Electron Spin Coherence Research Articles

Ultrafast all-optical coherence of molecular electron spins in room-temperature water solution.

The tunability and spatial precision of paramagnetic molecules makes them attractive for quantum sensing. However, usual microwave-based detection methods have poor temporal and spatial resolution, and optical methods compatible with room-temperature solutions have remained elusive. Here, we utilized pump-probe polarization spectroscopy to initialize and track electron spin coherence in a molecule. Designed to efficiently couple spins to light, aqueous K2IrCl6 enabled detection of few-picosecond free induction decay at room temperature and micromolar concentrations. Viscosity was found to strongly vary decoherence lifetimes. This approach has improved the experimental time-resolution by up to five orders of magnitude, making it possible to observe molecular electron spin coherence in a system that only exhibits coherence below 25 K with traditional techniques.

The contribution of methyl groups to electron spin decoherence of nitroxides in glassy matrices.

Long electron spin coherence lifetimes are crucial for high sensitivity and resolution in many pulse electron paramagnetic resonance (EPR) experiments aimed at measuring hyperfine and dipolar couplings, as well as in potential quantum sensing applications of molecular spin qubits. In immobilized systems, methyl groups contribute significantly to electron spin decoherence as a result of methyl torsional quantum tunneling. We examine the electron spin decoherence dynamics of the nitroxide radical 2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO) in both a methyl-free solvent and a methyl-containing solvent at cryogenic temperature. We model nitroxide and solvent methyl effects on decoherence using cluster correlation expansion (CCE) simulations extended to include methyl tunneling and compare the calculations to experimental data. We show that by using the methyl tunneling frequency as a fit parameter, experimental Hahn echo decays can be reproduced fairly well, allowing structural properties to be investigated in silico. In addition, we examine the Hahn echo of a hypothetical system with an unpaired electron and a single methyl to determine the effect of geometric configuration on methyl-driven electron spin decoherence. The simulations show that a methyl group contributes the most to electron spin decoherence if it is located between 2.5 and 6-7Å from the electron spin, with its orientation being of secondary importance.

Investigation of PCVSi− defect in 4H–SiC as a candidate for a qubit

Abstract Exploration of spin defects in semiconductors for possible qubits encourages the development of the quantum field. Silicon carbide (SiC) is a suitable platform to carry spin defects, due to its excellent electrical, mechanical and optical properties, together with its convenience for crystallographic growth and doping processes. In this study, a negatively charged phosphorus-vacancy (PCVSi −) defect, consisting of a silicon vacancy and nearby substitution of a phosphorus atom to a carbon atom in 4H–SiC, is investigated by first-principles calculations. This defect is demonstrated to possess a high spin (S = 1) with relatively low formation energy. Computed zero-phonon line energy and zero-field splitting parameters of this defect are close to those of neutral divacancy (VCVSi 0), negatively charged nitrogen-vacancy center (NCVSi −) and some other color centers, which indicate a similarity of both optical and spin properties among them. Moreover, the electron spin coherence time of this defect turns out to be 1.15–1.40 ms. Such a long coherence time provides the defect with reliability for quantum information processing. Our results show that the PCVSi − defect can be a promising candidate for a qubit.

A Paired-Ion Framework Composed of Vanadyl Porphyrin Molecular Qubits Extends Spin Coherence Times.

Molecular electron spin qubits arranged in precise arrays have great potential for use in quantum information science applications. Molecular qubits are synthetically versatile and can be placed in ordered arrangements upon incorporation into a new class of materials known as paired-ion frameworks (PIFs). A PIF composed of vanadyl porphyrin molecular qubits, VOTCPP-PIF-1, was synthesized as single crystals. Electron paramagnetic resonance spectroscopy was used to study their spin coherence at temperatures up to 293 K. A suspension of VOTCPP-PIF-1 at 5 K in dimethylformamide (DMF) had a spin-spin relaxation time (Tm) of 270 ns. In DMF-d7 and at 5 K, the coherence time of this material increased to 370 ns. This increase in Tm is attributed to the lower gyromagnetic ratio of 2H compared to 1H, which results in weaker electron-nuclear dipolar coupling that reduces the effect of nuclear spin flips on electron spin coherence. In toluene, crystals of VOTCPP-PIF-1 had a Tm of 31 ns at 293 K, demonstrating that PIFs are a promising platform for creating materials for quantum information science applications.

