208 Sensors and Actuators B, 6 (1992) 208-210
Langmuir-Blodgett film based membrane for DNA-probe biosensor
M. A. Karymov, A. A. Kruchinin, Yu. A. Tarantov, I. A. Balova, L. A. Remisova,
N. G. Sukhodolov and A. I. Yanklovich
Department of Chemistry, St. Petersburg University, Peterhof, St. Petersburg 198904 (Russia)
A. M. Yorkin
Department of Genetics, St. Petersburg University, Peterhof, St. Petersburg 198904 (Russia)
Abstract
Covalent attachment of DNA to diacetylene film produced on the surface of oxidized silicon by the Langmuir-
Blodgett technique has been studied. Coupling of phage M13 DNA with polymer film was carried out by the
carbodiimide method and by the formation of linker structures. Sorption capacity and hybridization efficiency
determined using the radioactive label 32p were about 10-20 pg mm -2 and near 100%, respectively.
1. Introduction
There is a growing interest in the development
of microelectronic sensors for detecting biological
substrata and antigens; the DNA-probe based sen-
sor is one of them [ 1]. This sensor can be used for
DNA detection in express diagnostics of gene
deaths and for specific bacterial gene (e.g. toxin
genes) disclosure. It should comprise a solid-state
transducer and a membrane with an immobilized
DNA-probe, the DNA having a specific nucleotide
sequence. Hybridization of a DNA-probe with
analyzed DNA will lead to a change of mass,
electrical charge or optical properties of the mem-
brane to be detected by gravimetric, potentiomet-
ric or optical transducers. Methods for the
membrane deposition on the surface of the solid
substrate should be compatible with microelec-
tronic technology, as well as allowing DNA immo-
bilization and hybridizatio n . It must also be
mechanically and electrically stable.
In this work a membrane for a DNA-probe
biosensor based on Langmuir-Blodgett (LB) di-
acetylene film with covalently bonded DNA has
been developed.
2. Experimental
Replicative and single-stranded forms of bacte-
riophage M 13 DNA with 6400 nucleotides pre-
pared by the routine method [2] were used in
experiments. The replicative form was labelled by
nick translation with [0~-32p] dNTP and had a
specific activity 3 x 109 cpm Ixg -1. An LS Beckman
100C counter was used to determine the DNA
sorption capacity of the diacetylene film and im-
mobilized DNA hybridization efficiency.
Diacetylene films were produced on the surface
of oxidized silicon wafers by the conventional LB
technique [3]. For this purpose the amphiphilic
diacetylene acids, 7,9-dokozadiynic CI2H25C=--C-
C-C-(CH2)sCOOH (C22 acid) and 3,5-octa-
decadiynic C~0H21C-C-C-C-(CH2)3COOH (C18
acid), were synthesized according to ref. 4, with
prototropic isomerization of diacetylene hydro-
carbons by lithium 2-aminoethylamide as a princi-
pal stage. The formed terminal isomer was
alkylated by to-Br alkanols with a covered hydroxyl
group. Using this method it was possible
to obtain amphiphilic diacetylene acids with a fixed
number of methylene groups between triple bonds
and a functional group from accessible initial
reagents by three stages of synthesis in one flask.
Polished silicon wafers were thermally oxidized
at 1100 °C in dry oxygen. The silicon dioxide film
thickness was 100 nm. The hydrophobization pro-
cedure included treatment in a 10% solution of
dimethyldichlorosilane in chloroform (20min at
room temperature) and subsequent annealing for
2 h at 180 °C in air. Previously hydrophobization
samples were boiled for 8 h in distilled water.
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