High-throughput First-principles Research Articles

Discovering novel γ-γ′ Pt-Al superalloys via lattice stability in Pt3Al induced by local atomic environment distortion

The strength of Pt-Al superalloys can be effectively improved using a coherent structure composed of a disordered γ phase and an ordered γ′ phase. However, γ′-Pt3Al has a cubic phase only at high temperatures and a tetragonal phase at low temperatures, thus breaking the coherent interface and deteriorating its mechanical properties. Here, high throughput first-principles calculations and rational experiments were conducted to discover novel γ-γ′ Pt-Al superalloys. The alloying strategy stabilizes the γ′ phase through the local charge distortion (LCD) or the local lattice distortion (LLD). Alloying elements, such as, Ti, Hf, and Ta, occupy the Al site in combination with Pt, making the spherical shape of change density in Pt3Al showing obvious directionality, i.e., LCD. Therefore, the stability of the γ′ phase is proposed at a lower alloying element concentration (3.125 at.%). However, alloying elements near Pt, e.g., Ni, Co, and Ru, tend to occupy the Pt site and induce LLD to stabilize the γ′ phase at higher alloying element concentration (12.5 at.%). The shape of the change density is similar to that of Pt3Al, and no obvious LCD is found when alloying elements occupy the Pt site. LCD-induced phase stability is observed exclusively at the Al site, whereas LLD-induced phase stability is solely present at the Pt site. The Pt-12Al-6X (X = Hf, Ti, Ta, Cr, and Ni in at.%) alloys were prepared, among which Pt-12Al-6Hf possessed a stable γ′ phase, a lower lattice misfit between γ and γ′, and a higher precipitation strengthening, resulting in its hardness (442.1 HV) surpassing that of Ni-based superalloys IN718 (413.6 HV). The γ′ phase in Pt-12Al-6Hf was characterized by high-resolution transmission electron microscopy, suggesting that the Pt site of the γ′ phase was occupied by Pt, while the Al site was shared by Pt, Al, and Hf. This is consistent with the calculated results.

Electrochemical stability of biodegradable Zn-Cu alloys through machine-learning accelerated high-throughput discovery.

Zn-Cu alloys have attracted great attention as biodegradable alloys owing to their excellent mechanical properties and biocompatibility, with corrosion characteristics being crucial for their suitability for biomedical applications. However, the unresolved identification of intermetallic compounds in Zn-Cu alloys affecting corrosion and the complexity of the application environment hamper the understanding of their electrochemical behavior. Utilizing high-throughput first-principles calculations and machine-learning accelerated evolutionary algorithms for screening the most stable compounds in Zn-Cu systems, a dataset encompassing the formation energy of 2033 compounds is generated. It reveals that most of the experimentally reported Zn-Cu compounds can be replicated, especially the structure of R32 CuZn5 is first discovered which possesses the lowest formation energy of -0.050 eV per atom. Furthermore, the simulated X-ray diffraction pattern matches perfectly with the experimental ones. By formulating 342 potential electrochemical reactions based on the binary compounds, the Pourbaix diagrams for Zn-Cu alloys are constructed to clarify the fundamental competition between different phases and ions. The calculated equilibrium potential of CuZn5 is higher than that of Zn through the forward reaction Zn + CuZn5 ⇌ CuZn5 + Zn2+ + 2e-, resulting in microcell formation owing to the stronger charge density localization in Zn compared to CuZn5. The presence of chlorine accelerates the corrosion of Zn through the reaction Zn + CuZn5 + 6Cl- + 6H2O ⇌ Cu + 6ZnOHCl + 6H+ + 12e-, where the formation of ZnOHCl disrupts the ZnO passive film and expands the corrosion pH range from 9.2 to 8.8. Our findings reveal an accurate quantitative corrosion mechanism for Zn-Cu alloys, providing an effective pathway to investigate the corrosion resistance of biodegradable alloys.

