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arXiv:1901.00247 · The Journal of Chemical Physics

Magnetic pulses enable multidimensional optical spectroscopy of dark states

Santiago Oviedo-Casado, František Šanda, Jürgen Hauer, Javier Prior

Published Feb 25, 2020• 0 citations
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Abstract

The study and manipulation of low dipole moment quantum states have been challenging due to their inaccessibility by conventional spectroscopic techniques. Controlling the spin in such states requires unfeasible strong magnetic fields to overcome typical decoherence rates. However, the advent of terahertz technology and its application in magnetic pulses opens up a new scenario. In this article, we focus on an electron-hole pair model to demonstrate that it is possible to control the precession of the spins and to modify the transition rates to different spin states. Enhancing transitions from a bright state to a dark state with different spins means that the latter can be revealed by ordinary spectroscopy. We propose a modification of the standard two-dimensional spectroscopic scheme in which a three pulse sequence is encased in a magnetic pulse. Its role is to drive transitions between a bright and a dark spin state, making the latter susceptible to spectroscopic investigation.

DOI
10.1063/1.5139409

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The study and manipulation of low dipole moment quantum states have been challenging due to their inaccessibility by conventional spectroscopic techniques. Controlling the spin in such states requires unfeasible strong magnetic fields to overcome typical decoherence rates. However, the advent of terahertz technology and its application in magnetic pulses opens up a new scenario. In this article, we focus on an electron-hole pair model to demonstrate that it is possible to control the precession of the spins and to modify the transition rates to different spin states. Enhancing transitions from a bright state to a dark state with different spins means that the latter can be revealed by ordinary spectroscopy. We propose a modification of the standard two-dimensional spectroscopic scheme in which a three pulse sequence is encased in a magnetic pulse. Its role is to drive transitions between a bright and a dark spin state, making the latter susceptible to spectroscopic investigation.
The study and manipulation of low dipole moment quantum states has been historically difficult due to their inaccessibility by conventional spectroscopic techniques. Controlling the spin in such states requires unfeasibly strong magnetic fields to overcome the typical decoherence rates. However, the advent of terahertz technology and its application to magnetic pulses opens up a new scenario. In this article, we employ an electron-hole pair model to demonstrate that it is possible to control the precession of the spins and to modify the transition rates to different spin states. Enhancing transitions from a bright state to a dark state with different spin means that the latter can be revealed by ordinary spectroscopy. We propose a modification of the standard two-dimensional spectroscopic scheme in which a three laser pulse sequence is encased in a circularly polarised magnetic pulse, whose role is to induce ultrafast coherent transitions between a bright and a dark spin state making the latter susceptible to spectroscopic investigation.
Dark excitons in quantum dots are not directly optically accessible, which has limited their use in practical applications. Nevertheless, they offer promising features such as substantially longer lifetimes compared to bright excitons, making them attractive candidates for quantum information processing. While previous theoretical and experimental studies have explored their potential, their full capabilities remain largely untapped. In this work, we demonstrate an all-optical storage and retrieval of the spin-forbidden dark exciton in a quantum dot from the ground state using chirped pulses and an in-plane magnetic field. Our experimental findings are in excellent agreement with theoretical predictions of the dynamics calculated using state-of-the-art product tensor methods. Our scheme enables an all-optical control of dark states without relying on any preceding decays. This opens up an unexplored dimension for optimal quantum control and time-bin entangled photon pair generation from quantum dots.
Because dark excitons in quantum dots are not directly optically accessible, so far they have not played a significant role in using quantum dots for photon generation. They possess significantly longer lifetimes than their brighter counterparts and hence offer enormous potential for photon storage or manipulation. In this work, we demonstrate an all-optical storage and retrieval of the spin-forbidden dark exciton in a quantum dot from the ground state employing chirped pulses and an in-plane magnetic field. Our experimental findings are in excellent agreement with theoretical predictions of the dynamics calculated using state-of-the-art product tensor methods. Our scheme enables an all-optical control of dark states without relying on any preceding decays. This opens up a new dimension for optimal quantum control and time-bin entangled photon pair generation from quantum dots.
Driving an open spin system by two strong, nearly degenerate fields enables addressing populations of individual spin states, characterisation of their interaction with thermal bath, and measurements of their relaxation/decoherence rates. With such addressing we observe nested magnetic resonances having nontrivial dependence on microwave field intensity: while the width of one of the resonances undergoes a strong power broadening, the other one exhibits a peculiar field-induced stabilization. We also observe light-induced narrowing of such composite resonances. The observations are explained by the dynamics of bright and dark superposition states and their interaction with reservoir.
We have studied experimentally spin-dependent photon echoes from excitons in an InGaAs/GaAs quantum well subject to a transverse magnetic field (Voigt geometry). Larmor precession of the spins of the electron and heavy hole in an exciton leads to a periodic transfer of coherence between bright and dark exciton states. The increase in dephasing time due to the transition to the dark states could be useful for coherent control development. A comprehensive analysis shows a good agreement between a four-wave mixing experiment and the predictions of a theoretical treatment based on a five-level exciton model comprising a ground state and two pairs of bright and dark states. The extracted optical dephasing time of bright and dark excitons is equal to 30 and 130 ps, respectively. Exploiting the photon echo reveals evidence of electron Larmor precession with in-plane ggg factor $|{g}_{e,\ensuremath{\perp}}|=0.44\ifmmode\pm\else\textpm\fi{}0.05$ and heavy hole precession as well. The precession frequency of the latter depends nonlinearly on the applied magnetic field, and the corresponding ggg factor reaches a value of $|{g}_{h,\ensuremath{\perp}}|\ensuremath{\approx}0.3$ at B=6B=6B=6 T. Estimates for the heavy hole ggg-factor spreading as well as the isotropic exchange interaction constant are provided.
Conventional control strategies for nitrogen-vacancy centers in quantum sensing are based on a two-level model of their triplet ground state. However, this approach fails in regimes of weak bias magnetic fields or strong microwave pulses, as we demonstrate. To overcome this limitation, we propose a novel control sequence that exploits all three levels by addressing a hidden Raman configuration with microwave pulses tuned to the zero-field transition. We report excellent performance in typical dynamical decoupling sequences, opening up the possibility for nano-NMR operation in low field environments.