US2002115079A1PendingUtilityA1

Process for detecting target nucleic acid, process for quantifying the same, and pyrylium compound for chemiluminescence analysis

Priority: Oct 3, 1996Filed: Aug 17, 2001Published: Aug 22, 2002
Est. expiryOct 3, 2016(expired)· nominal 20-yr term from priority
C12Q 1/6816C07D 335/02C12Q 1/6813C07D 309/34
56
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Claims

Abstract

The present invention provides a process for detecting or quantifying a target nucleic acid in a sample, the process comprising the steps of associating a chemiluminescent compound, capable of being associated with a double-stranded nucleic acid, with a double-stranded nucleic acid including the target nucleic acid, and detecting or measuring chemiluminescence derived from the chemiluminescent compound associated with the double-stranded nucleic acid. According to the process, the target nucleic acid in the sample can be highly sensitively detected, or precisely quantified.

Claims

exact text as granted — not AI-modified
What is claimed is:  
     
         1 . A process for detecting a target single-stranded nucleic acid having a first base sequence, said process comprising the steps of: 
 forming a double-stranded nucleic acid by hybridizing said target single-stranded nucleic acid with a probe nucleic acid having a second base sequence complementary to said first base sequence;    providing a chemiluminescent compound capable of being associated with a double-stranded nucleic acid, and then associating said chemiluminescent compound with the double-stranded nucleic acid resulting from said forming step; and    detecting luminescence from said chemiluminescent compound associated with said double-stranded nucleic acid.    
     
     
         2 . The process according to  claim 1 , wherein the luminescence-detecting step is conducted under a condition that only said chemiluminescent compound associated with said double-stranded nucleic acid can exhibit chemiluminescence.  
     
     
         3 . The process according to  claim 2 , wherein said condition is in an aqueous medium in which said chemiluminescent compound non-associated with a double-stranded nucleic acid does not exhibit chemiluminescence.  
     
     
         4 . The process according to  claim 3 , wherein said aqueous medium is water.  
     
     
         5 . The process according to  claim 3 , wherein said aqueous medium is an aqueous buffer solution.  
     
     
         6 . The process according to  claim 3 , wherein said aqueous medium is a mixture solution of water and an organic solvent miscible with water.  
     
     
         7 . The process according to  claim 6 , wherein said organic solvent comprises at least one solvent selected from the group consisting of methanol, ethanol, acetonitrile, dimethylformamide, dimethylsulfoxide, and isopropanol.  
     
     
         8 . The process according to  claim 6 , wherein said mixture solution has a content of said organic solvent falling within 2 to 50% by volume relative to water.  
     
     
         9 . The process according to  claim 8 , wherein said content falls within 5 to 20% by volume relative to water.  
     
     
         10 . The process according to  claim 3 , wherein pH of said aqueous medium ranges from 5 to 8.  
     
     
         11 . The process according to  claim 1 , wherein said chemiluminescent compound is capable of being inserted into the double helical structure of said double-stranded nucleic acid as an intercalator.  
     
     
         12 . The process according to  claim 11 , wherein said chemiluminescent compound is a pyrylium compound represented by the following formula [1]:  
       
         
           
           
               
               
           
         
       
       wherein: 
 X is O, S, Se or Te;  
 two of R 1 , R 2  and R 3  are independently a substituted or unsubstituted aryl group;  
 the other is a hydrogen atom, halogen atom, sulfonate group, amino group, styryl group, nitro group, hydroxyl group, carboxyl group, cyano group, substituted or unsubstituted alkyl group, substituted or unsubstituted cycloalkyl group, -A or -L-A, wherein: 
 L is -L 1 -, -L 2 -L 3 - or -L 4 -L 5 -L 6 -, wherein each of L 1  to L 6  is independently —(CH═CH)—, a divalent group derived from the substituted or unsubstituted aryl group, a substituted or unsubstituted lower alkylene group, or —CH═R 4 —, wherein R 4  is a ring structure having an oxo group; and  
 A is a substituted or unsubstituted aryl group, or —CH═R 5 , wherein R 5  is a substituted or unsubstituted heterocyclic ring, substituted or unsubstituted cycloalkyl group or substituted or unsubstituted aromatic ring; and  
 
 Y— is an anion.  
 
