Simulation analysis method for atomic layer deposition process of beta-phase gallium oxide material
By combining density functional theory and superlattice model, a growth substrate model was constructed and the reaction pathway was simulated, which solved the problems of high cost and low efficiency in the atomic layer deposition process of β-phase gallium oxide materials, and achieved accurate simulation and analysis of the atomic layer deposition process.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- HARBIN INST OF TECH
- Filing Date
- 2026-05-07
- Publication Date
- 2026-07-14
AI Technical Summary
In existing technologies, the simulation and analysis of the atomic layer deposition process of β-phase gallium oxide materials is costly and difficult to reveal the atomic-scale reaction mechanism, resulting in low efficiency in optimizing process parameters.
The simulation parameters were set using density functional theory, a superlattice model was constructed and surface hydrogen passivation was performed, a growth substrate model was built, the position of the bottom atomic layer was fixed and the precursor material was defined, multiple reaction pathways were simulated, and the reaction energy barrier and activation energy were determined.
It enables efficient and low-cost simulation and analysis of atomic layer deposition processes, shortens the research cycle, accurately captures key structural and energy data, reveals atomic-scale reaction mechanisms, and reduces material loss and equipment depreciation.
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Figure CN122392662A_ABST
Abstract
Description
Technical Field
[0001] This invention relates to the field of semiconductor material preparation technology, and more specifically, to a simulation analysis method, system, equipment, and medium for the atomic layer deposition process of β-phase gallium oxide material. Background Technology
[0002] Gallium oxide, as a fourth-generation semiconductor material, is widely used in power electronic devices and ultraviolet detectors. Among them, β-Ga₂O₃ is the most stable phase of gallium oxide. Atomic layer deposition (ALD) technology has become a key technology for preparing high-quality β-Ga₂O₃ thin films due to its ability to control film thickness and its conformal coverage of three-dimensional structures.
[0003] In related technologies, research on ALD processes for β-Ga2O3 mainly relies on experimental methods, such as using thermal ALD and plasma-enhanced ALD to simulate the reaction energy barriers and activation energies of the atomic layer deposition process of β-Ga2O3 materials. However, experimental methods have limitations such as high cost, long cycle time, and difficulty in revealing atomic-scale reaction mechanisms. This makes it impossible to effectively explain the entire ALD deposition process of β-Ga2O3 materials (including precursor adsorption, surface reactions, energy barrier calculations, etc.), thus making it difficult to efficiently optimize ALD process parameters. Summary of the Invention
[0004] The problem addressed by this invention is how to improve the efficiency of simulation analysis of the atomic layer deposition process of β-phase gallium oxide materials and reduce the cost of simulation analysis.
[0005] To address the aforementioned problems, this invention provides a simulation analysis method, system, equipment, and medium for the atomic layer deposition process of β-phase gallium oxide materials.
[0006] In a first aspect, the present invention provides a simulation analysis method for the atomic layer deposition process of β-phase gallium oxide materials, comprising: Set the simulation parameters for density functional theory; A superlattice model of β-phase gallium oxide material was constructed, and the superlattice model was subjected to surface hydrogen passivation treatment and structural relaxation optimization to obtain the growth substrate model of the β-phase gallium oxide material. By fixing the position of the bottom atomic layer of the growth substrate model and defining the precursor material, the simulated reaction environment of the β-phase gallium oxide material is obtained; Based on the simulated reaction environment and the simulated parameters, multiple reaction pathways of the atomic layer deposition process are simulated to obtain the stable intermediate structure corresponding to each reaction pathway. Based on the energy data of the stable intermediate structure corresponding to each reaction pathway, the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process are determined.
[0007] Optionally, setting the simulation parameters of density functional theory includes: Establish ion relaxation convergence criteria and energy barrier calculation methods for electronic structure calculations; The ion relaxation convergence criterion and the energy barrier calculation rule are used as the simulation parameters.
[0008] Optionally, the construction of the superlattice model for the β-phase gallium oxide material includes: Based on the crystal structure of the β-phase gallium oxide, a single lattice model of monoclinic β-phase gallium oxide containing multiple gallium oxide units is obtained. Based on the structural characteristics of the single-lattice model, a k-point grid of a preset size is generated; Based on the k-point grid, the superlattice model is obtained by extending it along the lattice vector direction of the single-lattice model.
[0009] Optionally, the step of performing surface hydrogen passivation treatment and structural relaxation optimization on the superlattice model to obtain the growth substrate model of the β-phase gallium oxide material includes: Hydrogen atom passivation is performed based on the surface atomic dangling bond distribution of the superlattice model to obtain a surface-saturated passivation model; Based on the ion relaxation convergence criterion in the simulation parameters, the passivation model is structurally relaxed to obtain a stable structural model with minimized energy. The lattice parameters are extracted from the stable structure model to obtain the growth substrate model.
[0010] Optionally, obtaining the simulated reaction environment for the β-phase gallium oxide material by fixing the position of the bottom atomic layer of the growth substrate model and defining the precursor material includes: Based on the structural characteristics of the growth substrate model, a bulk constraint condition is established by fixing the position of the bottom atomic layer of the growth substrate model. The position of the bottom atomic layer is the spatial coordinate of at least two atomic layers. Based on the precursor selection principle of atomic layer deposition process, trimethylgallium and oxygen are used as reactants; Based on the bulk constraint conditions and the reactants, the simulated reaction environment of the β-phase gallium oxide material is constructed.
