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Title: LDRD final report on adaptive-responsive nanostructures for sensing applications.

Abstract

Functional organic nanostructures such as well-formed tubes or fibers that can easily be fabricated into electronic and photonic devices are needed in many applications. Especially desirable from a national security standpoint are nanostructures that have enhanced sensitivity for the detection of chemicals and biological (CB) agents and other environmental stimuli. We recently discovered the first class of highly responsive and adaptive porphyrin-based nanostructures that may satisfy these requirements. These novel porphyrin nanostructures, which are formed by ionic self-assembly of two oppositely charged porphyrins, may function as conductors, semiconductors, or photoconductors, and they have additional properties that make them suitable for device fabrication (e.g., as ultrasensitive colorimetric CB microsensors). Preliminary studies with porphyrin nanotubes have shown that these nanostructures have novel optical and electronic properties, including strong resonant light scattering, quenched fluorescence, and electrical conductivity. In addition, they are photochemically active and capable of light-harvesting and photosynthesis; they may also have nonlinear optical properties. Remarkably, the nanotubes and potentially other porphyrin nanostructure are mechanically responsive and adaptive (e.g., the rigidity of the micrometers-long nanotubes is altered by light, ultrasound, or chemicals) and they self-heal upon removal the environmental stimulus. Given the tremendous degree of structural variation possible in the porphyrin subunits,more » additional types of nanostructures and greater control over their morphology can be anticipated. Molecular modification also provides a means of controlling their electronic, photonic, and other functional properties. In this work, we have greatly broadened the range of ionic porphyrin nanostructures that can be made, and determined the optical and responsivity properties of the nanotubes and other porphyrin nanostructures. We have also explored means for controlling their morphology, size, and placement on surfaces. The research proposed will lay the groundwork for the use of these remarkable porphyrin nanostructures in micro- and nanoscale devices, by providing a more detailed understanding of their molecular structure and the factors that control their structural, photophysical, and chemical properties.« less

Authors:
; ; ;
Publication Date:
Research Org.:
Sandia National Laboratories
Sponsoring Org.:
USDOE
OSTI Identifier:
875634
Report Number(s):
SAND2005-6252
TRN: US200603%%313
DOE Contract Number:
AC04-94AL85000
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEFENSE; CHEMICAL PROPERTIES; ELECTRIC CONDUCTIVITY; FABRICATION; FIBERS; FLUORESCENCE; LIGHT SCATTERING; MOLECULAR STRUCTURE; MORPHOLOGY; NANOSTRUCTURES; NATIONAL SECURITY; OPTICAL PROPERTIES; PHOTOCONDUCTORS; PHOTOSYNTHESIS; PORPHYRINS; Optics, Adaptive.; Nanostructures-Optical properties.; Photonic devices.

Citation Formats

Shelnutt, John Allen, van Swol, Frank B., Wang, Zhongchun, and Medforth, Craig J. LDRD final report on adaptive-responsive nanostructures for sensing applications.. United States: N. p., 2005. Web. doi:10.2172/875634.
Shelnutt, John Allen, van Swol, Frank B., Wang, Zhongchun, & Medforth, Craig J. LDRD final report on adaptive-responsive nanostructures for sensing applications.. United States. doi:10.2172/875634.
Shelnutt, John Allen, van Swol, Frank B., Wang, Zhongchun, and Medforth, Craig J. Tue . "LDRD final report on adaptive-responsive nanostructures for sensing applications.". United States. doi:10.2172/875634. https://www.osti.gov/servlets/purl/875634.
@article{osti_875634,
title = {LDRD final report on adaptive-responsive nanostructures for sensing applications.},
author = {Shelnutt, John Allen and van Swol, Frank B. and Wang, Zhongchun and Medforth, Craig J.},
abstractNote = {Functional organic nanostructures such as well-formed tubes or fibers that can easily be fabricated into electronic and photonic devices are needed in many applications. Especially desirable from a national security standpoint are nanostructures that have enhanced sensitivity for the detection of chemicals and biological (CB) agents and other environmental stimuli. We recently discovered the first class of highly responsive and adaptive porphyrin-based nanostructures that may satisfy these requirements. These novel porphyrin nanostructures, which are formed by ionic self-assembly of two oppositely charged porphyrins, may function as conductors, semiconductors, or photoconductors, and they have additional properties that make them suitable for device fabrication (e.g., as ultrasensitive colorimetric CB microsensors). Preliminary studies with porphyrin nanotubes have shown that these nanostructures have novel optical and electronic properties, including strong resonant light scattering, quenched fluorescence, and electrical conductivity. In addition, they are photochemically active and capable of light-harvesting and photosynthesis; they may also have nonlinear optical properties. Remarkably, the nanotubes and potentially other porphyrin nanostructure are mechanically responsive and adaptive (e.g., the rigidity of the micrometers-long nanotubes is altered by light, ultrasound, or chemicals) and they self-heal upon removal the environmental stimulus. Given the tremendous degree of structural variation possible in the porphyrin subunits, additional types of nanostructures and greater control over their morphology can be anticipated. Molecular modification also provides a means of controlling their electronic, photonic, and other functional properties. In this work, we have greatly broadened the range of ionic porphyrin nanostructures that can be made, and determined the optical and responsivity properties of the nanotubes and other porphyrin nanostructures. We have also explored means for controlling their morphology, size, and placement on surfaces. The research proposed will lay the groundwork for the use of these remarkable porphyrin nanostructures in micro- and nanoscale devices, by providing a more detailed understanding of their molecular structure and the factors that control their structural, photophysical, and chemical properties.},
doi = {10.2172/875634},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Tue Nov 01 00:00:00 EST 2005},
month = {Tue Nov 01 00:00:00 EST 2005}
}

