The interparticle Coulombic decay process (ICD) in a Coulomb-coupled pair of quantum dots (QDs) was predicted to feature electronic relaxation within one QD in conjunction with ionization of the other. In this work the QD model is extended from a pair to a triad of one excited and two ionizable QDs and in total three electrons. Analytical Wigner-Weisskopf expressions for the decay rates are formulated and confirmed with numerical electron dynamics calculations, suggesting a rate enhancement by a factor two that may be relevant for the competitiveness of ICD in QDs. Particularly, we compare two energetic scenarios, one allowing only for single ionization of the QD triad and one, not yet discussed in the community, potentially allowing for double ionization.
In this work, we investigate the capability of known quantum computing algorithms for fault-tolerant quantum computing to simulate the laser-driven electron dynamics of excitation and ionization processes in small molecules such as lithium hydride, which can be benchmarked against the most accurate time-dependent full configuration interaction (TD-FCI) calculations. The conventional TD-FCI wave packet propagation is reproduced using the Jordan−Wigner transformation for wave function and operators and the Trotter product formula for expressing the propagator. In addition, the time-dependent dipole moment, as an example of a time-dependent expectation value, is calculated using the Hadamard test. To include non-Hermitian operators in the ionization dynamics, a similar approach to the quantum imaginary time evolution (QITE) algorithm is employed to translate the propagator, including a complex absorption potential, into quantum gates. The computations are executed on a quantum computer simulator. By construction, all quantum computer algorithms, except for the QITE algorithm used only for ionization but not for excitation dynamics, would scale polynomially on a quantum computer with fully entangled qubits. In contrast, TD-FCI scales exponentially. Hence, quantum computation holds promises for substantial progress in the understanding of electron dynamics of excitation processes in increasingly large molecular systems, as has already been witnessed in electronic structure theory.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.