Long-lived Spin Coherence Research Articles

A quantum coherent spin in hexagonal boron nitride at ambient conditions.

Solid-state spin-photon interfaces that combine single-photon generation and long-lived spin coherence with scalable device integration-ideally under ambient conditions-hold great promise for the implementation of quantum networks and sensors. Despite rapid progress reported across several candidate systems, those possessing quantum coherent single spins at room temperature remain extremely rare. Here we report quantum coherent control under ambient conditions of a single-photon-emitting defect spin in a layered van der Waals material, namely, hexagonal boron nitride. We identify that the carbon-related defect has a spin-triplet electronic ground-state manifold. We demonstrate that the spin coherence is predominantly governed by coupling to only a few proximal nuclei and is prolonged by decoupling protocols. Our results serve to introduce a new platform to realize a room-temperature spin qubit coupled to a multiqubit quantum register or quantum sensor with nanoscale sample proximity.

Stark Tuning of Telecom Single-Photon Emitters Based on a Single Er3+

The implementation of scalable quantum networks requires photons at the telecom band and long-lived spin coherence. The single Er3+ in solid-state hosts is an important candidate that fulfills these critical requirements simultaneously. However, to entangle distant Er3+ ions through photonic connections, the emission frequency of individual Er3+ in solid-state matrix must be the same, which is challenging because the emission frequency of Er3+ depends on its local environment. Herein, we propose and experimentally demonstrate the Stark tuning of the emission frequency of a single Er3+ in a Y2SiO5 crystal by employing electrodes interfaced with a silicon photonic crystal cavity. We obtain a Stark shift of 182.9±0.8 MHz, which is approximately 27 times of the optical emission linewidth, demonstrating promising applications in tuning the emission frequency of independent Er3+ into the same spectral channels. Our results provide a useful solution for construction of scalable quantum networks based on single Er3+ and a universal tool for tuning emission of individual rare-earth ions.

Long-lived electron spin coherence in Ga-doped ZnO at room temperature

Electron spin dynamics are studied in Ga-doped ZnO single crystals by time-resolved Faraday and Kerr rotation spectroscopies. Long-lived spin coherence with two dephasing processes is discovered where the characteristic time is up to 5.2 ns at room temperature. Through the dependence measurements of laser wavelength and temperature, the room-temperature long-lived spin signal is attributed to localized electrons. The spin dephasing (relaxation) processes are independent of transverse (longitudinal) magnetic fields, indicating the spin dephasing not resulting from the g-factor inhomogeneity and electron-nuclear hyperfine interaction. It reveals that the two spin dephasing processes originate from two types of localized electrons, both of which are dominated by the anisotropic exchange Dzyaloshinskii-Moriya interaction between adjacent localized electrons.

Coupling light to a nuclear spin gas with a two-photon linewidth of five millihertz.

Nuclear spins of noble gases feature extremely long coherence times but are inaccessible to optical photons. Here, we realize a coherent interface between light and noble-gas spins that is mediated by alkali atoms. We demonstrate the optical excitation of the noble-gas spins and observe the coherent back action on the light in the form of high-contrast two-photon spectra. We report on a record two-photon linewidth of 5 ± 0.7 mHz above room temperature, corresponding to a 1-min coherence time. This experiment provides a demonstration of coherent bidirectional coupling between light and noble-gas spins, rendering their long-lived spin coherence accessible for manipulations in the optical domain.

Deep Three-Dimensional Solid-State Qubit Arrays with Long-Lived Spin Coherence

Three-dimensional arrays of silicon transistors increase the density of bits. Solid-state qubits are much larger so could benefit even more from using the third dimension given that useful fault-tolerant quantum computing will require at least 100,000 physical qubits and perhaps one billion. Here we use laser writing to create 3D arrays of nitrogen-vacancy centre (NVC) qubits in diamond. This would allow 5 million qubits inside a commercially available 4.5x4.5x0.5 mm diamond based on five nuclear qubits per NVC and allowing $(10 \mu m)^3$ per NVC to leave room for our laser-written electrical control. The spin coherence times we measure are an order of magnitude longer than previous laser-written qubits and at least as long as non-laser-written NVC. As well as NVC quantum computing, quantum communication and nanoscale sensing could benefit from the same platform. Our approach could also be extended to other qubits in diamond and silicon carbide.

Electromagnetic 0.1-100 kHz noise does not disrupt orientation in a night-migrating songbird implying a spin coherence lifetime of less than 10 µs.

