We establish sharp mixed spectral Barron regularity for eigenfunctions of molecular Coulomb Hamiltonians. The mixed norm is a Fourier $L^1$ norm with one isotropic weight and coordinate-product weights, and therefore detects regularity invisible to the isotropic Barron scale. For a nonempty set $I$ of electron indices on which the wave function is antisymmetric, we derive an explicit admissible region for the isotropic order $s$ and the coordinate orders $α,β$. This region is optimal as a uniform statement over the class of clamped-nuclei Coulomb Hamiltonians. For fixed-spin components with two occupied spin blocks, it reduces to $s+α+β<1$; in the fully spin-polarized class it reduces to $s+α<1$. In particular, if $\mathcal I_σ$ denotes the family of occupied same-spin blocks determined by $σ$, then every fixed-spin spatial component $ψ_σ$ satisfies, for every $0\leqα<1$, \[ \left(\sum_{I\in\mathcal I_σ}\prod_{i\in I}\langleξ_i\rangle^α\right)\widehat{ψ_σ}\in L^1(\mathbb{R}^{3N}). \] For a fully spin-polarized state, $\mathcal I_σ=\{\{1,\ldots,N\}\}$.
We establish sharp Barron regularity for Coulombic many-electron wave functions after extraction of the universal cut-off Jastrow factors. Following the factorization of Fournais et al.~\cite[Definition~1.4]{FournaisEtAl2005}, for a Coulombic eigenfunction $ψ$ we define the successive quotients by \[ φ=e^{-F_{2,\mathrm{cut}}}ψ\quad\text{and}\quad φ_3=e^{-F_{3,\mathrm{cut}}}φ=e^{-(F_{2,\mathrm{cut}}+F_{3,\mathrm{cut}})}ψ. \] Then \[ φ,φ_3\in\mathcal{B}^s(\mathbb{R}^{3N}) \qquad\text{for every }s<2. \] This range is optimal among universal factorizations. No factor depending only on the particle number and the nuclear data, but not on the eigenfunction or its eigenvalue, can make every corresponding quotient belong to $\mathcal{B}^2$. We also determine the exact endpoint growth. Writing $\varepsilon=2-s$, we prove that, for either $u=φ$ or $u=φ_3$, there is a computable constant $M$ independent of $\varepsilon$ such that \[ \left\|u\right\|_{\mathcal{B}^{2-\varepsilon}}\leq\frac{M}{\varepsilon^2}\left\|u\right\|_{\mathcal{B}^1}. \] For the unperturbed two-electron atom we prove, with a constant independent of $\varepsilon$, \[ \left|\left\|φ_3\right\|_{\mathcal{B}^{2-\varepsilon}}-\frac{32πZ\lvertφ_3(0,0)\rvert}{\varepsilon^2}\right|\leq\frac{C}{\varepsilon}. \] Hence the quadratic rate in the upper bound is sharp whenever $\lvertφ_3(0,0)\rvert\neq0$, as is the case for the ground state.