CAREER: Three-dimensional Nanoscale Device Fabrication via Molecular Programming and DNA-based Self-assembly

该学院早期职业发展（CAREER）资助支持开发一种新的纳米纤维方法，该方法基于DNA分子引导的纳米材料的自组装。大自然已经进化出以可持续的自下而上的方式将纳米材料自组装成复杂的三维几何形状的能力。相比之下，大多数人造设备都是通过理性的自上而下的过程组装的，这是非常不灵活，昂贵和不可持续的。本研究旨在将天然生物分子自组装和理性工程的优势联合收割机，通过编码分子识别到高性能材料中。其目标是开发一种新的纳米制造技术来制造复杂的纳米器件，而不使用昂贵的半导体工厂和方法。这种新的制造方法可以实现各种各样的应用，从具有前所未有的灵敏度的微型传感器到可以自我进化的电子设备。该研究与教育和推广计划相结合，该计划向从K-12到研究生水平的学生介绍自组装概念，并为多功能，可持续，负担得起和可访问的未来纳米制造培训劳动力。尽管经过数十年的发展，分子自组装尚未产生颠覆性的纳米制造方法。这在很大程度上是由于两个未解决的挑战：（i）在由不同的高性能纳米材料（如量子点和纳米线）构建的可实现架构中缺乏可编程的复杂性，以及（ii）缺乏将这些架构与现有设备集成的可扩展但精确的方法。这项研究旨在通过最大限度地提高编码到纳米材料组件和宏观器件中的分子识别量来应对这两个挑战。解决方案是将多个独特的DNA序列放置在纳米级和宏观级组件表面的精确位置上。对于纳米级组件，这是通过将纳米颗粒包裹到DNA折纸“套装”或盒子中来实现的，通过编程纳米颗粒-DNA相互作用，例如金属-嘌呤碱基，静电力，DNA-DNA配对等。这些多个独特DNA链的阵列共同作为分子邮政编码，允许纳米级组件自主识别和相互结合。对于宏观尺度的表面，这是通过用常规的光学光刻进行图案化，然后用标准的胺-羧基化学或用新的分子条形码方法进行DNA折纸缀合以将锚数千个独特的单链DNA固定在精确的位置来实现的。这种图案化的宏观器件表面为从纳米颗粒自组装的结构提供了大量的对接位点，从而产生最终器件。通过研究和理解自组装过程的热力学、纳米级结构、实验参数和最终器件的性能，这项研究推动了分子编程制造的极限。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

This Faculty Early Career Development (CAREER) grant supports the development of a new nanofabrication approach based on self-assembly of nanoscale materials guided by DNA molecules. Nature has evolved the ability to self-assemble nanomaterials into complex three-dimensional geometries in a sustainable bottom-up way. In contrast, most human-made devices are assembled through a rational top-down process which is highly inflexible, expensive, and unsustainable. This research seeks to combine the strengths of natural biomolecular self-assembly and rational engineering by encoding molecular recognition into high-performance materials. The goal is to develop a new nanomanufacturing technology to fabricate complex nanoscale devices, without using expensive semiconductor factories and methods. The new manufacturing approach enables a diverse range of applications, from tiny sensors with unprecedented sensitivity to electronic devices that can self-evolve. The research is integrated with an educational and outreach program that introduces self-assembly concepts to students from K-12 to graduate level and trains a workforce for versatile, sustainable, affordable, and accessible future nanomanufacturing.Despite decades of development, molecular self-assembly has not yet yielded a disruptive nanoscale manufacturing approach. This is largely due to two unsolved challenges: (i) the lack of programmable complexity in achievable architectures built from diverse, high-performance nanomaterials such as quantum dots and nanowires and (ii) the lack of scalable yet precise methods for integrating these architectures with existing devices. This research aims to meet both challenges by maximizing the amount of molecular recognition encoded into nanoscale material components and macroscale devices. The solution is to place multiple unique DNA sequences onto precise locations on surfaces of nanoscale and macroscale components. For nanoscale components this is achieved by wrapping nanoparticles into DNA origami “suits” or boxes via programming nanoparticle–DNA interactions, such as metal-purine base, electrostatic forces, DNA-DNA pairing, etc. These arrays of multiple unique DNA strands serve collectively as molecular zip codes allowing nanoscale components to autonomously recognize and bind to each other. For macroscale surfaces this is achieved by patterning with conventional optical lithography and then performing DNA origami conjugation with standard amine–carboxyl chemistry or with new molecular barcoding approaches to anchor thousands of unique single-stranded DNA in precise positions. This patterned macroscale device surface provides a multitude of docking sites for the architectures self-assembled from nanoparticles yielding the final device. By studying and understanding the thermodynamics of self-assembly processes, nanoscale structures, experimental parameters, and performance of the resulting devices, this research pushes the limits of what is possible to fabricate with molecular programming.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.