Nuclear Spin Coherence Times Research Articles

Pulsed optical pumping in electron spin vapor

Optically pumped atoms have essential applications in magnetic sensing, physics research, and inertial navigation. The polarization gradient caused by light absorption dramatically influences the performance of quantum sensors based on optical pumping. This paper presents a novel approach to address the trade-off between polarization gradient and sensitivity by introducing the pulsed optical pumping method. The interplay of pulsed optical pumping, relaxation, and diffusion processes leads to a more homogeneous distribution of electron spin. Experimental results indicate that the pulsed optical pumping technique increases the optically pumped magnetometer (OPM) signal strength by 12.8% and increases the nuclear spin coherence time by 12.29% in optically pumped co-magnetometer (OPCM). This technology has broad applications in sensors based on the optical pumping effect, such as OPM, OPCM, and nuclear magnetic resonance gyroscope, and holds immense promise for future advancements in the optical pumping field.

The quest for harnessing nuclear effects in graphene-based devices

The recent successes of superconducting qubits and the demonstration of quantum supremacy over classical bits herald a new era for information processing. Yet, the field is still in its infancy and there exist viable alternative candidates that can also store quantum information. In this review, we will highlight ideas, attempts, and the experimental progress to address nuclear spins in graphene, a readily available Dirac semimetal that consists of a single layer of carbon atoms. Carbon isotopes with a nuclear spin are rare in natural graphene. However, it is possible to enrich the spin-bearing 13C isotopes to produce large-scale graphene sheets, which constitute the testbed to store, transport, and retrieve spin information, or to engineer nanostructures. Here, the hyperfine interaction between the electron spins and the nuclear spins serves as an experimental control knob and mediator to address nuclear polarization and nuclear spin coherence times through electrical measurements. The exploitation of nuclear spins in graphene is thus an alluring perspective. We will discuss methods to synthesize 13C graphene and show experimental approaches and challenges to exploit the relatively weak hyperfine interaction in two-dimensional 13C graphene devices. The ultimate purpose, i.e., the exploitation of nuclear spins in graphene for information processing, is not within reach, but its potential for future applications merits a revisit of the current state-of-the-art.

Design Rules, Accurate Enthalpy Prediction, and Synthesis of Stoichiometric Eu3+ Quantum Memory Candidates.

Stoichiometric Eu3+ compounds have recently shown promise for building dense, optically addressable quantum memory as the cations' long nuclear spin coherence times and shielded 4f electron optical transitions provide reliable memory platforms. Implementing such a system, though, requires ultranarrow, inhomogeneous linewidth compounds. Finding this rare linewidth behavior within a wide range of potential chemical spaces remains difficult, and while exploratory synthesis is often guided by density functional theory (DFT) calculations, lanthanides' 4f electrons pose unique challenges for stability predictions. Here, we report DFT procedures that reliably reproduce known phase diagrams and correctly predict two experimentally realized quantum memory candidates. We are the first to synthesize the double perovskite halide Cs2NaEuF6. It is an air-stable compound with a calculated band gap of 5.0 eV that surrounds Eu3+ with mononuclidic elements, which are desirable for avoiding inhomogeneous linewidth broadening. We also analyze computational database entries to identify phosphates and iodates as the next generation of chemical spaces for stoichiometric quantum memory system studies. This work identifies new candidate platforms for exploring chemical effects on quantum memory candidates' inhomogeneous linewidth while also providing a framework for screening Eu3+ compound stability with DFT.

Coherent Control of a Nuclear Spin via Interactions with a Rare-Earth Ion in the Solid State

Individually addressed Er$^{3+}$ ions in solid-state hosts are promising resources for quantum repeaters, because of their direct emission in the telecom band and compatibility with silicon photonic devices. While the Er$^{3+}$ electron spin provides a spin-photon interface, ancilla nuclear spins could enable multi-qubit registers with longer storage times. In this work, we demonstrate coherent coupling between the electron spin of a single Er$^{3+}$ ion and a single $I=1/2$ nuclear spin in the solid-state host crystal, which is a fortuitously located proton ($^1$H). We control the nuclear spin using dynamical decoupling sequences applied to the electron spin, implementing one- and two-qubit gate operations. Crucially, the nuclear spin coherence time exceeds the electron coherence time by several orders of magnitude, because of its smaller magnetic moment. These results provide a path towards combining long-lived nuclear spin quantum registers with telecom-wavelength emitters for long-distance quantum repeaters.

