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Electrical devices employing molten compositions of biomoleculesRelated Patent Categories: Stock Material Or Miscellaneous Articles, Composite (nonstructural Laminate)Electrical devices employing molten compositions of biomolecules description/claimsThe Patent Description & Claims data below is from USPTO Patent Application 20060199016, Electrical devices employing molten compositions of biomolecules. Brief Patent Description - Full Patent Description - Patent Application Claims
RELATED APPLICATIONS [0001] This application Claims the benefit of U.S. Provisional Application No. 60/226,113, filed Aug. 18, 2000, the disclosure of which is incorporated herein by reference in its entirety. FIELD OF THE INVENTION [0003] The present invention relates to electrical devices, melt compositions of biomolecules such as nucleic acids, methods of making and using the same, and structures or devices incorporating the same. BACKGROUND OF THE INVENTION [0004] Nucleic acids may typically be manipulated in aqueous solution and may generally be associated with metal cations. For example, compositions of DNA may typically contain alkali metal countercations that render DNA a crystalline solid that is soluble only in water. [0005] In Gerald S. Manning, et al., "The Molecular Theory of Polyelectrolyte Solutions with Applications to the Electrostatic Properties of Polynucleotides", Quarterly Review of Biophysics II, 2:179-246 (1978), the authors discuss binding of various cationic substances with DNA in an aqueous environment. These cationic substances include metal cations, small cations with complex structures such as oligolysine and spermine, as well as high-molecular-weight cations such as polylysine. [0006] In M. Thomas Record, et al., "Thermodynamic Analysis of Ion Effects on the Binding and Conformational Equilibria of Proteins and Nucleic Acids: The Roles of Ion Association or Release, Screening, and Ion Effects on Water Activity", Quarterly Review of Biophysics II, 2:103-178 (1978), the authors discuss the various effects of low-molecular-weight electrolytes in the associations and interactions of proteins and nucleic acids. [0007] In Enders Dickinson, V, et al., "Hybrid Redox Polyether Melts Based on Polyether-Tailed Counterions", J. Am. Chem. Soc. 121:613-616 (1999), the authors propose transforming various ionic materials into room temperature molten salts by combining them with polyether-tailed counter ions such as polyether-tailed 2-sulfobenzoate and polyether-tailed triethylammonium. The ionic materials include ruthenium hexamine, metal trisbipyridines, metal trisphenanthrolines, and ionic forms of aluminum quinolate, anthraquinone, phthalocyanine, and porphyrins. The authors do not describe transforming nucleic acids into molten salts. [0008] In Mary Elizabeth Williams, et al., "Electron and Mass Transport in Hybrid Redox Polyether Melts: Co and Fe Bipyridines with Attached Polyether Chains", J. Am. Chem. Soc., 119: 1997-2005 (1997), the authors discuss how to discern charge transport by electron self exchange reactions from transport by physical diffusion so as to measure electron transfer rate constants in a series of undiluted metal complex molten salts [M(bpy(CO.sub.2MePEG).sub.2).sub.3].sup.+(ClO.sub.4).sub.2.sup.- where M=Co(II/I) and Fe(III/II) and MePEG is an oligomeric polyether of MW 150, 350, and 550 (the cation portion of which is shown below). In Enders Dickinson V, et al., "The Effect of Polyether Attachment on the Self-Exchange Barriers of Metal Tris(bipyridine) Molten Salts", J. Phys. Chem., 103:11028-11035 (1999), the authors propose highly viscous, room temperature molten salts that may be obtained by associating [M(bpy).sub.3].sup.2+ cations (where M=Ru or Co and bpy=2,2'-bipyridine) with polyether-tailed 2-sulfobenzoate anions. These articles do not discuss molten salts of nucleic acids, nor do the authors appear to recognize the benefits of forming redox-active melts where both the cation and the anion may be capable of electron transfer. [0009] In Yoshio Okahata, et al., "Anisotropic Electric Conductivity in an Aligned DNA Cast Film", J. Am. Chem. Soc., 120: 6165-6166 (1998), the authors propose an aligned DNA film as an anisotropic conductive film, in which counter Na.sup.