Tunnel-coupled pairs of optically active quantum dots-quantum dot molecules (QDMs)-offer the possibility to combine excellent optical properties such as strong light-matter coupling with two-spin singlet-triplet (S − T 0 ) qubits having extended coherence times. The S − T 0 basis formed using two spins is inherently protected against electric and magnetic field noise. However, since a single gate voltage is typically used to stabilize the charge occupancy of the dots and control the inter-dot orbital couplings, operation of the S − T 0 qubits under optimal conditions remains challenging. Here, an electric field tunable QDM that can be optically charged with one (1h) or two holes (2h) on demand is presented. A four-phase optical and electric field control sequence facilitates the sequential preparation of the 2h charge state and subsequently allows flexible control of the inter-dot coupling. Charges are loaded via optical pumping and electron tunnel ionization. Oneand two-hole charging efficiencies of (93.5 ± 0.8)% and (80.5 ± 1.3)% are achieved, respectively. Combining efficient charge state preparation and precise setting of inter-dot coupling allows for the control of few-spin qubits, as would be required for the on-demand generation of 2D photonic cluster states or quantum transduction between microwaves and photons.
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