Abstract
The study of charge and spin transport through semiconductor quantum dots is experiencing a renaissance due to recent advances in nanofabrication and the realization of quantum dots as candidates for quantum computing. In this work, we combine atomistic electronic structure calculations with quantum master equation methods to study the transport of electrons and holes through strongly confined quantum dots coupled to two leads with a voltage bias. We find that a competition between the energy spacing between the two lowest quasi-particle energy levels and the strength of the exchange interaction determines the spin states of the lowest two quasi-particle energy levels. Specifically, the low density of electron states results in a spin singlet being the lowest-energy two-electron state, whereas, in contrast, the high density of states and significant exchange interaction result in a spin triplet being the lowest-energy two-hole state. The exchange interaction is also responsible for spin blockades in transport properties, which could persist up to temperatures as high as 77 K for strongly confined colloidal quantum dots from our calculations. Finally, we relate these findings to the preparation and manipulation of singlet and triplet spin qubit states in quantum dots using voltage biases.
Original language | English |
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Pages (from-to) | 26661-26669 |
Number of pages | 9 |
Journal | Journal of Physical Chemistry C |
Volume | 125 |
Issue number | 48 |
DOIs | |
State | Published - 9 Dec 2021 |
Bibliographical note
Publisher Copyright:© 2021 American Chemical Society
Funding
This work was primarily supported by the Department of Energy, Photonics at Thermodynamic Limits Energy Frontier Research Center under Grant No. DE-SC0019140. J.P.P. acknowledges support from the Harvard University Center for the Environment. P.N. is a Moore Inventor Fellow through Grant GBMF8048 from the Gordon and Betty Moore Foundation. A.L. acknowledges support from the Israel Science Foundation, Grant No. 1364/21. W.D. acknowledges startup funding from Westlake University. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under Contract No. DE-AC02-05CH11231.
Funders | Funder number |
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Westlake University | |
U.S. Department of Energy | DE-AC02-05CH11231, DE-SC0019140 |
Center for the Environment, Harvard University | |
Israel Science Foundation | 1364/21 |