Two-Photon Interface of Nuclear Spins Based on the Optonuclear Quadrupolar Effect

Photons and nuclear spins are two well-known building blocks in quantum information science and technology. Establishing an efficient interface between optical photons and nuclear spins, while highly desirable for hybridizing these two quantum systems, is challenging because the interactions between nuclear spins and the environment are usually weak in magnitude, and there is also a formidable gap between nuclear spin frequencies and optical frequencies. In this work, we propose an opto-nuclear quadrupolar (ONQ) effect, whereby optical photons can be efficiently coupled to nuclear spins, similar to Raman scattering. Compared to previous works, ancilla electron spins are not required for the ONQ effect. This leads to advantages such as applicability in defect-free nonmagnetic crystals and longer nuclear spin coherence time. In addition, the frequency of the optical photons can be arbitrary, so they can be fine-tuned to minimize the material heating and to match telecom wavelengths for long-distance communications. Using perturbation theory and first-principles calculations, we demonstrate that the ONQ effect is stronger by several orders of magnitude than other nonlinear optical effects that could couple to nuclear spins. Based on this rationale, we propose promising applications of the ONQ effect, including quantum memory, quantum transduction, and materials isotope spectroscopy. We also discuss issues relevant to the experimental demonstration of the ONQ effect.

Extending the spin coherence lifetimes of Er3+167:Y2SiO5 at subkelvin temperatures

${\mathrm{Er}}^{3+}\text{:}{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ is a material of particular interest due to its suitability for telecom-band quantum memories and quantum transducers interfacing optical communication with quantum computers working in the microwave regime. Extending the coherence lifetimes of the electron spins and the nuclear spins is essential for implementing efficient quantum information processing based on such hybrid electron-nuclear spin systems. The electron spin coherence time of ${\mathrm{Er}}^{3+}\text{:}{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ is so far limited to several microseconds, and there are significant challenges in optimizing coherence lifetimes simultaneously for both the electron and nuclear spins. Here we perform a pulsed-electron-nuclear-double-resonance investigation for an ${\mathrm{Er}}^{3+}$-doped material at subkelvin temperatures. At the lowest working temperature, the electron spin coherence time reaches 290 $\ifmmode\pm\else\textpm\fi{}$ 17 $\mathrm{\ensuremath{\mu}}\mathrm{s}$, which has been enhanced by 40 times compared with the previous results. In the subkelvin regime, a rapid increase in the nuclear spin coherence time is observed, and the longest coherence time of 738 $\ifmmode\pm\else\textpm\fi{}$ 6 $\mathrm{\ensuremath{\mu}}\mathrm{s}$ is obtained. These extended coherence lifetimes could be valuable resources for further applications of ${\mathrm{Er}}^{3+}\text{:}{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ in fiber-based quantum networks.

Seconds-Scale Coherence on Nuclear Spin Transitions of Ultracold Polar Molecules in 3D Optical Lattices.

Ultracold polar molecules (UPMs) are emerging as a novel and powerful platform for fundamental applications in quantum science. Here, we report characterization of the coherence between nuclear spin levels of ultracold ground-state sodium-rubidium molecules loaded into a 3D optical lattice with a nearly photon scattering limited trapping lifetime of 9(1)seconds. After identifying and compensating the main sources of decoherence, we achieve a maximum nuclear spin coherence time of T_{2}^{*}=3.3(6) s with two-photon Ramsey spectroscopy. Furthermore, based on the understanding of the main factor limiting the coherence of the two-photon Rabi transition, we obtain a Rabi line shape with linewidth below 0.8Hz. The simultaneous realization of long lifetime and coherence time, and ultrahigh spectroscopic resolution in our system unveils the great potentials of Ultracold polar molecules in quantum simulation, computation, and metrology.

