We experimentally demonstrate that the decoherence of a spin by a spin bath can be completely eliminated by fully polarizing the spin bath. We use electron paramagnetic resonance at 240 gigahertz and 8 Tesla to study the spin coherence time $T_2$ of nitrogen-vacancy centers and nitrogen impurities in diamond from room temperature down to 1.3 K. A sharp increase of $T_2$ is observed below the Zeeman energy (11.5 K). The data are well described by a suppression of the flip-flop induced spin bath fluctuations due to thermal spin polarization. $T_2$ saturates at $\sim 250 μs$ below 2 K, where the spin bath polarization is 99.4 %.
Understanding and mitigating decoherence is a key challenge for quantum science and technology. The main source of decoherence for solid-state spin systems is the uncontrolled spin bath environment. Here, we demonstrate quantum control of a mesoscopic spin bath in diamond at room temperature that is composed of electron spins of substitutional nitrogen impurities. The resulting spin bath dynamics are probed using a single nitrogen-vacancy (NV) centre electron spin as a magnetic field sensor. We exploit the spin bath control to dynamically suppress dephasing of the NV spin by the spin bath. Fur…
We theoretically investigate spin decoherence of a single nitrogen-vacancy (NV) center in diamond. Using the spin coherent state P-representation method, coherence evolution of the NV center surrounded by nitrogen electron spins (N) is simulated. We find that spin decoherence time as well as free-induction decay of the NV center depend on the spatial configuration of N spins. Both the spin decoherence rate (1/T2) and dephasing rate (1/T2*) of the NV center increase linearly with the concentration of the N spins. Using the P-representation method, we also demonstrate extracting noise spectrum o…
Single-qubit sensing protocols can be used to measure qubit-bath coupling parameters. However, for sufficiently large coupling, the sensing protocol itself perturbs the bath, which is predicted to result in a characteristic response in the sensing measurements. Here, we observe this bath perturbation, also known as a quantum quench, by preparing the nuclear spin bath of a nitrogen-vacancy (NV) center in polarized initial states and performing phase-resolved spin echo measurements on the NV electron spin. These measurements reveal a time-dependent phase determined by the initial state of the ba…
Spin bath mediated long-lived coherent oscillations of NV centers in diamond
Bennett University（贝内特大学）；IIT Madras（印度理工学院马德拉斯分校）；Technische Universität Dortmund（多特蒙德工业大学）；Center For Quantum Information, Communication And Computing, IIT Madras（印度理工学院马德拉斯分校量子信息、通信与计算中心）；London center for Nanotechnology, UCL（伦敦纳米技术研究中心，伦敦大学学院）；SIAS, Krea University（克里亚大学SIAS学院）
The nitrogen-vacancy (NV) centre, as a promising candidate solid state system of quantum information processing, its electron spin coherence is influenced by the magnetic field fluctuations due to the local environment. In pure diamonds, the environment consists of hundreds of C-13 nuclear spins randomly spreading in several nanometers range forming a spin bath. Controlling and prolonging the electron spin coherence under the influence of spin bath are challenging tasks for the quantum information processing. On the other hand, for a given bath distribution, many of its characters are encoded …
We experimentally investigate the protection of electron spin coherence of nitrogen vacancy (NV) center in diamond by dynamical nuclear polarization. The electron spin decoherence of an NV center is caused by the magnetic ield fluctuation of the $^{13}$C nuclear spin bath, which contributes large thermal fluctuation to the center electron spin when it is in equilibrium state at room temperature. To address this issue, we continuously transfer the angular momentum from electron spin to nuclear spins, and pump the nuclear spin bath to a polarized state under Hartman-Hahn condition. The bath pola…
We study the dynamics of the quenched Anderson model at finite temperature using matrix product states. Exploiting a chain mapping for the electron bath, we investigate the entanglement structure in the MPS for various orderings of the two chains, which emerge from the thermofield transformation employed to deal with nonzero temperature. We show that merging both chains can significantly lower the entanglement at finite temperatures as compared to an intuitive nearest-neighbor implementation of the Hamiltonian. Analyzing the population of the free bath modes -- possible when simulating the ful…
Spin waves have risen as promising candidate information carriers for the next generation of information technologies. Recent experimental demonstrations of their detection using electron spins in diamond pave the way towards studying the back-action of a controllable paramagnetic spin bath on the spin waves. Here, we present a quantum theory describing the interaction between spin waves and paramagnetic spins. As a case study we consider an ensemble of nitrogen-vacancy spins in diamond in the vicinity of an Yttrium-Iron-Garnet thin film. We show how the back-action of the ensemble results in …
