Wafer-scale heterogeneous integration of self-powered lead-free metal halide UV photodetectors with ultrahigh stability and homogeneity

Recently, the newly-emerging lead-free metal-halide materials with less toxicity and superior optoelectronic properties have received wide attention as the safer and potentially more robust alternatives to lead-based perovskite counterparts. Among them, ternary copper halides (TCHs) have become a vital group due to their unique features, including abundant structural diversity, ease of synthesis, unprecedented optoelectronic properties, high abundance, and low cost. Although the recent efforts in this field have made certain progresses, some scientific and technological issues still remain unresolved. Herein, a comprehensive and up-to-date overview of recent progress on the fundamental characteristics of TCH materials and their versatile applications is presented, which contains topics such as: i) crystal and electronic structure features and synthesis strategies; ii) mechanisms of self-trapped excitons, luminescence regulation, and environmental stability; and iii) their burgeoning optoelectronic devices of phosphor-converted white light-emitting diodes (WLEDs), electroluminescent LEDs, anti-counterfeiting, X-ray scintillators, photodetectors, sensors, and memristors. Finally, the current challenges together with future perspectives on the development of TCH materials and applications are also critically described, which is considered to be critical for accelerating the commercialization of these rapidly evolving technologies. This article is protected by copyright. All rights reserved.

Recent Advances and Opportunities of Eco-Friendly Ternary Copper Halides: A New Superstar in Optoelectronic Applications.

The hexagonal phase of $\mathrm{AgBiS}{\mathrm{e}}_{2}$ has been discovered as a promising thermoelectric material for room-temperature applications. However, its basic conduction type is still ambiguous, and its current ZT value is pretty low. To improve the thermoelectric performance of $\mathrm{AgBiS}{\mathrm{e}}_{2}$, we apply band engineering to modify its band structure by introducing defects to increase the band degeneracy. From the calculated intrinsic point defect formation energies of $\mathrm{AgBiS}{\mathrm{e}}_{2}$ at different growth conditions, we clarify that the conducting behavior of $\mathrm{AgBiS}{\mathrm{e}}_{2}$ is a $p$-type semiconductor, and the Ag vacancy is the dominated acceptor. Based on scrutinizing the band structure of $\mathrm{AgBiS}{\mathrm{e}}_{2}$, two kinds of methodologies can be used to modify its band structure to achieve high band degeneracy: (i) shifting the Fermi level into the valence band using intrinsic defects, and (ii) converging several valence-band maxima by introducing extrinsic defects. We find that the intrinsic Ag vacancy is helpful to significantly increase the power factor, leading to a large ZT for Ag vacancy-doped $\mathrm{AgBiS}{\mathrm{e}}_{2}$: the maximum ZT value is increased to 0.3--0.5 at near room temperature. Based on analyzing the bonding characters and atomic energy levels in the compound, we predict several extrinsic dopants (Cu, Rh, and Pd) that can be used to converge three valence-band maxima. Our work provides methodologies to improve the room-temperature thermoelectric applications of $\mathrm{AgBiS}{\mathrm{e}}_{2}$ by tuning its band structures using intrinsic or extrinsic defects.

https://link.aps.org/accepted/10.1103/PhysRevB.99.155203

Thermoelectric optimization of AgBiS e 2 by defect engineering for room-temperature applications

Ultraviolet (UV) photodetectors, directly converting photons in the UV range into electrical signals, have been widely applied in areas such as life sciences, environmental monitoring, and aerospace. Environment-friendly all-inorganic lead-free perovskites with wide-bandgap (≥ 3.1 eV) are widely recognized for efficient absorption of the UV light and excellent optoelectronic properties and stability, rendering them ideal candidate materials for UV photodetectors. The aim of this review is to provide a comprehensive summary of the recent progress made on wide-bandgap all-inorganic lead-free perovskite UV photodetectors. According to the type of perovskite, UV photodetectors based on wide-bandgap all-inorganic lead-free perovskites are divided into three categories: oxide perovskite devices, halide double perovskite devices, and halide perovskite derivative devices. The advantages and challenges of wide-bandgap all-inorganic lead-free perovskite UV photodetectors are illustrated, and prospects of future research and promising breakthrough in applications are outlooked. This review tends to inspire the design of the new generation of UV photodetector and triggers new ideas on the development of perovskite materials in the field of UV detection. 