Quantum control of nuclear-spin qubits in a rapidly rotating diamond

Nuclear spins in certain solids couple weakly to their environment, making them attractive candidates for quantum information processing and inertial sensing. When coupled to the spin of an optically-active electron, nuclear spins can be rapidly polarized, controlled and read via lasers and radiofrequency fields. Possessing coherence times of several milliseconds at room temperature, nuclear spins hosted by a nitrogen-vacancy center in diamond are thus intriguing systems to observe how classical physical rotation at quantum timescales affects a quantum system. Unlocking this potential is hampered by precise and inflexible constraints on magnetic field strength and alignment in order to optically induce nuclear polarization, which restricts the scope for further study and applications. In this work, we demonstrate optical nuclear spin polarization and rapid quantum control of nuclear spins in a diamond physically rotating at $1\,$kHz, faster than the nuclear spin coherence time. Free from the need to maintain strict field alignment, we are able to measure and control nuclear spins in hitherto inaccessible regimes, such as in the presence of a large, time-varying magnetic field that makes an angle of more than $100^\circ$ to the nitrogen-lattice vacancy axis. The field induces spin mixing between the electron and nuclear states of the qubits, decoupling them from oscillating rf fields. We are able to demonstrate that coherent spin state control is possible at any point of the rotation, and even for up to six rotation periods. We combine continuous dynamical decoupling with quantum feedforward control to eliminate decoherence induced by imperfect mechanical rotation. Our work liberates a previously inaccessible degree of freedom of the NV nuclear spin, unlocking new approaches to quantum control and rotation sensing.

Enhancement of nuclear spin coherence times by driving dynamic nuclear polarization at defect centers in solids

The hyperpolarization of nuclear spins can enable powerful imaging and sensing techniques provided the hyperpolarization is sufficiently long-lived. Recent experiments on nanodiamond $^{13}$C nuclear spins demonstrate that relaxation times can be extended by three orders of magnitude by building up dynamic nuclear polarization (DNP) through the driving of electron-nuclear flip-flop processes at defect centers. This finding raises the question of whether the nuclear spin coherence times are also impacted by this hyperpolarization process. Here, we theoretically examine the effect of DNP on the nuclear spin coherence times as a function of the hyperpolarization drive time. We do this by developing a microscopic theory of DNP in a nuclear spin ensemble coupled to microwave-driven defect centers in solids and subject to spin diffusion mediated by internuclear dipolar interactions. We find that, similarly to relaxation times, the nuclear spin coherence times can be increased substantially by a few orders of magnitude depending on the driving time. Our theoretical model and results will be useful for current and future experiments on enhancing nuclear spin coherence times via DNP.

Noise-resilient architecture of a hybrid electron-nuclear quantum register in diamond

A hybrid quantum register consisting of nuclear spins in a solid-state platform coupled to a central electron spin is expected to combine the advantages of its elements. However, the potential to exploit long nuclear spin coherence times is severely limited by magnetic noise from the central electron spin during external interrogation. We overcome this obstacle and present protocols for addressing a decoherence-free nuclear spin subspace which was not accessible by previously existing methods. We demonstrate the efficacy of our protocols using detailed numerical simulations of a nitrogen-vacancy centre with nearby 13C nuclei, and show that the resulting hybrid quantum register is immune to electron spin noise and external magnetic field drifts. Our work takes an important step toward realising robust quantum registers that can be easily manipulated, entangled, and, at the same time, well isolated from external noise, with applications from quantum information processing and communication to quantum sensing.

Protecting a Diamond Quantum Memory by Charge State Control.

In recent years, solid-state spin systems have emerged as promising candidates for quantum information processing. Prominent examples are the nitrogen-vacancy (NV) center in diamond, phosphorus dopants in silicon (Si:P), rare-earth ions in solids, and VSi-centers in silicon-carbide. The Si:P system has demonstrated that its nuclear spins can yield exceedingly long spin coherence times by eliminating the electron spin of the dopant. For NV centers, however, a proper charge state for storage of nuclear spin qubit coherence has not been identified yet. Here, we identify and characterize the positively charged NV center as an electron-spin-less and optically inactive state by utilizing the nuclear spin qubit as a probe. We control the electronic charge and spin utilizing nanometer scale gate electrodes. We achieve a lengthening of the nuclear spin coherence times by a factor of 4. Surprisingly, the new charge state allows switching of the optical response of single nodes facilitating full individual addressability.

