DOE OSTI2014
Low temperature plasma (LTP) treatment of biological tissue is a promising path toward sterilization of bacteria due to its versatility and ability to operate under well-controlled and relatively mild conditions. The present collaborative research of an interdisciplinary team of investigators at University of Maryland, College Park (UMD), and University of California, Berkeley (UCB) focused on establishing our knowledge based with regard to low temperature plasma-induced chemical modifications in biomolecules that result in inactivation due to various plasma species, including ions, reactive radicals, and UV/VUV photons. The overall goals of the project were to identify and quantify the mechanisms by which low and atmospheric pressure plasma deactivates endotoxic biomolecules. Additionally, we wanted to understand the mechanism by which atmospheric pressure plasmas (APP) modify surfaces and how these modifications depend on the interaction of APP with the environment. Various low pressure plasma sources, a vacuum beam system and several atmospheric pressure plasma sources were used to accomplish this. In our work we elucidated for the first time the role of ions, VUV photons and radicals in biological deactivation of representative biomolecules, both in a UHV beam system and an inductively coupled, low pressure plasma system, and established the associated atomistic biomolecule changes. While we showed that both ions and VUV photons can be very efficient in deactivation of biomolecules, significant etching and/or deep modification (~200 nm) accompanied these biological effects. One of the most important findings in this work is the significant radical-induced deactivation and surface modification can occur with minimal etching. However, if radical fluxes and corresponding etch rates are relatively high, for example at atmospheric pressure, endotoxic biomolecule film inactivation may require near-complete removal of the film. These findings motivated further work at atmospheric pressure using several types of low temperature plasma sources, for which radical induced interactions generally dominate due to short mean free paths of ions and VUV photons. For these conditions we demonstrated the importance of environmental interactions when atmospheric pressure plasma sources are used to modify biomolecules. This is evident from both gas phase characterization data and in-situ surface characterization of treated biomolecules. Environmental interactions can produce unexpected outcomes due to the complexity of reactions of reactive species with the atmosphere which determines the composition of reactive fluxes and atomistic changes of biomolecules. Overall, this work clarified a richer spectrum of scientific opportunities and challenges for the field of low temperature plasma-biomolecule surface interactions than initially anticipated, in particular for plasma sources operating at atmospheric pressure. The insights produced in this work, e.g. demonstration of the importance of environmental interactions, are generally important for applications of APP to materials modifications. Thus one major contributions of this research has been the establishment of methodologies to more systematically study the interaction of plasma with bio-molecules. In particular, our studies of atmospheric pressure plasma sources using very well-defined experimental conditions enabled to combine atomistic surface modifications of biomolecules with changes in their biological function. The clarification of the role of ions, VUV photons and radicals in deactivation of biomolecules during low pressure and atmospheric pressure plasma-biomolecule interaction has broad implications, e.g. for the emerging field of plasma medicine. The development of methods to detect the effects of plasma treatment on immune-active biomolecules will be helpful in many future studies.