According to the currently prevailing theory, the magnetic compass sense in night-migrating birds relies on a light-dependent radical-pair-based mechanism. It has been shown that radio waves at megahertz frequencies disrupt magnetic orientation in migratory birds, providing evidence for a quantum-mechanical origin of the magnetic compass. Still, many crucial properties, e.g. the lifetime of the proposed magnetically sensitive radical pair, remain unknown. The current study aims to estimate the spin coherence time of the radical pair, based on the behavioural responses of migratory birds to broadband electromagnetic fields covering the frequency band 0.1-100 kHz. A finding that the birds were unable to use their magnetic compass under these conditions would imply surprisingly long-lived (greater than 10 µs) spin coherence. However, we observed no effect of 0.1-100 kHz radiofrequency (RF) fields on the orientation of night-migratory Eurasian blackcaps (Sylvia atricapilla). This suggests that the lifetime of the spin coherence involved in magnetoreception is shorter than the period of the highest frequency RF fields used in this experiment (i.e. approx. 10 µs). This result, in combination with an earlier study showing that 20-450 kHz electromagnetic fields disrupt magnetic compass orientation, suggests that the spin coherence lifetime of the magnetically sensitive radical pair is in the range 2-10 µs.

Transporting Long-Lived Quantum Spin Coherence in a Photonic Crystal Fiber.

Confining particles in hollow-core photonic crystal fibers has opened up new prospects to scale up the distance and time over which particles can be made to interact with light. However, maintaining long-lived quantum spin coherence and/or transporting it over macroscopic distances in a waveguide remain challenging. Here, we demonstrate coherent guiding of ground-state superpositions of ^{85}Rb atoms over a centimeter range and hundreds of milliseconds inside a hollow-core photonic crystal fiber. The decoherence is mainly due to dephasing from the residual differential light shift from the optical trap and the inhomogeneity of an ambient magnetic field. Our experiment establishes an important step towards a versatile platform that can lead to applications in quantum information networks and a matter wave circuit for quantum sensing.

Tailoring multilayer quantum wells for spin devices

The electron spin dynamics in multilayer GaAs/AlGaAs quantum wells, containing high-mobility dense two-dimensional electron gases, have been studied using time-resolved Kerr rotation and resonant spin amplification techniques. The electron spin dynamics was regulated through the wave function engineering and quantum confinement in multilayer quantum wells. We observed the spin coherence with a remarkably long dephasing time T2* > 13 ns for the structure doped beyond metal-insulator transition. Dyakonov-Perel spin relaxation mechanism, as well as the inhomogeneity of electron g-factor, was suggested as the major limiting factors for the spin coherence time. In the metallic regime, we found that the electron-electron collisions become dominant over microscopic scattering on the electron spin relaxation with the Dyakonov-Perel mechanism. Furthermore, the data analysis indicated that in our structure, due to the spin relaxation anisotropy, Dyakonov-Perel spin relaxation mechanism is efficient for the spins oriented in-plane and suppressed along the quantum well growth direction resulting in the enhancement of T2*. Our findings, namely, long-lived spin coherence persisting up to about room temperature, spin polarization decay time with and without a magnetic field, the spin-orbit field, single electron relaxation time, transport scattering time, and the electron-electron Coulomb scattering time highlight the attractiveness of n-doped multilayer systems for spin devices.

Spin relaxation of radicals in cryptochrome and its role in avian magnetoreception.

Long-lived spin coherence and rotationally ordered radical pairs have previously been identified as key requirements for the radical pair mechanism of the avian magnetic compass sense. Both criteria are hard to meet in a biological environment, where thermal motion of the radicals creates dynamic disorder and drives efficient spin relaxation. This has long been cited as a major stumbling block of the radical pair hypothesis. Here we combine Redfield relaxation theory with analytical solutions to a rotational diffusion equation to assess the impact of restricted rotational motion of the radicals on the operation of the compass. The effects of such motions are first investigated generally in small, model systems and are then critically examined in the magnetically sensitive flavin-tryptophan radical pair that is formed photochemically in the proposed magnetoreceptor protein, cryptochrome. We conclude that relaxation is slowest when rotational motion of the radicals within the protein is fast and highly constrained; that in a regime of slow relaxation, the motional averaging of hyperfine interactions has the potential to improve the sensitivity of the compass; and that consideration of motional effects can significantly alter the design criteria for an optimal compass. In addition, we demonstrate that motion of the flavin radical is likely to be compatible with its role as a component of a functioning radical-pair compass, whereas the motion of the tryptophan radical is less ideal, unless it is particularly fast.

