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arXiv:2509.14445 · Nature Communications

Coherent control of quantum-dot spins with cyclic optical transitions

Zhe Xian Koong, Urs Haeusler, Jan M. Kaspari, Christian Schimpf, Benyam Dejen, Ahmed M. Hassanen, Daniel Graham, Yusuf Karli, Ailton J. Garcia Jr, Melina Peter, Edmund Clarke, Maxime Hugues, Michał Gawełczyk, Armando Rastelli, Doris E. Reiter, Mete Atatüre, Dorian A. Gangloff

Published Jun 24, 2026• 1 citation
arXivHTMLPDF

Abstract

Solid-state spins are promising as interfaces from stationary qubits to single photons for quantum communication technologies. Semiconductor quantum dots have excellent optical coherence, exhibit near-unity collection efficiencies when coupled to photonic structures, and possess long-lived spins for quantum memory. However, the incompatibility of performing optical spin control and single-shot readout simultaneously has been a challenge faced by almost all solid-state emitters. To overcome this, we leverage light-hole mixing to realize a highly asymmetric lambda system in a negatively charged heavy-hole exciton in Faraday configuration. By compensating GHz-scale differential Stark shifts, induced by unequal coupling to Raman control fields, and by performing nuclear-spin cooling, we achieve quantum control of an electron-spin qubit with a π-pulse contrast of 97.4% while preserving spin-selective optical transitions with a cyclicity of 471 (50). We demonstrate this scheme for both GaAs and InGaAs quantum dots, and show that it is compatible with the operation of a nuclear quantum memory. Our approach thus enables repeated emission of indistinguishable photons together with qubit control, as required for single-shot readout, photonic cluster-state generation, and quantum repeater technologies.

