanical impact: Experimental and theoretical analyses

Supercooling is one of the major drawbacks that hinder the wide application of phase change thermal storage technology, where supercooling needs to be suppressed, or nucleation triggered at desired supercooling or time. The disturbance of mechanical impact can effectively promote nucleation. However, up to now, its nucleation mechanism has not been well explained, and the corresponding nucleation triggering technology has not been reasonably developed. In this paper, the effect of mechanical impact in supercooled water on nucleation is investigated experimentally by impact rod falling freely to hit the bottom of container. The nucleation temperature under impact at different heights of free fall are measured. The results show that 80% supercooling reduction can be achieved by a low impact energy of 0.007 J. In addition, we modify the existing model based on the experimental data to develop a revised model, which can estimate the impact stimulus required to trigger nucleation at desired supercooling. Moreover, the nucleation mechanism under impact based on classical nucleation theory is analyzed. By comparing the changes in pre-exponential factor and nucleation barrier with and without impact, the enhancement in nucleation rate under impact can be explained as a reduction on the free energy barrier for nucleation. Our experimental and theoretical analysis results preliminarily reveal the impact nucleation mechanism, which are expected to promote more in-depth research on the related topics. These results could also better serve to predict whether nucleation will occur in the supercooled water under mechanical impact, and to actively trigger nucleation or suppress supercooling as needed through mechanical impact.

Influences of Oxidation Degree and Size on the Ice Nucleation Efficiency of Graphene Oxide.

Figuring out the influences of carbonaceous particle properties on ice nucleation is important to atmospheric science, but it is still a challenge, especially for experimental investigations due to the coupling effect of multiple properties. Here we separately investigate the effects of oxidation degree and size, two typical and debated factors, on ice nucleation efficiency by choosing graphene oxide (GO) as the model. The results show that with the decrease of oxidation degree, ice nucleation efficiency increases through decreasing the ice nucleation free energy barrier () on GO surface. Interestingly, although the chosen GO sizes are sufficiently large compared with the sizes of critical ice nuclei, the increase of GO size leads to the increase of and thus the decrease of ice nucleation efficiency, unlike the general thought that is not affected by the particle size any more when the size of particle increases to several times that of the critical ice nucleus.

Computing free energy barriers for the nucleation of complex network mesophases.

A previously introduced framework to identify local order parameters (OPs) distinctive of incipient complex mesophases, such as bicontinuous network phases, is used in this work to evaluate nucleation free-energy barriers. The sampling techniques considered are the mean-first-passage-time (MFPT) method and novel variants of umbrella sampling, including Hybrid Monte Carlo (HMC) and a dual-OP-method that uses a blunter global OP for the umbrella bias while keeping record of configurations for analysis with a local OP. These methods were chosen for their ability to minimize or avoid frequent calculation of the expensive local OP, which makes their continuous on-the-fly tracking computationally very inefficient. These techniques were first validated by studying phase-transition barriers of model systems, i.e., the vapor-liquid nucleation of Lennard-Jones argon and a binary nanoparticle model. The disorder-to-order free energy barrier was then traced for the double gyroid and single diamond formed by mesoscopic bead-spring macromolecular models. The dual OP method was found to be the most robust and computationally efficient, since, unlike HMC, it does not require the expensive local OP to be computed on-the-fly, and unlike the MFPT method, it can negotiate large barriers aided by the biased sampling. The dual OP method requires, however, that a cheap global OP be identified and correlated (in a post-processing step) with the local OP that describes the structure of the critical nucleus, a process that can be aided by machine learning.

Enhanced Water Nucleation and Growth Based on Microdroplet Mobility on Lubricant-Infused Surfaces.

Lubricant-infused surfaces (LISs) can promote stable dropwise condensation and improve heat transfer rates due to a low nucleation free-energy barrier and high droplet mobility. Recent studies showed that oil menisci surrounding condensate microdroplets form distinct oil-rich and oil-poor regions. These topographical differences in the oil surface cause water microdroplets to rigorously self-propel long distances, continuously redistributing the oil film and potentially refreshing the surface for re-nucleation. However, the dynamic interplay between oil film redistribution, microdroplet self-propulsion, and droplet nucleation and growth is not yet understood. Using high-speed microscopy, we reveal that during water condensation on LISs, the smallest visible droplets (diameter: ∼1 μm, qualitatively representing nucleation) predominantly emerge in oil-poor regions due to a lower nucleation free-energy barrier. Considering the significant heat transfer performance of microdroplets (<10 μm) and transient characteristic of microdroplet movement, we compare the apparent nucleation rate density and water collection rate for LISs with oils of different viscosities and a solid hydrophobic surface at a wide range of subcooling temperatures. Generally, the lowest lubricant viscosity leads to the highest nucleation rate density. We characterize the length and frequency of microdroplet movement and attribute the nucleation enhancement primarily to higher droplet mobility and surface refreshing frequency. Interestingly and unexpectedly, hydrophobic surfaces outperform high-viscosity LISs at high subcooling temperatures but are generally inferior to any of the tested LISs at low temperature differences. To explain the observed nonlinearity between LISs and the solid hydrophobic surface, we introduce two dominant regimes that influence the condensation efficiency: mobility-limited and coalescence-limited. We compare these regimes based on droplet growth rates and water collection rates on the different surfaces. Our findings advance the understanding of dynamic water-lubricant interactions and provide new design rationales for choosing surfaces for enhanced dropwise condensation and water collection efficiencies.