[0011] Optionally, the reaction pathway includes a metal precursor half-reaction pathway and an oxidant half-reaction pathway; Based on the simulated reaction environment and the simulated parameters, multiple reaction pathways of the atomic layer deposition process are simulated to obtain stable intermediate structures corresponding to each reaction pathway, including: Based on the simulated reaction environment, the trimethylgallium precursor is placed at a preset surface position on the growth substrate model to determine the initial adsorption position of the trimethylgallium precursor. Based on the initial adsorption position, the atoms of the trimethylgallium precursor are moved multiple times by distribution movement control, and constraint relaxation is performed after each movement to obtain a stable intermediate configuration of the metal precursor half-reaction pathway. Based on the stable intermediate configuration of the metal precursor half-reaction pathway, the atoms of the oxygen precursor are controlled to move multiple times by distribution movement, and constraint relaxation is performed after each movement to obtain the stable intermediate configuration of the oxidant half-reaction pathway.
[0012] Optionally, determining the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process based on the energy data of the stable intermediate structure corresponding to each reaction pathway includes: Based on the energy data of the stable intermediate structure, a curve relationship between energy and reaction coordinates is constructed; Based on the aforementioned curve relationships, the transition state and steady state of each of the aforementioned reaction pathways are determined; By using the energy barrier calculation rules in the simulation parameters, and based on the energy extreme points corresponding to the transition and stable states of the reaction pathway, the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process are determined.
[0013] In a second aspect, the present invention provides a simulation and analysis system for the atomic layer deposition process of β-phase gallium oxide material, comprising: The parameter setting unit is used to set the simulation parameters for density functional theory. The model building unit is used to build a superlattice model of the β-phase gallium oxide material, and to perform surface hydrogen passivation treatment and structural relaxation optimization on the superlattice model to obtain the growth substrate model of the β-phase gallium oxide material. An environment construction unit is used to obtain a simulated reaction environment for the β-phase gallium oxide material by fixing the position of the bottom atomic layer of the growth substrate model and defining the precursor material; The simulation unit is used to simulate multiple reaction pathways of the atomic layer deposition process based on the simulated reaction environment and the simulation parameters, and to obtain a stable intermediate structure corresponding to each reaction pathway. An analysis unit is used to determine the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process based on the energy data of the stable intermediate structure corresponding to each reaction pathway.
[0014] Thirdly, an electronic device according to the present invention includes: a processor and a memory, the memory being used to store a computer program; When the computer program is loaded by the processor, it causes the processor to execute the simulation analysis method for the atomic layer deposition process of β-phase gallium oxide material as described above.
[0015] Fourthly, the present invention provides a computer-readable storage medium having a computer program stored thereon, wherein when the computer program is executed by a processor, it implements the simulation analysis method for the atomic layer deposition process of β-phase gallium oxide material as described above.
[0016] The present invention provides a simulation analysis method, system, equipment, and medium for the atomic layer deposition process of β-phase gallium oxide materials. By setting simulation parameters based on density functional theory, it provides a theoretical basis and calculation standard for the atomic scale, ensuring the accuracy and rationality of subsequent simulations. A superlattice model of β-phase gallium oxide is constructed and subjected to surface hydrogen passivation and structural relaxation optimization to obtain a growth substrate model that closely matches the actual deposition scenario, thereby restoring the crystal structure characteristics of β-phase gallium oxide (such as specific site distribution and interlayer structure). Subsequently, by fixing the position of the bottom atomic layer of the substrate model and defining the precursor material, a simulated reaction environment consistent with the essence of the atomic layer deposition process is established, realizing the core conditions of substrate fixation and reactant participation in the actual deposition process. Based on this, multiple reaction pathways are simulated using the above-mentioned simulated reaction environment and parameters, capturing the... The stable intermediate structures under each pathway cover the atomic-scale changes in key processes such as precursor adsorption, group migration, and reaction. Finally, the energy data of the stable intermediate structures are used to determine the reaction energy barrier and activation energy, quantifying the thermodynamic and kinetic characteristics of the deposition process. This fully replicates the entire process of β-phase gallium oxide atomic layer deposition, revealing the atomic-scale reaction mechanism. Compared with traditional experimental methods, this invention does not require investment in experimental equipment, high-purity precursor materials, or complex experimental environment construction, and avoids the time consumption and resource waste caused by the experimental process. Through theoretical simulation, multiple reaction pathways can be quickly traversed, key structural and energy data can be accurately captured, significantly shortening the research cycle and significantly reducing material consumption, equipment depreciation, and costs. This achieves efficient, low-cost, and accurate simulation analysis of the atomic deposition process. Attached Figure Description
[0017] Figure 1 This is a schematic flowchart of the simulation analysis method for the atomic layer deposition process of β-phase gallium oxide material according to an embodiment of the present invention; Figure 2 This is a schematic diagram of the superlattice model according to an embodiment of the present invention; Figure 3 This is a schematic diagram of the reaction pathway simulation process according to an embodiment of the present invention; Figure 4 This is a schematic diagram of the curve relationship in an embodiment of the present invention; Figure 5This is a schematic diagram of the simulation and analysis system for the atomic layer deposition process of β-phase gallium oxide material according to an embodiment of the present invention. Detailed Implementation
[0018] To make the above-mentioned objects, features, and advantages of the present invention more apparent and understandable, specific embodiments of the present invention will be described in detail below with reference to the accompanying drawings. Although some embodiments of the present invention are shown in the drawings, it should be understood that the present invention can be implemented in various forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided to provide a more thorough and complete understanding of the present invention. It should be understood that the accompanying drawings and embodiments of the present invention are for illustrative purposes only and are not intended to limit the scope of protection of the present invention.
