Helium isotopes are unrivalled tracers of the origins of melts in the Earth's convecting mantle but their role in determining melt contributions from the shallower and rigid lithospheric mantle is more ambiguous. We have acquired new He-3/He-4 data for olivine and pyroxene separates from 47 well-characterised mantle xenoliths from global on- and off-craton settings. When combined with existing data they demonstrate a new systematic relationship between fluid-hosted He-3/He-4 and major and trace element composition of host minerals and whole rock. We show that a significant proportion (>70 %) of mantle peridotites from continental off-craton settings with depleted major element compositions (e.g., olivine Mg# >= 89.5) have He-3/He-4 in the range of modern-day mid-ocean ridge basalt (MORB) source mantle (7-9 R-a) and we propose that they represent underplated melt residues, which initially formed in the convecting upper mantle. Furthermore, we observe that off-craton mantle xenoliths with signatures often attributed to enrichment by melts or fluids from 'ancient' subducted oceanic lithosphere have lower He-3/He-4 (<7 R-a). Modest correlations between He-3/He-4 and whole rock incompatible trace element signatures commonly used as proxies for metasomatism by small-fraction carbonatite and silicate melts or C-O-H fluids characterise lithospheric mantle with He-3/He-4 ranging from 5 to 8 R-a. Using a numerical model that integrates temperature-dependent melt extraction from the upper mantle with in-situ radiogenic ingrowth of He-4 in the continental mantle we show that the initial He-3/He-4 of continental lithosphere mantle has decreased over time. This is consistent with previous observations demonstrating that ancient (2.5-3.5 Ga) cratonic mantle has a depleted mineral chemistry (e.g., olivine Mg# = 91-94) and low He-3/He-4 (0.5-6.7 R-a), while continental off-craton mantle (<2.5 Ga) is more fertile (olivine Mg# = 88-92) and has less radiogenic He-3/He-4 (4-8.8 R-a). This relationship defines a 'global lithospheric mantle array' for intraplate peridotites on plots of He-3/He-4 vs olivine Mg#. Peridotites influenced by past and present subduction fluids, including those that contain amphibole, plot off this array. Our findings have broad implications for the He-3/He-4 signatures observed in continental magmas. Many of Earth's deepest melts, i.e. proto-kimberlites, are characterised by relatively low He-3/He-4. We attribute this to assimilation and incorporation of low He-3/He-4 cratonic mantle material during ascent of carbonate-rich melts through thick lithosphere, which overprints the original signatures. Moreover, our findings suggests that the lithospheric mantle acts as a long-term reservoir for other fluid-hosted volatiles (e.g., CO2, CH4, H2O), and in some cases able to sequester these over billion-year timescales until physio-chemical perturbation (e.g., during major rifting or heating events).