Long-range photon-mediated gate scheme between nuclear spin qubits in diamond

Defect centers in diamond are exceptional solid-state quantum systems that can have exceedingly long electron and nuclear spin coherence times. So far, single-qubit gates for the nitrogen nuclear spin, a two-qubit gate with a nitrogen-vacancy (NV) center electron spin, and entanglement between nearby nitrogen nuclear spins have been demonstrated. Here, we develop a scheme to implement a universal two-qubit gate between two distant nitrogen nuclear spins. Virtual excitation of an NV center that is embedded in an optical cavity can scatter a laser photon into the cavity mode; we show that this process depends on the nuclear spin state of the nitrogen atom. If two NV centers are simultaneously coupled to a common cavity mode and individually excited, virtual cavity photon exchange can mediate an effective interaction between the nuclear spin qubits, conditioned on the spin state of both nuclei, which implements a universal controlled-$\textit{Z}$ gate. We predict operation times below 100 nanoseconds, which is several orders of magnitude faster than the decoherence time of nuclear spin qubits in diamond.

Coherent storage of microwave excitations in rare-earth nuclear spins.

Interfacing between various elements of a computer--from memory to processors to long range communication--will be as critical for quantum computers as it is for classical computers today. Paramagnetic rare-earth doped crystals, such as Nd(3+):Y2SiO5(YSO), are excellent candidates for such a quantum interface: they are known to exhibit long optical coherence lifetimes (for communication via optical photons), possess a nuclear spin (memory), and have in addition an electron spin that can offer hybrid coupling with superconducting qubits (processing). Here we study two of these three elements, demonstrating coherent storage and retrieval between electron and (145)Nd nuclear spin states in Nd(3+):YSO. We find nuclear spin coherence times can reach 9 ms at ∼5 K, about 2 orders of magnitude longer than the electron spin coherence, while quantum state and process tomography of the storage or retrieval operation between the electron and nuclear spin reveal an average state fidelity of 0.86. The times and fidelities are expected to further improve at lower temperatures and with more homogeneous radio-frequency excitation.

High-fidelity readout and control of a nuclear spin qubit in silicon

Detection of nuclear spin precession is critical for a wide range of scientific techniques that have applications in diverse fields including analytical chemistry, materials science, medicine and biology. Fundamentally, it is possible because of the extreme isolation of nuclear spins from their environment. This isolation also makes single nuclear spins desirable for quantum-information processing, as shown by pioneering studies on nitrogen-vacancy centres in diamond. The nuclear spin of a (31)P donor in silicon is very promising as a quantum bit: bulk measurements indicate that it has excellent coherence times and silicon is the dominant material in the microelectronics industry. Here we demonstrate electrical detection and coherent manipulation of a single (31)P nuclear spin qubit with sufficiently high fidelities for fault-tolerant quantum computing. By integrating single-shot readout of the electron spin with on-chip electron spin resonance, we demonstrate quantum non-demolition and electrical single-shot readout of the nuclear spin with a readout fidelity higher than 99.8 percent-the highest so far reported for any solid-state qubit. The single nuclear spin is then operated as a qubit by applying coherent radio-frequency pulses. For an ionized (31)P donor, we find a nuclear spin coherence time of 60 milliseconds and a one-qubit gate control fidelity exceeding 98 percent. These results demonstrate that the dominant technology of modern electronics can be adapted to host a complete electrical measurement and control platform for nuclear-spin-based quantum-information processing.

Nuclear Spins of Ionized Phosphorus Donors in Silicon

We demonstrate the coherent control and electrical readout of ionized phosphorus donor nuclear spins in (nat)Si. By combining time-programed optical excitation with coherent electron spin manipulation, we selectively ionize the donors depending on their nuclear spin state, exploiting a spin-dependent recombination process at the Si/SiO(2) interface, and find a nuclear spin coherence time of 18 ms for the ionized donors. The presented technique allows for spectroscopy of ionized-donor nuclear spins and enhances the sensitivity of electron nuclear double resonance to a level of 3000 nuclear spins.

Magnetic Field Dependence of Quadrupolar Splitting and Nuclear Spin Coherence Time in a Strained (110) GaAs Quantum Well

We investigated the magnetic field dependence of quadrupolar splitting and phase relaxation time of nuclear spins in an n-GaAs/AlGaAs (110) quantum well (QW) by optically detected nuclear magnetic resonance (NMR). The NMR spectra show large quadrupolar splitting induced by an internal field gradient in the QW epilayer. At lower magnetic fields, the quadrupolar splitting become much enhanced, resulting in the appearance of the second order magnetic field dependence of the quadrupole interaction in the NMR spectra. It is also shown that the intrinsic coherence time and the effective coherence time for resonant transitions become shorter as a result that the energy splitting between the two levels becomes small and incoherent transition is occurred by irradiation of an rf magnetic field.

