Defect-free single-atom arrays in optical tweezers are a promising platform for scalable quantum computing, quantum simulation, and quantum metrology. Extending single-species arrays to mixed-species ones promises to offer other possibilities. In our recent proof-of-principle realization of defect-free two-dimensional assembly of mixed-species ${}^{87}\mathrm{Rb}$ and ${}^{85}\mathrm{Rb}$ atom arrays [C. Sheng et al., Phys. Rev. Lett. 128, 083202 (2022)], the filling fractions were limited by imperfect atom transfer and algorithmic limitations during the rearrangement process. To scale up defect-free mixed-species atom arrays, we increase the tweezer-array size, improve atom-transfer efficiency, and upgrade the heuristic heteronuclear algorithm—removing the need for subpartitioning, incorporating flexibility moves to overcome path blocking, enabling efficient multicycle rearrangement, and thereby achieving higher success rates in larger arrays. Consequently, we successfully created defect-free arrays containing 120 mixed-species atoms. The resulting filling fraction and defect-free probability improved to 98.3(1)% and 14(2)%, respectively. We anticipate that the enhanced algorithm can be extended to other atomic species combinations, making these mixed-species arrays readily available for studies of many-body physics, quantum error correction, and quantum metrology.

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• Coherent control
• Cooling & trapping
• Quantum information with atoms & light
• Alkali metals
• Atomic gases
• Nanotechnology
• Atom & ion cooling
• Optical tweezers