Long-lived nanosecond spin coherence in high-mobility 2DEGs confined in double and triple quantum wells

We investigated the spin coherence of high-mobility two-dimensional electron gases confined in multilayer GaAs quantum wells. The dynamics of the spin polarization was optically studied using pump-probe techniques: time-resolved Kerr rotation and resonant spin amplification. For double and triple quantum wells doped beyond the metal-to-insulator transition, the spin-orbit interaction was tailored by the sample parameters of structural symmetry (Rashba constant), width, and electron density (Dresselhaus linear and cubic constants) which allow us to attain long dephasing times in the nanoseconds range. The determination of the scales, namely, transport scattering time, single-electron scattering time, electron-electron scattering time, and spin polarization decay time further supports the possibility of using n-doped multilayer systems for developing spintronic devices.

Long-lived nanosecond spin relaxation and spin coherence of electrons in monolayer MoS2 and WS2

A range of semiconductors can host both spin and valley polarizations. Optical experiments on single layers of transition metal dichalcogenides now show that inter-valley scattering can accelerate spin relaxation. The recently discovered monolayer transition metal dichalcogenides (TMDCs) provide a fertile playground to explore new coupled spin–valley physics1,2,3. Although robust spin and valley degrees of freedom are inferred from polarized photoluminescence (PL) experiments4,5,6,7,8, PL timescales are necessarily constrained by short-lived (3–100 ps) electron–hole recombination9,10. Direct probes of spin/valley polarization dynamics of resident carriers in electron (or hole)-doped TMDCs, which may persist long after recombination ceases, are at an early stage11,12,13. Here we directly measure the coupled spin–valley dynamics in electron-doped MoS2 and WS2 monolayers using optical Kerr spectroscopy, and reveal very long electron spin lifetimes, exceeding 3 ns at 5 K (two to three orders of magnitude longer than typical exciton recombination times). In contrast with conventional III–V or II–VI semiconductors, spin relaxation accelerates rapidly in small transverse magnetic fields. Supported by a model of coupled spin–valley dynamics, these results indicate a novel mechanism of itinerant electron spin dephasing in the rapidly fluctuating internal spin–orbit field in TMDCs, driven by fast inter-valley scattering. Additionally, a long-lived spin coherence is observed at lower energies, commensurate with localized states. These studies provide insight into the physics underpinning spin and valley dynamics of resident electrons in atomically thin TMDCs.

Long-lived spin coherence of indirect excitons in GaAs coupled quantum wells

We study spatially indirect excitons confined in a symmetric GaAs double quantum well. We show that the spin polarisation of very dilute gases can be optically imprinted, in both pure and superposition states. In the regime where indirect excitons can be localized, we observe at 350 mK that the excitons spin degree of freedom is frozen with a relaxation time comparable to the coherence time and to the radiative lifetime .

Spin-dependent electronic processes and long-lived spin coherence of deep-level trap sites in CdS nanocrystals

Carrier trapping in colloidal nanocrystals represents a major energy loss mechanism for excitonic states crucial to devices. Surprisingly little is known about the influence of the spin degree of freedom on the nature of these intrinsic trap centers or the types of coupling that these states experience. Here, a pulsed microwave optically detected magnetic resonance study is presented that aims to probe the interaction pathways existing between shallow band-edge trap states and the deep-level emissive chemical defect states responsible for the broad, low-energy emission common to CdS nanocrystals. Due to long spin coherence times (${T}_{2}$) of these states, Rabi flopping detected in the luminescence under magnetic resonance provides access to information regarding the modes of coupling of shallow-trapped electron-hole pairs, both of isolated species and of those in proximity to the emissive defect. Corresponding optically detected spin-echo experiments expose an extraordinarily long intrinsic spin coherence time (${T}_{2}\ensuremath{\approx}1.6$ \ensuremath{\mu}s) for colloidal nanocrystals, and an electron spin-echo envelope modulation indicative of local spin interactions. This effect provides opportunities for gaining the detailed chemical and structural information needed in order to eliminate energy loss mechanisms during the synthetic process.