Control of light-induced torque in quantum well waveguides through electron spin coherence

We explore the mechanical effects of light interacting with a quantum well waveguide, specifically focusing on the emergence of quantized torque. We investigate the response of the waveguide to the influence of two intense coupling fields in conjunction with two weaker fields. We find that the electron spin coherence plays a crucial role in amplifying the torque applied to the waveguide emitters. This heightened torque, in turn, triggers a distinctive circular current flow pattern within the waveguide. Furthermore, we explore different scenarios for modulating the torque by adjusting system parameters, thereby establishing a means to control current flow. The emergence of a light-induced quantized torque not only illuminates the interplay between quantum emitters and electromagnetic fields but also opens up exciting possibilities for innovative approaches to govern induced-torque behavior within quantum well waveguides.

Electric Field Effects in Hybrid Perovskites Studied via Picosecond Kerr Microscopy.

We present time-resolved Kerr rotation (TRKR) spectra in thin films of CH3NH3PbI3 (MAPI) hybrid perovskite using a unique picosecond microscopy technique at 4 K having a spatial resolution of 2 μm and temporal resolution of 1 ps, subjected to both an in-plane applied magnetic field up to 700 mT and an electric field up to 104 V/cm. We demonstrate that the obtained TRKR dynamics and spectra are substantially inhomogeneous across the MAPI films with prominent resonances at the exciton energy and interband transition of this compound. From the obtained quantum beating response as a function of magnetic field in the Voigt configuration, we also extract the inhomogeneity of the electron and hole Lande g-values and spin coherence time, T2*. We also report the TRKR dependence on both the applied magnetic field and electric field. From the change in the quantum beating dynamics, we found that T2* substantially decreases upon the application of an electric field. At the same time, from the induced spatial TRKR changes, we show that the electric field induced effects are caused by ion migration in the MAPI films.

Precise Characterization of a Waveguide Fiber Interface in Silicon Carbide.

Spin-active optical emitters in silicon carbide are excellent candidates toward the development of scalable quantum technologies. However, efficient photon collection is challenged by undirected emission patterns from optical dipoles, as well as low total internal reflection angles due to the high refractive index of silicon carbide. Based on recent advances with emitters in silicon carbide waveguides, we now demonstrate a comprehensive study of nanophotonic waveguide-to-fiber interfaces in silicon carbide. We find that across a large range of fabrication parameters, our experimental collection efficiencies remain above 90%. Further, by integrating silicon vacancy color centers into these waveguides, we demonstrate an overall photon count rate of 181 kilo-counts per second, which is an order of magnitude higher compared to standard setups. We also quantify the shift of the ground state spin states due to strain fields, which can be introduced by waveguide fabrication techniques. Finally, we show coherent electron spin manipulation with waveguide-integrated emitters with state-of-the-art coherence times of T 2 ∼ 42 μs. The robustness of our methods is very promising for quantum networks based on multiple orchestrated emitters.

Optical and microstructural characterization of Er3+ doped epitaxial cerium oxide on silicon

Rare-earth ion dopants in solid-state hosts are ideal candidates for quantum communication technologies, such as quantum memories, due to the intrinsic spin–photon interface of the rare-earth ion combined with the integration methods available in the solid state. Erbium-doped cerium oxide (Er:CeO2) is a particularly promising host material platform for such a quantum memory, as it combines the telecom-wavelength (∼1.5μm) 4f–4f transition of erbium, a predicted long electron spin coherence time when embedded in CeO2, and a small lattice mismatch with silicon. In this work, we report on the epitaxial growth of Er:CeO2 thin films on silicon using molecular beam epitaxy, with controlled erbium concentration between 2 and 130 parts per million (ppm). We carry out a detailed microstructural study to verify the CeO2 host structure and characterize the spin and optical properties of the embedded Er3+ ions as a function of doping density. In as-grown Er:CeO2 in the 2–3 ppm regime, we identify an EPR linewidth of 245(1) MHz, an optical inhomogeneous linewidth of 9.5(2) GHz, an optical excited state lifetime of 3.5(1) ms, and a spectral diffusion-limited homogeneous linewidth as narrow as 4.8(3) MHz. We test the annealing of Er:CeO2 films up to 900 °C, which yields narrowing of the inhomogeneous linewidth by 20% and extension of the excited state lifetime by 40%.

