High-Entropy Halide Perovskite Crystals via Mild-Temperature Self-Assembly
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Solution Overview
Problem
High-entropy materials require extreme temperatures and complex processing techniques for synthesis, making it challenging to form single-phase crystalline solid solutions and scale up production for large-scale applications, with unpredictable outcomes even under these conditions.
Innovation Solution
A room-temperature-solution and low-temperature-solution synthesis process is developed for high-entropy semiconductor single crystals using halide-based perovskites, leveraging self-assembly of stabilized complexes in multi-element inks to form Cs2MCl6 vacancy-ordered double perovskite structures with near-equimolar metal cations, allowing for the creation of high-entropy materials with soft, easily reconfigurable lattices.
Engineering Contradictions & Design Principles
Engineering Contradiction Analysis
1Manufacturing precision
If extreme temperature synthetic procedures (over 1,000°C) and complex processing techniques (hot rolling) are used, then single-phase crystalline solid solutions can be formed, but the stability of other materials in device architecture is compromised and energy consumption increases
Solution Approach 1:
The invention fundamentally changes the synthesis temperature parameter from extreme temperatures (>1,000°C) to mild temperatures (room temperature to 80°C). This parameter change enables the formation of high-entropy perovskite single crystals without compromising the stability of other device materials, as the mild conditions are compatible with standard device architecture components.
Solution Approach 2:
The invention replaces mechanical processing techniques (hot rolling) with solution-based chemical synthesis. By dissolving precursors in solution and allowing self-assembly at low temperatures, the process eliminates the need for complex mechanical processing while achieving single-phase crystalline formation through controlled precipitation and crystal growth mechanisms.
2Manufacturing precision
If extreme temperature synthetic procedures (over 1,000°C) are used, then high-entropy materials can be synthesized, but extensive energy input makes it challenging to scale up production
Solution Approach 1:
The invention changes the temperature parameter from >1,000°C to room temperature or 80°C, dramatically reducing energy input. This enables scalable production of high-entropy materials for large-scale applications, as the mild conditions require minimal energy while still achieving single-phase crystalline formation through solution chemistry and self-assembly processes.
3Manufacturing precision
If extreme temperature and complex processing techniques are used, then single-phase high-entropy materials can be formed, but the process is incompatible with stability of other materials in device architecture
Solution Approach 1:
By changing the synthesis temperature parameter to mild conditions (room temperature to 80°C), the invention eliminates the harmful thermal effects that would destabilize other device materials. The low-temperature solution process allows single-phase high-entropy perovskite formation without exposing surrounding device components to extreme heat, preserving overall device architecture stability.
4Manufacturing precision
If traditional high-temperature synthesis is used, then crystalline solid solutions can be formed, but the extensive energy input and complex processing make it challenging to scale up
Solution Approach 1:
The invention replaces energy-intensive mechanical processing (hot rolling at >1,000°C) with solution-based chemical synthesis at room temperature or 80°C. This substitution enables scalable production through simple solution mixing, precipitation, and crystal growth processes that can be easily scaled up without requiring complex high-temperature equipment or extensive energy infrastructure.
Applied Scientific Principles
This section explains which scientific principles are used to turn an abstract innovation direction into a practical engineering solution.
Function Achieved in This Case
The process enables the formation of stable, single-phase high-entropy semiconductor single crystals with enhanced durability and unique optical properties, suitable for large-scale applications in devices like LEDs and computer chips, while reducing energy input and synthesis complexity.
Implementation Method 1
designed on the cubic Cs2MCl6 (M=Zr4+, Sn4+, Te4+, Hf4+, Re4+, Os4+, Ir4+ or Pt4+) vacancy-ordered double perovskite structure from the self-assembly of stabilized complexes in multi-element inks
Data Source
AI summary
High-entropy materials according to the formula Cs2{M}Cl6 are provided. {M} is a combination of at least five metal cations each occupying the M-site of the high-entropy material as a random alloy, e.g., in near-equimolar ratios. The high-entropy materials provided herein includes five or six-element halide perovskite semiconductor single crystals of the Cs2{SnTeReOsIrPt}1Cl6 family and the Cs2{ZrSnTeHfRePt}1Cl6 family. Also provided are methods of generating a high-entropy material, e.g., metal halide perovskite high-entropy semiconductor single crystals, by contacting Cs+ molecules with at least five different [MCl6]2− molecules in a solvent, forming via a self-assembly process the high-entropy material according to the formula Cs2{M}Cl6. The method is conducted at milder temperature (e.g., at a temperature of 100° C. or lower) relative to traditional methods of high-entropy material synthesis which typically requires procedures of over 1,000° C.