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Journal of the Optical Society of America B

Double-excitation transfer in dimer and trimer three-level systems using laser pulses and single photons

Abuenameh Aiyejina, Ethan Wyke, Roger Andrews, Andrew D. Greentree

Published May 30, 2024• 2 citations
Publisher

Abstract

We derive and simulate the wavefunctions and double-excitation probabilities for dimer and trimer three-level systems. Perfect state transfer occurs for pulse strengths that are odd multiples of π /2 when the parameter Jt equals odd multiples of π /2 and π /2 for the dimer and trimer, respectively. Near-perfect state transfer with a single photon occurred for photon coupling strength g =2 J when Jt=1.99,19.87 in the dimer and Jt=2.62,25.51 in the trimer. The nature of perfect state transfer is due to localization and transfer of double excitations for given pulse strengths and times.

DOI
10.1364/josab.523990

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We derive and simulate the wavefunctions and double-excitation probabilities for dimer and trimer three-level systems. Perfect state transfer occurs for pulse strengths that are odd multiples of π /2 when the parameter Jt equals odd multiples of π /2 and π /2 for the dimer and trimer, respectively. Near-perfect state transfer with a single photon occurred for photon coupling strength g =2 J when Jt=1.99,19.87 in the dimer and Jt=2.62,25.51 in the trimer. The nature of perfect state transfer is due to localization and transfer of double excitations for given pulse strengths and times.
We analyze a quantum wire that consists of a linear chain of three qutrits with nearest-neighbor interactions and detuning on the central qutrit. We derive the detuning conditions for perfect state transfer of a double excitation and for maximal entanglement between the first and third qutrits. We also analytically determine the times for perfect state transfer and maximal entanglement, which are found to be periodic. We also show that perfect state transfer is a necessary condition for maximal entanglement, with the first occurrence of maximal entanglement at half the time for the first occurrence of perfect state transfer.
In this paper, the theory of the transfer efficiency of a light-harvesting system consisting of a trimer ring coupled to an acceptor site is presented. When the ring has a prepared excitation or is excited using a laser pulse, the maximum transfer efficiency is approximately 0.5, while a near-perfect transfer efficiency is generated by a single photon. The near-perfect efficiency results from the creation of a dark state by the photon, which suppresses the effect of spontaneous decay from the donor.
Compared to single-photon rates, multiphoton excitation rates of atoms and molecules are generally quite small, even at high laser intensities, at least in a 2-level system. Small multiphoton coupling strengths, large ac Stark shifts, and ionization all inhibit real population transfer between bound states. However, it has recently been shown that a 3-level system consisting of a ground state and a pair of nearly degenerate strongly coupled upper states greatly enhances the multiphoton coupling with the ground state, while also greatly reducing the ac Stark shift of the ground state. In this paper I will derive an analytic expression for the n-photon Rabi frequency, for this system, in the case of degenerate upper states, as well as an expression for the level shifts induced in the case of nondegenerate upper states. Numerical calculations based on the 3-level system are presented to verify the analytic results and to show that high-order \ensuremath{\pi} pulses can be driven at moderate field strengths. To demonstrate the feasibility of this process in a real physical system, I will present fully correlated 2-electron calculations in a model one-dimensional molecular potential, including ionization that show a 12-photon \ensuremath{\pi} pulse driven with near-infrared photons. In other words, a single excited state 18.6 eV above the ground state can be populated with over 90% efficiency with little ionization while the ground state is almost completely depopulated. Besides the possibility of producing an amplifying medium in the vacuum ultraviolet, this 3-level configuration may open the door to other strong field effects previously restricted to single-photon interactions, such as adiabatic passage and inner-shell ionization.
Due to their excellent optical properties, quantum dots are promising for applications in photonic quantum technologies. For on-demand single-photon generation, a two-level system given by an excitonic transition is typically excited with a resonant laser pulse of area π. This prepares the two-level system in its excited state from where it spontaneously emits a single photon. However, emission that occurs already during the presence of the laser pulse allows for re-excitation and, thus, multi-photon emission which limits the single-photon purity [1]. In contrast, when exciting the system with a pulse of area 2π, the system is expected to be returned to the ground state. However, in this case emission during the presence of the pulse is most likely to occur when the system is in its excited state – exactly after an area of π has been absorbed. This restarts the Rabi oscillation with a pulse area of π remaining in the pulse which leads to re-excitation with near-unity probability and the emission of a second photon within the excited state lifetime [2,3]. Finally, we present the generation of single photons with ultra-low multi-photon probability [4]. Using two-photon excitation of the bi-exciton suppresses re-excitation and improves the single photon purity by several orders of magnitude for short pulses. [1] K. A. Fischer, et al., New J. Phys. 18, 113053 (2016) [2] K. A. Fischer, et al., Nature Physics 13, 649-654 (2017) [3] K. A. Fischer, et al., Quantum Sci. Technol. 3, 014006 (2017) [4] L. Hanschke et al., arxiv: 1801.01672 (2018)