Probing Kinetics and Mechanism of Formation of Mixed Metallic Nanoparticles in a Polymer Membrane by Galvanic Replacement between Two Immiscible Metals: Case Study of Nickel/Silver Nanoparticle Synthesis.

Galvanic replacement between metals has received notable research interest for the synthesis of heterometallic nanostructures. The growth pattern of the nanostructures depends on several factors such as extent of lattice mismatch, adhesive interaction between the metals, cohesive forces of the individual metals, etc. Due to the difficulties in probing ultrafast kinetics of the galvanic replacement reaction and particle growth in solution, real-time mechanistic investigations are often limited. As a result, the growth mechanism of one metal on the surface of another metal at the nanoscale is poorly understood so far. In the present work, we could successfully probe the galvanic replacement of silver ions with nickel nanoparticles, stabilized in a polymer membrane, using two complementary methods, namely, small-angle X-ray scattering (SAXS) and radiolabeling, and the results are supported by density functional theory (DFT) computations. The silver-nickel system has been chosen for the present investigation because of the high degree of bulk immiscibility caused by the large lattice mismatch (15.9%) and the weak adhesive interaction, which makes it a perfect model system for immiscible metal pairs. Membrane, as a host medium, plays a crucial role in retarding the kinetics of atomic and particle rearrangements (nucleation and growth) due to slower mobility of the atoms (monomers) and particles within the polymer network. This allowed us to examine the real-time concentration of silver monomers during galvanic replacement of silver ions with nickel nanoparticles and evolution of Ni/Ag nanoparticles. From combined experiment and DFT computations, it has been demonstrated, for the first time to the best of our knowledge, that the majority of silver atoms, which are produced on the nickel nanoparticle surface by galvanic reactions, do not form traditional core-shell nanostructures with nickel and undergo a self-governing sequential nucleation and growth of silver nanoparticles via formation of intermediate prenucleation silver clusters, leading to the formation of mixed metallic nanoparticles in the membrane. The surface of NiNPs has a heterogeneous effect on the silver nucleation pathway, which is evident from the reduced critical free energy barrier of nucleation (ΔGcrit). The present work establishes an original mechanistic pathway based on a sequential nucleation model for formation of mixed metallic nanoparticles by the galvanic replacement route, which opens up future possibilities for size-controlled synthesis in mixed systems.

Suppression of ice nucleation in supercooled water under temperature gradients

Understanding the behaviours of ice nucleation in non-isothermal conditions is of great importance for the preparation and retention of supercooled water. Here ice nucleation in supercooled water under temperature gradients is analyzed thermodynamically based on classical nucleation theory (CNT). Given that the free energy barrier for nucleation is dependent on temperature, different from a uniform temperature usually used in CNT, an assumption of linear temperature distribution in the ice nucleus was made and taken into consideration in analysis. The critical radius of the ice nucleus for nucleation and the corresponding nucleation model in the presence of a temperature gradient were obtained. It is observed that the critical radius is determined not only by the degree of supercooling, the only dependence in CNT, but also by the temperature gradient and even the Young’s contact angle. Effects of temperature gradient on the change in free energy, critical radius, nucleation barrier and nucleation rate with different contact angles and degrees of supercooling are illustrated successively. The results show that a temperature gradient will increase the nucleation barrier and decrease the nucleation rate, particularly in the cases of large contact angle and low degree of supercooling. In addition, there is a critical temperature gradient for a given degree of supercooling and contact angle, at the higher of which the nucleation can be suppressed completely.

Equivalence between condensation and boiling in a Lennard-Jones fluid.

