Recent progress in the design of IR nonlinear optical materials by partial chemical substitution: Structural evolution and performance optimization

The fabrication of heterojunctions is an intriguing approach to boost the reactivity of catalysts. However, facile preparation of desirable heterojunction materials remains a challenge. Here, novel CoPS3/CoS2 heterojunctions are created by an intuitive phosphatization process on the basis of structurally flexible cobalt sulfide precursors. Significant stress effect exists at these heterogeneous interfaces, resulting in lattice distortions and the exposure of more active sites. The interface interaction also modifies the catalyst's electronic structure to improve its electrical conductivity and hydrogen adsorption capabilities. Notably, the overpotential of the CoPS3/CoS2 heterojunction for electrocatalytic hydrogen evolution reaction is just 36.3 mV, which is far superior to those of single‐component catalysts and competitive with comparable catalysts reported. This work not only offers an innovative electrocatalyst but also a strategy that can be used to create heterojunctions based on related transition metal thiophosphates.

Interfacial Engineering of Cobalt Thiophosphate with Strain Effect and Modulated Electron Structure for Boosting Electrocatalytic Hydrogen Evolution Reaction

Oxychalcogenides capable of exhibiting excellent balance among large second‐harmonic generation (SHG) response, wide band gap (Eg), and suitable birefringence (Δn) are ideal materials class for infrared nonlinear optical (IR NLO) crystals. However, rationally designing a new high‐performance oxychalcogenide IR NLO crystal still faces a huge challenge because it requires the optimal orientations of the heteroanionic groups in oxychalcogenide. Herein, a series of antiperovskite‐type oxychalcogenides, Ae3Q[GeOQ3] (Ae = Ba, Sr; Q = S, Se), which were synthesized by employing the antiperovskite‐type Ba3S[GeS4] as the structure template. Their structures feature novel three‐dimensinoal frameworks constructed by distorted [QAe6] octahedra, which are further filled by [GeOQ3] tetrahedra to form antiperovskite‐type structures. Based on the unique antiperovskite‐type structures, the favorable alignment of the polarizable [GeOQ3] tetrahedra and distorted [QAe6] octahedra have been achieved. These contribute the ideal combination of large SHG response (0.7–1.5 times that of AgGaS2), wide Eg (3.52–4.10 eV), and appropriate Δn (0.017–0.035) in Ae3Q[GeOQ3]. Theoretical calculations and crystal structure analyses revealed that the strong SHG and wide Eg could be attributed to the polarizable [GeOQ3] tetrahedra and distorted [QAe6] octahedra. This research provides a new exemplification for the design of high‐performance IR NLO materials.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202204755

The Antiperovskite‐Type Oxychalcogenides Ae3Q[GeOQ3] (Ae = Ba, Sr; Q = S, Se) with Large Second Harmonic Generation Responses and Wide Band Gaps

Ag-based chalcogenides and derivatives as promising infrared nonlinear optical materials

Inorganic chalcogenides have been studied as the most promising infrared (IR) nonlinear optical (NLO) candidates for the past decades. However, it is proven difficult to discover high-performance materials that combine the often-incompatible properties of large energy gap (Eg ) and strong second harmonic generation (SHG) response (deff ), especially for rare-earth chalcogenides. Herein, centrosymmetric Cs3 [Sb3 O6 ][Ge2 O7 ] is selected as a maternal structure and a new noncentrosymmetric rare-earth oxychalcogenide, namely, Nd3 [Ga3 O3 S3 ][Ge2 O7 ], is successfully designed and obtained by the module substitution strategy for the first time. Especially, Nd3 [Ga3 O3 S3 ][Ge2 O7 ] is the first case of breaking the trade-off relationship between wide Eg (>3.5 eV) and large deff (>0.5 × AgGaS2 ) in rare-earth chalcogenide system, and thus displays an outstanding IR-NLO comprehensive performance. Detailed structure analyses and theoretical studies reveal that the NLO effect originates mainly from the cooperation of heteroanionic [GaO2 S2 ] and [NdO2 S6 ] asymmetric building blocks. This work not only presents an excellent rare-earth IR-NLO candidate, but also plays a crucial role in the rational structure design of other NLO materials in which both large Eg and strong deff are pursued.

Rational Design of a Rare-Earth Oxychalcogenide Nd3 [Ga3 O3 S3 ][Ge2 O7 ] with Superior Infrared Nonlinear Optical Performance.

The achievement of balanced performance with a strong second-harmonic generation (SHG) response, proper birefringence, and wide band gap concurrently is a crucial but challenging task in infrared nonlinear optical (IR-NLO) crystals. Here, we theoretically confirmed that the heteroanionic oxysulfide tetrahedron would produce improved polarizability anisotropy and quadratic hyperpolarizability compared with the monoanionic oxide or sulfide tetrahedra. When this anion-mixing strategy was applied, melilite oxysulfide with the four representative members A2GeGa2OS6 (A = Ca, Sr) and Sr2MGe2OS6 (M = Zn, Cd) was successfully discovered as a promising IR-NLO material system. Remarkably, compared with the monoanionic melilite oxides, these compounds exhibited unbiased performances of proper birefringences (0.106-0.143), strong SHG responses (>10× melilite oxide Ba2CdGe2O7, 1.3-2.1× AgGaS2 (AGS) @1570 nm) with phase-matchable ability, wide band gaps (2.95-3.15 eV), and large laser-induced damage thresholds (LIDTs, 5.6-13.4× AGS). The high structure tolerance of melilite offers a great possibility to improve the SHG response via tuning the orbital composition and hybridization near band edges. This work provides an effective approach for the design of high-performance IR-NLO materials.