Wide-bandgap All-inorganic Lead-free Perovskites for Ultraviolet Photodetectors

Despite the fact that research into most high-performance thermoelectric (TE) materials is focused on tellurides, compelling demand has arisen to replace tellurium (Te) with selenium (Se) due to the scarcity of Te. Silver bismuth diselenide (AgBiSe2, ABS) has been widely studied in relation to thermoelectric applications due to its intrinsically low thermal conductivity. However, its low power factor (PF) has been considered as an underlying issue preventing improvements of the TE properties of ABS. Here, it is demonstrated that a high PF can be achieved by incorporating Cu into the ABS system via the nestification of conduction bands when a disordering between Ag and Bi occurs. Degenerate electronic bands simultaneously increase the density-of-states effective mass and carrier concentration while not reducing the carrier mobility significantly. Therefore, improved TE performance with a maximum PF of 8.2 μW cm−1 K−2 and a peak zT value of 1.14 was achieved at 773 K, opening a new horizon for the development of environmentally benign TE materials with high performance capabilities.

Order-disorder transition-induced band nestification in AgBiSe2–CuBiSe2 solid solutions for superior thermoelectric performance

Polarization-sensitive photodetectors are the core of optics applications and have been successfully demonstrated in photodetectors based on the newly-emerging metal-halide perovskites. However, achieving high polarization sensitivity is still extremely challenging. In addition, most of the previously reported photodetectors were concentrated on 1D lead-halide perovskites and 2D asymmetric intrinsic structure materials, but suffered from being external bias driven, lead-toxicity, poor stability and complex processes, severely limiting their practical applications. Here, we demonstrate a high-performance polarization-sensitive and stable polarization-sensitive UV photodetector based on a dendritic crystal lead-free metal-halide CsCu2I3/GaN heterostructure. By combining the anisotropic morphology and asymmetric intrinsic structure of CsCu2I3 dendrites with the isotropic material GaN film, a high specific surface area and built-in electric field are achieved, exhibiting an ultra-high polarization selectivity up to 28.7 and 102.8 under self-driving mode and -3 V bias, respectively. To our knowledge, such a high polarization selectivity has exceeded those of all of the reported perovskite-based devices, and is comparable to, or even superior to, those of the conventional 2D heterostructure materials. Interestingly, the unsealed device shows outstanding stability, and can be stored for over 2 months, and effectively maintained the performance even after repeated heating (373K)-cooling (300K) for different periods of time in ambient air, indicating a remarkable temperature tolerance and desired compatibility for applications under harsh conditions. Such excellent performance and simple method strongly show that the CsCu2I3/GaN heterojunction photodetector has great potential in practical applications with high polarization-sensitivity. This work provides a new insight into designing novel high-performance polarization-sensitive optoelectronic devices.

A high-performance polarization-sensitive and stable self-powered UV photodetector based on a dendritic crystal lead-free metal-halide CsCu2I3/GaN heterostructure.

AgBiSe2 and AgSbSe2, two typical examples of Te-free I–V–VI2 chalcogenides, are drawing much attention due to their promising thermoelectric performance Both compounds were synthesized via melting and consolidated by spark plasma sintering The role of annealing on the transport properties of polymorphous AgBiSe2 and monophase AgSbSe2 was studied Annealing has a greater impact on AgBiSe2 than AgSbSe2, which is ascribed to the temperature dependent phase transition of AgBiSe2 Unannealed AgBiSe2 shows p–n switching, but annealed AgBiSe2 exhibits n-type semiconducting behavior over the whole measurement temperature range By performing high-temperature Hall measurements, we attribute this intriguing variation to the change in the amount of Ag vacancies and mid-temperature rhombohedral phase after annealing Both AgBiSe2 and AgSbSe2 exhibit low thermal conductivity values, which are ∼040–050 W m−1 K−1 for AgSbSe2 and ∼045–070 W m−1 K−1 for AgBiSe2, respectively The maximum ZT value of AgBiSe2 is enhanced from 018 to 021 after annealing Pristine AgSbSe2 presents a ZT value as high as 060 at 623 K, although slight deterioration emerges after annealing

/pdf/comparing-the-role-of-annealing-on-the-transport-properties-45e8jaznfk.pdf

Comparing the role of annealing on the transport properties of polymorphous AgBiSe2 and monophase AgSbSe2

High-Performance Self-Driven Single GaN-Based p–i–n Homojunction One-Dimensional Microwire Ultraviolet Photodetectors

Realization of Specific Localized Surface Plasmon Resonance in Au-Modified Ni Nanoplasmonics for Efficient Detection

High-Performance Self-Driven Single Gan-Based P-I-N Homojunction One-Dimensional Microwire Ultraviolet Photodetector

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