Doping strategies for β-Ga2O3 based on high-throughput first-principles calculations

β-Ga2O3 is a promising material for advanced optoelectronic semiconductors due to its wide bandgap and high breakdown voltage. However, achieving efficient p-type doping remains a challenge. This investigation employs high-throughput (HT) first-principles calculations to explore doping effects in β-Ga2O3 systematically. The results of HT first-principles calculations indicate that changes in the Fermi levels (EF) can reflect the type of dopant elements. We systematically evaluated nine candidate dopants using GGA+U calculations. Through analysis of the (0/−1) transition levels, the ability to form shallow acceptors gradually decreases in the order of Zn, Mg, Cu, Hg, and Ag. Interestingly, due to the GGA+U optimization process considering electron correlation and localization effects, Mg-doped β-Ga2O3 exhibits an impurity level near the conduction band minimum (CBM), contributed by Mg2p and O2p orbitals. Mulliken population analysis reveals that Cu exhibits the highest charge density after doping compared to Hg, Zn, and Mg. Additionally, Ag-doped β-Ga2O3 shows potential for UV device applications within the 200 nm to 280 nm spectrum. The insights from this study delineate effective p-type doping strategies for β-Ga2O3, contributing to the advancement of optoelectronic device development involving semiconductors.

Improving TiB2 dispersion in Al-Si composites by interfacial projection: High-throughput first-principles calculations and experimental verification

The dispersion of reinforced particles is crucial in improving the mechanical properties of ceramic particles reinforced Al matrix composites. In this work, a novel interfacial projection strategy was proposed to improve the dispersion of TiB2 particles in Al-Si composites through high-throughput first-principles calculations with the experimental verification. Firstly, the Al(111)/TiB2(0001) interface model was constructed. Then, the pre-substitution of Si at 2 at. % concentration was employed to simulate the solutionized Al matrix. Secondly, alloying behaviors of 55 elements (10 substitution sites per element) in the Si-Al(111)/TiB2(0001) interface were studied by high-throughput first-principles calculations in terms of the relative interface formation energy and the relative work of adhesion. With these values, a theoretical alloying map for evaluating the dispersion ability of these alloying elements was plotted. Accordingly, the copper mold experiments were conducted to validate the theoretical alloying map. Based on the electron analysis, the enhanced interface bonds by alloying primarily attributed to electron accumulations around Si atom, indicating that the pre-substitution Si atom was vital for a reliable simulation result. Generally, this interfacial projection strategy provides a precise and potent approach in designing high-performance Al matrix composites, and should be applicable to other reinforced particles.

Pressure-Induced Re-Entrant Superconductivity in Transition Metal Dichalcogenide TiSe2.

Transition metal dichalcogenide TiSe2 exhibits a superconducting dome within a low pressure range of 2-4GPa, which peaks with the maximal transition temperature Tc of ≈1.8 K. Here it is reported that applying high pressure induces a new superconducting state in TiSe2, which starts at ≈16GPa with a substantially higher Tc that reaches 5.6 K at ≈21.5GPa with no sign of decline. Combining high-throughput first-principles structure search, X-ray diffraction, and Raman spectroscopy measurements up to 30GPa, It is found that TiSe2 undergoes a first-order structural transition from the 1T phase under ambient pressure to a new 4O phase under high pressure. Comparative ab initio calculations reveal that while the conventional phonon-mediated pairing mechanism may account for the superconductivity observed in 1T-TiSe2 under low pressure, the electron-phonon coupling of 4O-TiSe2 is too weak to induce a superconducting state whose transition temperature is as high as 5.6 K under high pressure. The new superconducting state found in pressurized TiSe2 requires further study on its underlying mechanism.

Accelerating ferroelectric materials discovery through high-throughput first-principles screening and experimental validation

We conducted high-throughput screening of ferroelectrics using first-principles calculations based on an existing crystal structure database. We focused on nonpolar structures with polar instability, to efficiently screen materials for their potential to undergo ferroelectric phase transitions from oxide materials in crystal structure databases. Our screening criteria included computational feasibility (excluding partial occupation), the absence of hazardous elements, and a maximum of 250 atoms in the conventional cell. Through this screening, we identified 47 ferroelectric candidates, 8 of which have already been reported as ferroelectrics. To validate our screening approach, we synthesized and evaluated several candidate materials with Dion–Jacobson-type structures, and measured their dielectric and ferroelectric properties. Although the ferroelectric behavior was not initially identified in these materials, our experiments confirmed their properties. Finally, we discovered a new ferroelectric material, CsCa2Nb3O10, which exhibited a ferroelectric phase transition at 28 K, clearly demonstrating the effectiveness of our screening strategy.