+ cations were exchanged completely to cationic amphiphiles. The authors report that the aligned DNA film was prepared as follows. An aqueous solution of DNA from Salmon testes (average MW 1.3.times.10.sup.6, ca. 2000 bp) was mixed with an aqueous solution of a cationic amphiphile, N,N,N-trimethyl-N-(3,6,9,12-tetraoxadocosyl) ammonium bromide, (CH.sub.3).sub.3N(CH.sub.2CH.sub.2O).sub.4(CH.sub.2).sub.9(CH.sup.3).sup.- +Br.sup.-. The precipitated DNA-lipid polyion complex (1:1 ratio of phosphate anion to cationic amphiphile) was collected and solubilized in chloroform/ethanol (4:1 v/v). The solution (40 mg/mL, 4 wt %) was cast on a Teflon plate, and the solvent was evaporated slowly under saturated solvent vapor at room temperature. The obtained self-standing film (ca. 60 microns thick) was transparent, flexibly strong, and water-insoluble. The reference does not propose molten salts of polynucleic acids that are liquid. Furthermore, the precipitated DNA-lipid polyanion complex discussed by the authors is not soluble in water. [0010] Various references have discussed the possibility of electron transport through DNA. For example, in Danny Porath, et al., "Direct Measurement of Electrical Transport Through DNA Molecules", Nature, 403: 635-638 (2000), the authors present measurements of electrical transport through individual-10.4 nm-long, double-stranded poly(G)-poly(C) DNA molecules connected to two metal nanoelectrodes, that may indicate large-bandgap semiconducting behavior. In Frederick D. Lewis, et al., "Distance-Dependent Electron Transfer in DNA Hairpins", Science, 277: 673-676 (1997), the authors discuss the distance dependence of photoinduced electron transfer in duplex DNA, and state that while kinetic analysis suggests that duplex DNA is somewhat more effective than proteins as a medium for electron transfer, it does not function as a molecular wire. In Joshua Jortner, et al., "Charge Transfer and Transport in DNA", Proc. Natl. Acad. Sci., 95: 12759-12765 (1998), the authors explore charge migration in DNA and advance two distinct mechanisms of charge separation in a donor-bridge-acceptor system. In Daniel B. Hall, et al., "Oxidative DNA Damage Through Long-range Electron Transfer", Nature, 382: 731-735 (1996), the authors note that the DNA double helix, which contains a .alpha.-stacked array of heterocyclic base pairs, could be a suitable medium for the migration of charge over long molecular distances. In Hans-Werner Fink & Christian Schonenberger, "Electrical Conduction Through DNA Molecules", Nature, 398: 407-410 (1999), the authors report direct measurements of electrical current as a function of the potential applied across a few DNA molecules associated into single ropes at least 600 nm long, which indicate effective conduction through the ropes. In Gary B. Schuster, "Long-Range Charge Transfer in DNA: Transient Structural Distortions Control the Distance Dependence, Acc. Chem. Res., 33: 253-260 (2000), the author proposes a mechanism for long-range charge transport in DNA that depends on its spontaneous structural distortion. This mechanism is referred to as phonon-assisted polaron hopping. In Frederick D. Lewis, et al., "Direct Measurement of Hole Transport Dynamics in DNA", Nature, 406: 51-53 (2000), the authors propose that electrons and holes can migrate from the locus of formation to trap sites, and such migration can occur through either a single step "super exchange" mechanism or a multistep charge transport "hopping" mechanism. These references do not describe molten salts of nucleic acids, and do not suggest how to obtain such molten salts. [0011] Several authors have proposed the use of nucleic acids in molecular electronics. For example, in Robert Elghanian, et al., "Selective Colorimetric Detection of Polynucleotides Based on the Distance-Dependent Optical Properties of Gold Nanoparticles", Science, 277: 1078-1081 (1997), the authors discuss the use of nucleic acids to form a polymeric network of nanoparticles. In Chad A Mirkin, "Programming the Assembly of Two- and Three-Dimensional Architectures with DNA and Nanoscale Inorganic Building Blocks", Inorg. Chem., 39:2258-2272 (2000), the author discusses the development of biological-based-methods for directing the assembly of nanoscale inorganic building blocks into functional materials. The author proposes using DNA as a synthetically programmable assembler. In J. J. Hopfield, et al., "A Molecular Shift Register Based on Electron Transfer", Science, 241: 817-820 (1988), the authors propose an electronic shift-register memory at the molecular level. The authors mention that