     
     
         13 . The process according to  claim 12 , wherein L in said formula [1] is any one of the groups represented by the following formulae [2] to [6], respectively:  
       
         
           
           
               
               
           
         
       
       wherein Z is a hydrogen atom or a substituted or unsubstituted lower alkyl group, n is 0, 1 or 2, and φ is a substituted or o-, m- or p-phenylene group.  
     
     
         14 . The process according to  claim 12 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [7]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y — is an anion.  
     
     
         15 . The process according to  claim 14 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         16 . The process according to  claim 12 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [8]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         17 . The process according to  claim 16 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         18 . The process according to  claim 12 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [9]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         19 . The process according to  claim 18 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         20 . The process according to  claim 12 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [10]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         21 . The process according to  claim 20 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         22 . The process according to  claim 12 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [11]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         23 . The process according to  claim 22 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         24 . The process according to  claim 12 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [12]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         25 . The process according to  claim 24 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         26 . The process according to  claim 12 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [13]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         27 . The process according to  claim 26 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         28 . The process according to  claim 12 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [14]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         29 . The process according to  claim 28 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         30 . The process according to  claim 12 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [15]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         31 . The process according to  claim 30 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         32 . The process according to  claim 12 , wherein at least one hydrophilic group is introduced into at least one substituent of said pyrylium compound.  
     
     
         33 . The process according to  claim 1 , wherein said chemiluminescent compound is inserted into said double-stranded nucleic acid by groove binding.  
     
     
         34 . The process according to  claim 1 , wherein said luminescence-detecting step includes allowing said chemiluminescent compound and said double-stranded nucleic acid to coexist with an oxalic ester and hydrogen peroxide.  
     
     
         35 . The process according to  claim 34 , wherein said oxalic ester is bisdinitrophenyl oxalate.  
     
     
         36 . The process according to  claim 1 , wherein said step of forming a double-strand ed nucleic acid includes immobilizing said target nucleic acid or said probe nucleic acid to a solid phase previous to hybridizing said target nucleic acid with said probe nucleic acid.  
     
     
         37 . The process according to  claim 1 , wherein said step of forming a double-stranded nucleic acid includes the steps of: 
 immobilizing said target nucleic acid to a solid phase;    preparing as said probe nucleic acid, a single-stranded nucleic acid capable of binding with said target nucleic acid through complementary sequences at 3′-end regions of the target nucleic acid and the single-stranded nucleic acid;    hybridizing said target nucleic acid with said probe nucleic acid to form a double-stranded nucleic acid; and    polymerizing nucleotides to the 3′-ends of said target nucleic acid and said probe nucleic acid by extension reaction to extend a double-stranded portion in said double-stranded nucleic acid.    
     
     
         38 . The process according to  claim 1 , wherein said step of forming a double-stranded nucleic acid includes the steps of: 
 preparing as said probe nucleic acid, a single-stranded nucleic acid capable of binding with said target nucleic acid through complementary sequences at 3′-end regions of the target nucleic acid and the single-stranded nucleic acid; immobilizing said probe nucleic acid to a solid phase;    hybridizing said target nucleic acid with said probe nucleic acid to form a double-stranded nucleic acid; and    polymerizing nucleotides to the 3′-ends of said target nucleic acid and said probe nucleic acid by extension reaction to extend a double-stranded portion in said double-stranded nucleic acid.    
     
     
         39 . The process according to  claim 36 ,  37  or  38 , wherein said solid phase comprises a plastic plate.  
     
     
         40 . The process according to  claim 1 , wherein said target nucleic acid is DNA or RNA.  
     
     
         41 . The process according to  claim 40 , wherein said DNA is cDNA.  
     
     
         42 . The process according to  claim 40 , wherein said RNA is mRNA, tRNA or rRNA.  
     
     
         43 . The process according to  claim 1 , wherein said probe nucleic acid is DNA or RNA.  
     
     
         44 . The process according to  claim 1 , wherein said target nucleic acid is mRNA comprising a base sequence corresponding to oligoriboadenylic acid at 3′-end region thereof, and said probe nucleic acid comprises a base sequence corresponding to oligodeoxyribothymidylic acid or polydeoxyribothymidylic acid, the base sequence relating to hybridization with said target nucleic acid.  
     
     
         45 . A process for quantifying a target single-stranded nucleic acid having a first base sequence, said process comprising the steps of: 
 forming a double-stranded nucleic acid by hybridizing said target single-stranded nucleic acid with a probe nucleic acid having a second base sequence complementary to said first base sequence;    providing a chemiluminescent compound capable of being associated with a double-stranded nucleic acid, and then associating said chemiluminescent compound with the double-stranded nucleic acid resulting from said forming step; and    measuring luminescence from said chemiluminescent compound associated with said double-stranded nucleic acid.    
     
