The present disclosure, among other things, provides a composition of a particle including a substrate; at least a first condensation layer comprising at least a first dopant entity; and at least a second layer comprising a second dopant entity. In some embodiments, different dopant entities are included in different layers. In some embodiments, such dopant entities are or comprise detectable entities. This, in some embodiments, provided technologies achieve multi-modality particles. Among the many advantages of provided technologies include the ability to image particles by a plurality of distinct imaging modalities and/or in a plurality of contexts (e.g., pre-surgical, intraoperative and/or post-surgical environments). The present invention provides methods that include a single administration of particles to a subject, followed by a plurality of steps that comprise imaging the administered particles, which steps may utilize different imaging technologies and/or be performed at different times and/or in different environments.