Heteroanionic Melilite Oxysulfide: A Promising Infrared Nonlinear Optical Candidate with a Strong Second-Harmonic Generation Response, Sufficient Birefringence, and Wide Bandgap.

Two-dimensional (2D) materials catalysts provide an atomic scale view on fascinating arena for understanding the mechanism of electrocatalytic carbon dioxide reduction (CO2 ECR). Here, we successfully exfoliated both layered and nonlayered ultra-thin metal phosphorous trichalcogenides (MPCh3) nanosheets via wet grinding exfoliation (WGE), and systematically investigated the mechanism of MPCh3 as catalysts for CO2 ECR. Unlike the layered CoPS3 and NiPS3 nanosheets, the active Sn atoms tend to be exposed on the surfaces of nonlayered SnPS3 nanosheets. Correspondingly, the nonlayered SnPS3 nanosheets exhibit clearly improved catalytic activity, showing formic acid selectivity up to 31.6% with -7.51 mA cm-2 at -0.65 V vs. RHE. The enhanced catalytic performance can be attributed to the formation of HCOO* via the first proton-electron pair addition on the SnPS3 surface. These results provide a new avenue to understand novel CO2 ECR mechanism of Sn-based and MPCh3-based catalysts.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/anie.202217253

Exfoliated 2D Layered and Nonlayered Metal Phosphorous Trichalcogenides Nanosheets as Promising Electrocatalysts for CO2 Reduction.

A new noncentrosymmetric (NCS) quaternary sulfide, SrAgAsS4, was obtained via the strategy of aliovalent substitution based on centrosymmetric (CS) SrGa2S4. The new compound features two-dimensional [AgAsS4]2- layers, which are composed of alternately connected [AsS4] tetrahedra and [AgS4] tetrahedra. Importantly, SrAgAsS4 exhibits a strong phase-matched second-harmonic generation response (1.35 × AgGaS2 at 2100 nm) and has a suitable birefringence (0.15@2100 nm) and moderate band gap (2.31 eV). The first-principles calculations revealed the significant contribution of [AsS4] and [AgS4] tetrahedra to its optical properties. This work will promote the application of the aliovalent substitution strategy in the design of NCS-structure-based functional materials.

SrAgAsS4: A Noncentrosymmetric Sulfide with Good Infrared Nonlinear Optical Performance Induced by Aliovalent Substitution from Centrosymmetric SrGa2S4.

Chalcogenides, which refer to chalcogen anions, have attracted considerable attention in multiple fields of applications, such as optoelectronics, thermoelectrics, transparent contacts, and thin film transistors. In comparison to oxide counterparts, chalcogenides have demonstrated higher mobility and \textit{p}-type dopability, owing to larger orbital overlaps between metal-X covalent chemical bondings and higher-energy valence bands derived by p-orbitals. Despite the potential of chalcogenides, the number of successfully synthesized compounds remains relatively low compared to oxides, suggesting the presence of numerous unexplored chalcogenides with fascinating physical characteristics. In this study, we implemented a systematic high-throughput screening process combined with first-principles calculations on ternary chalcogenides using 34 crystal structure prototypes. We generated a computational material database containing over 400,000 compounds by exploiting the ion-substitution approach at different atomic sites with elements in the periodic table. The thermodynamic stabilities of the candidates were validated using the chalcogenides included in the Open Quantum Materials Database. Moreover, we trained a model based on Crystal Graph Convolutional Neural Networks to predict the thermodynamic stability of novel materials. Furthermore, we theoretically evaluated the electronic structures of the stable candidates using accurate hybrid functionals. A series of in-depth characteristics, including the carrier effective masses, electronic configuration, and photovoltaic conversion efficiency, was also investigated. Our work provides useful guidance for further experimental research in the synthesis and characterization of such chalcogenides as promising candidates, as well as charting the stability and optoelectronic performance of ternary chalcogenides.

Accelerated Screening of Ternary Chalcogenides for High-Performance Optoelectronic Materials

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Papers

Heteroanionic Melilite Oxysulfide: A Promising Infrared Nonlinear Optical Candidate with a Strong Second-Harmonic Generation Response, Sufficient Birefringence, and Wide Bandgap.

Exfoliated 2D Layered and Nonlayered Metal Phosphorous Trichalcogenides Nanosheets as Promising Electrocatalysts for CO2 Reduction.

SrAgAsS4: A Noncentrosymmetric Sulfide with Good Infrared Nonlinear Optical Performance Induced by Aliovalent Substitution from Centrosymmetric SrGa2S4.

Accelerated Screening of Ternary Chalcogenides for High-Performance Optoelectronic Materials