Due to interest in both solid state based quantum computing architectures and the application of quantum mechanical systems to nanomagnetometry, there has been considerable recent attention focused on understanding the microscopic dynamics of solid state spin baths and their effects on the coherence of a controllable, coupled central electronic spin. Many analytic approaches are based on simplified phenomenological models in which it is difficult to capture much of the complex physics associated with this system. Conversely, numerical approaches reproduce this complex behaviour, but are limite…
Artificial atom qubits in diamond have emerged as leading candidates for a range of solid-state quantum systems, from quantum sensors to repeater nodes in memory-enhanced quantum communication. Inversion-symmetric group IV vacancy centers, comprised of Si, Ge, Sn and Pb dopants, hold particular promise as their neutrally charged electronic configuration results in a ground-state spin triplet, enabling long spin coherence above cryogenic temperatures. However, despite the tremendous interest in these defects, a theoretical understanding of the electronic and spin structure of these centers rema…
Vacancy aggregation enhances NV- spin coherence in diamond: a cluster-correlation-expansion study of multi-vacancy spin baths in semiconductors
University of Tsukuba（筑波大学）；Institute of Pure and Applied Sciences（纯理与应用科学研究院）；Japanese-French Laboratory for Semiconductor Physics and Technology J-FAST（日法半导体物理与技术实验室（J-FAST））；CNRS（法国国家科学研究中心）；University Grenoble Alpes（格勒诺布尔阿尔卑斯大学）；Grenoble INP（格勒诺布尔国立理工学院）
We develop a quantum theory for a variety of nuclear spin dynamics such as dephasing, relaxation, squeezing, and narrowing due to the hyperfine interaction with a generic, dissipative electronic system. The first-order result of our theory reproduces and generalizes the nonlinear Hamiltonian for nuclear spin squeezing [M. S. Rudner, Phys. Rev. Lett. 107, 206806 (2011)]. The second-order result of our theory provides a good explanation to the experimentally observed $^{13}$C nuclear spin bath narrowing in diamond nitrogen-vacancy center [E. Togan, Nature 478, 497 (2011)
We simulate the dynamics of varying density quasi-two-dimensional spin ensembles in solid-state systems, focusing on the nitrogen-vacancy centers in diamond. We consider the effects of various control sequences on the averaged dynamics of large ensembles of spins, under a realistic "spin-bath" environment. We reveal that spin locking is efficient for decoupling spins initialized along the driving axis, both from coherent dipolar interactions and from the external spin-bath environment, when the driving is two orders of magnitude stronger than the relevant coupling energies. Since the applicati…
A promising approach for multi-qubit quantum registers is to use optically addressable spins to control multiple dark electron-spin defects in the environment. While recent experiments have observed signatures of coherent interactions with such dark spins, it is an open challenge to realize the individual control required for quantum information processing. Here we demonstrate the initialisation, control and entanglement of individual dark spins associated to multiple P1 centers, which are part of a spin bath surrounding a nitrogen-vacancy center in diamond. We realize projective measurements …
A First-principles Computational Framework for Quantum Decoherence in Complex Diamond Spin Environments
Sungkyunkwan University（成均馆大学）；Ajou University（亚洲大学）；University of Chicago（芝加哥大学）；Korea Institute of Science and Technology（韩国科学技术院）；Korean Research Institute of Standards and Science（韩国计量科学研究院）；Ulm University（乌尔姆大学）；Korea University of Science and Technology（韩国科学技术院）；Argonne National Laboratory（阿贡国家实验室）
Knowing a quantum system's environment is critical for its practical use as a quantum device. Qubit sensors can reconstruct the noise spectral density of a classical bath, provided long enough coherence time. Here we present a protocol that can unravel the characteristics of a more complex environment, comprising both unknown coherently coupled quantum systems, and a larger quantum bath that can be modeled as a classical stochastic field. We exploit the rich environment of a Nitrogen-Vacancy center in diamond, tuning the environment behavior with a bias magnetic field, to experimentally demons…
Decoherence of quantum objects in noisy environments is important in quantum sciences and technologies. It is generally believed that different processes coupled to the same noise source should have similar decoherence behaviors and stronger noises would cause faster decoherence. Here we show that in a quantum bath, the case can be the opposite. In particular, we predict that the multi-transition of a nitrogen-vacancy center spin-1 in diamond can have longer coherence time than the single-transitions, even though the former suffers twice stronger noises from the nuclear spin bath than the latt…
