Bulk metallic glasses (BMGs), or amorphous metal alloys, have a unique combination of properties such as high strength, large elastic strain limit (up to 2%), corrosion resistance and formability. These unique properties make them candidates for precision mechanical elements, hinge supports, contact surfaces as well as miniaturized systems (MEMS). However, their limited ductility hinders further realizations of their industrial potential. Under uniaxial tension tests, metallic glass fails in a brittle manner with unstable propagation of a single shear band. There is a need to understand the conditions for shear band nucleation and propagation in order to achieve a superior material system with adequate toughness to ensure in-service reliability;This dissertation focuses on understanding the nucleation and propagation mechanisms of shear bands in BMGs under constrained deformation. The nature of the work is primarily experimental with integrated finite element simulations to elucidate the observed trends. Wedge indentation with a circular profile of different radii is used to provide a stable loading path for in situ monitoring of shear band nucleation, propagation in Vitreloy-1. Detailed analyses of the in-plane finite deformation fields are carried out using digital image correlation. The incremental surface analysis showed that multiple shear bands are developed beneath the indenter. The observed pattern closely follow the traces of slip line field for a pressure sensitive material. The first shear bands initiate in the bulk beneath the indenter when a critical level of mean pressure is achieved. Two distinct shear band patterns are developed, that conform to either the alpha or beta lines for each sector. The deformation zones developed under indenters with different radii were found to be self-similar;The evolution of shear bands beneath the indenter is also characterized into two different categories. A set of primary bands is identified to evolve with the process zone front and presents an included angle of 78°-80°. The other set of bands evolves at a later stage of loading within the originally formed ones but with consistently higher included angle of around 87°. The band spacing is found to scale with the local average of maximum in-plane shear strain such that the local strain energy is minimized. The measurements shed light on the critical shear strain needed to initiate these bands. The richness of the shear band network establishes a basis for calibration of constitutive models;Experimental in-plane deformation maps show the amount of total strain that builds prior to the initiation of localized deformation. Furthermore, the maps help examine the change imposed on the surrounding strain field by the appearance of shear bands. It was verified that shear bands relax the asymptotic field by changing the order of singularity. Finally, it was seen that the shear bands are not the only accumulation of permanent deformation but that the surrounding material can accrue relatively high level of inelastic deformation (up to 5%);To rationalize these findings, the Johnson cavity expansion model is adapted and modified to account for pressure-dependent yielding conditions. The elasto-plastic boundary from such analysis is used to scale the experimental measurements for all indenter radii, loading level and spatial position beneath the indenter. The continuum finite element simulations have shown that the macroscopic measurements of force-depth indentation curves would predict a lower value of the pressure sensitivity than those observed from the detailed microscopic measurements. Moreover, a transition from pressure insensitive response to progressive pressure sensitivity is observed by decreasing the indenter radius, or in effect by increasing the level of hydrostatic pressure under the indenter. This leads to the belief that the BMG's pressure sensitivity parameter is in itself dependent on the level of the applied pressure. These observations give detailed insight on the post-yield behavior of BMGs, which cannot be obtained from macroscopic uniaxial tension or compression tests;Despite the richness of the shear band details, the current framework has provided several notable results. First, the macroscopic trends, force-indentation depth response and the extent of deformation zones are well captured for this constrained deformation mode by continuum models that address only the onset of yielding. Second, the apparent pressure dependence of the shear band angle on the macroscopic measurements is minimal. Third, the initiation point, and not the shear band development is of critical importance. These findings would formulate the basis for simulation of shear band nucleation, propagation and interactions. They would also elucidate the role of secondary particle inclusion for toughening;Another form of inhomogeneous deformation in the form of shear bands is also studied in constrained layer of ductile metal subjected to shearing deformation. The material system utilized was comprised of a ductile layer of tin based solder, encapsulated within relatively hard copper shoulders. The experimental configuration provides pure shear state within the constrained solder layer. Different Pb/Sn compositions are tested with grain size approaching the film thickness. The in-plane strain distribution within the joint thickness is measured by a microscopic digital image correlation system. The toughness evolution within such highly gradient deformation field is monitored qualitatively through a 2D surface scan with a nanoindenter. The measurements showed a highly inhomogeneous deformation field within the film with discreet shear bands of concentrated strain. The localized shear bands showed long-range correlations of the order of 2-3 grain diameter. A size-dependent macroscopic response on the layer thickness is observed. However, the corresponding film thickness is approximately 100-1000 times larger than those predicted by non-local continuum theories and discreet dislocation.