We experimentally demonstrate how coherent population trapping (CPT) for donor-bound electron spins in GaAs results in autonomous feedback that prepares stabilized states for the spin polarization of nuclei around the electrons. CPT was realized by excitation with two lasers to a bound-exciton state. Transmission studies of the spectral CPT feature on an ensemble of electrons directly reveal the statistical distribution of prepared nuclear-spin states. Tuning the laser driving from blue to red detuned drives a transition from one to two stable states. Our results have importance for ongoing research on schemes for dynamic nuclear-spin polarization, the central spin problem, and control of spin coherence.
We experimentally demonstrate how coherent population trapping (CPT) for donor-bound electron spins in GaAs results in autonomous feedback that prepares stabilized states for the spin polarization of nuclei around the electrons. CPT was realized by excitation with two lasers to a bound-exciton state. Transmission studies of the spectral CPT feature on an ensemble of electrons directly reveal the statistical distribution of prepared nuclear-spin states. Tuning the laser driving from blue to red detuned drives a transition from one to two stable states. Our results have importance for ongoing research on schemes for dynamic nuclear-spin polarization, the central spin problem, and control of spin coherence.
Feedback control is a powerful tool to stabilize systems for which precision control is difficult to impose directly, such as the environment of an open quantum system. Reduction of noise from the environment is a major challenge on the road to harnessing delicate quantum effects such as superposition and entanglement. In particular, spin states of defects and quantum dots in semiconductors display promising coherence properties for future applications, often being limited by disturbance from disordered nuclear spins in their environment. Here we show how optical coherent population trapping (CPT) of the spin of localized semiconductor electrons stabilizes the surrounding nuclear spins via feedback control. We find distinct control regimes for different signs of laser detuning and examine the transition from an unpolarized, narrowed state to a polarized state possessing a bistability. The narrowing of the state protects the electron spin against dephasing and yields self-improving CPT. Our analysis is relevant for a variety of solid-state systems where hyperfine-induced dephasing is a limitation for using electron spin coherence.
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.
Summary form only given. Semiconductor quantum dots (QD) offer the current state-of-the-art in intensity and coherence for single photon generation, as well as serving as a testbed for various novel approaches to quantum networking. Their high brightness provides a means to produce high-bandwidth spin-photon entanglement [1]. However, the purity and usefulness of the generated entangled state is severely limited by the coherence time of the QD charge carrier spin, typically on the order of 2ns for electrons in a self-assembled InGaAs QD. This limit is imposed by low-frequency fluctuations of the Overhauser field generated by host nuclear spins, affecting the electron spin resonance frequency.Here, we measure an extension of T2 by over an order of magnitude, enabled by prior preparation of the surrounding nuclear spin bath. The interplay of dynamic nuclear polarization and coherent population trapping (CPT) can lead to a controllable mechanism that locks the nuclear spins, and thereby reduces the Overhauser field fluctuations [2,3]. We use the lambda-scheme formed by an optical transition between bound electron and negatively-charged exciton in Voigt geometry at a field of 5T. There, we use the CPT dark-state resonance as a means to lock the polarization state of the nuclear spins surrounding the electron spin. Using ultrafast optical spin rotations, we perform a Ramsey sequence following a CPT preparation of the nuclear spins, to measure the Free Induction Decay of the electron spin coherence [4]. With a pulse sequence composed of 70μs of CPT preparation, followed by 70μs of repeated Ramsey measurements, as shown in Fig. 1a, we observe coherent electron spin oscillations at a Ramsey delay of 29ns, as shown in Fig. 1b. The oscillations are free of the deleterious effects of nuclear polarization typical in such measurements [5], indicating the stabilization of the mean Overhauser field to a fixed value. The measured T2 of 39ns is over an order of magnitude longer than the Ti of 3ns measured on the system with unprepared nuclear spins, as shown in Fig. 1c.
We report experimental studies of coherent spin dynamics of donor-bound electrons in high-purity GaAs by using transient differential transmission. The donor-bound exciton transitions, which are not visible in the linear absorption spectrum, are spectrally resolved in the nonlinear differential transmission spectra. The spin beats in the transient differential transmission response, arising from electron spin precession in an external magnetic field, are investigated with the pump and probe coupling to various donor-bound exciton transitions. The spectral dependence of the spin beats provides important information on the polarization selection rule for the underlying donor-bound exciton transitions. The polarization selection rules deduced from these experiments indicate that contributions from higher-energy donor-bound exciton transitions can severely limit the effectiveness of optical spin control using mechanisms such as polarization-dependent optical Stark shifts.
We show that a quantum interference effect in optical absorption from two electronic spin states of a solid-state emitter can be used to prepare the surrounding environment of nuclear spins in well-defined states, thereby suppressing electronic spin dephasing. The coupled electron-nuclei system evolves into a coherent population trapping state by optical-excitation-induced nuclear-spin diffusion for a broad range of initial optical detunings. The spectroscopic signature of this evolution where the single-electron strongly modifies its environment is a drastic broadening of the dark resonance in optical absorption experiments. The large difference in electronic and nuclear time scales allows us to verify the preparation of nuclear spins in the desired state.
Abstract We employ the electronic spin of a single nitrogen-vacancy (NV) defect in diamond to detect and control the quantum state of remote nuclear spins coupled by hyperfine interaction. More precisely, our work focuses on individual 13C 13 C nuclei featuring a moderate hyperfine coupling strength ( ∼1 ∼ 1 MHz) with the NV’s electron spin. Two different methods providing an efficient room-temperature polarization of these peculiar 13C 13 C nuclear spins are described. The first one is based on a polarization transfer from the NV electron spin to the 13C 13 C nucleus, which is mediated by the anisotropic component of the hyperfine interaction. The second one relies on coherent population trapping (CPT) within a Λ Λ -type energy-level configuration in the microwave domain, which enables to initialize the 13C 13 C nuclear spin in any quantum state superposition on the Bloch sphere. This CPT protocol is performed in an unusual regime for which relaxation from the excited level of the Λ Λ -scheme is externally triggered by optical pumping and separated in time from coherent microwave excitations. For these two polarization techniques, we investigate the impact of optical illumination on the nuclear spin polarization efficiency. This work adds new methods to the quantum toolbox used for coherent control of individual nuclear spins in diamond, which might find applications in quantum metrology. Graphical Abstract