Identifying weakly coupled nuclear spins around single electron spins is a key step of implementing quantum information processing using coupled electron-nuclei spin systems or sensing like single spin nuclear magnetic resonance detection using diamond defect spins. Dynamical decoupling control of the center electron spin with periodic pulse sequences [e.g., the Carre-Purcell-Meiboom-Gill (CPMG) sequence] has been successfully used to identify single nuclear spins and to resolve structure of nuclear spin clusters. Here, we design a new type of pulse sequences by replacing the repetition unit (…
We theoretically study the decoherence and the dynamical decoupling control of nitrogen-vacancy center electron spins in high-purity diamond, where the hyperfine interaction with $^{13}$C nuclear spins is the dominating decoherence mechanism. The decoherence is formulated as the entanglement between the electron spin and the nuclear spins, which is induced by nuclear spin bath evolution conditioned on the electron spin state. The nuclear spin bath evolution is driven by elementary processes such as single spin precession and pairwise flip-flops. The importance of different elementary processes…
The quantum Zeno and anti-Zeno paradigms have thus far addressed the evolution control of a quantum system coupled to an immutable bath via non-selective measurements performed at appropriate intervals. We fundamentally modify these paradigms by introducing, theoretically and experimentally, the concept of controlling the bath state via selective measurements of the system (a qubit). We show that at intervals corresponding to the anti-Zeno regime of the system-bath exchange, a sequence of measurements has strongly correlated outcomes. These correlations can dramatically enhance the bath-state …
New magnetometry techniques based on Nitrogen Vacancy (NV) defects in diamond have received much attention of late as a means to probe nanoscale magnetic environments. The sensitivity of a single NV magnetometer is primarily determined by the transverse spin relaxation time, $T_2$. Current approaches to improving the sensitivity employ crystals with a high NV density at the cost of spatial resolution, or extend $T_2$ via the manufacture of novel isotopically pure diamond crystals. We adopt a complementary approach, in which optimal dynamic decoupling techniques extend coherence times out to th…
We model the decoherence and dephasing of nitrogen vacancy (NV) centers in diamond due to a noisy paramagnetic bath, with and without the presence of a rf field that couples levels of the ground electronic state manifold, using a simple quantum mechanical model that allows for analytical solutions. The model treats the NV three-level ground state system in the presence of fluctuating magnetic fields that arise from the environment, and that result in decoherence, dephasing and dissipation. We show that all 9 eigenmodes of the three-level system are coupled to each other due to interaction with…
We demonstrate that the spin decoherence of nitrogen vacancy (NV) centers in diamond can be suppressed by a transverse magnetic field if the electron spin bath is the primary decoherence source. The NV spin coherence, created in "a decoherence-free subspace" is protected by the transverse component of the zero-field splitting, increasing the spin-coherence time about twofold. The decoherence due to the electron spin bath is also suppressed at magnetic fields stronger than ~25 gauss when applied parallel to the NV symmetry axis. Our method can be used to extend the spin-coherence time of simila…
In this paper, we study the electron spin decoherence of single defects in silicon carbide (SiC) nuclear spin bath. We find that, although the natural abundance of $^{29}\rm{Si}$ ($p_{\rm{Si}}=4.7\%$) is about 4 times larger than that of $^{13}{\rm C}$ ($p_{\rm{C}}=1.1\%$), the electron spin coherence time of defect centers in SiC nuclear spin bath in strong magnetic field ($B>300~\rm{Gauss}$) is longer than that of nitrogen-vacancy (NV) centers in $^{13}{\rm C}$ nuclear spin bath in diamond. The reason for this counter-intuitive result is the suppression of heteronuclear-spin flip-flop proces…
We report on the noise spectrum experienced by few nanometer deep nitrogen-vacancy centers in diamond as a function of depth, surface coating, magnetic field and temperature. Analysis reveals a double-Lorentzian noise spectra consistent with a surface electronic spin bath, with slower dynamics due to spin-spin interactions and faster dynamics related to phononic coupling. These results shed new light on the mechanisms responsible for surface noise affecting shallow spins at semiconductor interfaces, and suggests possible directions for further studies. We demonstrate dynamical decoupling from …
