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Heteronuclear Rydberg molecules

We report the creation of heteronuclear ultralong-range Rydberg-molecule dimers by excitation of minority $^{88}\text{Sr}$ atoms to $5sns\,^3S_1$ Rydberg states ($n=31-39$) in a dense background of $^{84}\text{Sr}$. We observe an isotope shift of the $ν=0$ vibrational state over this range of $n$ and compare our measurements with a theoretical prediction and a simple scaling argument. With the appropriate choice of principal quantum number the isotope shift is sufficiently large to produce heteronuclear dimers with almost perfect fidelity. When the spectral selectivity is limited, we obtain a lower bound on the ratio of heteronuclear to homonuclear excitation probability of 30 to 1 by measuring the scaling of the molecular excitation rate with varying relative densities of $^{88}\text{Sr}$ and $^{84}\text{Sr}$ in the ultracold mixture.