Terahertz signature detection of biological samples in aqueous solution remains a great challenge due to the strong terahertz absorption of water. Here we propose a new preparation process for fabricating a microfluidic chip and use it as an effective sensor to probe the terahertz absorption signatures of microcystin aptamer (a linear single-stranded DNA with 60 nucleotides) dissolved in TE buffer with different concentrations. The microfluidic chip made of silicon includes thousands of 2.4 μm × 2.4 μm square-cross-section channels. One repeatable terahertz absorption signature is detected and recognized around 830 GHz, fitted to a Lorentz oscillator. This signature is theorized to originate from the bending of hydrogen bonds formed between adjacent hydrated DNA bases surrounded by water molecules. Furthermore, the low-lying vibrational modes are also investigated by molecular dynamics simulations which suggest that strong resonant oscillations are highly probable in the 815–830 GHz frequency band.
To reduce the intense terahertz (THz) wave absorption of water and increase the signal-to-noise ratio, the THz spectroscopy detection of biomolecules usually operates using the nanofluidic channel technologies in practice. The effects of confinement due to the existence of nanofluidic channels on the conformation and dynamics of biomolecules are well known. However, studies of confinement effects on the THz spectra of biomolecules are still not clear. In this work, extensive all-atom molecular dynamics simulations are performed to investigate the THz spectra of the glycine oligopeptide solutions in free and confined environments. THz spectra of the oligopeptide solutions confined in carbon nanotubes (CNTs) with different radii are calculated and compared. Results indicate that with the increase of the degree of confinement (the reverse of the radius of CNT), the THz absorption coefficient decreases monotonically. By analyzing the diffusion coefficient and dielectric relaxation dynamics, the hydrogen bond life, and the vibration density of the state of the water molecules in free solution and in CNTs, we conclude that the confinement effects on the THz spectra of biomolecule solutions are mainly to slow down the dynamics of water molecules and hence to reduce the THz absorption of the whole solution in confined environments.
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