Decoherence of quantum objects is critical to modern quantum sciences and technologies. It is generally believed that stronger noises cause faster decoherence. Strikingly, recent theoretical research discovers the opposite case for spins in quantum baths. Here we report experimental observation of the anomalous decoherence effect for the electron spin-1 of a nitrogen-vacancy centre in high-purity diamond at room temperature. We demonstrate that under dynamical decoupling, the double-transition can have longer coherence time than the single-transition, even though the former couples to the nucl…
The degree of non-Markovianity of a continuous bath can be quantified by means of the coherence. This simple measure is experimentally accessible through Ramsey spectroscopy, but it is limited to incoherent dynamical maps. We propose an extension of this measure and discuss its application to color centers in diamond, where the optical coherence between two orbital states is affected by interactions with a structured phonon bath. By taking realistic phonon spectral density functions into account, we show that this measure is well-behaved at arbitrary temperatures and that it provides additiona…
We demonstrate a robust experimental method for determining the depth of individual shallow Nitrogen-Vacancy (NV) centers in diamond with $\sim1$ nm uncertainty. We use a confocal microscope to observe single NV centers and detect the proton nuclear magnetic resonance (NMR) signal produced by objective immersion oil, which has well understood nuclear spin properties, on the diamond surface. We determine the NV center depth by analyzing the NV NMR data using a model that describes the interaction of a single NV center with the statistically-polarized proton spin bath. We repeat this procedure f…
We present a combined theoretical and experimental study of solid-state spin decoherence in an electronic spin bath, focusing specifically on ensembles of nitrogen vacancy (NV) color centers in diamond and the associated substitutional nitrogen spin bath. We perform measurements of NV spin free induction decay times $T_2^*$ and spin-echo coherence times $T_2$ in 25 diamond samples with nitrogen concentrations [N] ranging from 0.01 to 300\,ppm. We introduce a microscopic model and perform numerical simulations to quantitatively explain the degradation of both $T_2^*$ and $T_2$ over four orders …
Efficient polarization of organic molecules is of extraordinary relevance when performing nuclear magnetic resonance (NMR) and imaging. Commercially available routes to dynamical nuclear polarization (DNP) work at extremely low-temperatures, thus bringing the molecules out of their ambient thermal conditions and relying on the solidification of organic samples. In this work we investigate polarization transfer from optically-pumped nitrogen vacancy centers in diamond to external molecules at room temperature. This polarization transfer is described by both an extensive analytical analysis and …
Heat-Bath Algorithmic cooling (HBAC) techniques provide ways to selectively enhance the polarization of target quantum subsystems. However, the cooling in these techniques are bounded. Here we report the first experimental observation of the HBAC cooling bound. We use HBAC to hyperpolarize nuclear spins in diamond. Using two carbon nuclear spins as the source of polarization (reset) and the 14N nuclear spin as the computation bit, we demonstrate that repeating a single cooling step increases the polarization beyond the initial reset polarization and reaches the cooling limit of HBAC. We benchm…
Controlling the interaction of a single quantum system with its environment is a fundamental challenge in quantum science and technology. We dramatically suppress the coupling of a single spin in diamond with the surrounding spin bath by using double-axis dynamical decoupling. The coherence is preserved for arbitrary quantum states, as verified by quantum process tomography. The resulting coherence time enhancement is found to follow a general scaling with the number of decoupling pulses. No limit is observed for the decoupling action up to 136 pulses, for which the coherence time is enhanced …
We present an experimental and theoretical study of electronic spin decoherence in ensembles of nitrogen-vacancy (NV) color centers in bulk high-purity diamond at room temperature. Under appropriate conditions, we find ensemble NV spin coherence times (T_2) comparable to that of single NVs, with T_2 > 600 microseconds for a sample with natural abundance of 13C and paramagnetic impurity density ~10^15 cm^(-3). We also observe a sharp decrease of the coherence time with misalignment of the static magnetic field relative to the NV electronic spin axis, consistent with theoretical modeling of NV c…
We investigate bright fluorescence of nitrogen (NV)- and silicon-vacancy color centers in pyramidal, single crystal diamond tips which are commercially available as atomic force microscope probes. We coherently manipulate NV electronic spin ensembles with $T_2 = 7.7(3)\,μ$s. Color center lifetimes in different tip heights indicate effective refractive index effects and quenching. Using numerical simulations, we verify enhanced photon rates from emitters close to the pyramid apex; a situation promising for scanning probe sensing.
