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In this thesis the control of ultrafast (10⁻¹³ s) optical pulses used for metrological applications has been investigated. Two different measurement set-ups have been considered, both based around the `pump-probe' technique, where an optical pulse is divided into two parts, one to `pump' or excite a physical system of interest, the other to `probe' or measure the outcome. In both cases the measurement uses electro-optic sampling (EOS), where an electric field is measured by detecting changes in the optical probe pulse polarisation after interaction with the field. In the first study, a method for wavelength metrology in the terahertz (THz) region has been demonstrated by producing an optical pulse shaper and genetic algorithm to control pump pulses and so indirectly influence the THz spectra they generate. In the second study an OPO (optical parametric oscillator) has been developed to provide ultrafast optical pulses for the generation of < 100 fs electrical pulses for metrology using quantum interference control (QUIC). QUIC electrical signals have been demonstrated successfully by charge accumulation measurements and the QUIC electrical pulse temporally measured using EOS, though the low signal levels due to power restrictions mean the QUIC electrical pulse is unsuitable for metrology at this time. Finally, a portable optical pulse measurement device based around frequency-resolved optical gating (FROG) has been designed, built and tested. This has been shown to be capable of retrieving amplitude and phase information in both the temporal and spectral domains for optical pulses as short as 20 fs duration. The ability to characterise shaped pulses also has been demonstrated successfully, with the requirements for full automation identified.