[0019] It should be understood that the various steps described in the method embodiments of the present invention may be performed in different orders and / or in parallel. Furthermore, the method embodiments may include additional steps and / or omit the steps shown. The scope of the present invention is not limited in this respect.
[0020] The term "comprising" and its variations as used herein are open-ended, meaning "including but not limited to"; the term "based on" means "at least partially based on"; the term "one embodiment" means "at least one embodiment"; the term "another embodiment" means "at least one additional embodiment"; the term "some embodiments" means "at least some embodiments"; and the term "optionally" means "optional embodiments". Definitions of other terms will be given in the following description. It should be noted that the concepts of "first," "second," etc., mentioned in this invention are used only to distinguish different devices, modules, or units, and are not intended to limit the order of functions performed by these devices, modules, or units or their interdependencies.
[0021] It should be noted that the terms "a" and "a plurality of" used in this invention are illustrative rather than restrictive. Those skilled in the art should understand that, unless otherwise expressly indicated in the context, they should be understood as "one or more".
[0022] Combination Figure 1 As shown in the embodiment of the present invention, a simulation analysis method for the atomic layer deposition process of β-phase gallium oxide material includes: Set the simulation parameters for density functional theory.
[0023] Specifically, setting the simulation parameters of density functional theory is crucial for providing a theoretical basis and computational standard for atomic-scale calculations of the atomic layer deposition process of β-phase gallium oxide materials. By selecting appropriate density functional theory-related computational configurations, the electronic structure and properties of β-phase gallium oxide materials can be characterized, laying a unified computational foundation for subsequent model construction, reaction simulation, and energy calculation, thus ensuring the accuracy and rationality of the entire simulation process.
[0024] A superlattice model of β-phase gallium oxide material was constructed, and the superlattice model was subjected to surface hydrogen passivation treatment and structural relaxation optimization to obtain the growth substrate model of the β-phase gallium oxide material.
[0025] Specifically, the superlattice model is constructed to fit the crystal structure of β-phase gallium oxide, while surface hydrogen passivation can eliminate the instability caused by dangling bonds on the model surface. Structural relaxation optimization can enable the model to reach the stable state with the lowest energy. The resulting growth substrate model can truly reflect the structural characteristics and physicochemical properties of β-phase gallium oxide as a deposition substrate, providing a carrier for the construction of the subsequent simulation reaction environment.
[0026] By fixing the position of the bottom atomic layer of the growth substrate model and defining the precursor material, the simulated reaction environment of the β-phase gallium oxide material is obtained.
[0027] Specifically, a simulated reaction environment is constructed by fixing the position of the bottom atomic layer of the growth substrate model and defining the precursor material. Fixing the position of the bottom atomic layer of the substrate corresponds to the fixed state of the substrate during actual deposition, avoiding interference from irrelevant atomic movements in the reaction simulation. Selecting a precursor material compatible with the β-phase gallium oxide atomic layer deposition process can recreate the real-world reaction scenario involving the reactants. The simulated reaction environment built by combining these two methods can typically accurately replicate the process conditions during β-phase gallium oxide atomic layer deposition, providing a realistic physicochemical basis for subsequent reaction simulations. This environment preserves the structural stability of the substrate during deposition while ensuring that the types of reactants are consistent with the actual process. It provides reliable scenario support for simulating the complete process of precursor adsorption, diffusion, reaction, and product desorption on the substrate surface, allowing atomic-scale reaction simulations to realistically reflect the material interactions and dynamic changes during actual deposition.
[0028] Based on the simulated reaction environment and the simulated parameters, multiple reaction pathways of the atomic layer deposition process are simulated to obtain stable intermediate structures corresponding to each reaction pathway.
[0029] Specifically, by simulating a series of core processes such as precursor adsorption, group migration, and reaction on the substrate surface, potential reaction pathways are explored. At the same time, by using structural relaxation and other methods, the energy stability of the obtained intermediate structure is ensured, thus fully capturing the dynamic changes at the atomic level during the deposition process.
[0030] Based on the energy data of the stable intermediate structure corresponding to each reaction pathway, the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process are determined.
[0031] Specifically, the reaction energy barrier and activation energy are key thermodynamic and kinetic parameters characterizing the ease and rate of reaction. By analyzing the energy data under different reaction pathways, the advantages and disadvantages of each reaction path can be quantified, the dominant reaction mechanism of the β-phase gallium oxide atomic layer deposition process can be clarified, and a systematic mechanism explanation of the entire deposition process can be completed to achieve the goal of simulation analysis.
[0032] The present invention provides a simulation analysis method for the atomic layer deposition process of β-phase gallium oxide. By setting simulation parameters based on density functional theory, it provides a theoretical foundation and calculation standard for the atomic scale, ensuring the accuracy and rationality of subsequent simulations. A superlattice model of β-phase gallium oxide is constructed and subjected to surface hydrogen passivation and structural relaxation optimization to obtain a growth substrate model that closely matches the actual deposition scenario, thereby restoring the crystal structure characteristics of β-phase gallium oxide (such as specific site distribution and interlayer structure). Subsequently, by fixing the position of the bottom atomic layer of the substrate model and defining the precursor material, a simulated reaction environment consistent with the essence of the atomic layer deposition process is established, realizing the core conditions of substrate fixation and reactant participation in the actual deposition process. Based on this, multiple reaction pathways are simulated using the above-mentioned simulated reaction environment and parameters, capturing the characteristics of each pathway. The stable intermediate structure covers the atomic-scale changes in key processes such as precursor adsorption, group migration, and reaction. Finally, the energy data of the stable intermediate structure is used to determine the reaction energy barrier and activation energy, quantifying the thermodynamic and kinetic characteristics of the deposition process. This fully replicates the entire process of β-phase gallium oxide atomic layer deposition, revealing the atomic-scale reaction mechanism. Compared with traditional experimental methods, this invention does not require investment in experimental equipment, high-purity precursor materials, or complex experimental environment construction, and avoids the time consumption and resource waste caused by the experimental process. Through theoretical simulation, multiple reaction pathways can be quickly traversed, and key structural and energy data can be accurately captured, which greatly shortens the research cycle and significantly reduces material consumption, equipment depreciation, and costs. It achieves efficient, low-cost, and accurate simulation analysis of the atomic deposition process.