In this report, the polarization properties of the photoluminescence emitted by single nitrogen-vacancy (NV) color centers in diamond are investigated using resonant excitation at cryogenic temperature. We first underline that the two excited-state orbital branches are associated with two orthogonal transition dipoles. Using selective excitation of one dipole, we then show that the photoluminescence is partially unpolarized owing to fast relaxation between the two orbitals induced by the thermal bath. This result might be important in the context of the realization of indistinguishable single …
Quantum entanglement, the essential resource for quantum information processing, has rich dynamics under different environments. Probing different entanglement dynamics typically requires exquisite control of complicated system-environment coupling in real experimental systems. Here, by a simple control of the effective solid-state spin bath in a diamond sample, we observe rich entanglement dynamics, including the conventional asymptotic decay as well as the entanglement sudden death, a term coined for the phenomenon of complete disappearance of entanglement after a short finite time interval.…
The dynamics of single electron and nuclear spins in a diamond lattice with different 13C nuclear spin concentration is investigated. It is shown that coherent control of up to three individual nuclei in a dense nuclear spin cluster is feasible. The free induction decays of nuclear spin Bell states and single nuclear coherences among 13C nuclear spins are compared and analyzed. Reduction of a free induction decay time T2* and a coherence time T2 upon increase of nuclear spin concentration has been found. For diamond material with depleted concentration of nuclear spin, T2* as long as 30 micros…
We study the longitudinal relaxation of a nitrogen-vacancy (NV) center surrounded by a $^{13}$C nuclear spin bath in diamond. By means of cluster-correlation expansion (CCE), we numerically demonstrate the decay process of electronic state induced by cross relaxation at low temperature. It is shown that the CCE method is not only capable of describing pure-dephasing effect at large-detuning regime, but it can also simulate the quantum dynamics of populations in the nearly resonant regime. We present a proposal to slow down the decay of NV center via implementing quantum Zeno effect (QZE). The …
Under ambient conditions, spin impurities in solid-state systems are found in thermally-mixed states and are optically "dark", i.e., the spin states cannot be optically controlled. Nitrogen-vacancy (NV) centers in diamond are an exception in that the electronic spin states are "bright", i.e., they can be polarized by optical pumping, coherently manipulated with spin-resonance techniques, and read out optically, all at room temperature. Here we demonstrate a dressed-state, double-resonance scheme to transfer polarization from bright NV electronic spins to dark substitutional-Nitrogen (P1) elect…
We present a measurement scheme capable of achieving the quantum limit of parameter estimation using an adaptive strategy that minimizes the parameter's variance at each step. The adaptive rule we propose makes the scheme robust against errors, in particular imperfect readouts, a critical requirement to extend adaptive schemes from quantum optics to solid-state sensors. Thanks to recent advances in single-shot readout capabilities for electronic spins in the solid state (such as Nitrogen Vacancy centers in diamond), this scheme can be as well applied to estimate the polarization of a spin bath…
Quantum registers of nuclear spins coupled to electron spins of individual solid-state defects are a promising platform for quantum information processing. Pioneering experiments selected defects with favourably located nuclear spins having particularly strong hyperfine couplings. For progress towards large-scale applications, larger and deterministically available nuclear registers are highly desirable. Here we realize universal control over multi-qubit spin registers by harnessing abundant weakly coupled nuclear spins. We use the electron spin of a nitrogen-vacancy centre in diamond to selec…
We consider a protocol for the control of few-qubit registers comprising one electronic spin embedded in a nuclear spin bath. We show how to isolate a few proximal nuclear spins from the rest of the environment and use them as building blocks for a potentially scalable quantum information processor. We describe how coherent control techniques based on magnetic resonance methods can be adapted to these electronic-nuclear solid state spin systems, to provide not only efficient, high fidelity manipulation of the registers, but also decoupling from the spin bath. As an example, we analyze feasible…
The studies of many-body dynamics of interacting spin ensembles, as well as quantum sensing in solid state systems, are often limited by the need for high spin concentrations, along with efficient decoupling of the spin ensemble of interest from its spin-bath environment. In particular, for an ensemble of nitrogen-vacancy (NV) centers in diamond, high conversion efficiencies between nitrogen (P1) defects and NV centers are essential, while maintaining long coherence times of an NV ensemble. In this work, we study the effect of electron irradiation on the conversion efficiency and the coherence…
Nonradiative transfer processes are often regarded as loss channels for an optical emitter1, since they are inherently difficult to be experimentally accessed. Recently, it has been shown that emitters, such as fluorophores and nitrogen vacancy centers in diamond, can exhibit a strong nonradiative energy transfer to graphene. So far, the energy of the transferred electronic excitations has been considered to be lost within the electron bath of the graphene. Here, we demonstrate that the trans-ferred excitations can be read-out by detecting corresponding currents with picosecond time resolution…
