The Two-Higgs Doublet Model (2HDM) is a well-motivated theoretical framework that provides additional sources of CP Violation (CPV) beyond the Standard Model (SM). After studying the vacuum topology of a general (convex) 2HDM potential, we unambiguously identify three origins of CPV: (i) Spontaneous CPV (SCPV), where the vacuum manifold has at least two degenerate CPV minima disconnected by domain walls, (ii) Explicit CPV (ECPV) with one single CPV ground state, and (iii) Mixed Spontaneous and Explicit CPV (MCPV), where the theory possesses more than one non-degenerate CPV local minimum. Most importantly, we define a novel complex parameter rCP whose norm and phase control the three different realisations of CPV, at least at the tree level. In all these scenarios, only two CPV phases can be made independent, as any third CPV parameter will always be constrained via the CP-odd tadpole condition. Since ECPV vanishes in 2HDMs where SM Higgs alignment is achieved naturally through accidental continuous symmetries, we analyse the possibility of maximising CPV through soft and explicit breaking of these symmetries. We derive upper limits on key CPV parameters that quantify the degree of SM misalignment from constraints due to the non-observation of an electron Electric Dipole Moment (EDM). Finally, we delineate the CP-violating parameter space of the so-constrained naturally aligned 2HDMs that can further be probed at the CERN Large Hadron Collider (LHC).
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