     
         46 . The process according to  claim 45 , wherein the luminescence-measuring step is conducted under a condition that only said chemiluminescent compound associated with said double-stranded nucleic acid can exhibit chemiluminescence.  
     
     
         47 . The process according to  claim 46 , wherein said condition is in an aqueous medium in which said chemiluminescent compound non-associated with a double-stranded nucleic acid does not exhibit chemiluminescence.  
     
     
         48 . The process according to  claim 47 , wherein said aqueous medium is water.  
     
     
         49 . The process according to  claim 47 , wherein said aqueous medium is an aqueous buffer solution.  
     
     
         50 . The process according to  claim 47 , wherein said aqueous medium is a mixture solution of water and an organic solvent miscible with water.  
     
     
         51 . The process according to  claim 50 , wherein said organic solvent comprises at least one solvent selected from the group consisting of methanol, ethanol, acetonitrile, dimethylformamide, dimethylsulfoxide, and isopropanol.  
     
     
         52 . The process according to  claim 50 , wherein said mixture solution has a content of said organic solvent falling within 2 to 50% by volume relative to water.  
     
     
         53 . The process according to  claim 52 , wherein said content falls within 5 to 20% by volume relative to water.  
     
     
         54 . The process according to  claim 47 , wherein pH of said aqueous medium ranges from 5 to 8.  
     
     
         55 . The process according to  claim 45 , wherein said chemiluminescent compound is capable of being inserted into the double helical structure of said double-stranded nucleic acid as an intercalator.  
     
     
         56 . The process according to  claim 55 , wherein said chemiluminescent compound is a pyrylium compound represented by the following formula [1]:  
       
         
           
           
               
               
           
         
       
       wherein: 
 X is O, S, Se or Te;  
 two of R 1 , R 2  and R 3  are independently a substituted or unsubstituted aryl group;  
 the other is a hydrogen atom, halogen atom, sulfonate group, amino group, styryl group, nitro group, hydroxyl group, carboxyl group, cyano group, substituted or unsubstituted alkyl group, substituted or unsubstituted cycloalkyl group, -A or -L-A, wherein: 
 L is -L 1 -, -L 2 -L 3 - or -L 4 -L 5 -L 6 -, wherein each of L 1  to L 6  is independently —(CH═CH)—, a divalent group derived from the substituted or unsubstituted aryl group, a substituted or unsubstituted lower alkylene group, or —CH═R 4 —, wherein R 4  is a ring structure having an oxo group; and  
 A is a substituted or unsubstituted aryl group, or —CH═R 5 , wherein R 5  is a substituted or unsubstituted heterocyclic ring, substituted or unsubstituted cycloalkyl group or substituted or unsubstituted aromatic ring; and  
 
 Y— is an anion.  
 
     
     
         57 . The process according to  claim 56 , wherein L in said formula [1] is any one of the groups represented by the following formulae [2] to [6], respectively:  
       
         
           
           
               
               
           
         
       
       -φ-(CH═CH)n-   [3]; —CH═CH-φ-CH═CH—  [4];  
       
         
           
           
               
               
           
         
       
       wherein Z is a hydrogen atom or a substituted or unsubstituted lower alkyl group, n is 0, 1 or 2, and φ is a substituted or unsubstituted o-, m- or p-phenylene group.  
     
     
         58 . The process according to  claim 56 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [7]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         59 . The process according to  claim 58 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         60 . The process according to  claim 56 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [8]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         61 . The process according to  claim 60 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         62 . The process according to  claim 56 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [9]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         63 . The process according to  claim 62 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         64 . The process according to  claim 56 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [10]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         65 . The process according to  claim 64 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         66 . The process according to  claim 56 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [11]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         67 . The process according to  claim 66 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         68 . The process according to  claim 56 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [12]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         69 . The process according to  claim 68 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         70 . The process according to  claim 56 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [13]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         71 . The process according to  claim 70 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         72 . The process according to  claim 56 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [14]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         73 . The process according to  claim 72 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         74 . The process according to  claim 56 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [15]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         75 . The process according to  claim 74 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         76 . The process according to  claim 56 , wherein at least one hydrophilic group is introduced into at least one substituent of said pyrylium compound.  
     