Long Electron Spin Coherence Times of Atomic Hydrogen Trapped in Silsesquioxane Cages.

Encapsulated atomic hydrogen in cube-shaped octasilsesquioxane (POSS) cages of the Si8O12R8 type (where R is an organic group) is one of the simplest alternative stable systems to paramagnetic endofullerenes that have been regarded as key elements of spin-based quantum technologies. Apart from common sources of decoherence such as nuclear spin and spectral diffusion, all H@POSS species studied so far suffer from additional shortening of T2 at low temperatures due to methyl group rotations. Here we eliminate this factor for the first time by studying the smallest methyl-free derivative with R = H, namely, H@T8H8. By applying dynamical decoupling methods, we measure electron spin coherence times T2 up to 280 ± 76 μs at T = 90 K and observe a linear dependence of the decoherence rate 1/T2 on trapped hydrogen concentrations, which we attribute to the spin dephasing mechanism of instantaneous diffusion and a nonuniform spatial distribution of encapsulated H atoms.

Efficient two-dimensional Fraunhofer diffraction pattern via electron spin coherence

In this letter, we have discussed the two-dimensional diffraction pattern via electron spin coherence in a GaAs quantum dot. Impulsive stimulated Raman excitation utilizing coherent optical fields is employed for the purpose of regulating the electron spin coherence within a charged ensemble of GaAs quantum dots, by means of an intermediate charged exciton (trion) state. We show that for the coupling two-dimensional standing wave (SW) field in the x and y directions, the two-dimensional Fraunhofer pattern can be formed for a weak probe light. By using the experimental parameters and controlling the Rabi frequency of the SW field and relative phase between applied lights, the symmetry and asymmetry diffraction pattern are obtained for the weak probe light due to the four-wave mixing mechanism. Our proposed model may have potential applications in high-capacity optical communications and quantum information technologies.

Operating mode dependent energy transfer efficiency in a quantum well waveguide

In this paper, we delve into the intricate interplay between optical fields with varying relative phases in a closed-loop configuration semiconductor quantum well waveguide with four distinct energy levels, and how it impacts the Fraunhofer diffraction patterns obtained via four-wave mixing. By harnessing a strong control field, a standing wave driving field, and two weak probe and signal fields, we drive the waveguide to generate these patterns with maximum efficiency. To achieve this, we consider three distinct light-matter interaction scenarios, where the system is first set up in either a lower electromagnetically induced transparency or a coherent population trapping state, followed by a final state that enables electron spin coherence (ESC) induction. Our results reveal that the efficiency of Fraunhofer diffraction in the quantum well waveguide can be enhanced significantly under specific parameter regimes via the spin coherence effect. Further investigation of the light-matter interaction in the ESC zone, where only one of the control fields is a standing wave field, demonstrates that spin coherence facilitates more efficient transfer of energy from the probe light to the third and fourth orders, highlighting its crucial role in shaping the diffraction patterns.

Room Temperature Electron Spin Coherence in Photogenerated Molecular Spin Qubit Candidates.

One of the main challenges in the emerging field of molecular spintronics is the identification of new spin qubit materials for quantum information applications. In this regard, recent work has shown that photoexcited chromophore-radical systems are promising candidates to expand our repertoire of suitable candidate molecules. Here, we investigate a series of three chromophore-radical compounds composed of a perylene diimide (PDI) chromophore and a stable 2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO) radical by transient electron paramagnetic resonance (EPR) techniques. We explore the influence of isotope labeling of the TEMPO moiety on the EPR spectra and electron spin coherence times of the molecular quartet states generated upon photoexcitation and illustrate that (i) a coherent manipulation of the spin state is possible in these systems even at room temperature and that (ii) a spin coherence time of 0.7 μs can be achieved under these conditions. This demonstration of electron spin coherence at ambient temperatures paves the way for practical applications of such systems in functional molecular devices.

Thermally Ultrarobust S = 1/2 Tetrazolinyl Radicals: Synthesis, Electronic Structure, Magnetism, and Nanoneedle Assemblies on Silicon Surface.