[0033] Optionally, setting the simulation parameters of density functional theory includes: Establish ion relaxation convergence criteria and energy barrier calculation methods for electronic structure calculations; The ion relaxation convergence criterion and the energy barrier calculation rule are used as the simulation parameters.
[0034] Specifically, firstly, based on the crystal structure characteristics of β-phase gallium oxide and the computational requirements of the atomic layer deposition process, the ion relaxation convergence criteria are determined, namely, setting the cutoff energy of the plane wave basis set, the force threshold for ion position relaxation, and the spin polarization configuration to ensure that ion motion reaches a stable state during structure optimization. Simultaneously, a suitable energy barrier calculation method is selected, which can capture the energy characteristics of the transition state during the reaction process. Finally, the above two key configurations are integrated into complete simulation parameters. In a preferred embodiment of the invention, the Vienna Ab initio Simulation Software (VASP) package is used as the computational tool, and the PBE exchange correlation function based on the Projected Augmented Wave (PAW) method is selected. The PBE exchange correlation function is an approximate description of the exchange energy originating from the identical fermion properties of electrons and the correlation energy originating from electron quantum correlation in a multi-electron system, directly determining the computational accuracy and reliability. Using the PBE exchange correlation function in the ALD deposition simulation of β-phase gallium oxide, the electronic structure, atomic binding energy, and reaction path energy changes of the material are determined. The ion relaxation convergence criterion was set as follows: a plane wave basis cutoff energy of 400 eV, allowing ion positions to relax until the force on the atom is less than 0.04 eV / Å, and all calculations were performed using spin polarization settings. The energy barrier calculation method used was the push elastic band method, combined with Baader population analysis to assist in obtaining the atomic charge distribution. By calculating the energy of the initial, intermediate, and final states of the reaction and searching for the transition state, the migration energy barrier during the deposition of β-phase gallium oxide atomic layers was solved. The above ion relaxation convergence criterion and energy barrier calculation method were used together as simulation parameters for subsequent simulation analysis.
[0035] In this embodiment of the invention, by defining the ion relaxation convergence criterion and the energy barrier calculation method and integrating them into the simulation parameters, not only is a calculation benchmark provided for the simulation of the atomic layer deposition process of β-phase gallium oxide materials, but the deviation of simulation results caused by fuzzy parameter settings is effectively avoided, ensuring the accuracy of electronic structure calculation and energy barrier analysis; at the same time, the selected ion relaxation convergence criterion can accurately adapt to the crystal structure and physicochemical properties of β-phase gallium oxide, and the energy barrier calculation method can efficiently capture the energy change characteristics of atomic-scale reactions, significantly improving the reliability of the entire simulation analysis method.
[0036] Optionally, the construction of the superlattice model for the β-phase gallium oxide material includes: Based on the crystal structure of the β-phase gallium oxide, a single lattice model of monoclinic β-phase gallium oxide containing multiple gallium oxide units is obtained. Based on the structural characteristics of the single-lattice model, a k-point grid of a preset size is generated; Based on the k-point grid, the superlattice model is obtained by extending it along the lattice vector direction of the single-lattice model.
[0037] Specifically, firstly, based on the stable monoclinic crystal system of β-phase gallium oxide, a single-lattice model containing a specific number of gallium oxide units is selected as the foundation to ensure that the model closely matches the actual crystal structure of the material. Next, combining the structural characteristics of the single-lattice model, such as atomic arrangement and site distribution, a suitable preset size k-point grid is determined to provide accuracy support for the subsequent calculation of the electronic structure of the extended model. Finally, using the k-point grid as the calculation benchmark, the single-lattice model is periodically extended along the lattice vector direction to extend the single-lattice model into a superlattice model that meets the requirements of atomic layer deposition simulation. Specifically, in a preferred embodiment of the present invention, based on the monoclinic crystal structure of β-phase gallium oxide, a monoclinic β-Ga₂O₃ single-lattice model containing four gallium oxide units is selected; combining the distribution characteristics of the two inequivalent gallium atom sites and three inequivalent oxygen atom sites in this single-lattice model, as well as the interlayer alternation structure, a 2×2×1 k-point grid is generated; based on the k-point grid, the model is expanded along the lattice vector direction to finally obtain a β-phase gallium oxide superlattice model with a crystal unit length of 9.138, a width of 11.632, and a height of 33.6453, combined with... Figure 2 As shown, the superlattice model exhibits a characteristic of alternating pure octahedral structures and tetrahedral and octahedral structures.