     
         77 . The process according to  claim 45 , wherein said chemiluminescent compound is inserted into said double-stranded nucleic acid by groove binding.  
     
     
         78 . The process according to  claim 45 , wherein said luminescence-measuring step includes allowing said chemiluminescent compound and said double-stranded nucleic acid to coexist with an oxalic ester and hydrogen peroxide.  
     
     
         79 . The process according to  claim 78 , wherein said oxalic ester is bisdinitrophenyl oxalate.  
     
     
         80 . The process according to  claim 45 , wherein said step of forming a double-stranded nucleic acid includes immobilizing said target nucleic acid or said probe nucleic acid to a solid phase previous to hybridizing said target nucleic acid with said probe nucleic acid.  
     
     
         81 . The process according to  claim 45 , wherein said step of forming a double-stranded nucleic acid includes the steps of: 
 immobilizing said target nucleic acid to a solid phase;    preparing as said probe nucleic acid, a single-stranded nucleic acid capable of binding with said target nucleic acid through complementary sequences at 3′-end regions of the target nucleic acid and the single-stranded nucleic acid;    hybridizing said target nucleic acid with said probe nucleic acid to form a double-stranded nucleic acid; and    polymerizing nucleotides to the 3′-ends of said target nucleic acid and said probe nucleic acid by extension reaction to extend a double-stranded portion in said double-stranded nucleic acid.    
     
     
         82 . The process according to  claim 45 , wherein said step of forming a double-stranded nucleic acid includes the steps of: 
 preparing as said probe nucleic acid, a single-stranded nucleic acid capable of binding with said target nucleic acid through complementary sequences at 3′-end regions of the target nucleic acid and the single-stranded nucleic acid;    immobilizing said probe nucleic acid to a solid phase;    hybridizing said target nucleic acid with said probe nucleic acid to form a double-stranded nucleic acid; and    polymerizing nucleotides to the 3′-ends of said target nucleic acid and said probe nucleic acid by extension reaction to extend a double-stranded portion in said double-stranded nucleic acid.    
     
     
         83 . The process according to  claim 80 ,  81  or  82 , wherein said solid phase comprises a plastic plate.  
     
     
         84 . The process according to  claim 45 , wherein said target nucleic acid is DNA or RNA.  
     
     
         85 . The process according to  claim 84 , wherein said DNA is cDNA.  
     
     
         86 . The process according to  claim 84 , wherein said RNA is mRNA, tRNA or rRNA.  
     
     
         87 . The process according to  claim 45 , wherein said probe nucleic acid is DNA or RNA.  
     
     
         88 . The process according to  claim 45 , wherein said target nucleic acid is MRNA comprising a base sequence corresponding to oligoriboadenylic acid at 3′-end region thereof, and said probe nucleic acid comprises a base sequence corresponding to oligodeoxyribothymidylic acid or polydeoxyribothymidylic acid, the base sequence relating to hybridization with said target nucleic acid.  
     
     
         89 . A process for detecting a target double-stranded nucleic acid comprising the steps of: 
 providing a chemiluminescent compound capable of being associated with a double-stranded nucleic acid, and then associating said chemiluminescent compound with the target double-stranded nucleic acid; and    detecting luminescence from said chemiluminescent compound associated with said target double-stranded nucleic acid.    
     
     
         90 . The process according to  claim 89 , wherein the luminescence-detecting step is conducted under a condition that only said chemiluminescent compound associated with said double-stranded nucleic acid can exhibit chemiluminescence.  
     
     
         91 . The process according to  claim 90 , wherein said condition is in an aqueous medium in which said chemiluminescent compound non-associated with a double-stranded nucleic acid does not exhibit chemiluminescence.  
     
     
         92 . The process according to  claim 91 , wherein said aqueous medium is water.  
     
     
         93 . The process according to  claim 91 , wherein said aqueous medium is an aqueous buffer solution.  
     
     
         94 . The process according to  claim 91 , wherein said aqueous medium is a mixture solution of water and an organic solvent miscible with water.  
     
     
         95 . The process according to  claim 94 , wherein said organic solvent comprises at least one solvent selected from the group consisting of methanol, ethanol, acetonitrile, dimethylformamide, dimethylsulfoxide, and isopropanol.  
     
     
         96 . The process according to  claim 94 , wherein said mixture solution has a content of said organic solvent falling within 2 to 50% by volume relative to water.  
     
