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Consider a second-order, right-invariant, subelliptic differential operator \\(H\\) on \\(G,\\) and the associated semigroup \\(S_t=e^{-tH}.\\) The author identifies an ideal \\textbf{n\\('\\)} of \\textbf{g} such that \\(H\\) satisfies global regularity estimates for spatial derivatives of all orders, when the derivatives are taken in the direction of \\textbf{n\\('\\)}. The regularity is expressed as \\(L_2\\) estimates for derivatives of the semigroup, and as Gaussian bounds for derivatives of the heat kernel. The boundedness in \\(L_p,\\) \\(1<p<\\infty,\\) is obtained of some associated Riesz transform operators. It is shown that \\textbf{n\\('\\)} is the largest ideal of \\textbf{g} for which the regularity results hold. Various algebraic characterizations of \\textbf{n\\('\\)} are given. In particular, \\textbf{n\\('\\)}=\\textbf{s} \\(\\oplus\\) \\textbf{n} where \\textbf{n} is the nilradical of \\textbf{g} and \\textbf{s} is the largest semisimple ideal of \\textbf{g}. Additional features of this article include an exposition of the structure theory for \\(G\\) in Section 2, and a concept of twisted multiplication on Lie groups which includes semidirect products in the 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