Resonant spin amplification of resident electrons in CdTe/(Cd,Mg)Te quantum wells subject to tilted magnetic fields

Electron spin coherence in CdTe/(Cd,Mg)Te quantum wells is studied experimentally and theoretically in tilted external magnetic fields generated by a superconducting vector magnet. The long-lived spin coherence is measured by pump-probe Kerr rotation in the resonant spin amplification (RSA) regime. The shape of RSA signals is very sensitive to weak magnetic field components deviating from the Voigt or Faraday geometries.

Quantum hologram of macroscopically entangled light via the mechanism of diffuse light storage

In this paper, we consider a quantum memory scheme for light diffusely propagating through a spatially disordered atomic gas. A unique characteristic is enhanced trapping of the signal light pulse by quantum multiple scattering, which can be naturally integrated with the mechanism of stimulated Raman conversion into a long-lived spin coherence. Then, the quantum state of the light can be mapped onto the disordered atomic spin subsystem and can be stored in it for a relatively long time. The proposed memory scheme can be applicable for storage of the macroscopic analogue of the Ψ( − ) Bell state and the prepared entangled atomic state performs its quantum hologram, which suggests the possibility of further quantum information processing.

Long-lived, room-temperature electron spin coherence in colloidal CdS quantum dots

Time-resolved Faraday rotation spectroscopy is used to study the electron spin coherence in colloidal CdS quantum dots. Long-lived spin coherence with dephasing time T2*>3ns has been found at room temperature. Spin dynamics unaffected by the faster carrier recombination suggests the spin signal coming from the residual electrons in the dots. A small external transverse magnetic field of 50 mT can extend T2* ∼ 2 times longer compared with that in zero magnetic field. Hyperfine interaction between electron and nuclear spins limits the dephasing time in zero or low magnetic field, while for higher magnetic fields, inhomogeneous dephasing becomes to dominate the spin dynamics.

Long-lived electron spin coherence in CdSe/Zn(S,Se) self-assembled quantum dots

The electron spin coherence in $n$-doped and undoped, self-assembled CdSe/Zn(S,Se) quantum dots has been studied by time-resolved pump-probe Kerr rotation. Long-lived spin coherence persisting up to 13 ns after spin orientation has been found in the $n$-doped quantum dots, outlasting significantly the lifetimes of charge neutral and negatively charged excitons of 350--530 ps. The electron spin dephasing time as long as 5.6 ns has been measured in a magnetic field of 0.25 T. Hyperfine interaction of resident electrons with nuclear spin fluctuations is suggested as the main limiting factor for the dephasing time. The efficiency of this mechanism in II-VI and III-V quantum dots is analyzed.

Stationary light pulse in solids with long-lived spin coherence

We present a detailed analysis of stationary light pulses (SLP's) for the case of inhomogeneous broadening in both optical and spin transitions, which is normally found in solid materials with long-lived spin coherence. By solving the Langevin equations of motion for the density matrix elements under the integral over the entire range of the inhomogeneous broadenings, the necessary conditions for creating the SLP in a solid are obtained. Then the decay and diffusion processes that the SLP undergoes are analyzed. The characteristics of such processes are studied based on the analytic solution of the SLP with a slowly varying envelope. The dependence of SLP lifetime on inhomogeneous broadenings of spin and optical transitions, which can be regarded as the laser linewidth in the repump scheme, has been discussed.

High-speed spatially multimode atomic memory

We study the coherent storage and retrieval of a very short multimode light pulse in an atomic ensemble. We consider a quantum memory process based on the conversion of a signal pulse into a long-lived spin coherence via light matter interaction in an on-resonant $\ensuremath{\Lambda}$ -type system. In order to study the writing and reading processes we analytically solve the partial differential equations describing the evolution of the field and of the atomic coherence in time as well as in space. We show how to optimize the process for writing as well as for reading. If the medium length is fixed, for each length, there is an optimal value of the pulse duration. We discuss the information capacity of this memory scheme and we estimate the number of transverse modes that can be stored as a quantum hologram.

Quantum memory for light via a stimulated off-resonant Raman process: Beyond the three-levelΛ-scheme approximation

We consider a quantum memory scheme based on the conversion of a signal pulse into a long-lived spin coherence via stimulated off-resonant Raman process. For a storing medium consisting of alkali-metal atoms, we have calculated the Autler-Townes resonance structure created by a strong control field. By taking into account the upper hyperfine states of the ${D}_{1}$ optical transition, we show important deviations from the predictions of the usual three-level $\ensuremath{\Lambda}$-scheme approximation and we demonstrate an enhancement of the process for particular detunings of the control. We estimate the memory efficiency one can obtain using this configuration.