     
         97 . The process according to  claim 96 , wherein said content falls within 5 to 20% by volume relative to water.  
     
     
         98 . The process according to  claim 91 , wherein pH of said aqueous medium ranges from 5 to 8.  
     
     
         99 . The process according to  claim 89 , wherein said chemiluminescent compound is capable of being inserted into the double helical structure of said double-stranded nucleic acid as an intercalator.  
     
     
         100 . The process according to  claim 99 , wherein said chemiluminescent compound is a pyrylium compound represented by the following formula [1]:  
       
         
           
           
               
               
           
         
       
       wherein: 
 X is O, S, Se or Te;  
 two of R 1 , R 2  and R 3  are independently a substituted or unsubstituted aryl group;  
 the other is a hydrogen atom, halogen atom, sulfonate group, amino group, styryl group, nitro group, hydroxyl group, carboxyl group, cyano group, substituted or unsubstituted alkyl group, substituted or unsubstituted cycloalkyl group, -A or -L-A, wherein: 
 L is -L 1 -, -L 2 -L 3 - or -L 4 -L 5 -L 6 -, wherein each of L 1  to L 6  is independently —(CH═CH)—, a divalent group derived from the substituted or unsubstituted aryl group, a substituted or unsubstituted lower alkylene group, or —CH═R 4 —, wherein R 4  is a ring structure having an oxo group; and  
 A is a substituted or unsubstituted aryl group, or —CH═R 5 , wherein R 5  is a substituted or unsubstituted heterocyclic ring, substituted or unsubstituted cycloalkyl group or substituted or unsubstituted aromatic ring; and  
 
 Y— is an anion.  
 
     
     
         101 . The process according to  claim 100 , wherein L in said formula [1] is any one of the groups represented by the following formulae [2] to [6], respectively:  
       
         
           
           
               
               
           
         
       
       -φ-(CH═CH) n-   [3]; —CH═CH-φ-CH═CH—  [];  
       
         
           
           
               
               
           
         
       
       wherein Z is a hydrogen atom or a substituted or unsubstituted lower alkyl group, n is 0, 1 or 2, and φ is a substituted or unsubstituted o-, m- or p-phenylene group.  
     
     
         102 . The process according to  claim 100 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [7]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         103 . The process according to  claim 102 , wherein X is or S, and Y is I or ClO 4 .  
     
     
         104 . The process according to  claim 100 , wherein said chemiluminescent compound represented by said formula [1] is compound represented by the following formula [8]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         105 . The process according to  claim 104 , wherein X is or S, and Y is I or ClO 4 .  
     
     
         106 . The process according to  claim 100 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [9]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         107 . The process according to  claim 106 , wherein X is or S, and Y is I or ClO 4 .  
     
     
         108 . The process according to  claim 100 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [10]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         109 . The process according to  claim 108 , wherein X is or S, and Y is I or ClO 4 .  
     
     
         110 . The process according to  claim 100 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [11]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         111 . The process according to  claim 110 , wherein X is or S, and Y is I or ClO 4 .  
     
     
         112 . The process according to  claim 100 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [12]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         113 . The process according to  claim 112 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         114 . The process according to  claim 100 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [13]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         115 . The process according to  claim 114 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         116 . The process according to  claim 100 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [14]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         117 . The process according to  claim 116 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         118 . The process according to  claim 100 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [15]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         119 . The process according to  claim 118 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         120 . The process according to  claim 100 , wherein at least one hydrophilic group is introduced into at least one substituent of said pyrylium compound.  
     
     
         121 . The process according to  claim 89 , wherein said luminescence-detecting step includes allowing said chemiluminescent compound and said double-stranded nucleic acid to coexist with an oxalic ester and hydrogen peroxide.  
     
     
         122 . The process according to  claim 121 , wherein said oxalic ester is bisdinitrophenyl oxalate.  
     
     
         123 . The process according to  claim 89 , wherein said chemiluminescent compound is inserted into said double-stranded nucleic acid by groove binding.  
     
     
         124 . A process for quantifying a target double-stranded nucleic acid comprising the steps of: 
 providing a chemiluminescent compound capable of being associated with a double-stranded nucleic acid, and then associating said chemiluminescent compound with the target double-stranded nucleic acid; and    measuring luminescence from said chemiluminescent compound associated with said target double-stranded nucleic acid.    
     