[0038] In this embodiment of the invention, by selecting a single-lattice model that precisely matches the essence of the β-phase gallium oxide crystal structure, generating an adaptive k-point grid, and expanding the lattice vector direction, the constructed superlattice model can realistically reproduce the core features of the atomic site distribution and interlayer structure of β-phase gallium oxide, and its lattice parameters are in high agreement with experimental measurements. At the same time, the reasonable k-point grid setting ensures the accuracy of subsequent simulation calculations, and the size of the expanded superlattice model meets the requirements of the atomic layer deposition process simulation. It provides a structurally accurate and reliable model carrier for subsequent surface hydrogen passivation treatment, reaction environment construction, and reaction pathway simulation, effectively improving the realism and accuracy of the entire simulation analysis method.
[0039] Optionally, the step of performing surface hydrogen passivation treatment and structural relaxation optimization on the superlattice model to obtain the growth substrate model of the β-phase gallium oxide material includes: Hydrogen atom passivation is performed based on the surface atomic dangling bond distribution of the superlattice model to obtain a surface-saturated passivation model; Based on the ion relaxation convergence criterion in the simulation parameters, the passivation model is structurally relaxed to obtain a stable structural model with minimized energy. The lattice parameters are extracted from the stable structure model to obtain the growth substrate model.
[0040] Specifically, for the dangling bonds formed on the surface of the superlattice model due to atomic unsaturation, a hydrogen atom-oriented encapsulation method is used for passivation treatment. The combination of hydrogen atoms and dangling bonds eliminates surface instability, resulting in a surface-saturated passivated model. Then, according to the preset ion relaxation convergence criteria in the simulation parameters, the passivated model is structurally relaxed, allowing atoms in the model, except for the fixed layer, to freely adjust their positions until the forces acting on the atoms meet the convergence threshold and the total energy of the system reaches its minimum, forming a stable structural model with minimized energy. Finally, key lattice parameters such as lattice constant and atomic site distribution are extracted from the stable structural model, ultimately obtaining a growth substrate model that conforms to the actual crystal characteristics of β-phase gallium oxide. In a preferred embodiment of the present invention, for a β-phase gallium oxide superlattice model containing four gallium oxide units and expanded by a 2×2×1 k-point grid, hydrogen atoms are used to encapsulate these dangling bonds one by one according to the distribution of gallium and oxygen atoms on the surface, resulting in a passivation model with saturated surface atomic valence bonds. Subsequently, based on the ion relaxation convergence criteria in the simulation parameters (plane wave basis set cutoff energy 400 eV, ion position relaxation threshold 0.04 eV / Å, and spin polarization setting), structural relaxation optimization is performed on the passivation model. During the process, the position of the bottom atomic layer of the model is fixed, and the remaining atomic layers are allowed to relax freely until the total energy of the system tends to stabilize. After relaxation is completed, lattice parameters with a length of 9.138, a width of 11.632, and a height of 33.6453 are extracted from the stable structural model, along with the distribution data of two non-equivalent gallium atom sites and three non-equivalent oxygen atom sites, finally forming a β-phase gallium oxide growth substrate model.
[0041] In this embodiment of the invention, hydrogen atom passivation effectively eliminates surface dangling bonds in the superlattice model, avoiding interference from surface instability on subsequent deposition simulation. Meanwhile, structural relaxation optimization based on ion relaxation convergence criteria ensures that the model energy is in the lowest stable state, making the crystal structure of the model highly consistent with the lattice characteristics of actual β-phase gallium oxide.
[0042] Optionally, obtaining the simulated reaction environment for the β-phase gallium oxide material by fixing the position of the bottom atomic layer of the growth substrate model and defining the precursor material includes: Based on the structural characteristics of the growth substrate model, a bulk constraint condition is established by fixing the position of the bottom atomic layer of the growth substrate model. The position of the bottom atomic layer is the spatial coordinate of at least two atomic layers. Based on the precursor selection principle of atomic layer deposition process, trimethylgallium and oxygen are used as reactants; Based on the bulk constraint conditions and the reactants, the simulated reaction environment of the β-phase gallium oxide material is constructed.
[0043] Specifically, based on the crystal structure stability requirements of the growth substrate model and the fixed state of the substrate in actual deposition, the three-dimensional spatial coordinates of at least two layers of atoms at the bottom are locked to restrict the movement of these atoms, establishing a bulk constraint condition to ensure that the substrate model maintains structural stability in subsequent reaction simulations. Then, following the selection principle in atomic layer deposition (ALD) that the precursor must be compatible with the target material and have moderate reactivity, trimethylgallium and oxygen are selected as reactants for β-phase gallium oxide deposition, which aligns with the combination logic of precursors in the actual process. Finally, the established bulk constraint condition is combined with the selected reactants to replicate the core scenario of substrate fixation and reactant participation in the actual ALD process, thereby constructing a simulated reaction environment for β-phase gallium oxide materials that can support subsequent reaction pathway simulations. In a preferred embodiment of the present invention, for a β-phase gallium oxide growth substrate model that has undergone surface hydrogen passivation and structural relaxation optimization and contains two inequivalent gallium atom sites and three inequivalent oxygen atom sites, the spatial coordinates of the bottom three atomic layers of the model are fixed according to its interlayer structure characteristics, so that they cannot move in subsequent simulations, thus establishing stable bulk phase constraints. Based on the selection principle that the precursor in the atomic layer deposition process must be able to provide the target element and the reaction must be controllable, trimethylgallium (Ga(CH3)3) is determined as the gallium source and oxygen (O2) is determined as the oxygen source, and both are used as reactants. The growth substrate model with the bottom atomic layers fixed is combined with the trimethylgallium and oxygen reactants to build a simulated reaction environment that fits the actual process, wherein the trimethylgallium is initially placed 3 Å away from the surface of the substrate model to prepare for subsequent deposition simulation.