Magnetic Field Dependence of Quadrupolar Splitting and Nuclear Spin Coherence Time in a Strained (110) GaAs Quantum Well

Magnetic Field Dependence of Quadrupolar Splitting and Nuclear Spin Coherence Time in a Strained (110) GaAs Quantum Well

Theory of the electron and nuclear spin coherence times of shallow donor spin qubits in isotopically and chemically purified zinc oxide

In this article, I present a theoretical study of the electron and nuclear spin coherence times of shallow donor spin qubits in zinc oxide (ZnO) at low temperature. The influence of different spin-phonon processes as well as different spin-spin processes on the spin coherence time of shallow donors in ZnO is considered, both in the case of an electron spin qubit and in the case of a nuclear spin qubit encoded on a shallow donor. It is estimated that the electron spin coherence time of an isolated indium shallow donor in natural quasi-intrinsic ZnO is on the order of hundreds of microseconds, limited by the nuclear spectral diffusion process. The electron spin coherence time of an isolated indium shallow donor can be extended to few milliseconds in isotopically and chemically purified quasi-intrinsic ZnO. In this optimal case, the electron spin coherence time of an isolated indium shallow donor is only limited by a spin-lattice decoherence process. It is also estimated that the nuclear spin coherence time of an isolated indium shallow donor in natural quasi-intrinsic ZnO is on the order of hundreds of milliseconds, limited by the nuclear spectral diffusion process. The nuclear spin coherence time of an isolated indium shallow donor can be extended to few seconds in isotopically and chemically purified quasi-intrinsic ZnO. In this optimal case, the nuclear spin coherence time of an isolated indium shallow donor is only limited by the cross relaxation decoherence process. This study thus shows the great potential of electron and nuclear spin qubits encoded on shallow donors in isotopically and chemically purified quasi-intrinsic ZnO for the implementation of quantum processor and/or quantum memories.

Nuclear spins as quantum memory in semiconductor nanostructures

We theoretically consider solid state nuclear spins in a semiconductor nanostructure environment as long-lived, high-fidelity quantum memory. In particular, we calculate, in the limit of a strong applied magnetic field, the fidelity versus time of P donor nuclear spins in random bath environments of Si and GaAs, and the lifetime of excited intrinsic spins in polarized Si and GaAs environments. In the former situation, the nuclear spin dephases due to spectral diffusion induced by the dipolar interaction among nuclei in the bath. We calculate the decay of nuclear spin quantum memory in the context of Hahn and Carr-Purcell-Meiboom-Gill (CPMG) refocused spin echoes using a formally exact cluster expansion technique which has previously been successful in dealing with electron spin dephasing in a solid state nuclear spin bath. With decoherence dominated by transverse dephasing (T2), we find it feasible to maintain high fidelity (losses of less than 10^{-6}) quantum memory on nuclear spins for times of the order of 100 microseconds (GaAs:P) and 1 to 2 milliseconds (natural Si:P) using CPMG pulse sequences of just a few (~2-4) applied pulses. We also consider the complementary situation of a central flipped intrinsic nuclear spin in a bath of completely polarized nuclear spins where decoherence is caused by the direct flip-flop of the central spin with spins in the bath. Exact numerical calculations that include a sufficiently large neighborhood of surrounding nuclei show lifetimes on the order of 1-5 ms for both GaAs and natural Si. Our calculated nuclear spin coherence times may have significance for solid state quantum computer architectures using localized electron spins in semiconductors where nuclear spins have been proposed for quantum memory storage.

Electric field tunability of nuclear and electronic spin dynamics due to the hyperfine interaction in semiconductor nanostructures.

We present formulas for the nuclear and electronic spin relaxation times due to the hyperfine interaction for nanostructed systems and show that the times depend on the square of the local density of electronic states at the nuclear position. A drastic sensitivity (orders of magnitude) of the electronic and nuclear spin coherence times to small electric fields is predicted for both uniformly distributed nuclear spins and delta-doped layers of specific nuclei. This sensitivity is robust to nuclear spin diffusion.