In the midst of the NISQ era of quantum computers, the challenges are gravitating to encompass both architecting and full-stack engineering aspects, which are inherently algorithm-driven, so that there starts to be a convergence of bottom-up and top down design approaches, what we coin as the Quantum Architecting (QuArch) era. In face of many-fold diverse design proposals, in this paper it is postulated and proposed to apply the so-called Design Space Exploration (DSE) to the full vertical stack of quantum systems as an instrumental methodology to address such design diversity challenge. This structured design means, based upon composing a multidimensional input design space together with compressing the set of output performance metrics into an optimization-oriented overall figure of merit, provides a framework and method for optimization, for performance comparison. It yields as well a way to discriminate among alternative techniques at all layers and across layers, eventually as a structured and comprehensive design-oriented formal framework to address the quantum system design and evaluation complexity. The paper concludes by illustrating instances of this methodology in optimizing and comparing mapping techniques to address the resource-constrained current NISQ quantum chips, and to carry out a quantitative gap analysis of scalability trends aiming manycore distributed quantum architectures.