one scheme to build such a register may take advantage of the linear structure of DNA to which sequence-specific chromophore-bearing groups could be bound. However, methods for carrying out such a scheme are not provided. In Leonard M. Adelman, "Molecular Computation of Solutions to Combinatorial Problems", Science, 266: 1021-1024 (1994), the author proposes carrying out computations at the molecular level using the tools of molecular biology to solve an instance of the directed Hamiltonian path problem. A small graph was encoded in molecules of DNA, and the "operations" of the computation were performed with standard protocols and enzymes. In Michael C. Pirrung, et al., "The Arrayed Primer Extension Method for DNA Microchip Analysis: Molecular Computation of Satisfaction Problems", J. Am. Chem. Soc., 122: 1873-1882 (2000), the authors discuss a DNA computer which may be capable of solving nondeterministic polynomial time (NP)-complete problems (those whose time-complexity function rises exponentially with the problem size) in polynomial time using an arrayed primer extension method. These methods are based on template-dependent extension of DNA primers bound to a solid phase with a labeled dideoxyribonucleotide terminator, followed by detection of the label so added. These references do not describe molten salts of nucleic acids, nor do they appear to recognize the usefulness of such molten salts in molecular electronic applications. SUMMARY OF THE INVENTION [0012] A first aspect of the invention is a composition comprising a salt of an organic polymer ion and a polymer (generally polyether or polysiloxane) counterion; the organic polymer ion selected from the group consisting of polypeptides, polynucleic acids, polystyrenes, and polysaccharides (these including copolymers thereof or compounds to which other groups have been joined, such as glycoproteins); wherein at least one of the organic polymer ion and the polymer counterion is redox active, and having the general formula X.sup..+-. Z.sup..+-., where X is an organic polymer ion and Z is a polymer counterion, subject to the proviso that when X is positively charged then Z is negatively charged, and when X is negatively charged then Z is positively charged ("charge" herein referring to a net positive or negative charge; for example a net positive or negative charge resulting from an absence or excess of electrons, respectively, or a net positive charge (creating a cation) or a net negative charge (creating an anion)). In general, the composition is a melt, preferably at temperatures at which electronic devices such as computers are typically used (e.g., about -50 or -25 to about 100.degree. C.). In some embodiments, the organic polymer ion is an anion and the counterion is a cation; In other embodiments, the organic polymer ion is a cation and the counterion is an anion. In some embodiments either the organic polymer ion is redox active or the polyether counterion is redox active; in other embodiments, both the organic polymer ion and the polyether counterion are redox active. The molar ratio of the organic polymer ion to the polymer counterion (e.g., X and Z in the general formula above) in the composition may be any suitable ratio, such as from about 20:1 or 10:1 to about 1:10 or 1:20. The organic polymer ion may have any suitable molecular weight, such as from about 1, 10 or 100 to 1,000, 10,000, or 100,000 kilodaltons, or more. The polymer counterion may likewise have any suitable molecular weight such as from about 0.2, 0.3, 1, 10 or 100 to 1,000, 10,000, or 100,000 kilodaltons, or more. [0013] A further aspect of the invention is a method of depositing a material on a substrate, comprising the step of coating at least one surface portion of a substrate with a composition described above. The method may optionally further include the step of solidifying the composition on the substrate. In general, the substrate is a solid substrate and the at least one surface portion is an external surface portion, or the substrate may be a porous substrate and the at least one surface portion may include an internal surface portion. The substrate may be a metal, semiconductor, polymeric, or any other suitable material. [0014] A further aspect of the present invention is a structure comprising: (a) a substrate; and (b) a coating on the substrate, the coating comprising a composition as described above. In one embodiment, the substrate is an electrode. [0015] A