Halide perovskites, as a new material category, have provided growing numbers of breakthroughs in photovoltaic, photodetector and sensing, laser, light emitting diode, X and γ-ray detector, photocatalyst, memory, transducer, transistor, ferroelectric, photothermal conversion, thermoelectric, and more, with great potential but also challenges. These materials have also provided a new platform to discover, understand, and apply new phenomena such as unique polaronic charge behavior, ultraslow hot carrier cooling, nontrivial edge sate, versatile lower dimensional lattice tunability to such as 2D multiple quantum well (MQW) with abnormal light-matter transferring properties, etcetera. However, the material discovery rate and the synthesis of the halide perovskites still restricted by their very low-yield (10-35%) and time-consuming (0.1-10 mm³ h^-1) synthesis. In addition, the synthesis and manufacturing of the halide perovskites are crucial to their structural and microscopic features at various scales from lattice (e.g., distortion, strain, and defects), grain (e.g., size, orientation, and grain boundary), morphology and topography (e.g., homogeneity, surface roughness, and surface traps), all of which could synergistically affect the final physical property and their overall reliability in real implementations.

Prior manufacturing of halide perovskite mainly includes liquifying the perovskite into solution followed by solidifying it into film or single crystals and vaporizing the perovskite through high-vacuum thermal deposition techniques. The former plays a dominant role in the field of thin film perovskite photoelectronics such as photovoltaics and light emission diodes (LEDs) but represents an inefficient and effortful way for bulk crystal synthesis, which has already set the limits on not only the application or measurement that requires a bulk sample but also limits the high-throughput material discovery of new crystals. Also, intrinsic material issues such as purity due to residual solvent molecules and impurity species from solution as well as the defects and lattice distortions that are ‘frozen’ during the nonequilibrium crystallization, remain to address. Further manufacturing difficulties including complex post-deposition treatment (e.g., anti-solvent, two/multi-step treatment, annealing, surface passivation), batch-to-batch consistency and reproducibility, up-scalability and mass-productivity, capital expense on solvent materials and energy input for solvent removing, as well as raw material waste from deposition (e.g., spin-coating), and eco-concern on solvent toxicity, can bring multiple risks to the technical transition.

In parallel, vapor-based methods for perovskite synthesis have been attempted with controllable purity, yield, and scalability as well as exemption of those solvent-related concerns. Such a vapor technique could be more practically reliable as learned from the prior success of commercialized organic light emitting diode (OLED) since the vapor method can minimize moisture and oxygen concentration within the final products and thereby a higher level of efficiency and lifetime compared to the wet methods. Unlike organics, vapor deposition of halide perovskite requires simultaneous sublimation of its multiple precursors. While technically monitoring the evaporation rate of the low-molecular-weight ammonium halide and accurately controlling the stoichiometry remain challenging, which is also accompanied by other issues such as low material usage (e.g., 10%) and unwanted decomposition through outgassing in high-vacuum due to the weak bonding nature of halide perovskites. On the other hand, the current synthesis of bulk perovskite materials for applications in X-/γ-ray detection, photo-sensing, and thermoelectric still relay on the low-yield (10-35 %) and time-consuming (0.1-10 mm³ h^-1) wet chemistry methods. Recent studies reveal the melting method to synthesize the bulk sample but critically limited to a specific composition (i.e., all-inorganic) due to the conflict between the high reaction temperature (over 500 °C) and the intermediate decomposition temperature of general halide perovskites. All of these have already set up the barrier for not only mass production for real applications but also the high-throughput discovery of advanced perovskite materials with unique properties.

To overcome these barriers, we report the first attempt on a universal solid state-based route for synthesizing high-quality perovskites via a field-assisted sintering technique (FAST) using simultaneous electric field and mechanical stress that directly densifies the perovskites from solid precursors into high-quality bulk crystals within a few minutes (Figure 1). This synthetic route for halide perovskites outpaces prior liquid- and vapor-based methods by nature of high-throughput, 100% material usage, oxygen- and moisture-free, hazardous solvent-free, and capability of producing high-quality large bulk crystals in a short time. We employed different perovskite compositions and geometric designs for demonstration in this work and established such perovskite synthetic route with the uniqueness of ultrahigh yield, quick process, and solvent-free, along with bulk products of exceptional quality approaching single crystal. This method enables the discovery, investigation, and application of innovative perovskites in terms of time-/yield-/effort-efficiency and sample quality. To show the remarkable performance of the synthesized materials, we exemplify the applications of FAST-perovskites in detection, photovoltaic, thermoelectric, and other potential applications for opening extra chapters for future research and technological development. The newly synthesized material products will have the potential to address the bottleneck issues in existing relevant fields, such as the instability and toxicity in solar cells, low performance in piezoelectric and thermoelectric, and the potential for new applications such as intelligent image sensing and/or artificial synaptic memory. Development of this new high-throughput synthetic technique can catalyze the advance of multiple fields since it enables materials fabrication with various size and shapes (Figure 2), proper composition at each lattice site with expected properties, non-stoichiometric compounds, grain size control and refinements, dopant manipulation, defect engineering, and large-scale production of halide perovskites.