Abstract We report a general synthetic route toward helical ladder polymers with varying spring constants, built with chirality‐assisted synthesis (CAS). Under tension and compression, these shape‐persistent structures do not unfold, but rather stretch and compress akin classical Hookean springs. Our synthesis is adaptable to helices with different pitch and diameter, which allowed us to investigate how molecular flexibility in solution depends on the exact geometry of the ladder polymers. Specifically, we showed with molecular dynamic simulations and by measuring the longitudinal1H NMR relaxation times (T1) for our polymers at different Larmor frequencies, that increasing the helix diameter leads to increased flexibility. Our results present initial design rules for tuning the mechanical properties of intrinsically helical ladder polymers in solution, which will help inspire a new class of robust, spring‐like molecular materials with varying mechanical properties. 
                        more » 
                        « less   
                    
                            
                            A universal all-solid synthesis for high throughput production of halide perovskite
                        
                    
    
            Abstract Halide perovskites show ubiquitous presences in growing fields at both fundamental and applied levels. Discovery, investigation, and application of innovative perovskites are heavily dependent on the synthetic methodology in terms of time-/yield-/effort-/energy- efficiency. Conventional wet chemistry method provides the easiness for growing thin film samples, but represents as an inefficient way for bulk crystal synthesis. To overcome these, here we report a universal solid state-based route for synthesizing high-quality perovskites, by means of simultaneously applying both electric and mechanical stress fields during the synthesis, i.e., the electrical and mechanical field-assisted sintering technique. We employ various perovskite compositions and arbitrary geometric designs for demonstration in this report, and establish such synthetic route with uniqueness of ultrahigh yield, fast processing and solvent-free nature, along with bulk products of exceptional quality approaching to single crystals. We exemplify the applications of the as-synthesized perovskites in photodetection and thermoelectric as well as other potentials to open extra chapters for future technical development. 
        more » 
        « less   
        
    
                            - Award ID(s):
- 1916707
- PAR ID:
- 10499952
- Publisher / Repository:
- Nature
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 13
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
- 
            
- 
            A diastereoselective synthesis of the β-anomer of glycinamide ribonucleotide (β-GAR) has been developed. The synthesis was accomplished in nine steps from D-ribose and occurred in 5% overall yield. The route provided material on the multi-milligram scale. The synthetic β-GAR formed was remarkably resistant to anomerization both in solution and as a solid.more » « less
- 
            Chalcogenide perovskites are promising semiconductor materials with attractive optoelectronic properties and appreciable stability, making them enticing candidates for photovoltaics and related electronic applications. Traditional synthesis methods for these materials have long suffered from high‐temperature requirements of 800–1000 °C. However, the recently developed solution processing route provides a way to circumvent this. By utilizing barium thiolate and ZrH2, this method is capable of synthesizing BaZrS3perovskite at modest temperatures (500–600 °C), generating crystalline domains on the order of hundreds of nanometers in size. Herein, a systematic study of this solution processing route is done to gain a mechanistic understanding of the process and to supplement the development of device quality fabrication methodologies. A barium polysulfide liquid flux is identified as playing a key role in the rapid synthesis of large‐grain BaZrS3perovskite at modest temperatures. Additionally, this mechanism is successfully extended to the related BaHfS3perovskite. The reported findings identify viable precursors, key temperature regimes, and reaction conditions that are likely to enable the large‐grain chalcogenide perovskite growth, essential toward the formation of device‐quality thin films.more » « less
- 
            Abstract The design of multifunctional alloys with multiple chemical components requires controllable synthesis approaches. Physical vapor deposition techniques, which result in thin films (<1 μm), have previously been demonstrated for micromechanical devices and metallic combinatorial libraries. However, this approach deviates from bulk-like properties due to the residual stress derived in thin films and is limited by total film thickness. Here, we report a route to obtain ternary Ni-Mn-Sn alloy thick films with controllable compositions and thicknesses by annealing electrochemically deposited multi-layer monatomic (Ni, Mn, Sn) films, deposited sequentially from separate aqueous deposition baths. We demonstrate (1) controllable compositions, with high degree of uniformity, (2) smooth films, and (3) high reproducibility between film transformation behavior. Our results demonstrate a positive correlation between alloy film thicknesses and grain sizes, as well as consistent bulk-like transformation behavior.more » « less
- 
            Abstract In response to environmental stressors, biological systems exhibit extraordinary adaptive capacity by turning destructive environmental stressors into constructive factors; however, the traditional engineering materials weaken and fail. Take the response of polymers to an aquatic environment as an example: Water molecules typically compromise the mechanical properties of the polymer network in the bulk and on the interface through swelling and lubrication, respectively. Here, we report a class of 3D-printable synthetic polymers that constructively strengthen their bulk and interfacial mechanical properties in response to the aquatic environment. The mechanism relies on a water-assisted additional cross-linking reaction in the polymer matrix and on the interface. As such, the typically destructive water can constructively enhance the polymer’s bulk mechanical properties such as stiffness, tensile strength, and fracture toughness by factors of 746% to 790%, and the interfacial bonding by a factor of 1,000%. We show that the invented polymers can be used for soft robotics that self-strengthen matrix and self-heal cracks after training in water and water-healable packaging materials for flexible electronics. This work opens the door for the design of synthetic materials to imitate the constructive adaptation of biological systems in response to environmental stressors, for applications such as artificial muscles, soft robotics, and flexible electronics.more » « less
 An official website of the United States government
An official website of the United States government 
				
			 
					 
					
 
                                    