Exciton dephasing in lead sulfide quantum dots by X-point phonons

Using a sensitive transient four-wave mixing technique in heterodyne detection, we measured the ground-state excitonic dephasing in PbS colloidal quantum dots of 4-6-nm diameter in the temperature range from 5 to 100 K. We observe an ultrafast (<100 fs) initial decay followed by a component of about 300 fs at 5 K, which becomes faster with decreasing dot size and increasing temperature. This dynamics is attributed to pure dephasing of phonon-assisted transitions in the peculiar band structure of PbS, which allows coupling to phonons with wave vectors both near the Brillouin zone center and near the (100) zone edge, the X point. We estimate an upper limit of 7% for the weight of the zero-phonon line with 2.6-ps spin-flip limited dephasing.