[0044] In this embodiment of the invention, a bulk phase constraint condition is established by fixing at least two layers of atoms at the bottom of the growth substrate model, which effectively simulates the stable state of the substrate in actual deposition, avoids the interference of random movement of substrate atoms on the reaction simulation, and ensures the specificity of the reaction process; trimethylgallium and oxygen are selected as reactants to reduce the chemical environment in which the precursor participates in the reaction; the simulated reaction environment is constructed based on the bulk phase constraint condition and reactants.
[0045] Optionally, the reaction pathway includes a metal precursor half-reaction pathway and an oxidant half-reaction pathway; Based on the simulated reaction environment and the simulated parameters, multiple reaction pathways of the atomic layer deposition process are simulated to obtain stable intermediate structures corresponding to each reaction pathway, including: Based on the simulated reaction environment, the trimethylgallium precursor is placed at a preset surface position on the growth substrate model to determine the initial adsorption position of the trimethylgallium precursor. Based on the initial adsorption position, the atoms of the trimethylgallium precursor are moved multiple times by distribution movement control, and constraint relaxation is performed after each movement to obtain a stable intermediate configuration of the metal precursor half-reaction pathway. Based on the stable intermediate configuration of the metal precursor half-reaction pathway, the atoms of the oxygen precursor are controlled to move multiple times by distribution movement, and constraint relaxation is performed after each movement to obtain the stable intermediate configuration of the oxidant half-reaction pathway.
[0046] Specifically, based on the surface characteristics of the growth substrate model in the simulated reaction environment, the trimethylgallium precursor is placed at a fixed distance from the substrate surface to determine its initial adsorption position. Then, based on this initial adsorption position, the methyl and hydrogen atoms in the trimethylgallium are moved stepwise. After each movement, constraints are applied to the model, and structural relaxation is performed according to the relaxation criteria in the simulation parameters to ensure the energy stability of the intermediate configurations formed after each movement, thereby obtaining a series of stable intermediate configurations for the metal precursor half-reaction pathway. Finally, based on the final stable configuration of the metal precursor half-reaction, the same stepwise movement method is used to control the interaction between oxygen atoms in the oxygen precursor and the substrate surface and residual groups in the metal precursor. After each movement, a constraint relaxation operation is performed to capture the stable intermediate configurations of the oxidant half-reaction pathway. In a preferred embodiment of the invention, combined with... Figure 3 As shown, the trimethylgallium precursor was placed at a preset position 3 Å away from the surface of the growth substrate model to determine its initial adsorption state. Based on this initial position, one methyl group in the trimethylgallium was moved closer to a hydrogen atom on the substrate surface. After the movement, the position of the methyl group was fixed and constrained relaxation was performed according to the simulation parameters (cutoff energy 400 eV, force threshold 0.04 eV / Å). Then, the remaining methyl and hydrogen atoms were moved in sequence, and the movement, constraint, and relaxation steps were repeated to obtain three stable intermediate configurations of "adsorption-group migration-preliminary reaction" in the metal precursor half-reaction pathway. Based on the final configuration of the metal precursor half-reaction, an oxygen precursor was introduced into the simulation environment. The oxygen atoms were moved stepwise to combine with the hydrogen atoms and methyl groups remaining on the substrate surface. After each movement, the position of the oxygen atoms was fixed and constrained relaxation was performed to obtain two stable intermediate configurations of "oxygen atom adsorption-bonding reaction-product formation" in the oxidant half-reaction pathway, which fully covered the key reaction stages of the entire deposition cycle.
[0047] In this embodiment of the invention, the entire deposition process is simulated by splitting it into two half-reaction pathways, which not only fits the process characteristics of alternating atomic layer deposition, but also accurately captures the atomic-scale changes in each reaction stage, avoiding the problem of missing intermediate states caused by a one-time simulation of the entire cycle.
[0048] Optionally, determining the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process based on the energy data of the stable intermediate structure corresponding to each reaction pathway includes: Based on the energy data of the stable intermediate structure, a curve relationship between energy and reaction coordinates is constructed; Based on the aforementioned curve relationships, the transition state and steady state of each of the aforementioned reaction pathways are determined; By using the energy barrier calculation rules in the simulation parameters, and based on the energy extreme points corresponding to the transition and stable states of the reaction pathway, the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process are determined.