     
         125 . The process according to  claim 124 , wherein the luminescence-measuring step is conducted under a condition that only said chemiluminescent compound associated with said double-stranded nucleic acid can exhibit chemiluminescence.  
     
     
         126 . The process according to  claim 125 , wherein said condition is in an aqueous medium in which said chemiluminescent compound non-associated with a double-stranded nucleic acid does not exhibit chemiluminescence.  
     
     
         127 . The process according to  claim 126 , wherein said aqueous medium is water.  
     
     
         128 . The process according to  claim 126 , wherein said aqueous medium is an aqueous buffer solution.  
     
     
         129 . The process according to  claim 126 , wherein said aqueous medium is a mixture solution of water and an organic solvent miscible with water.  
     
     
         130 . The process according to  claim 129 , wherein said organic solvent comprises at least one solvent selected from the group consisting of methanol, ethanol, acetonitrile, dimethylformamide, dimethylsulfoxide, and isopropanol.  
     
     
         131 . The process according to  claim 129 , wherein said mixture solution has a content of said organic solvent falling within 2 to 50% by volume relative to water.  
     
     
         132 . The process according to  claim 131 , wherein said content falls within 5 to 20% by volume relative to water.  
     
     
         133 . The process according to  claim 126 , wherein pH of said aqueous medium ranges from 5 to 8.  
     
     
         134 . The process according to  claim 124 , wherein said chemiluminescent compound is capable of being inserted into the double helical structure of said double-stranded nucleic acid as an intercalator.  
     
     
         135 . The process according to  claim 134 , wherein said chemiluminescent compound is a pyrylium compound represented by the following formula [1]:  
       
         
           
           
               
               
           
         
       
       wherein: 
 X is O, S, Se or Te;  
 two of R 1 , R 2  and R 3  are independently a substituted or unsubstituted aryl group;  
 the other is a hydrogen atom, halogen atom, sulfonate group, amino group, styryl group, nitro group, hydroxyl group, carboxyl group, cyano group, substituted or unsubstituted alkyl group, substituted or unsubstituted cycloalkyl group, -A or -L-A, wherein: 
 L is -L 1 -, -L 2 -L 3 - or -L 4 -L 5 -L 6 -, wherein each of L 1  to L 6  is independently —(CH═CH)—, a divalent group derived from the substituted or unsubstituted aryl group, a substituted or unsubstituted lower alkylene group, or —CH═R 4 —, wherein R 4  is a ring structure having an oxo group; and  
 A is a substituted or unsubstituted aryl group, or —CH═R 5 , wherein R 5  is a substituted or unsubstituted heterocyclic ring, substituted or unsubstituted cycloalkyl group or substituted or unsubstituted aromatic ring; and  
 
 Y— is an anion.  
 
     
     
         136 . The process according to  claim 135 , wherein L in said formula [1] is any one of the groups represented by the following formulae [2] to [6], respectively:  
       
         
           
           
               
               
           
         
       
       -φ- (CH═CH) n-   [3]; —CH═CH-φ-CH═CH—  [4];  
       
         
           
           
               
               
           
         
       
       wherein Z is a hydrogen atom or a substituted or unsubstituted lower alkyl group, n is 0, 1 or 2, and φ is a substituted or unsubstituted o-, m- or p-phenylene group.  
     
     
         137 . The process according to  claim 135 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [7]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         138 . The process according to  claim 137 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         139 . The process according to  claim 135 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [8]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         140 . The process according to  claim 139 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         141 . The process according to  claim 135 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [9]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         142 . The process according to  claim 141 , wherein X is or S, and Y is I or ClO 4 .  
     
     
         143 . The process according to  claim 135 , wherein said chemiluminescent compound represented by said formula [1] is a compound represented by the following formula [10]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         144 . The process according to  claim 143 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         145 . The process according to  claim 135 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [11]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         146 . The process according to  claim 145 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         147 . The process according to  claim 135 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [12]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         148 . The process according to  claim 147 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         149 . The process according to  claim 135 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [13]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         150 . The process according to  claim 149 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         151 . The process according to  claim 135 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [14]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         152 . The process according to  claim 151 , wherein X is or S, and Y is I or ClO 4 .  
     
     
         153 . The process according to  claim 135 , wherein said chemiluminescent compound represented by said formula [1] is the compound represented by the following formula [15]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         154 . The process according to  claim 153 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         155 . The process according to  claim 135 , wherein at least one hydrophilic group is introduced into at least one substituent of said pyrylium compound.  
     
