On the structure and desorption dynamics of DNA bases adsorbed on gold:: A temperature-programmed study

被引:133
作者
Östblom, M
Liedberg, B [1 ]
Demers, LM
Mirkin, CA
机构
[1] Linkoping Univ, Dept Phys Chem & Biol, Div Mol Phys, S-58183 Linkoping, Sweden
[2] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[3] Northwestern Univ, Ctr Nanofabricat & Mol Self Assembly, Evanston, IL 60208 USA
关键词
D O I
10.1021/jp051617b
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The structure and desorption dynamics of mono- and multilayer samples of adenine, cytosine, guanine, and thymine on polycrystalline gold thin films are studied using temperature-programmed desorption-infrared reflection absorption spectroscopy (TPD-IRAS) and temperature-programmed desorption-mass spectroscopy (TPD-MS). It is shown that the pyrimidines, adenine and guanine, adsorb to gold in a complex manner and that both adhesive (adenine) and cohesive (guanine) interactions contribute the apparent binding energies to the substrate surface. Adenine displays at least two adsorption sites, including a high-energy site (210 degrees C, similar to 136 kJ/mol), wherein the molecule coordinates to the gold substrate via the NH2 group in an sp(3)-like, strongly perturbed, nonplanar configuration. The purines, cytosine and thymine, display a less complicated adsorption/desorption behavior. The desorption energy for cytosine (160 degrees C, similar to 122 kJ/mol) is similar to those obtained for adenine and guanine, but desorption occurs from a single site of dispersed, nonaggregated cytosine. Thymine desorbs also from a single site but at a significantly lower energy (100 degrees C, similar to 104 kJ/mol). Infrared data reveal that the monolayer architectures discussed herein are structurally very different from those observed for the bases in the bulk crystalline state. It is also evident that both pyrimidines and purines adsorb on gold with the plane of the molecule in a nonparallel orientation with respect to the substrate surface. The results of this work are discussed in the context of improving the understanding of the design of capturing oligonucleotides or DNA strands for bioanalytical applications, in particular, for gold nanoparticle-based assays.
引用
收藏
页码:15150 / 15160
页数:11
相关论文
共 54 条
  • [1] Neutron inelastic scattering, optical spectroscopies, and scaled quantum mechanical force fields for analyzing the vibrational dynamics of pyrimidine nucleic acid bases. Thymine
    Aamouche, A
    Ghomi, M
    Coulombeau, C
    Grajcar, L
    Baron, MH
    Jobic, H
    Berthier, G
    [J]. JOURNAL OF PHYSICAL CHEMISTRY A, 1997, 101 (10) : 1808 - 1817
  • [2] Vibrational modes in thymine molecule from an ab initio MO calculation
    Aida, M
    Kaneko, M
    Dupuis, M
    Ueda, T
    Ushizawa, K
    Ito, G
    Kumakura, A
    Tsuboi, M
    [J]. SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 1997, 53 (03) : 393 - 407
  • [3] Surface enhanced vibrational spectra of thymine
    Aroca, R
    Bujalski, R
    [J]. VIBRATIONAL SPECTROSCOPY, 1999, 19 (01) : 11 - 21
  • [4] In situ infrared study of cytosine adsorption on gold electrodes
    Ataka, K
    Osawa, M
    [J]. JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1999, 460 (1-2) : 188 - 196
  • [5] Real-time multicolor DNA detection with chemoresponsive diffraction gratings and nanoparticle probes
    Bailey, RC
    Nam, JM
    Mirkin, CA
    Hupp, JT
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (44) : 13541 - 13547
  • [6] DIRECT MEASUREMENT OF HYDROGEN-BONDING IN DNA NUCLEOTIDE BASES BY ATOMIC-FORCE MICROSCOPY
    BOLAND, T
    RATNER, BD
    [J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1995, 92 (12) : 5297 - 5301
  • [7] 2-DIMENSIONAL ASSEMBLY OF PURINES AND PYRIMIDINES ON AU(111)
    BOLAND, T
    RATNER, BD
    [J]. LANGMUIR, 1994, 10 (10) : 3845 - 3852
  • [8] DNA-modified core-shell Ag/Au nanoparticles
    Cao, YW
    Jin, R
    Mirkin, CA
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2001, 123 (32) : 7961 - 7962
  • [9] Self-assembly of adenine on Cu(110) surfaces
    Chen, Q
    Frankel, DJ
    Richardson, NV
    [J]. LANGMUIR, 2002, 18 (08) : 3219 - 3225
  • [10] Thermal desorption behavior and binding properties of DNA bases and nucleosides on gold
    Demers, LM
    Östblom, M
    Zhang, H
    Jang, NH
    Liedberg, B
    Mirkin, CA
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2002, 124 (38) : 11248 - 11249