[0049] Specifically, firstly, energy data for all stable intermediate structures in each reaction pathway are collected, with the reaction coordinates (e.g., relative atomic distances, reaction progress) on the horizontal axis and energy values on the vertical axis. A continuous curve relationship between energy and the reaction coordinates is constructed. Then, based on this continuous curve relationship, the stable structures corresponding to energy minima (i.e., stable states) are identified, including reactant states, intermediate product states, final product states, and structures corresponding to energy maxima (i.e., transition states), thus clarifying the key energy nodes for each reaction step. Finally, the preset energy barrier calculation rules in the simulation parameters are called, such as using the push elastic band method to calculate the activation energy of each reaction step by the energy difference between the transition state and the preceding stable state. The total reaction energy barrier is determined by comparing the maximum difference between the energies of all transition states and the initial stable state in the same reaction pathway. In a preferred embodiment of the present invention, energy data of three stable intermediate structures in the metal precursor half-reaction pathway and two stable intermediate structures in the oxidant half-reaction pathway are collected, wherein the energy values of each stable intermediate structure are -1.5 eV, -1.2 eV, -1.8 eV, -1.6 eV, and -2.0 eV, respectively. Using the relative atomic distance as the reaction coordinate, the energy data are correlated with the corresponding reaction coordinate to plot a curve showing the change in energy with the reaction coordinate. Based on this curve, five stable states (corresponding to each stable intermediate structure) corresponding to the energy minimum points and two transition states (corresponding to the intermediate transition structures in the methyl migration process and the oxygen atom bonding process, respectively) are identified. The energy barrier calculation rule for the elastic band in the simulation parameters is called, and the energy difference between the first transition state and the preceding stable state is calculated to be 0.44 eV (i.e., the activation energy of this step), and the energy difference between the second transition state and the preceding stable state is 0.55 eV. Simultaneously, the total reaction energy barrier is determined to be 0.99 eV, completing the quantification of the energy parameters of the β-phase gallium oxide atomic layer deposition process. Combined with... Figure 4 As shown, Figure 4The three sub-figures a, b, and c all use relative distance (horizontal axis, unit Å) as the reaction coordinate and relative energy (vertical axis, unit eV) as the energy index. Among them, figure a corresponds to the adsorption process of trimethylgallium precursor on the surface of hydrogen-encapsulated β-phase gallium oxide substrate, with the horizontal axis representing the relative distance between gallium atoms and the substrate surface (3.0-1.5 Å), showing the energy change when the precursor approaches the substrate; figure b corresponds to the reaction step of methyl (CH3) moving towards hydrogen atoms on the substrate surface, with the horizontal axis representing the relative distance between CH atoms (2.0-1.2 Å), and the reaction energy barrier of this step is marked as 0.44 eV; figure c corresponds to the model relaxation and subsequent reaction process, with the horizontal axis representing the relative distance between CH3 group and the substrate surface (2.8-3.8 Å), and the energy barrier is marked as 0.55 eV and the total reaction energy barrier as 0.99 eV, which as a whole presents the key energy fluctuation characteristics of the metal precursor half-reaction pathway of β-phase gallium oxide material in ALD deposition.
[0050] In this embodiment of the invention, by constructing a curve relationship between energy and reaction coordinates, the energy evolution law of the reaction process is clearly presented, facilitating intuitive identification of the transition state and the steady state, and avoiding the problem that single energy data cannot reflect the whole picture of the reaction. Based on the curve relationship and the preset energy barrier calculation rules, the energy extreme points of the transition state and the steady state are determined, providing a precise data source for the calculation of the energy barrier and activation energy, ensuring the objectivity and accuracy of the calculation results; the final reaction energy barrier and activation energy quantification data can directly characterize the reaction difficulty and rate control steps of the β-phase gallium oxide atomic layer deposition process, effectively making up for the shortcomings of traditional experimental methods in quantifying reaction energy characteristics, and significantly improving the practical value of simulation analysis.
[0051] Combination Figure 5 As shown, another embodiment of the present invention provides a simulation and analysis system for the atomic layer deposition process of β-phase gallium oxide material, comprising: The parameter setting unit is used to set the simulation parameters for density functional theory. The model building unit is used to build a superlattice model of the β-phase gallium oxide material, and to perform surface hydrogen passivation treatment and structural relaxation optimization on the superlattice model to obtain the growth substrate model of the β-phase gallium oxide material. An environment construction unit is used to obtain a simulated reaction environment for the β-phase gallium oxide material by fixing the position of the bottom atomic layer of the growth substrate model and defining the precursor material; The simulation unit is used to simulate multiple reaction pathways of the atomic layer deposition process based on the simulated reaction environment and the simulation parameters, and to obtain a stable intermediate structure corresponding to each reaction pathway. An analysis unit is used to determine the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process based on the energy data of the stable intermediate structure corresponding to each reaction pathway.
[0052] The simulation and analysis system for the atomic layer deposition process of β-phase gallium oxide material of the present invention has the same advantages over the prior art as the simulation and analysis method for the atomic layer deposition process of β-phase gallium oxide material described above, and will not be repeated here.
[0053] Another embodiment of the present invention provides an electronic device, comprising: a processor and a memory, wherein the memory is used to store a computer program; When the computer program is loaded by the processor, it causes the processor to execute the simulation analysis method for the atomic layer deposition process of β-phase gallium oxide material as described above.
[0054] The electronic device of the present invention has the same advantages over the prior art as the simulation analysis method of the atomic layer deposition process of β-phase gallium oxide material described above, and will not be repeated here.
[0055] Another embodiment of the present invention provides a computer-readable storage medium having a computer program stored thereon. When the computer program is executed by a processor, it implements the simulation analysis method for the atomic layer deposition process of β-phase gallium oxide material as described above.
[0056] The advantages of the computer-readable storage medium of the present invention compared to the prior art are the same as the advantages of the simulation analysis method for the atomic layer deposition process of β-phase gallium oxide material compared to the prior art, and will not be repeated here.
[0057] While the present invention has been disclosed above, its scope of protection is not limited thereto. Those skilled in the art can make various changes and modifications without departing from the spirit and scope of the present invention, and all such changes and modifications will fall within the scope of protection of the present invention.
Claims
1. A simulation and analysis method for the atomic layer deposition process of β-phase gallium oxide materials, characterized in that, include: Set the simulation parameters for density functional theory; A superlattice model of β-phase gallium oxide material was constructed, and the superlattice model was subjected to surface hydrogen passivation treatment and structural relaxation optimization to obtain the growth substrate model of the β-phase gallium oxide material. By fixing the position of the bottom atomic layer of the growth substrate model and defining the precursor material, the simulated reaction environment of the β-phase gallium oxide material is obtained; Based on the simulated reaction environment and the simulated parameters, multiple reaction pathways of the atomic layer deposition process are simulated to obtain the stable intermediate structure corresponding to each reaction pathway. Based on the energy data of the stable intermediate structure corresponding to each reaction pathway, the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process are determined.
