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US4704353A Expired / Lapsed US ⏱️ 0.0 years remaining

Photoresponsive redox detection and discrimination

Assignee: Molecular Devices LLC
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Filing: 1984-04-27
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Granted: 1987-11-03
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Expires: 2004-04-27
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Abstract

Abstract Devices and methods are provided for making a plurality of determinations of the local (site-specific) redox state of a liquid system, by employing a photoresponsive element, which can be independently irradiated at different sites to provide independently detectable signals.

Inventors

  • 👤 Gillian M. K. Humphries
  • 👤 John W. Parce
  • 👤 Harden M. McConnell

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-10-27 11:52
CPC Classifications
G; G01; G01N; G01N33/00; G01N33/48; G01N33/50; G01N33/53; G01N33/543; G01N33/54366; G01N33/54373; G01N33/5438; C; C12; C12Q; C12Q1/00; C12Q1/001; C12Q1/004; G01N27/00; G01N27/26; G01N27/28; G01N27/30; G01N27/305; Y; Y10; Y10S; Y10S435/00; Y10S435/966; Y10S435/973; Y10S436/00; Y10S436/805; Y10S436/806; Y10S436/807; Y10S436/827; Y10S436/904

Claims Analysis

Total Claims: 41
Claim 1
Independent Claim 154 words
A photoresponsive device for making at different sites a plurality of determinations of a redox substance capable of modifying an electrical signal resulting from irradiation of a photoresponsive element, said device comprising: a photoresponsive element having an irradiation receiving surface; irradiation means for irradiating at least two sites on said surface to provide distinguishable signals; a counterelectrode; means for polarizing said element with respect to said counterelectrode; first container means for retaining media in which said substance is to be determined in a photoresponsive modifying relationship to at least two sites; second container means for maintaining a first electrolyte in electrical communication with said photoresponsive element; third container means for maintaining a second electrolyte in electrical communication with said counterelectrode; means for providing electrical communication between electrolyte in said second and third container means without mixing of said first and second electrolytes; and means for measuring the electrical photoresponse during irradiation of a site.
Claim 2
Dependent Claim 154 words
A photoresponsive device for making at different sites a plurality of determinations of a redox substance capable of modifying an electrical signal resulting from irradiation of a photoresponsive element, said device comprising: a photoresponsive element having an irradiation receiving surface; irradiation means for irradiating at least two sites on said surface to provide distinguishable signals; a counterelectrode; means for polarizing said element with respect to said counterelectrode; first container means for retaining media in which said substance is to be determined in a photoresponsive modifying relationship to at least two sites; second container means for maintaining a first electrolyte in electrical communication with said photoresponsive element; third container means for maintaining a second electrolyte in electrical communication with said counterelectrode; means for providing electrical communication between electrolyte in said second and third container means without mixing of said first and second electrolytes; and means for measuring the electrical photoresponse during irradiation of a site.
Claim 3
Dependent Claim 17 words
A device according to claim 1, wherein said photoresponsive element is a monolithic doped silicon semiconductor wafer.
Claim 4
Dependent Claim 21 words
A device according to claim 1, including a clear sheet in close spaced apart parallel juxtaposition to said irradiation receiving surface.
Claim 5
Dependent Claim 19 words
A device according to claim 1, wherein said irradiation means is an LED array programmed to provide light pulses.
Claim 6
Dependent Claim 24 words
A device according to claim 1, wherein said container means is a plurality of channels, each of said channels associated with an irradiation site.
Claim 7
Dependent Claim 24 words
A device according to claim 1, wherein said container means is a plurality of compartments, each of said compartments associated with an irradiation site.
Claim 8
Dependent Claim 24 words
A device according to claim 1, wherein a portion of said element is coated with a lipid bilamellar layer for contact with said media.
Claim 9
Dependent Claim 29 words
A device according to claim 7, wherein said lipid bilamellar layer is coated on said irradiation receiving surface and has a specific binding pair member bound to said layer.
Claim 10
Independent Claim 139 words