Open-shell organic molecules, including S = 1/2 radicals, may provide enhanced properties for several emerging technologies; however, relatively few synthesized to date possess robust thermal stability and processability. We report the synthesis of S = 1/2 biphenylene-fused tetrazolinyl radicals 1 and 2. Both radicals possess near-perfect planar structures based on their X-ray structures and density-functional theory (DFT) computations. Radical 1 possesses outstanding thermal stability as indicated by the onset of decomposition at 269 °C, based on thermogravimetric analysis (TGA) data. Both radicals possess very low oxidation potentials <0 V (vs. SCE) and their electrochemical energy gaps, Ecell ≈ 0.9 eV, are rather low. Magnetic properties of polycrystalline 1 are characterized by superconducting quantum interference device (SQUID) magnetometry revealing a one-dimensional S = 1/2 antiferromagnetic Heisenberg chain with exchange coupling constant J'/k ≈ -22.0 K. Radical 1 in toluene glass possesses a long electron spin coherence time, Tm ≈ 7 μs in the 40-80 K temperature range, a property advantageous for potential applications as a molecular spin qubit. Radical 1 is evaporated under ultrahigh vacuum (UHV) forming assemblies of intact radicals on a silicon substrate, as confirmed by high-resolution X-ray photoelectron spectroscopy (XPS). Scanning electron microscope (SEM) images indicate that the radical molecules form nanoneedles on the substrate. The nanoneedles are stable for at least 64 hours under air as monitored by using X-ray photoelectron spectroscopy. Electron paramagnetic resonance (EPR) studies of the thicker assemblies, prepared by UHV evaporation, indicate radical decay according to first-order kinetics with a long half-life of 50 ± 4 days at ambient conditions.

Coherence protection of spin qubits in hexagonal boron nitride

Spin defects in foils of hexagonal boron nitride are an attractive platform for magnetic field imaging, since the probe can be placed in close proximity to the target. However, as a III-V material the electron spin coherence is limited by the nuclear spin environment, with spin echo coherence times of ∽100 ns at room temperature accessible magnetic fields. We use a strong continuous microwave drive with a modulation in order to stabilize a Rabi oscillation, extending the coherence time up to ∽ 4μs, which is close to the 10 μs electron spin lifetime in our sample. We then define a protected qubit basis, and show full control of the protected qubit. The coherence times of a superposition of the protected qubit can be as high as 0.8 μs. This work establishes that boron vacancies in hexagonal boron nitride can have electron spin coherence times that are competitive with typical nitrogen vacancy centres in small nanodiamonds under ambient conditions.

Distance measurements between 5 nanometer diamonds - single particle magnetic resonance or optical super-resolution imaging?

5 nanometer sized detonation nanodiamonds (DNDs) are studied as potential single-particle labels for distance measurements in biomolecules. Nitrogen-vacancy (NV) defects in the crystal lattice can be addressed through their fluorescence and optically-detected magnetic resonance (ODMR) of a single particle can be recorded. To achieve single-particle distance measurements, we propose two complementary approaches based on spin-spin coupling or optical super-resolution imaging. As a first approach, we try to measure the mutual magnetic dipole-dipole coupling between two NV centers in close DNDs using a pulse ODMR sequence (DEER). The electron spin coherence time, a key parameter to reach long distance DEER measurements, was prolonged using dynamical decoupling reaching T 2,DD ≈ 20 μs, extending the Hahn echo decay time T 2 by one order of magnitude. Nevertheless, an inter-particle NV-NV dipole coupling could not be measured. As a second approach, we successfully localize the NV centers in DNDs using STORM super-resolution imaging, achieving a localization precision of down to 15 nm, enabling optical nanometer-scale single-particle distance measurements.

Highly efficient exchange of orbital angular momentum of light via electron spin coherence

In this letter we analysed the efficient exchange of orbital angular momentum (OAM) of light in a double V-type semiconductor quantum well via electron spin coherence. We found that due to the four-wave mixing (FWM) mechanism the OAM state of the vortex light can transfer from applied lights to a new generated signal beam when the efficiency of the FWM processes is enough high. We also shown that the absorption spectrum of the new generated light depends on the OAM number and azimuthal angle of the optical vortex light. We realized that for some specific parametric conditions the absorption spectrum of the generated light becomes negative which corresponds to the lasing without inversion.