2. The simulation and analysis method for the atomic layer deposition process of β-phase gallium oxide material according to claim 1, characterized in that, The setting of simulation parameters for density functional theory includes: Establish ion relaxation convergence criteria and energy barrier calculation methods for electronic structure calculations; The ion relaxation convergence criterion and the energy barrier calculation rule are used as the simulation parameters.
3. The simulation and analysis method for the atomic layer deposition process of β-phase gallium oxide material according to claim 1, characterized in that, The construction of the superlattice model for β-phase gallium oxide material includes: Based on the crystal structure of the β-phase gallium oxide, a single lattice model of monoclinic β-phase gallium oxide containing multiple gallium oxide units is obtained. Based on the structural characteristics of the single-lattice model, a k-point grid of a preset size is generated; Based on the k-point grid, the superlattice model is obtained by extending it along the lattice vector direction of the single-lattice model.
4. The simulation and analysis method for the atomic layer deposition process of β-phase gallium oxide material according to claim 2, characterized in that, The process of performing surface hydrogen passivation and structural relaxation optimization on the superlattice model to obtain the growth substrate model of the β-phase gallium oxide material includes: Hydrogen atom passivation is performed based on the surface atomic dangling bond distribution of the superlattice model to obtain a surface-saturated passivation model; Based on the ion relaxation convergence criterion in the simulation parameters, the passivation model is structurally relaxed to obtain a stable structural model with minimized energy. The lattice parameters are extracted from the stable structure model to obtain the growth substrate model.
5. The simulation and analysis method for the atomic layer deposition process of β-phase gallium oxide material according to claim 1, characterized in that, The process of obtaining the simulated reaction environment for the β-phase gallium oxide material by fixing the position of the bottom atomic layer of the growth substrate model and defining the precursor material includes: Based on the structural characteristics of the growth substrate model, a bulk constraint condition is established by fixing the position of the bottom atomic layer of the growth substrate model. The position of the bottom atomic layer is the spatial coordinate of at least two atomic layers. Based on the precursor selection principle of atomic layer deposition process, trimethylgallium and oxygen are used as reactants; Based on the bulk constraint conditions and the reactants, the simulated reaction environment of the β-phase gallium oxide material is constructed.
6. The simulation and analysis method for the atomic layer deposition process of β-phase gallium oxide material according to claim 5, characterized in that, The reaction pathways include the metal precursor half-reaction pathway and the oxidant half-reaction pathway; Based on the simulated reaction environment and the simulated parameters, multiple reaction pathways of the atomic layer deposition process are simulated to obtain stable intermediate structures corresponding to each reaction pathway, including: Based on the simulated reaction environment, the trimethylgallium precursor is placed at a preset surface position on the growth substrate model to determine the initial adsorption position of the trimethylgallium precursor. Based on the initial adsorption position, the atoms of the trimethylgallium precursor are moved multiple times by distribution movement control, and constraint relaxation is performed after each movement to obtain a stable intermediate configuration of the metal precursor half-reaction pathway. Based on the stable intermediate configuration of the metal precursor half-reaction pathway, the atoms of the oxygen precursor are controlled to move multiple times by distribution movement, and constraint relaxation is performed after each movement to obtain the stable intermediate configuration of the oxidant half-reaction pathway.
7. The simulation and analysis method for the atomic layer deposition process of β-phase gallium oxide material according to claim 2, characterized in that, The step of determining the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process based on the energy data of the stable intermediate structure corresponding to each reaction pathway includes: Based on the energy data of the stable intermediate structure, a curve relationship between energy and reaction coordinates is constructed; Based on the aforementioned curve relationships, the transition state and steady state of each of the aforementioned reaction pathways are determined; By using the energy barrier calculation rules in the simulation parameters, and based on the energy extreme points corresponding to the transition and stable states of the reaction pathway, the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process are determined.
8. A simulation and analysis system for the atomic layer deposition process of β-phase gallium oxide material, characterized in that, include: The parameter setting unit is used to set the simulation parameters for density functional theory. The model building unit is used to build a superlattice model of the β-phase gallium oxide material, and to perform surface hydrogen passivation treatment and structural relaxation optimization on the superlattice model to obtain the growth substrate model of the β-phase gallium oxide material. An environment construction unit is used to obtain a simulated reaction environment for the β-phase gallium oxide material by fixing the position of the bottom atomic layer of the growth substrate model and defining the precursor material; The simulation unit is used to simulate multiple reaction pathways of the atomic layer deposition process based on the simulated reaction environment and the simulation parameters, and to obtain a stable intermediate structure corresponding to each reaction pathway. An analysis unit is used to determine the reaction energy barrier and activation energy of the β-phase gallium oxide material during the atomic layer deposition process based on the energy data of the stable intermediate structure corresponding to each reaction pathway.
9. An electronic device, characterized in that, include: Processor and memory, the memory being used to store computer programs; When the computer program is loaded by the processor, it causes the processor to execute a simulation analysis method for the atomic layer deposition process of β-phase gallium oxide material as described in any one of claims 1-7.
10. A computer-readable storage medium having a computer program stored thereon, characterized in that, When the computer program is executed by the processor, it implements a simulation analysis method for the atomic layer deposition process of β-phase gallium oxide material as described in any one of claims 1-7.