     
         156 . The process according to  claim 124 , wherein said luminescence-measuring step includes allowing said chemiluminescent compound and said double-stranded nucleic acid to coexist with an oxalic ester and hydrogen peroxide.  
     
     
         157 . The process according to  claim 156 , wherein said oxalic ester is bisdinitrophenyl oxalate.  
     
     
         158 . The process according to  claim 124 , wherein said chemiluminescent compound is inserted into said double-stranded nucleic acid by groove binding.  
     
     
         159 . A process for detecting a target single-stranded nucleic acid having a first base sequence, said process comprising the steps of: 
 forming a double-stranded nucleic acid by hybridizing said target single-stranded nucleic acid with a probe nucleic acid having a second base sequence complementary to said first base sequence;    providing a compound which can be intercalated into a double-stranded nucleic acid and which is capable of exhibiting chemiluminescence only in a hydrophobic condition, and then intercalating said compound into the double-stranded nucleic acid resulting from said forming step; and    placing in an aqueous medium said double-stranded nucleic acid into which said compound is intercalated together with a reagent capable of causing said compound to exhibit chemiluminescence, and detecting the resulting chemiluminescence.    
     
     
         160 . A process for quantifying a target single-stranded nucleic acid having a first base sequence, said process comprising the steps of: 
 forming a double-stranded nucleic acid by hybridizing said target single-stranded nucleic acid with a probe nucleic acid having a second base sequence complementary to said first base sequence;    providing a compound which can be intercalated into a double-stranded nucleic acid and which is capable of exhibiting chemiluminescence only in a hydrophobic condition, and then intercalating said compound into the double-stranded nucleic acid resulting from said forming step; and    placing in an aqueous medium said double-stranded nucleic acid into which said compound is intercalated together with a reagent capable of causing said compound to exhibit chemiluminescence, and measuring the resulting chemiluminescence.    
     
     
         161 . A process for detecting a target double-stranded nucleic acid comprising the steps of: 
 providing a compound which can be intercalated into a double-stranded nucleic acid and which is capable of exhibiting substantial chemiluminescence only in a hydrophobic condition, and then intercalating said compound into said target double-stranded nucleic acid; and    placing in an aqueous medium said double-stranded nucleic acid into which said compound is intercalated together with a reagent capable of causing said compound to exhibit chemiluminescence, and detecting the resulting chemiluminescence.    
     
     
         162 . A process for quantifying a target double-stranded nucleic acid comprising the steps of: 
 providing a compound which can be intercalated into a double-stranded nucleic acid and which is capable of exhibiting substantial chemiluminescence only in a hydrophobic condition, and then intercalating said compound into said target double-stranded nucleic acid; and    placing in an aqueous medium said double-stranded nucleic acid into which said compound is intercalated together with a reagent capable of causing said compound to exhibit chemiluminescence, and measuring the resulting chemiluminescence.    
     
     
         163 . The detecting process according to  claim 159  or  161 , wherein said compound is a pyrylium compound represented by the following formula [1]:  
       
         
           
           
               
               
           
         
       
       wherein: 
 X is O, S, Se or Te;  
 two of R 1 , R 2  and R 3  are independently a substituted or unsubstituted aryl group;  
 the other is a hydrogen atom, halogen atom, sulfonate group, amino group, styryl group, nitro group, hydroxyl group, carboxyl group, cyano group, substituted or unsubstituted alkyl group, substituted or unsubstituted cycloalkyl group, -A or -L-A, wherein: 
 L is -L 1 -, -L 2 -L 3 - or -L 4 -L 5 -L 6 -, wherein each of L 1  to L 6  is independently —(CH═CH)—, a divalent group derived from the substituted or unsubstituted aryl group, a substituted or unsubstituted lower alkylene group, or —CH═R 4 —, wherein R 4  is a ring structure having an oxo group; and  
 A is a substituted or unsubstituted aryl group, or —CH═R 5 , wherein R 5  is a substituted or unsubstituted heterocyclic ring, substituted or unsubstituted cycloalkyl group or substituted or unsubstituted aromatic ring; and  
 
 Y— is an anion.  
 