further aspect of the present invention is a method of making a molten salt, the method comprising the steps of: (a) providing an organic polymer ion selected from the group consisting of polypeptides, polynucleic acids, polystyrenes, and polysaccharides; (b) providing a polymer (typically a polyether or polysiloxane) counterion; and (c) combining the organic polymer ion with the polymer counterion to make a molten salt thereof. [0016] A further aspect of the present invention is a method of forming a structure, comprising the steps of: (a) forming a molten salt of a composition as described above, and (b) solidifying, immobilizing, applying or shaping the molten salt to form a structure. [0017] A further aspect of the present invention is an electrical device such as a memory device, the device comprising: (a) a first electrode; (b) a storage medium electrically coupled to the electrode, the storage medium comprising an ionic liquid melt (including but not limited to the compositions described above), the ionic liquid melt comprising at least a first redox active compound. The device may include a second electrode electrically coupled to the storage medium. In some embodiments, the storage medium is contained within an enclosed and/or sealed chamber. In some embodiments, the ionic liquid melt further comprises a second redox active compound that together with the first redox active compound form a redox active pair. Such a device may be a refreshable memory device. In general, the storage medium is not covalently bonded to the first electrode. [0018] A more particular aspect of the present invention is a composition comprising a salt, for example a molten salt, of a polynucleic acid anion and a polyether cation. The polyether cation may have a polyether tail group having the formula: --(R.sup.1O).sub.n--R.sup.2 wherein: R.sup.1 is a substituted or unsubstituted, linear or branched, aliphatic or cycloaliphatic group, having between 1 and 10 carbons, that is saturated, partially saturated, or unsaturated; R.sup.2 is a substituted or unsubstituted, linear or branched, aliphatic or cycloaliphatic group, having between 1 and 8 carbons, that is saturated, partially saturated, or unsaturated; and n is typically an integer between 1, 2 or 3 and 15, 25 or 50. In addition to the foregoing, analogous materials in which the tail is a siloxane (such as poly-dimethylsiloxane) rather than a polyether may also be prepared. [0019] The polynucleic acid may be polydeoxyribonucleic acid, polyribonucleic acid, etc. The polyether tail group may comprise polyethylene or polypropylene glycol. In a particular embodiment, R.sup.1 is an unsubstituted, saturated C.sub.1 to C.sub.4 alkyl group. In another particular embodiment, R.sup.2 is an unsubstituted, saturated C.sub.1 to C.sub.8 alkyl group. In another particular embodiment, R.sup.2 is an unsubstituted, saturated C.sub.1 to C.sub.4 alkyl group such as a methyl group. [0020] A further aspect of the present invention is a composition, preferably comprising a salt of a polynucleic acid anion and a polyether cation, said salt in the absence of any diluting solvent preferably being present as a molten salt. In a particular embodiment, the salt is amorphous (non-crystalline) and has a glass transition temperature between about -50 or -25 and 100.degree. C. (i.e., temperatures at which electronic devices such as computers are typically used). [0021] A further aspect of the present invention is a method of depositing a polynucleic acid on a substrate, comprising the step of: coating at least one surface portion of a substrate with a composition comprising a salt of a polynucleic acid anion and a polyether cation, said salt being present as a molten salt. The coating step may be followed by the step of solidifying, adhering and/or immobilizing the composition on said substrate. In a preferred embodiment, the substrate is a solid substrate and said at least one surface portion is an external surface portion. The substrate may also be a porous substrate, and said at least one surface portion may include an internal surface portion (e.g., a interior wall of a pore). Suitable substrates include but are not limited to metals, semiconductors, and polymeric materials. In a particular embodiment, the substrate comprises an electrode. Continue reading about Electrical devices employing molten compositions of biomolecules... 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