DOI
10.1038/s41467-026-74590-z

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Solid-state spins are promising as interfaces from stationary qubits to single photons for quantum communication technologies. Semiconductor quantum dots have excellent optical coherence, exhibit near-unity collection efficiencies when coupled to photonic structures, and possess long-lived spins for quantum memory. However, the incompatibility of performing optical spin control and single-shot readout simultaneously has been a challenge faced by almost all solid-state emitters. To overcome this, we leverage light-hole mixing to realize a highly asymmetric lambda system in a negatively charged heavy-hole exciton in Faraday configuration. By compensating GHz-scale differential Stark shifts, induced by unequal coupling to Raman control fields, and by performing nuclear-spin cooling, we achieve quantum control of an electron-spin qubit with a π-pulse contrast of 97.4% while preserving spin-selective optical transitions with a cyclicity of 471 (50). We demonstrate this scheme for both GaAs and InGaAs quantum dots, and show that it is compatible with the operation of a nuclear quantum memory. Our approach thus enables repeated emission of indistinguishable photons together with qubit control, as required for single-shot readout, photonic cluster-state generation, and quantum repeater technologies.
Abstract Solid-state spins are promising as interfaces from stationary qubits to single photons for quantum communication technologies. Semiconductor quantum dots have excellent optical coherence, exhibit near-unity collection efficiencies when coupled to photonic structures, and possess long-lived spins for quantum memory. However, the incompatibility of performing optical spin control and single-shot readout simultaneously has been a challenge faced by almost all solid-state emitters. To overcome this, we leverage light-hole mixing to realize a highly asymmetric lambda system in a negatively charged heavy-hole exciton in Faraday configuration. By compensating GHz-scale differential Stark shifts, induced by unequal coupling to Raman control fields, and by performing nuclear-spin cooling, we achieve quantum control of an electron-spin qubit with a π-pulse contrast of 97.4% while preserving spin-selective optical transitions with a cyclicity of 471 (50). We demonstrate this scheme for both GaAs and InGaAs quantum dots, and show that it is compatible with the operation of a nuclear quantum memory. Our approach thus enables repeated emission of indistinguishable photons together with qubit control, as required for single-shot readout, photonic cluster-state generation, and quantum repeater technologies.
Single spins in semiconductor quantum dots form a promising platform for solid-state quantum information processing. The spin-up and spin-down states of a single electron or hole, trapped inside a quantum dot, can represent a single qubit with a reasonably long decoherence time. The spin qubit can be optically coupled to excited (charged exciton) states that are also trapped in the quantum dot, which provides a mechanism to quickly initialize, manipulate and measure the spin state with optical pulses, and to interface between a stationary matter qubit and a 'flying' photonic qubit for quantum communication and distributed quantum information processing. The interaction of the spin qubit with light may be enhanced by placing the quantum dot inside a monolithic microcavity. An entire system, consisting of a two-dimensional array of quantum dots and a planar microcavity, may plausibly be constructed by modern semiconductor nano-fabrication technology and could offer a path toward chip-sized scalable quantum repeaters and quantum computers. This article reviews the recent experimental developments in optical control of single quantum dot spins for quantum information processing. We highlight demonstrations of a complete set of all-optical single-qubit operations on a single quantum dot spin: initialization, an arbitrary SU(2) gate, and measurement. We review the decoherence and dephasing mechanisms due to hyperfine interaction with the nuclear-spin bath, and show how the single-qubit operations can be combined to perform spin echo sequences that extend the qubit decoherence from a few nanoseconds to several microseconds, more than 5 orders of magnitude longer than the single-qubit gate time. Two-qubit coupling is discussed, both within a single chip by means of exchange coupling of nearby spins and optically induced geometric phases, as well as over longer-distances. Long-distance spin-spin entanglement can be generated if each spin can emit a photon that is entangled with the spin, and these photons are then interfered. We review recent work demonstrating entanglement between a stationary spin qubit and a flying photonic qubit. These experiments utilize the polarization- and frequency-dependent spontaneous emission from the lowest charged exciton state to single spin Zeeman sublevels.
New technologies based on the properties of quantum mechanics promise to revolutionise the way information is processed by outperforming what is possible using classical devices. Examples include massively parallel processing using quantum computers, verifiably secure communication using quantum cryptography, and measurement with sensitivity beyond classical limitation with quantum metrology. Realising the full potential of these technologies necessitates the ability to communicate quantum information over large distances, a key requirement for future quantum networks. However, developing practical implementations of long-distance quantum communication is challenging as it necessitates three major ingredients: light-matter interfaces, elementary quantum operations, and quantum memories. This thesis describes work that has been undertaken to address these requirements using semiconductor nanotechnology. We have first demonstrated that single InAs quantum dots embedded inside conventional diode structures constitute high-fidelity controllable interfaces between optical qubits and solid-state qubits. Indeed, the polarisation state of a photon was transferred into the spin state of an electron-hole pair and eventually restored through radiative recombination of the electron and the hole with a fidelity up to 95%. Moreover, spins