A method for substantially simultaneously determining a redox substance in a plurality of volumes of an electrically responsive medium, employing a photoresponsive element having a common lead through an electrical circuit to a counterelectrode, wherein said substance is capable of modulating the photoresponse of said element; said method comprising: directing said medium into photoresponsive modifying relationship with a photoresponsive surface of said element; maintaining electrical communication between said element and said counterelectrode through an electrically responsive fluid or gel; irradiating said surface at a plurality of sites in relation to individual volumes at different times in a predetermined sequence for defined periods of time at each of said sites; and determining by means of said circuit the presence of said substance in each of said volumes by the effect of said substance on the photoresponse resulting from said irradiation.
Claim 11
Independent Claim 139 words
A method for substantially simultaneously determining a redox substance in a plurality of volumes of an electrically responsive medium, employing a photoresponsive element having a common lead through an electrical circuit to a counterelectrode, wherein said substance is capable of modulating the photoresponse of said element; said method comprising: directing said medium into photoresponsive modifying relationship with a photoresponsive surface of said element; maintaining electrical communication between said element and said counterelectrode through an electrically responsive fluid or gel; irradiating said surface at a plurality of sites in relation to individual volumes at different times in a predetermined sequence for defined periods of time at each of said sites; and determining by means of said circuit the presence of said substance in each of said volumes by the effect of said substance on the photoresponse resulting from said irradiation.
Claim 12
Dependent Claim 38 words
A method according to claim 9, wherein said circuit includes means for polarizing said element in relation to said counterelectrode and means for measuring the current necessary to restore the level of polarization during irradiation of said surface.
Claim 13
Dependent Claim 21 words
A method according to claim 9, wherein said circuit includes means for varying the light intensity in relation to said photoresponse.
Claim 14
Dependent Claim 37 words
A method according to claim 9, wherein said circuit includes means for fixing the potential between said photoresponsive element and counterelectrode and for fixing the intensity of said irradiation and determining the DC component of the photoresponse.
Claim 15
Dependent Claim 13 words
A method according to claim 9, wherein said substance is an inorganic ion.
Claim 16
Dependent Claim 15 words
A method according to claim 9, wherein said photoresponsive element is a monolithic doped semiconductor.
Claim 17
Dependent Claim 16 words
A method according to claim 9, wherein said volumes are portions of at least one stream.
Claim 18
Dependent Claim 18 words
A method according to claim 9, wherein each of said volumes is physically separated from the other volumes.
Claim 19
Dependent Claim 17 words
A method according to claim 9, wherein said substance is methylene blue, Meldola blue, or phenazine methosulfate.
Claim 20
Dependent Claim 34 words
A method according to claim 9, wherein said circuit maintains said element and counterelectrode at a predetermined potential difference and measures the current necessary to restore the potential difference upon irradiation of said surface.
Claim 21
Dependent Claim 16 words
A method according to claim 9, wherein said substance is a result of an enzymatic reaction.
Claim 22
Dependent Claim 26 words
A method according to claim 19, wherein said substance is reduced or oxidized indirectly through one or more intermediate compounds by the product of said enzyme.
Claim 23
Dependent Claim 12 words
A method according to claim 19, wherein said enzyme is an oxidoreductase.
Claim 24
Dependent Claim 12 words
A method according to claim 21, wherein said oxidoreductase is a peroxidase.
Claim 25
Dependent Claim 12 words
A method according to claim 21, wherein said enzyme is a dehydrogenase.
Claim 26
Independent Claim 257 words
A method for determining the presence of an analyte in a sample, which analyte is a member of a first specific binding pair consisting of ligand and receptor, said method employing: (a) a photoresponsive electrode having an irradiation surface; (b) a counterelectrode; (c) an electrical circuit connecting said photoresponsive electrodes and counterelectrode and maintaining said electrodes in a predetermined potential relationship; (d) a binding surface for binding a member of a specific binding pair, which surface is said irradiation surface or a facing surface in close spaced apart juxtaposition to said irradiation surface; and (e) specific binding means for specifically binding one of said members of said first specific binding pair to said binding surface; said method comprising: in an aqueous assay medium, combining components with said specific binding means, said assay components including a sample, a labeled specific binding pair member, which labeled specific binding pair member is a member of said first pair or capable of binding to, either directly or indirectly, a member of said first pair, wherein said label is a member of a system capable of modulating the electrical photoresponse of said photoresponsive electrode by means of a change in redox potential, and any additional members of said system; irradiating a plurality of sites on said irradiation surface in relation to individual volumes of said combined components at different times in accordance with a predetermined schedule; and determining the electrical photoresponse as modulated by said system by means of said circuit as indicative of the presence of said analyte in said sample.