Automated design of hybrid halide perovskite monolayers for band gap engineering

The recent experimental confirmation of perovskite monolayers has sparked ongoing efforts in their prediction and synthesis, showcasing their flexible tunable band gap and potential in advanced functional devices. Although large-scale computational designs have been successfully performed for inorganic perovskite monolayers, the complexity introduced by organic cations hinders the same approaches applied to the hybrid halide perovskite monolayers. To address this challenge, we have proposed a high-throughput first-principles computational workflow that automates the design of hybrid halide perovskite monolayers. We strategically reduce the complexity of the configurations by analyzing the orientation of cations and the structural symmetry. Over 400 hybrid halide perovskite monolayers have been designed, and their structures and fundamental properties are stored in the database. Correlation analyses show a strong correlation between band gaps and metal-halogen-metal bond angles or metal-halogen bond lengths, consistent with prior studies for bulk and layered perovskites. The underlying physics that the band gap is modulated by the antibonding in the metal-halogen bond makes band gap engineering of hybrid halide perovskite monolayers feasible. Accordingly, initial research on lateral heterojunctions and solar cells has been conducted to explore the potential practical applications of the designed hybrid halide perovskite monolayers. Our study lays the foundation for further exploration of hybrid halide perovskite monolayers and highlights promising opportunities for their potential applications in electronic and optical devices.

Grain boundary engineering in Nickel-rich cathode: A combination of high-throughput first-principles and interpretable machine learning study

One of the primary challenges in commercializing nickel (Ni)-rich layered cathodes for lithium-ion batteries (LIBs) is addressing the problem of crack formation during cell cycling. These cracks quickly spread along grain boundaries (GBs), causing capacity and voltage degradation. GB engineering, a classical technique for strengthening materials that has been largely unexplored in LIBs, could potentially inhibit intergranular fractures and significantly extend battery life. In this study, we employed a synergistic approach that combined high-throughput first-principles calculations and an interpretable machine learning (ML) framework to assess the feasibility of enhancing GBs through segregation-induced strengthening via doping. As a result, we generated a comprehensive database containing 64 elements doped at 4 sites in ∑3 [100](012) GB of LiNiO2, representing the largest database for first-principle-aided GB engineering in LIBs to date. This database further enabled the implementation of an interpretable ML workflow to uncover the fundamental principles governing dopant segregation and GB strengthening. Based on the insights gained from this research, we provide practical and promising recommendations for dopant elements that can effectively anchor and reinforce GBs, such as Mg, Al, Si, Ti, Cr, Mn, Fe, Cu, Zn, Hf, and Ce, with some already demonstrated success in experiments. This work on GB engineering serves as a foundation for the development of advanced, doped cathode materials for next-generation batteries.

Discovery of atomic clock-like spin defects in simple oxides from first principles

Virtually noiseless due to the scarcity of spinful nuclei in the lattice, simple oxides hold promise as hosts of solid-state spin qubits. However, no suitable spin defect has yet been found in these systems. Using high-throughput first-principles calculations, we predict spin defects in calcium oxide with electronic properties remarkably similar to those of the NV center in diamond. These defects are charged complexes where a dopant atom — Sb, Bi, or I — occupies the volume vacated by adjacent cation and anion vacancies. The predicted zero phonon line shows that the Bi complex emits in the telecommunication range, and the computed many-body energy levels suggest a viable optical cycle required for qubit initialization. Notably, the high-spin nucleus of each dopant strongly couples to the electron spin, leading to many controllable quantum levels and the emergence of atomic clock-like transitions that are well protected from environmental noise. Specifically, the Hanh-echo coherence time increases beyond seconds at the clock-like transition in the defect with 209Bi. Our results pave the way to designing quantum states with long coherence times in simple oxides, making them attractive platforms for quantum technologies.

