Phonon dispersion of oriented DNA by inelastic x-ray scattering

Abstract

Films of oriented deoxyribonucleic acid (DNA), prepared by the wet spinning method, have been studied using inelastic x-ray scattering. Spectra were recorded within the range of energy transfers -30< homega <30 meV at momentum transfers homegaQ ranging from 2.5 to 30 nm(-1) whereby the direction of Q essentially coincided with the helical axis. Measurements at ambient temperature cover samples in the A, B, C, and D conformations of DNA. Within the limits of the instrumental resolution, the spectra were analyzed by the response of a damped harmonic oscillator delivering dispersion and damping of modes having displacements with nonzero projections onto Q, i.e., essentially the compression waves traveling along the helical axis. The longitudinal speed of sound resulting from the sinusoidal dispersion varies only weakly with conformation. Our sound speed values are compared to results from Brillouin spectroscopy. The dispersion curves exhibit a minimum at about the inverse rise per residue, which -- together with strong elastic scattering -- reflect the large degree of disorder. Overdamping of the modes is observed for Q>5 nm(-1). The possibility that the observed large damping parameters are due to several contributing modes is discussed in terms of a simple model calculation for an idealized double helix. Whereas the quasicrystalline approximation for an effective disordered chain could well describe the sinusoidal dispersion, it fails to reproduce the observed damping by one order of magnitude. Our results indicate that the high-frequency dynamics of DNA is liquidlike and is most appropriately described by instantaneous normal modes of short correlation length.