Claim 27
Independent Claim 257 words
A method for determining the presence of an analyte in a sample, which analyte is a member of a first specific binding pair consisting of ligand and receptor, said method employing: (a) a photoresponsive electrode having an irradiation surface; (b) a counterelectrode; (c) an electrical circuit connecting said photoresponsive electrodes and counterelectrode and maintaining said electrodes in a predetermined potential relationship; (d) a binding surface for binding a member of a specific binding pair, which surface is said irradiation surface or a facing surface in close spaced apart juxtaposition to said irradiation surface; and (e) specific binding means for specifically binding one of said members of said first specific binding pair to said binding surface; said method comprising: in an aqueous assay medium, combining components with said specific binding means, said assay components including a sample, a labeled specific binding pair member, which labeled specific binding pair member is a member of said first pair or capable of binding to, either directly or indirectly, a member of said first pair, wherein said label is a member of a system capable of modulating the electrical photoresponse of said photoresponsive electrode by means of a change in redox potential, and any additional members of said system; irradiating a plurality of sites on said irradiation surface in relation to individual volumes of said combined components at different times in accordance with a predetermined schedule; and determining the electrical photoresponse as modulated by said system by means of said circuit as indicative of the presence of said analyte in said sample.
Claim 28
Dependent Claim 16 words
A method according to claim 24, wherein said photoresponsive semiconductor is a doped monolithic silicon wafer.
Claim 29
Dependent Claim 12 words
A method according to claim 24, wherein said label is an enzyme.
Claim 30
Dependent Claim 17 words
A method according to claim 24, wherein said specific binding means is a second ligand and receptor.
Claim 31
Dependent Claim 18 words
A method according to claim 27, wherein said second ligand and receptor are a saccharide and a lectin.
Claim 32
Dependent Claim 21 words
A method according to claim 27, wherein said second ligand and receptor are a ligand and a natural receptor or antibody.
Claim 33
Independent Claim 155 words
A method for determining the presence of an enzyme substrate in a medium, wherein the product of said substrate results in the production of a product, capable of producing either directly or indirectly a detectable redox potential, said method employing: (a) a photoresponsive semiconductor electrode having an irradiation surface; (b) at least one counterelectrode; (c) an electrical circuit connecting said photoresponsive electrode and counterelectrode and maintaining said electrodes in a predetermined potential relationship; (d) a binding surface for binding said enzyme at a plurality of sites; said method comprising: contacting said enzyme at each of said sites with an aqueous medium containing said substrate and any additional components necessary for the enzymatic catalyzed reaction; irradiating said sites on said irradiation surface at different times in accordance with a predetermined schedule; and determining the electrical photoresponse as modified by said system by means of said circuit as a measure of the amount of said substrate present.
Claim 34
Independent Claim 155 words
A method for determining the presence of an enzyme substrate in a medium, wherein the product of said substrate results in the production of a product, capable of producing either directly or indirectly a detectable redox potential, said method employing: (a) a photoresponsive semiconductor electrode having an irradiation surface; (b) at least one counterelectrode; (c) an electrical circuit connecting said photoresponsive electrode and counterelectrode and maintaining said electrodes in a predetermined potential relationship; (d) a binding surface for binding said enzyme at a plurality of sites; said method comprising: contacting said enzyme at each of said sites with an aqueous medium containing said substrate and any additional components necessary for the enzymatic catalyzed reaction; irradiating said sites on said irradiation surface at different times in accordance with a predetermined schedule; and determining the electrical photoresponse as modified by said system by means of said circuit as a measure of the amount of said substrate present.