Hyperfine interactions and coherent spin dynamics of isotopically purified 167Er3+ in polycrystalline Y2O3

167Er3+ doped solids are a promising platform for quantum technology due to erbium’s telecom C-band optical transition and its long hyperfine coherence times. We experimentally study the spin Hamiltonian and dynamics of 167Er3+ spins in Y2O3 using electron paramagnetic resonance (EPR) spectroscopy. The anisotropic electron Zeeman, hyperfine and nuclear quadrupole matrices are fitted using data obtained by X-band (9.5 GHz) EPR spectroscopy. We perform pulsed EPR spectroscopy to measure spin relaxation time T 1 and coherence time T 2 for the 3 principal axes of an anisotropic g tensor. Long electronic spin coherence time up to 24.4 μs is measured for lowest g transition at 4 K, exceeding previously reported values at much lower temperatures. Measurements of decoherence mechanism indicates T 2 limited by spectral diffusion and instantaneous diffusion. Long spin coherence times, along with a strong anisotropic hyperfine interaction makes 167Er3+:Y2O3 a rich system and an excellent candidate for spin-based quantum technologies.

Electron-spin spectral diffusion in an erbium doped crystal at millikelvin temperatures

Erbium doped crystals offer a versatile platform for hybrid quantum devices because they combine magnetically sensitive electron-spin transitions with telecom-wavelength optical transitions. At the high doping concentrations necessary for many quantum applications, however, strong magnetic interactions of the electron-spin bath lead to excess spectral diffusion and rapid decoherence. Here we lithographically fabricate a 4.4 GHz superconducting planar microresonator on a ${\text{CaWO}}_{4}$ crystal doped with Er ions at a concentration of 20 ppm relative to Ca. Using the microwave resonator, we characterize the spectral diffusion processes that limit the electron-spin coherence of Er ions at millikelvin temperatures by applying two- and three-pulse echo sequences. The coherence time shows a strong temperature dependence, reaching 1.3 ms at 23 mK for an electron-spin transition of $^{167}\mathrm{Er}$.

Room-Temperature Quantitative Quantum Sensing of Lithium Ions with a Radical-Embedded Metal-Organic Framework.

Recent advancements in quantum sensing have sparked transformative detection technologies with high sensitivity, precision, and spatial resolution. Owing to their atomic-level tunability, molecular qubits and ensembles thereof are promising candidates for sensing chemical analytes. Here, we show quantum sensing of lithium ions in solution at room temperature with an ensemble of organic radicals integrated in a microporous metal-organic framework (MOF). The organic radicals exhibit electron spin coherence and microwave addressability at room temperature, thus behaving as qubits. The high surface area of the MOF promotes accessibility of the guest analytes to the organic qubits, enabling unambiguous identification of lithium ions and quantitative measurement of their concentration through relaxometric and hyperfine spectroscopic methods based on electron paramagnetic resonance (EPR) spectroscopy. The sensing principle presented in this work is applicable to other metal ions with nonzero nuclear spin.

Electron spin coherence on a solid neon surface

A single electron floating on the surface of a condensed noble-gas liquid or solid can act as a spin qubit with ultralong coherence time, thanks to the extraordinary purity of such systems. Previous studies suggest that the electron spin coherence time on a superfluid helium (He) surface can exceed 100 s. In this paper, we present theoretical studies of the electron spin coherence on a solid neon (Ne) surface, motivated by our recent experimental realization of single-electron charge qubit on solid Ne. The major spin decoherence mechanisms investigated include the fluctuating Ne diamagnetic susceptibility due to thermal phonons, the fluctuating thermal current in normal metal electrodes, and the quasi-statically fluctuating nuclear spins of the 21Ne ensemble. We find that at a typical experimental temperature about 10 mK in a fully superconducting device, the electron spin decoherence is dominated by the third mechanism via electron–nuclear spin–spin interaction. For natural Ne with 2700 ppm abundance of 21Ne, the estimated inhomogeneous dephasing time is around 0.16 ms, already better than most semiconductor quantum-dot spin qubits. For commercially available, isotopically purified Ne with 1 ppm of 21Ne, can be 0.43 s. Under the application of Hahn echoes, the coherence time T 2 can be improved to 30 ms for natural Ne and 81 s for purified Ne. Therefore, the single-electron spin qubits on solid Ne can serve as promising new spin qubits.