Argonne National Laboratory

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Programmable Assembly of Colloidal Crystals with DNA

XSD/CMS Special Colloquium
Andrew Senesi, Northwestern University
January 17, 2013 3:30PM to 4:30PM
Building 433
Nano-structured materials and their assemblies have generated considerable scientific and industrial interest as a result of new chemical and physical interactions as their size is reduced and they are positioned into well-defined spatial arrangements. Indeed, a grand challenge in nanotechnology is to construct materials comprised of positionally encoded elements (i.e. nanoparticles) with fine control over spacing, symmetry, and composition, with single- or sub-nanometer precision and registry. The ability to exercise such control over multiple length scales and in three dimensions for a single system would, in principle, provide researchers with a route to fabrication “materials by design”, in which one could design and build a functional system with programmed chemical and physical properties, useful in material synthesis, optics, biomedicine, energy, and catalysis. In this talk, I will discuss recent progress towards this goal, by using DNA as a programmable ligand to direct the assembly of nanoparticles into crystalline arrays.

DNA is ideally suited for this purpose, as synthetically tunable variations in nucleotide sequence allow for precise engineering of the nanoparticle’s hydrodynamic radius and binding properties. These factors, in turn, dictate the crystallographic symmetry and lattice parameters of the assembly. By further employing a DNA-functionalized substrate, thin-film nanoparticle superlattices can be grown in a layer-by-layer fashion with fine control over the number of particle layers in the assembly (i.e. film thickness). Importantly, the judicious choice of DNA substrate-particle interconnects allows one to tune the interfacial energy between various crystal planes and the substrate, and thereby control crystal orientation. A theoretical framework to understand these results is presented. These nanoparticle superlattices can further be patterned in arbitrary locations on a substrate using molecular printing techniques such as dip-pen nanolithography (DPN) and polymer pen lithography (PPL).

The principles developed in this work represent a major advance in the bottom-up synthesis of nanomaterials and a major step towards the integration of nanoscale materials into functional device architectures. Lastly, ultrafast pump-probe studies of third-generation materials for future photovoltaics will be presented. One such novel photovoltaic material uses heavy O doping of ZnTe to generate the formation of an intermediate band within the forbidden gap, in order to improve the matching of semiconductor absorption and solar spectra. This approach is believed to become useful for realization of single junction solar cells with very high efficiencies. However, the implementation of such devices requires advanced characterization techniques. Multiphoton optical pulse excitations are demonstrated to induce multiband charge transfer dynamics in ZnTe:O films as revealed when monitoring the time-resolved photoluminescence signals.