Claim 35
Dependent Claim 12 words
A method according to claim 30, wherein said enzyme is horseradish peroxidase.
Claim 36
Dependent Claim 12 words
A method according to claim 30, wherein said enzyme is glucose oxidase.
Claim 37
Independent Claim 142 words
A method for determining the presence of one or more microorganisms in a medium, said method employing: (a) a photoresponsive electrode having an irradiation surface having a plurality of sites; (b) at least one counterelectrode; (c) an electrical circuit connecting said photoresponsive electrode and counterelectrode and maintaining said electrodes in a predetermined potential relationship; said method comprising: contacting said medium at each of said sites under conditions where said microorganism remains viable and produces at least one metabolic product capable of modulating the photoresponsive of said photoresponsive electrode by means of a change in the detectable redox potential of said medium; irradiating said sites on said irradiation surface at different times in accordance with a predetermined schedule; and determining the electrical photoresponse as modified by said metabolic product by means of said circuit as an indication of the presence of a microorganism.
Claim 38
Independent Claim 142 words
A method for determining the presence of one or more microorganisms in a medium, said method employing: (a) a photoresponsive electrode having an irradiation surface having a plurality of sites; (b) at least one counterelectrode; (c) an electrical circuit connecting said photoresponsive electrode and counterelectrode and maintaining said electrodes in a predetermined potential relationship; said method comprising: contacting said medium at each of said sites under conditions where said microorganism remains viable and produces at least one metabolic product capable of modulating the photoresponsive of said photoresponsive electrode by means of a change in the detectable redox potential of said medium; irradiating said sites on said irradiation surface at different times in accordance with a predetermined schedule; and determining the electrical photoresponse as modified by said metabolic product by means of said circuit as an indication of the presence of a microorganism.
Claim 39
Dependent Claim 20 words
A method according to claim 33, wherein said microorganism is bound by a specific receptor in juxtaposition to said site.
Claim 40
Independent Claim 138 words
A method for detecting the presence of an analyte in a medium, said method employing: (a) a photoresponsive electrode having an irradiation surface having a plurality of sites; (b) at least one counterelectrode; (c) an electrical circuit connecting said photoresponsive electrode and counterelectrode and maintaining said electrodes in a predetermined potential relationship; said method comprising: contacting said medium at each of said sites, wherein said medium contains horseradish peroxidase, hydrogen peroxide and methylene blue, and the amount of horseradish peroxidase in said medium is related to the amount of analyte in said medium, said horseradish peroxidase catalyzing the oxidation of methylene blue; irradiating said sites on said irradiation surface at different times in accordance with a predetermined schedule; and determining the electrical photoresponse as a result of the reaction of the methylene blue at each of said sites.
Claim 41
Independent Claim 138 words
A method for detecting the presence of an analyte in a medium, said method employing: (a) a photoresponsive electrode having an irradiation surface having a plurality of sites; (b) at least one counterelectrode; (c) an electrical circuit connecting said photoresponsive electrode and counterelectrode and maintaining said electrodes in a predetermined potential relationship; said method comprising: contacting said medium at each of said sites, wherein said medium contains horseradish peroxidase, hydrogen peroxide and methylene blue, and the amount of horseradish peroxidase in said medium is related to the amount of analyte in said medium, said horseradish peroxidase catalyzing the oxidation of methylene blue; irradiating said sites on said irradiation surface at different times in accordance with a predetermined schedule; and determining the electrical photoresponse as a result of the reaction of the methylene blue at each of said sites.

References Cited (Backward Citations)

US4020830A Cited
US4020830B1 Cited
US4238757A Cited
US4486272A Cited
US4562157A Cited
US4591550A Cited

USPTO Annuity & Maintenance Windows

Annuity Stage Window Opens Payment Deadline Surcharge Period Until Estimated Fee Status
3.5 Years (Year 4) 1990-11-02 1991-05-04 1991-11-03 $2000.00 Window Closed / Lapsed
7.5 Years (Year 8) 1994-11-02 1995-05-04 1995-11-03 $3760.00 Window Closed / Lapsed
11.5 Years (Year 12) 1998-11-02 1999-05-04 1999-11-03 $7700.00 Window Closed / Lapsed

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