We quantify sequential and nonsequential contributions in two-photon double ionization of helium atoms by intense ultrashort extreme-ultraviolet pulses with central photon energies ℏω ctr near the sequential double-ionization threshold. If the spectrum of such pulses overlaps both the sequential (ℏω > 54.4 eV) and nonsequential (ℏω < 54.4 eV) double-ionization regimes, the sequential and nonsequential doubleionization mechanisms are difficult to distinguish. By tracking the double-ionization asymmetry in joint photoelectron angular distributions, we introduce the two-electron forward-backward-emission asymmetry as a measure that allows the distinction of sequential and nonsequential contributions. Specifically, for ℏω ctr ¼ 50 eV pulses with a sine-squared temporal profile, we find that the sequential double-ionization contribution is the largest at a pulse length of 650 as, due to competing temporal and spectral constraints. In addition, we validate a simple heuristic expression for the sequential double-ionization contribution in comparison with ab initio calculations. DOI: 10.1103/PhysRevLett.115.183002 PACS numbers: 32.80.Rm, 33.80.Rv, 42.50.Hz In 1975, the mechanism of nonsequential double ionization was revealed in the photoionization of alkaline earth atoms [1]. It is enabled by strong electronic correlation and thus clearly distinct from the sequential double-ionization mechanism. Nonsequential double ionization was observed for noble gas atoms in 1982 [2] and received rapidly increasing attention from both experimentalists [3-9] and theorists [10][11][12][13].Photoelectron angular distributions of single-photon double ionization were found to owe their structure partly to (dipole) selection rules [11,14,15] and to consist of symmetrical and antisymmetrical contributions (with regard to electron exchange), that each can be written as the product of an angular and a correlation factor [11]. For coplanar emission geometry, where the emitted-electron momenta and polarization axis of the linearly polarized extremeultraviolet (XUV) pulse lie in a plane, and for equal energy sharing (equal asymptotic kinetic energies E 1 and E 2 of the photoelectrons), the angular factor becomes j cos θ 1 þ cos θ 2 j 2 , where θ 1 and θ 2 are photoelectron emission angles relative to the polarization direction of the ionizing light, while the electron correlation factor follows as expf−4 ln 2½ðθ 12 − πÞ=θ 1=2 2 g, with the mutual emission angle θ 12 ¼ jθ 1 − θ 2 j. The adjustable parameter, θ 1=2 , is related to the significance of correlation in the double-ionization process [11]. The antisymmetrical contribution and back-to-back electron emission vanish at equal energy sharing but become progressively more prominent for increasingly nonequal energy sharing, as the antisymmetrical contribution j cos θ 1 − cos θ 2 j 2 gradually appears in joint photoelectron angular distributions [10,11,16].