Unraveling the Emerging Photocatalytic, Thermoelectric, and Topological Properties of Intercalated Architecture MZX (M = Ga and In; Z = Si, Ge and Sn; X = S, Se, and Te) Monolayers.

The continuous advancements in studying two-dimensional (2D) materials pave the way for groundbreaking innovations across various industries. In this study, by employing density functional theory calculations, we comprehensively elucidate the electronic structures of MZX (M = Ga and In; Z = Si, Ge, and Sn; X = S, Se, and Te) monolayers for their applications in photocatalytic, thermoelectric, and spintronic fields. Interestingly, GaSiS, GaSiSe, InSiS, and InSiSe monolayers are identified to be efficient photocatalysts for overall water splitting with band gaps close to 2.0 eV, suitable band edge positions, and excellent optical harvest ability. In addition, the InSiTe monolayer exhibits a ZT value of 1.87 at 700 K, making it highly appealing for applications in thermoelectric devices. It is further highlighted that GaSnTe, InSnS, and InSnSe monolayers are predicted to be 2D topological insulators (TIs) with bulk band gaps of 115, 54, and 152 meV, respectively. Current research expands the family of 2D GaGeTe materials and establishes a path toward the practical utilization of MZX monolayers in energy conversion and spintronic devices.

Promising M2CO2/MoX2 (M = Hf, Zr; X = S, Se, Te) Heterostructures for Multifunctional Solar Energy Applications.

Two-dimensional van der Waals (vdW) heterostructures are potential candidates for clean energy conversion materials to address the global energy crisis and environmental issues. In this work, we have comprehensively studied the geometrical, electronic, and optical properties of M2CO2/MoX2 (M = Hf, Zr; X = S, Se, Te) vdW heterostructures, as well as their applications in the fields of photocatalytic and photovoltaic using density functional theory calculations. The lattice dynamic and thermal stabilities of designed M2CO2/MoX2 heterostructures are confirmed. Interestingly, all the M2CO2/MoX2 heterostructures exhibit intrinsic type-II band structure features, which effectively inhibit the electron-hole pair recombination and enhance the photocatalytic performance. Furthermore, the internal built-in electric field and high anisotropic carrier mobility can separate the photo-generated carriers efficiently. It is noted that M2CO2/MoX2 heterostructures exhibit suitable band gaps in comparison to the M2CO2 and MoX2 monolayers, which enhance the optical-harvesting abilities in the visible and ultraviolet light zones. Zr2CO2/MoSe2 and Hf2CO2/MoSe2 heterostructures possess suitable band edge positions to provide the competent driving force for water splitting as photocatalysts. In addition, Hf2CO2/MoS2 and Zr2CO2/MoS2 heterostructures deliver a power conversion efficiency of 19.75% and 17.13% for solar cell applications, respectively. These results pave the way for exploring efficient MXenes/TMDCs vdW heterostructures as photocatalytic and photovoltaic materials.

Out-of-plane polarization modulated band alignments inß-In2X3/α-In2X3(X = S and Se) vdW heterostructures.

The construction of two-dimensional (2D) van der Waals (vdW) heterostructures is an effective strategy to overcome the intrinsic disadvantages of individual 2D materials. Herein, by employing first-principles calculations, the electronic structures and potential applications in the photovoltaic field of theß-In2X3/α-In2X3(X = S and Se) vdW heterostructures have been systematically unraveled. Interestingly, the band alignments ofß-In2S3/α-In2S3,ß-In2Se3/α-In2Se3, andß-In2Se3/α-In2S3heterostructures can be transformed from type-I to type-II by switching the polarization direction ofα-In2X3layers. It is highlighted that the light-harvesting ability of theß-In2X3/α-In2X3vdW heterostructures is significantly higher than the corresponding monolayers in nearly the entire visible light region. Interestingly, type-IIß-In2S3/α-In2Se3↓ heterostructure can achieve the power conversion efficiency of 17.9%, where theα-In2Se3layer acts as a donor and theß-In2S3layer displays as the acceptor. The present research not only provides an in-depth understanding that the out-of-plane polarization ofα-In2X3monolayers can efficiently modulate the band edge alignment of theß-In2X3/α-In2X3vdW heterostructures, but also paves the way for the application of these heterostructures in the field of photovoltaics and optoelectronics.

Deciphering the roles of ammonium doping for lead-free (NH4)xCs3-xCu2I5 perovskites to regulate the photoelectronic properties.

Inorganic ammonium (NH4+) is the simplest amine cation with perfect symmetry, the smallest radius and many H atoms, allowing itself to be used as a potential dopant in achieving high-quality perovskite materials. As a composition-modulation strategy, NH4+-doped (NH4)xCs3-xCu2I5 (0 < x < 1.5) lead-free perovskites were successfully synthesized via the eco-friendly ball milling method in this work. As the ammonium content increases, the lattice constants of (NH4)xCs3-xCu2I5 shrink and the grain sizes increase. The doping of NH4+ effectively passivates the lattice defects, suppresses the non-radiative recombination and tunes the energy band structure, resulting in better fluorescence properties. UV-pumped deep-blue LEDs based on (NH4)xCs3-xCu2I5 phosphors were fabricated, which showed improved performance and tunable emission. These results demonstrate the potential of the NH4+-doping strategy for improving the performance of lead-free perovskite optoelectronics.