Effect of alloying elements on zinc-induced liquid metal embrittlement in steels: A first-principles study

Liquid metal embrittlement (LME) induced by Zn melt in galvanized steels during spot-welding poses a significant challenge to the advancement of the automotive industry. A critical strategy to address this challenge is identifying promising alloying elements capable of mitigating LME. High-throughput first-principles calculations were employed to investigate the segregation behavior of 22 common alloying elements at the Σ5(310) grain boundary of iron and their impact on the grain boundary energy. The results indicate that volume distortion upon doping of the alloying elements predominantly influences their segregation behavior, while the weak bonding between Zn and Fe is responsible for the grain boundary embrittlement. Exploration of solute interaction between Zn and the other alloying element in the Fe grain boundary model reveals that the attraction between metallic doping elements and Zn correlates with both the elastic effects and the magnetic properties of the dopant, while the repulsion between non-metallic elements and Zn is primarily governed by the elastic effects. Separating the grain boundary strengthening energy into mechanical and chemical contributions shows that they correlate linearly with variations in volume of the doping site and changes in bond energy for bonds associated with the doping site at the grain boundary, respectively. Accordingly, the strengthening effect of the doping elements can be estimated by evaluating the induced changes in local volume and bond energies on grain boundaries. Furthermore, potential alloying elements to mitigate the Zn-induced LME are screened and discussed, with B and Mo being the most promising candidates.

Anisotropic materials with abnormal Poisson's ratios and acoustic velocities.

Isotropic materials are required to adhere to various mechanical principles due to their limited thermal stability. For instance, it is essential for Poisson's ratio to be within the range of -1 to 0.5, and the longitudinal wave velocity must exceed the transverse wave velocity. Nevertheless, perfect crystals, as anisotropic materials, have the ability to defy conventional rules. Through the integration of high-throughput processes and first-principles calculations, a comprehensive exploration of known materials was conducted, resulting in the establishment of a database featuring an extreme anisotropic mechanism. This included the identification of abnormal Poisson's ratios (with the directional Poisson's ratio ranging from -3.00 to 3.67), the discovery of extreme negative linear compressibility, the determination of the upper and lower limits of the sound velocity, and other associated properties. Several materials with abnormal Poisson's ratios (<-1 or >0.5) were listed, and their peculiar mechanical behavior, wherein the volume decreased counterintuitively with uniaxial tension, was discussed. Finally, this study focused on the velocities of longitudinal and transverse waves, with specific emphasis on materials exhibiting transverse wave velocities that exceeded the longitudinal wave velocities.

A substitutional quantum defect in WS2 discovered by high-throughput computational screening and fabricated by site-selective STM manipulation

Point defects in two-dimensional materials are of key interest for quantum information science. However, the parameter space of possible defects is immense, making the identification of high-performance quantum defects very challenging. Here, we perform high-throughput (HT) first-principles computational screening to search for promising quantum defects within WS2, which present localized levels in the band gap that can lead to bright optical transitions in the visible or telecom regime. Our computed database spans more than 700 charged defects formed through substitution on the tungsten or sulfur site. We found that sulfur substitutions enable the most promising quantum defects. We computationally identify the neutral cobalt substitution to sulfur (CoS0\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${}_{{{{{{{{\\rm{S}}}}}}}}}^{0}$$\\end{document}) and fabricate it with scanning tunneling microscopy (STM). The CoS0\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${}_{{{{{{{{\\rm{S}}}}}}}}}^{0}$$\\end{document} electronic structure measured by STM agrees with first principles and showcases an attractive quantum defect. Our work shows how HT computational screening and nanoscale synthesis routes can be combined to design promising quantum defects.

Theoretical Study of the Competition Mechanism of Alloying Elements in L12-(Nix1Crx2Cox3)3Al Precipitates

The impact of variations in the content of single alloying element on the properties of alloy materials has been extensively discussed, but the influence of this change on the content of multiple alloying elements in the alloy materials has been disregarded, as the performances of alloy materials should be determined by the collective influence of multiple alloying elements. To address the aforementioned issue, the present study conducted a comprehensive investigation into the impact of variations in the content of alloying elements, namely Ni, Cr, and Co, on the structural and mechanical properties of L12-(Nix1Crx2Cox3)3Al precipitates using the high-throughput first-principles calculations and the partial least squares (PLS) regression, and the competitive mechanism among these three elements was elucidated. The findings demonstrate that the same alloying element may exhibit opposite effects in both single element analysis and comprehensive multi-element analysis, for example, the effect of Ni element on elastic constant C11, and the influence of Cr element on Vickers hardness and yield strength. The reason for this is that the impact of the content of other two alloying elements is ignored in the single element analysis. Meanwhile, the Co element demonstrates a significant competitive advantage in the comparative analysis of three alloying elements for different physical properties. Therefore, the methodology proposed in this study will facilitate the elucidation of competition mechanisms among different alloy elements and offer a more robust guidance for experimental preparation.

