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Exciton delocalization in dye aggregate systems is a phenomenon that is revealed by spectral features, such as Davydov splitting, J- and H-aggregate behavior, and fluorescence suppression. Using DNA as an architectural template to assemble dye aggregates enables specific control of the aggregate size and dye type, proximal and precise positioning of the dyes within the aggregates, and a method for constructing large, modular two- and three-dimensional arrays. Here, we report on dye aggregates, organized via an immobile Holliday junction DNA template, that exhibit large Davydov splitting of the absorbance spectrum (125 nm, 397.5 meV), J- and H-aggregate behavior, and near-complete suppression of the fluorescence emission (∼97.6% suppression). Because of the unique optical properties of the aggregates, we have demonstrated that our dye aggregate system is a viable candidate as a sensitive absorbance and fluorescence optical reporter. DNA-templated aggregates exhibiting exciton delocalization may find application in optical detection and imaging, light-harvesting, photovoltaics, optical information processing, and quantum computing. [ABSTRACT FROM AUTHOR]

The magnetomechanical behavior of ferromagnetic shape memory alloys such as Ni-Mn-Ga, and hence the relationship between structure and nanoscale magnetomechanical properties, is of interest for their potential applications in actuators. Furthermore, due to its crystal structure, the behavior of Ni-Mn-Ga is anisotropic. Accordingly, nanoindentation and magnetic force microscopy were used to probe the nanoscale mechanical and magnetic properties of electropolished single crystalline 10M martensitic Ni-Mn-Ga as a function of the crystallographic c-axis (easy magnetization) direction relative to the indentation surface (i.e., c-axis in-plane versus out-of-plane). Load-displacement curves from 5–10 mN indentations on in-plane regions exhibited pop-in during loading, whereas this phenomenon was absent in out-of-plane regions. Additionally, the reduced elastic modulus measured for the c-axis out-of-plane orientation was ∼50% greater than for in-plane. Although heating above the transition temperature to the austenitic phase followed by cooling to the room temperature martensitic phase led to partial recovery of the indentation deformation, the magnitude and direction of recovery depended on the original relative orientation of the crystallographic c-axis: positive recovery for the in-plane orientation versus negative recovery (i.e., increased indent depth) for out-of-plane. Moreover, the c-axis orientation for out-of-plane regions switched to in-plane upon thermal cycling, whereas the number of twins in the in-plane regions increased. We hypothesize that dislocation plasticity contributes to the permanent deformation, while pseudoelastic twinning causes pop-in during loading and large recovery during unloading in the c-axis in-plane case. Minimization of indent strain energy accounts for the observed changes in twin orientation and number following thermal cycling. [ABSTRACT FROM AUTHOR]

Coherent exciton delocalization in dye aggregate systems gives rise to a variety of intriguing optical phenomena, including J- and H-aggregate behavior and Davydov splitting. Systems that exhibit coherent exciton delocalization at room temperature are of interest for the development of artificial light-harvesting devices, colorimetric detection schemes, and quantum computers. Here, we report on a simple dye system templated by DNA that exhibits tunable optical properties. At low salt and DNA concentrations, a DNA duplex with two internally functionalized Cy5 dyes (i.e., dimer) persists and displays predominantly J-aggregate behavior. Increasing the salt and/or DNA concentrations was found to promote coupling between two of the DNA duplexes via branch migration, thus forming a four-armed junction (i.e., tetramer) with H-aggregate behavior. This H-tetramer aggregate exhibits a surprisingly large Davydov splitting in its absorbance spectrum that produces a visible color change of the solution from cyan to violet and gives clear evidence of coherent exciton delocalization. [ABSTRACT FROM AUTHOR]