Technical Report:

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  • Solid-state lighting (SSL) technologies, based on semiconductor light emitting devices, have the potential to reduce worldwide electricity consumption by more than 10%, which could significantly reduce U.S. dependence on imported energy and improve energy security. The III-nitride (AlGaInN) materials system forms the foundation for white SSL and could cover a wide spectral range from the deep UV to the infrared. For this LDRD program, we have investigated the synthesis of single-crystalline III-nitride nanowires and heterostructure nanowires, which may possess unique optoelectronic properties. These novel structures could ultimately lead to the development of novel and highly efficient SSL nanodevice applications. GaNmore » and III-nitride core-shell heterostructure nanowires were successfully synthesized by metal organic chemical vapor deposition (MOCVD) on two-inch wafer substrates. The effect of process conditions on nanowire growth was investigated, and characterization of the structural, optical, and electrical properties of the nanowires was also performed.« less
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  • Electrochemically formed porous silicon (PS) was reported in 1991 to exhibit visible photoluminescence. This discovery could lead to the use of integrated silicon-based optoelectronic devices. This LDRD addressed two general goals for optical emission from Si: (1) investigate the mechanisms responsible for light emission, and (2) tailor the microstructure and composition of the Si to obtain photoemission suitable for working devices. PS formation, composition, morphology, and microstructure have been under investigation at Sandia for the past ten years for applications in silicon-on-insulator microelectronics, micromachining, and chemical sensors. The authors used this expertise to form luminescent PS at a variety ofmore » wavelengths and have used analytical techniques such as in situ Raman and X-ray reflectivity to investigate the luminescence mechanism and quantify the properties of the porous silicon layer. Further, their experience with ion implantation in Si lead to an investigation into alternate methods of producing Si nanostructures that visibly luminesce.« less
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  • This project is aimed to gain added durability by supporting ripening-resistant dendritic platinum and/or platinum-based alloy nanostructures on carbon. We have developed a new synthetic approach suitable for directly supporting dendritic nanostructures on VXC-72 carbon black (CB), single-walled carbon nanotubes (SWCNTs), and multi-walled carbon nanotubes (MWCNTs). The key of the synthesis is to creating a unique supporting/confining reaction environment by incorporating carbon within lipid bilayer relying on a hydrophobic-hydrophobic interaction. In order to realize size uniformity control over the supported dendritic nanostructures, a fast photocatalytic seeding method based on tin(IV) porphyrins (SnP) developed at Sandia was applied to the synthesismore » by using SnP-containing liposomes under tungsten light irradiation. For concept approval, one created dendritic platinum nanostructure supported on CB was fabricated into membrane electrode assemblies (MEAs) for durability examination via potential cycling. It appears that carbon supporting is essentially beneficial to an enhanced durability according to our preliminary results.« less