High-throughput first-principles study on the effect of Ni segregation on the formation of Cr-depleted zone and corrosion resistance of S32205 duplex stainless steels

Recent studies have found that in the absence of Cr carbide precipitation, co-segregation of Cr and other elements at the interface between α-Fe and γ-Fe can also lead to the formation of Cr-depleted zones, leading to intergranular corrosion. The study employed three-dimensional atomic probes, focused ion beams, and high-throughput first-principles calculation techniques to investigate the impact of Ni atoms on the α-Fe/γ-Fe interface of UNS S32205 duplex stainless steels. The goal was to analyze the formation of Cr-depleted zones and interface corrosion resistance. The results indicate that both Ni and Cr atoms are segregated at the interface between α-Fe and γ-Fe phases; The strong interaction between Ni and Cr atoms hinders Cr segregation at the interface and slows down the formation of Cr-depleted zones; co-segregation of Ni and Cr can improve the stability of the α-Fe/γ-Fe phase interface, reduce the generation of microcracks, and reduce the stability of Cl atom adsorption in the cracks. This establishes the theoretical basis for further suppressing the formation of Cr-depleted zones and preventing intergranular corrosion.

Band Alignment of Oxides by Learnable Structural-Descriptor-Aided Neural Network and Transfer Learning.

The band alignment of semiconductors, insulators, and dielectrics is relevant to diverse material properties and device structures utilizing their surfaces and interfaces. In particular, the ionization potential and electron affinity are fundamental quantities that describe surface-dependent band-edge positions with respect to the vacuum level. Their accurate and systematic determination, however, demands elaborate experiments or simulations for well-characterized surfaces. Here, we report machine learning for the band alignment of nonmetallic oxides using a high-throughput first-principles calculation data set containing about 3000 oxide surfaces. Our neural network accurately predicts the band positions for relaxed surfaces of binary oxides simply by using the information on bulk structures and surface termination planes. Moreover, we extend the model to naturally include multiple-cation effects and transfer it to ternary oxides. The present approach enables the band alignment of a vast number of solid surfaces, thereby opening the way to a systematic understanding and materials screening.

Chemical-substitution-driven giant anomalous Hall and Nernst effects in magnetic cubic Heusler compounds

Chemical substitution efficiently optimizes the physical properties of Heusler compounds, especially their anomalous transport properties, including anomalous Hall conductivity (AHC) and anomalous Nernst conductivity (ANC). This study systematically investigates the effect of chemical substitution on AHC and ANC in 1493 magnetic cubic Heusler compounds using high-throughput first-principles calculations. Notable trends emerge in Co- and Rh-based compounds, where chemical substitution effectively enhances the AHC and ANC. Intriguingly, certain chemically substituted candidates exhibit outstanding enhancement in AHCs and ANCs, such as (Co0.8Ni0.2)2FeSn with considerable AHC and ANC values of −2567.78 Scm−1 and 8.27 Am−1K−1, respectively, and (Rh0.8Ru0.2)2MnIn with an AHC of 1950.49 Scm−1. In particular, an extraordinary ANC of 8.57 Am−1K−1 is identified exclusively in Rh2Co0.7Fe0.3In, nearly double the maximum value of 4.36 Am−1K−1 observed in the stoichiometric Rh2CoIn. A comprehensive band structure analysis underscores that the notable enhancement in ANC arises from the creation and modification of the energy-dependent nodal lines through chemical substitution. This mechanism generates a robust Berry curvature, resulting in significant ANCs. These findings emphasize the pivotal role of chemical substitution in engineering high-performance materials, thereby expanding the horizons of transport property optimization within Heusler compounds.

Tuning the Surface Stability and Li/Na Storage of MXenes by Controlling the Surface Termination Coverage.