Condensation and boiling are phase transitions highly relevant to industry, geology, and atmospheric science. These phase transitions are initiated by the nucleation of a drop in a supersaturated vapor and of a bubble in an overstretched liquid, respectively. The surface tension between both phases, liquid and vapor, is a key parameter in the development of such nucleation stage. Whereas the surface tension can be readily measured for a flat interface, there are technical and conceptual limitations to obtain it for the curved interface of the nucleus. On the technical side, it is quite difficult to observe a critical nucleus in experiments. From a conceptual point of view, the interfacial free energy depends on the choice of the dividing surface, being the surface of tension the one relevant for nucleation. We bypass the technical limitation by performing simulations of a Lennard-Jones fluid where we equilibrate critical nuclei (both drops and bubbles). Regarding the conceptual hurdle, we find the relevant cluster size by searching the radius that correctly predicts nucleation rates and nucleation free energy barriers when combined with Classical Nucleation Theory. With such definition of the cluster size we find the same value of the surface tension for drops and bubbles of a given radius. Thus, condensation and boiling can be viewed as two sides of the same coin. Finally, we combine the data coming from drops and bubbles to obtain, via two different routes, estimates of the Tolman length, a parameter that allows describing the curvature dependence of the surface tension in a theoretical framework.

Wettability behavior and anti-icing property of superhydrophobic coating on HTV silicone rubber

Composite insulators, which use high temperature vulcanized (HTV) silicone rubber as shed material, are widely applied in transmission lines. Ice accumulation on their surfaces may inflict flashover accident and even massive power outage. In this study, a superhydrophobic (SH) coating on HTV silicone rubber was fabricated by the sol–gel process combined with the plasma jet treatment method. It was found that the as-prepared SH coating exhibited prominent superhydrophobicity and an excellent self-cleaning property with a water contact angle of 160.15°, a contact angle hysteresis of 0.60°, a sliding angle of 1.8°, and a surface free energy of 0.1421 mN/m. The anti-icing behavior of water droplets on the as-prepared SH coating surface was investigated at a low temperature of −30 °C and compared with that of the HTV silicone rubber surface. The results indicated that the freezing time on the SH coating was postponed obviously and was as long as 150 s. The SH coating surface exhibited about 5.6 times delay in freezing at −30 °C compared with the HTV silicone rubber surface. Furthermore, heterogeneous nucleation theory and heat transfer theory were introduced to explain the difference in freezing time between the as-prepared SH coating and HTV silicone rubber. It could be concluded that the SH coating had a large nucleation free energy barrier and a low heat transfer rate between the droplet and the surface and, thus, was able to effectively delay the freezing time.

The effect of grafting density on the crystallization behavior of one‐dimensional confined polymers

AbstractGrafting density and confinement scale of the nano‐area are significant elements affecting the crystallization behavior of polymers. In this work, the crystallization processes of confined and unconfined polymer systems with different grafting density were systematically studied by MC simulation. The results show that when the grafting density of confined systems is low, the crystallization rate is faster and the final crystallinity is higher. However, the crystallization ability is reduced for higher grafting density. We found that for this confined system, the segmental density of interfacial region is larger, and the movement of chain segment is lower. Due to the higher grafting density, the crowding effect of polymer chains is strong, which leads to the intermolecular nucleation. The critical nucleation free energy barrier is higher. Moreover, only homogeneous nucleation occurs in confined polymer systems. With the increasing grafting density, the crystals change from lying on the substrate surface to being perpendicular to the substrate surface in unconfined polymer systems. The crystals are mainly lying on the substrate surface in confined polymer systems. These simulation results are helpful to understand the microscopic mechanism of crystallization behaviors of polymer nanocomposites and provide a theoretical basis for the design of nanocomposites with excellent physical properties.

Heterogeneous nucleation of YBCO via fluorine based MOD process: thermodynamic and kinetic approach

The nucleation of YBa2Cu3O7−δ (YBCO) film deposited via metal organic decomposition (MOD) approach is a complex process that has a key role in YBCO film crystalline orientation and, consequently, superconducting properties. Up to now, several studies have been carried out to clarify this step in the fluorine based MOD route which employs only or partially metals trifluoroacetate for the precursor solution preparation. However, these previous works provided only qualitative indications, whereas a quantitative theoretical investigation seems to be still lacking.In this paper, the free energy for critical nucleus formation of fluorine based MOD YBCO has been determined according to the classical nucleation theory. The volume contribution to the free energy is computed using thermodynamic data on (Y, Ba, Cu, O) systems available from the literature. The free energy barrier for nucleation depends upon nucleus orientation, via the work of adhesion and surface energies of vacuum/nucleus interfaces. The model is applied to describe heterogeneous nucleation of YBCO on (001) SrTiO3 single crystal and provides quantitative information on nucleation barriers as a function of temperature and both precursor and gas phase compositions. Through a kinetic approach, the energy barriers are further employed to estimate the fraction of c-oriented nuclei as a function of temperature and water partial pressure.Comparison with experimental data from literature lends support to the proposed computations. Therefore, the results shown in this work may be useful in designing the YBCO deposition process in order to obtain films with superior superconducting properties avoiding expensive and time-consuming experimental optimizations.