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arXiv:2203.00712 · Nano Letters

SUPER Scheme in Action: Experimental Demonstration of Red-Detuned Excitation of a Quantum Emitter

Yusuf Karli, Florian Kappe, Vikas Remesh, Thomas K. Bracht, Julian Münzberg, Saimon Filipe Covre da Silva, Tim Seidelmann, V. M. Axt, Armando Rastelli, Doris E. Reiter, Gregor Weihs

Published Jul 6, 2022• 64 citations
arXivHTMLPDF

Abstract

The quest for the perfect single-photon source includes finding the optimal protocol for exciting the quantum emitter. Coherent optical excitation was, up until now, achieved by tuning the laser pulses to the transition frequency of the emitter, either directly or in average. Recently, it was theoretically discovered that an excitation with two red-detuned pulses is also possible where neither of which would yield a significant upper-level population individually. We show that the so-called swing-up of quantum emitter population (SUPER) scheme can be implemented experimentally with similar properties to existing schemes by precise amplitude shaping of a broadband pulse. Because of its truly off-resonant nature, this scheme has the prospect of powering high-purity photon sources with superior photon count rate.

DOI
10.1021/acs.nanolett.2c01783

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The quest for the perfect single-photon source includes finding the optimal protocol for exciting the quantum emitter. Coherent optical excitation was, up until now, achieved by tuning the laser pulses to the transition frequency of the emitter, either directly or in average. Recently, it was theoretically discovered that an excitation with two red-detuned pulses is also possible where neither of which would yield a significant upper-level population individually. We show that the so-called swing-up of quantum emitter population (SUPER) scheme can be implemented experimentally with similar properties to existing schemes by precise amplitude shaping of a broadband pulse. Because of its truly off-resonant nature, this scheme has the prospect of powering high-purity photon sources with superior photon count rate.
In the SUPER scheme (Swing-UP of the quantum EmitteR population), excitation of a quantum emitter is achieved with two off-resonant, red-detuned laser pulses. This allows the generation of high-quality single photons without the need of complex laser stray light suppression or careful spectral filtering. In the present work, we extend this promising method to quantum emitters, specifically semiconductor quantum dots, inside a resonant optical cavity. A significant advantage of the SUPER scheme is identified in that it eliminates re-excitation of the quantum emitter by suppressing photon emission during the excitation cycle. This, in turn, leads to almost ideal single-photon purity, overcoming a major factor typically limiting the quality of photons generated with quantum emitters in high-quality cavities. We further find that for cavity-mediated biexciton emission of degenerate photon pairs, the SUPER scheme leads to near-perfect biexciton initialization with very high values of polarization entanglement of emitted photon pairs. Published by the American Physical Society 2024
The swing-up of quantum emitter population (SUPER) scheme allows to populate the excited state of a quantum emitter with near-unity fidelity using two red-detuned laser pulses. Its off-resonant, yet fully coherent nature has attracted significant interest in quantum photonics as a valuable tool for preparing single-photon sources in their excited state on demand, while simultaneously ensuring straightforward spectral filtering of the laser. However, the physical understanding of this mechanism in terms of energy exchange between the electromagnetic field and the emitter is still lacking. Here, we present a fully quantized model of the swing-up excitation and demonstrate that it is in fact a multi-photon process, where one of the modes loses two or more photons while the other gains at least one. Our findings provide an unexpected physical interpretation of the SUPER scheme and unveil a new non-linear interaction between single emitters and multiple field modes.
The swing-up of quantum emitter population (SUPER) scheme allows to populate the excited state of a quantum emitter with near-unity fidelity using two red-detuned laser pulses. Its off-resonant yet fully coherent nature has attracted significant interest in quantum photonics as a valuable tool for preparing single-photon sources in their excited state on demand while simultaneously ensuring straightforward spectral filtering of the laser. However, the physical understanding of this mechanism in terms of energy exchange between the electromagnetic field and the emitter is still lacking. Here, we present a fully quantized model of the swing-up excitation and demonstrate that it is in fact a multi-photon process, where one of the modes loses two or more photons while the other gains at least one. Our findings provide an unexpected physical interpretation of the SUPER scheme and unveil a new non-linear interaction between single emitters and multiple field modes.
Coherent control of quantum emitters is essential for scalable quantum photonic technologies. The recently proposed swing up of the quantum emitter population (SUPER) scheme allows efficient and coherent state preparation via off-resonant, red-detuned laser pulses, simplifying laser suppression and enhancing photon collection. We present a systematic study of SUPER excitation applied to a single GaAs quantum dot in a low- Q micropillar cavity. We first identify the optimal excitation conditions for SUPER, and then compare the key figures of merit against the well-established two-photon excitation (TPE). Despite requiring higher excitation powers, SUPER achieves near-unity population inversion of the exciton state ( ∼ 95 % ) and high single-photon purity ( g ( 2 ) = 0.03 ) comparable to that under TPE, while also exhibiting a shortened decay time ( ∼ 200 ps) reducing the time jitter in the exciton population. A polarization-resolved analysis reveals that when both excitation and collection are aligned with one of the exciton dipoles, SUPER results in highly polarized single-photon emission, exceeding the resonant TPE saturation by a factor of 1.45. Under optimized excitation conditions, we also observe biexciton preparation via a distinct SUPER resonance, constituting an experimental demonstration of biexciton preparation using SUPER. These findings are in good agreement with a proposed four-level theoretical model that incorporates the biexciton state. Furthermore, we report that, strikingly, a slight misalignment of laser polarization induces an additional SUPER resonance that selectively populates the orthogonal exciton dipole, without altering the nominal excitation polarization. This unexpected behavior reveals a new degree of freedom for coherent state preparation. Our findings establish the SUPER scheme as a versatile tool for state-selective exciton and biexciton control, with strong potential for quantum photonic applications.
The Swing-UP of the quantum EmitteR population (SUPER) two-color pulsed excitation scheme allows for robust and close to 100\% excitation of a two-level quantum emitter using only red detuned light. We analyze the underlying counterintuitive dynamics using a full quantum input-output description of the in- and outgoing light pulses for the case of two coherent free-space input pulses at realistic photon numbers. At the microscopic level, the SUPER mechanism exhibits its nonlinear three-photon Raman-type character, leading to a net photon-number change of −2-2−2 in one mode and +1+1+1 in the other, as was first guessed from cavity-enhanced model descriptions at low photon numbers. We confirm that in free space, a sufficiently high pulse photon number, much larger than one, is required to achieve high-fidelity inversion. To treat the large coherent-state amplitudes (photon numbers) relevant for SUPER, we extend the quantum input-output formalism to include a cumulant expansion approach. With an interaction-picture formulation, the few exchanged photons that govern the nontrivial dynamics enable direct full-quantum calculations in truncated Hilbert spaces, including treatments in a displacement frame and for initial Fock-state pulses.