This thesis, entitled Ground state properties of Mn and Mo using laser spectroscopic methods was submitted to The University of Manchester by Miss Frances Claire Charlwood on 2nd October 2010 for the degree Doctor of Philosophy (PhD).An optical study of Mn and Mo isotopes has been performed in two contrasting regions of the nuclear chart. Collinear laser spectroscopic methods were employed using the Ion Guide Separator On-Line (IGISOL) at the University of Jyväskylä, Finland. Optical pumping in an ion-trap with the use of frequency quadrupled titanium sapphire lasers, greatly improved the efficiency of the spectroscopy performed.For the first time, the change in mean-square charge radius was determined for ground and isomeric states in 50-56Mn with a sharp shell closure seen across N = 28. Nuclear quadrupole moments in 50m,53,54,56Mn were also extracted, displaying trends similar to those of the charge radii. Newly extracted hyperfine structures and isotope shifts of 90-92,94-98,100,102-106,108Mo span the N = 50 shell closure and well-known N = 60 shape change. Unlike the Z = 38 - 41 isotopic chains, Mo exhibits a smooth increase in mean-square charge radius, with no sudden onset of deformation at N = 60. These measurements signify the end point of this strongly deformed A ∼ 100 region in both Z and N.In the Z ∼ 40 region, the charge radii follow the trends in the mass measurements near perfectly. However, in the Mn measurements a clear disparity between the mass and charge radii measurements is seen across the N = 28 magic shell closure. The absence of any shell effects in the Mn mass measurements show the importance of charge radii measurements, with pertinent implications for future investigations in the N = 40 region.Additionally, a portable data acquisition system for laser spectroscopy has been successfully tested. It is based on the LabJack system which will directly interface to a USB connection. It is able to register individual photons from amplified and converted photomultiplier tube signals (with bunched or continuous ion beams). The device drives a Cooknell voltage supply, which steps the voltage across the laser-ion interaction region. The introduction of an accurate 100 ms time window into the LabJack system has enabled a precise photon detection system for future off-line testing and on-line use. Further to this, a new method of locating hyperfine resonances has been introduced into our spectroscopy.