We describe several two-dimensional NMR experiments to facilitate the analysis of overcrowded proton-decoupled deuterium spectra of chiral molecules oriented in poly-gamma-benzyl-L-glutamate liquid crystalline solutions. These 2D NMR experiments allow the correlation between the components of each quadrupolar doubtet in the deuterium spectra and then their assignment on the basis of chemical shift. The 2D pulse sequences proposed in this work were developed using the Cartesian spin-operator formalism for spin I = 1 nuclei with a small quadrupolar moment, such as deuterons in high magnetic field. The features and analytical potentialities of each pulse sequence are discussed and compared. Illustrative applications of these sequences in natural abundance deuterium NMR spectroscopyusing a 9.4 T magnetic field and standard NMR equipment are reported and examined. With this technique, it is demonstrated that quantitative measurements are possible within a precision of 10%.