2D transition metal carbides and/or nitrides, MXenes, are a class of widely studied materials with great potential for energy storage applications. The control of surface chemistry is an effective approach for preparing novel MXenes and modifying their electrochemical properties. However, an in-depth and systematic atomic-scale study of the effect of surface termination on MXene stability and electrochemical performance is scarce and thus is highly desired. Here, through high-throughput first-principles calculations, 28 stable chalcogen-functionalized M2CTz (M = V, Nb, and Ta, T = S, Se, and Te) under different chemical environments are identified. The reduction of termination coverage improves electrical conductivity but weakens in-plane stiffness. Intriguingly, based on charge transfer mechanism, the diffusion barrier of lithium/sodium atoms on the M2CTz exhibits a volcano-like relationship with termination coverage, and the ion diffusion channel formed in half termination coverage greatly accelerates lithium ion diffusion and returns to or exceeds sodium ion diffusion rate at full termination coverage. V2CSe2/Nb2CSz not only displays the large lithium/sodium capacity (592/409-466 mAhg-1) but also exhibits low barrier energy and open-circuit voltage, suggesting a promising candidate anode material for lithium/sodium-ion batteries. These findings provide insights into the design and fabrication of MXenes and tuning the electrochemical performance of MXenes by controlling termination coverage.

Tunable magnetic anisotropy of Os-Ru dimer on 2D transition metal chalcogenides substrates

The precise manipulation of atoms enables the creation of distinct materials from the bottom up to construct devices with breakthrough performance, especially in the field of quantum technologies. A large magnetic anisotropy energy (MAE) is important to realize bit storage of information in magnetic memory devices. As the smallest magnetic nanostructure, substrate-supported transition metal dimers are potential atomic-scale storage medium to obtain large MAEs. Using high-throughput first-principles calculations, we have performed a systematic investigation of the MAE of 76 heterodimensional systems consisting of zero-dimensional Os-Ru dimer and experimentally synthesized two-dimensional transition metal dichalcogenides (TMDs). Huge MAEs in the range of 102.09–247.69 meV were found in 13 of these heterodimensional systems. In particular, the Os-Ru@T-ZrSe2 with the largest MAE of 247.69 meV corresponds to a theoretical blocking temperature (67 K) in terms of a relaxation time of 10 years and a storage density of 281 Tb·inch−2. The underlying mechanism for the significant enhancement of MAE is attributed to the rearrangement of the in-plane molecular orbitals near the Fermi level, which is closed relative to the electron transfer capability between the Os-Ru dimer and the TMD substrates. In addition, we have also constructed a heat map for TMD-supported Os-Ru dimer, showing the degree of correlation between MAEs and feature descriptors. Our work not only suggests an effective way to improve MAE of transition metal dimers but also extracts relatively simple rules for substrate selection.

Lead-Free Double Perovskites: A Review of the Structural, Optoelectronic, Mechanical, and Thermoelectric Properties Derived from First-Principles Calculations, and Materials Design Applicable for Pedagogical Purposes

Metal halide perovskite materials have shown significant advancements in their application as light absorbers in perovskite solar cells, with power conversion efficiencies reaching 27%. However, lead-based perovskites pose a concern due to their toxicity and stability issues in moisture, UV radiation, and heat. This has led to a pressing need to explore substitute materials that do not contain lead but maintain the remarkable characteristics of lead-based perovskites. This review article focuses on halide double perovskites characterised by the A2B’B”X6 composition, highlighting their structural, optical, thermoelectric, and mechanical capabilities. Additionally, the review evaluates several materials databases to investigate materials suitable for high-throughput first-principles calculations integrated inside density functional theory. The review aims to identify novel perovskite materials, offer a thorough evaluation of the potential benefits and drawbacks associated with this class of materials, and, from the pedagogical standpoint, discover effective instructional frameworks.

Superalkali halide perovskites with suitable direct band gaps for photovoltaic applications.

The construction of superalkali halide perovskites has attracted attention for the development of new photovoltaic materials, but stable superalkalis have not been found until now. Herein, to construct new three-dimensional superalkali halide perovskites with a MI3 frame (M = Sn and Pb), a new Li(H2O)3+ superalkali cation is designed and selected based on low vertical ionization potential, suitable tolerance factor, small ionic radius and large dissociation energy. High-throughput first-principles calculations show that superalkalis with lower vertical ionization potentials exhibit stronger interactions with the MI3 frame. The normal and cubic Li(H2O)3MI3 perovskites and cubic Li(H2O)4PbI3 perovskites have direct band gaps, s-p and p-p electron transitions, effective carrier masses of less than 0.45me and exciton binding energies of less than 291 meV. Moreover, the cubic Li(H2O)3PbI3 perovskite with a direct band gap of 1.40 eV can in theory show a power conversion efficiency of 33.49%. These results strongly suggest that superalkali cations with large dissociation energy can be used to develop stable superalkali perovskites for photovoltaic applications.