were manipulated using subnanosecond modulation of a vertical electric field applied to the quantum dots. By controlling this electrical modulation, we demonstrated elementary phase-shift and spin-flip gate operations with near-unity fidelities. An electron-hole pair confi ned in a single quantum dot has a short radiative lifetime limiting therefore its use as an excitonic quantum memory. The solution we proposed was to use a quantum dot molecule to control the spatial separation of the electron and the hole and therefore prevent their recombination. Comprehensive studies of electric field eff ects upon the photoluminescence of quantum dot molecules lead to a clear understanding and a good control over their physical properties. Single photons were stored in individual quantum dot molecules up to 1μs and read out on a subnanosecond time scale. Moreover, the circular polarisation of individual photons was transferred into the spin state of electron-hole pairs with a fidelity above 90%, which does not degrade for storage times up to the 12.5 ns repetition period of the experiment. Our work on single quantum dots could be extended in the near future to allow for two-qubits quantum operations by con fining a second electron-hole pair to be electrically manipulated. Storage of a superposition of spin states in a quantum dot molecule should also be possible if the spin states are made degenerate, which is feasible using the electric fi eld dependence of the energy splitting between the spin states discussed in this thesis. We believe that combining both approaches will lead to the development of a controllable multi-qubit quantum memory for polarised light, a building block for long distance quantum communication based on semiconductor nanotechnology.
Coherent spin-photon interfaces are essential for scalable quantum networks, but their realization requires optically bright transitions, long-lived spin coherence, and complete coherent control. Donor-bound electron spins in II-VI semiconductors offer an attractive platform for optically active spin qubits because they combine strong donor-bound exciton transitions in a direct-bandgap material with a potentially nuclear-spin-free environment. However, coherent control of an individual optically active donor spin has remained elusive. Here we demonstrate optical initialization, coherent control, and readout of a single donor-bound electron spin in ZnSe. Using spin-selective donor-bound exciton optical transitions, we initialize the electron spin and directly resolve its spin-relaxation dynamics. We achieve coherent spin control with off-resonant picosecond optical pulses, as demonstrated by spin Rabi oscillations and Ramsey interference. We further coherently drive two spin-selective optical transitions and observe high-contrast coherent population trapping, demonstrating the formation of an optically controlled dark state. At higher driving strengths, multiple dark resonances reveal the hyperfine interaction between the electron and the I = 3/2 Cl nucleus. These results establish the first coherent optical control of a single donor electron spin in a II-VI semiconductor and identify isolated optical donors as a promising platform for solid-state optically active qubits.
Single spins confined in semiconductor quantum dots - artificial atoms in the solid-state - are attractive candidates for quantum mechanical bits, the fundamental units and building blocks of a quantum computer. The ability to address quantum dot spins optically allows us to initialise and manipulate the state of the quantum bit. Gaining information on the qubit, for example by reading out its state, not only requires state-selective optical excitation, but also access to the single photons scattered in response by the quantum dot. Further, for a distributed computer architecture where nodes of few quantum bits are interlinked via optical communication channels photonic quantum bits are required to faithfully transmit the quantum information. In this thesis we advocate resonant excitation of quantum dot transitions and collection of the resonance fluorescence to address two outstanding challenges: generating dephasing-free single photons for use as flying quantum bits and single-shot spin readout. To this end we investigate the spectral and first-order coherence properties of quantum dot resonance fluorescence. In particular, we directly observe highly coherent scattering in the low Rabi frequency limit which has remained unexplored for solid-state single photon emitters so far. At the same time, interactions with the semiconductor environment are revealed and quantified through their optical signatures: exciton-phonon coupling, nuclear spin dynamics and local electric field fluctuations signal a departure from the ideal atom-like behaviour. Taking advantage of the laser-like coherence of single phase-locked quantum dot photons in the Heitler regime, we demonstrate near-ideal two-photon quantum interference. This benchmark measurement is a precursor for the photonic entanglement of distant quantum dot spins in a quantum optical network, and the results here predict a high fidelity operation. Finally, moving to tunnel-coupled quantum dot molecules we show that the overlap of carrier wave functions in two closely spaced quantum dots forms new spin-selective optical transitions not available in single quantum dots. Then, the presence or absence of scattered photons reveals the electron spin. Intermittency in the quantum dot resonance fluorescence allowed us, for the first time, to observe spin quantum jumps in real-time. Both achievements - highly coherent photons and spin readout - provide the missing link to attempt creation of a small-scale quantum network now.
We demonstrate high-fidelity reversible transfer of quantum information from the polarization of photons into the spin state of an electron-hole pair in a semiconductor quantum dot. Moreover, spins are electrically manipulated on a subnanosecond time scale, allowing us to coherently control their evolution. By varying the area of the electrical pulse, we demonstrate phase-shift and spin-flip gate operations with near-unity fidelities. Our system constitutes a controllable quantum interface between flying and stationary qubits, an enabling technology for quantum logic in the solid state.