     
     
         164 . The quantifying process according to  claim 160  or  162 , wherein said compound is a pyrylium compound represented by the following formula [1]:  
       
         
           
           
               
               
           
         
       
       wherein: 
 X is O, S, Se or Te;  
 two of R 1 , R 2  and R 3  are independently a substituted or unsubstituted aryl group;  
 the other is a hydrogen atom, halogen atom, sulfonate group, amino group, styryl group, nitro group, hydroxyl group, carboxyl group, cyano group, substituted or unsubstituted alkyl group, substituted or unsubstituted cycloalkyl group, -A or -L-A, wherein: 
 L is -L 1 -, -L 2 -L 3 - or -L 4 -L 5 -L 6 -, wherein each of L 1  to L 6  is independently —(CH═CH)—, a divalent group derived from the substituted or unsubstituted aryl group, a substituted or unsubstituted lower alkylene group, or —CH═R 4 —, wherein R 4  is a ring structure having an oxo group; and  
 A is a substituted or unsubstituted aryl group, or —CH═R 5 , wherein R 5  is a substituted or unsubstituted heterocyclic ring, substituted or unsubstituted cycloalkyl group or substituted or unsubstituted aromatic ring; and  
 
 Y— is an anion.  
 
     
     
         165 . A pyrylium compound represented by the following formula [1] for use in chemiluminescence analysis:  
       
         
           
           
               
               
           
         
       
       wherein: 
 X is O, S, Se or Te;  
 two of R 1 , R 2  and R 3  are independently a substituted or unsubstituted aryl group;  
 the other is a hydrogen atom, halogen atom, sulfonate group, amino group, styryl group, nitro group, hydroxyl group, carboxyl group, cyano group, substituted or unsubstituted alkyl group, substituted or unsubstituted cycloalkyl group, -A or -L-A, wherein: 
 L is -L 1 -, -L 2 -L 3 - or -L 4 -L 5 -L 6 -, wherein each of L 1  to L 6  is independently —(CH═CH)—, a divalent group derived from the substituted or unsubstituted aryl group, a substituted or unsubstituted lower alkylene group, or —CH═R 4 —, wherein R 4  is a ring structure having an oxo group; and  
 
 A is a substituted or unsubstituted aryl group, or —CH═R 5 , wherein R 5  is a substituted or unsubstituted heterocyclic ring, substituted or unsubstituted cycloalkyl group or substituted or unsubstituted aromatic ring; and  
 Y— is an anion.  
 
     
     
         166 . The pyrylium compound according to  claim 165 , wherein L in said formula [1] is any one of the groups represented by the following formulae [2] to [6], respectively:  
       
         
           
           
               
               
           
         
       
       -φ-(CH═CH) n-   [3]; —CH═CH-φ-CH═CH—  [4];  
       
         
           
           
               
               
           
         
       
       wherein Z is a hydrogen atom or a substituted or unsubstituted lower alkyl group, n is 0, 1 or 2, and φ is a substituted or unsubstituted o-, m- or p-phenylene group.  
     
     
         167 . The pyrylium compound according to  claim 165 , represented by the following formula [7]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         168 . The pyrylium compound according to  claim 167 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         169 . The pyrylium compound according to  claim 165 , represented by the following formula [8]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         170 . The pyrylium compound according to  claim 169 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         171 . The pyrylium compound according to  claim 165 , represented by the following formula [9]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         172 . The pyrylium compound according to  claim 171 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         173 . The pyrylium compound according to  claim 165 , represented by the following formula [10]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         174 . The pyrylium compound according to  claim 173 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         175 . The pyrylium compound according to  claim 165 , represented by the following formula [11]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         176 . The pyrylium compound according to  claim 175 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         177 . The pyrylium compound according to  claim 165 , represented by the following formula [12]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         178 . The pyrylium compound according to  claim 177 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         179 . The pyrylium compound according to  claim 165 , represented by the following formula [13]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         180 . The pyrylium compound according to  claim 179 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         181 . The pyrylium compound according to  claim 165 , represented by the following formula [14]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         182 . The pyrylium compound according to  claim 181 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         183 . The pyrylium compound according to  claim 165 , represented by the formula [15]:  
       
         
           
           
               
               
           
         
       
       wherein X is O, S, Se, or Te, and Y— is an anion.  
     
     
         184 . The pyrylium compound according to  claim 183 , wherein X is O or S, and Y is I or ClO 4 .  
     
     
         185 . The pyrylium compound according to  claim 165 , wherein at least one hydrophilic group is introduced into at least one substituent of said pyrylium compound.

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