Spin Bath Research Articles

RIDME Spectroscopy: New Topics Beyond the Determination of Electron Spin-Spin Distances.

Relaxation-induced dipolar modulation enhancement (RIDME) is a pulse EPR experiment originally designed to determine distances between spin labels. However, RIDME has several features that make it an efficient tool in a number of "nonconventional" applications, away from the original purpose of this pulse experiment. RIDME appears to be an interesting experiment to probe longitudinal electron spin dynamics, e.g., in relation to qubits research, to probe distributions of exchange couplings, useful for the design of molecular magnets, and to determine important details of electron spin interactions with the nuclear spin bath, which is related to the dynamic nuclear polarization and soft materials research. We also anticipate interesting applications of RIDME in the structural biology of biopolymers as well as their interactions, aggregation, and phase separation. It is not excluded that in the near future such "nonconventional" topics could grow in number and evolve into the main application area of RIDME.

Spin coherence in strongly coupled spin baths in quasi-two-dimensional layers

We investigate the spin-coherence decay of NV− spins interacting with the strongly coupled bath of nitrogen defects in diamond layers. For thin diamond layers, we demonstrate that the spin-coherence times exceed those of bulk diamond, thus allowing to surpass the limit imposed by high-defect concentrations in bulk. We show that the stretched-exponential parameter for the short-time spin-coherence decay is governed by the hyperfine interaction in the bath, thereby constraining random-noise models. We introduce a method based on the cluster-correlation expansion applied to strongly interacting bath partitions instead of individual spins. Our results facilitate material development for quantum-technology devices. Published by the American Physical Society 2024

Probing coherence properties of shallow implanted NV ensembles under different oxygen terminations

Abstract Nitrogen vacancy (NV) color centers in diamond have shown great potential for various applications in quantum technology due to their long coherence times, high sensitivity to magnetic fields and atomic scale resolution. However, one major challenge in utilizing near surface NV centers is the decoherence caused by spins and charges fluctuating on the surface, which affects the spin properties of the sensors. To reduce the induced noise, various oxygen surface treatments such as low power oxygen plasma treatment and annealing under oxygen atmosphere have been explored to terminate the diamond surface and reduce its impact on NV coherence. We showed that the NV center’s coherence time can be enhanced up to a factor of 3 over a large spectral range of noise. Double electron–electron resonance measurements revealed an extra source of decoherence, scaling similarly as the P1 spin bath. The improvement in coherence times is accompanied with an increase in measured ketone/ether content and reduction of sp2 signal in x-ray photoelectron spectroscopy measurements. Finally we compared the performance of different NV ensembles and surface treatments for sensing external proton spins. The oxygen annealing is an effective procedure of enhancing the spin coherence times and reducing broad band spin noise experienced by shallow implanted ensemble NV centers in diamond.

Computationally Driven Discovery of T Center-like Quantum Defects in Silicon.

Quantum technologies would benefit from the development of high-performance quantum defects acting as single-photon emitters or spin-photon interfaces. Finding such a quantum defect in silicon is especially appealing in view of its favorable spin bath and high processability. While some color centers in silicon have been emerging in quantum applications, there remains a need to search for and develop new high-performance quantum emitters. By searching a high-throughput computational database of more than 22,000 charged complex defects in silicon, we identify a series of defects formed by a group III element combined with carbon ((A-C)Si with A = B, Al, Ga, In, Tl) and substituting on a silicon site. These defects are analogous structurally, electronically, and chemically to the well-known T center in silicon ((C-C-H)Si), and their optical properties are mainly driven by an unpaired electron on the carbon p orbital. They all emit in the telecom, and some of these color centers show improved properties compared to the T center in terms of computed radiative lifetime, emission efficiency, or smaller optical linewidth. The kinetic barrier computations and previous experimental evidence show that these T center-like defects can be formed through the capture of a diffusing carbon by a substitutional group III atom. We also show that the synthesis of hydrogenated T center-like defects followed by a dehydrogenation annealing step could facilitate the formation of these defects. Our work motivates further studies on the synthesis and control of this new family of quantum defects and demonstrates the use of high-throughput computational screening to discover new color center candidates.

Programmable adiabatic demagnetization for systems with trivial and topological excitations

We propose a simple, robust protocol to prepare a low-energy state of an arbitrary Hamiltonian on a quantum computer or programmable quantum simulator. The protocol is inspired by the adiabatic demagnetization technique, used to cool solid-state systems to extremely low temperatures. A fraction of the qubits (or spins) is used to model a spin bath that is coupled to the system. By an adiabatic ramp down of a simulated Zeeman field acting on the bath spins, energy and entropy are extracted from the system. The bath spins are then measured and reset to the polarized state, and the process is repeated until convergence to a low-energy steady state is achieved. We demonstrate the protocol via application to the quantum Ising model. We study the protocol's performance in the presence of noise and show how the information from the measurement of the bath spins can be used to monitor the cooling process. The performance of the algorithm depends on the nature of the excitations of the system; systems with non-local (topological) excitations are more difficult to cool than those with local excitations. We explore the possible mitigation of this problem by trapping topological excitations.

Spin relaxation dynamics with a continuous spin environment: The dissipaton equation of motion approach.

We investigate the quantum dynamics of a spin coupling to a bath of independent spins via the dissipaton equation of motion (DEOM) approach. The bath, characterized by a continuous spectral density function, is composed of spins that are independent level systems described by the su(2) Lie algebra, representing an environment with a large magnitude of anharmonicity. Based on the previous work by Suarez and Silbey [J. Chem. Phys. 95, 9115 (1991)] and by Makri [J. Chem. Phys. 111, 6164 (1999)] that the spin bath can be mapped to a Gaussian environment under its linear response limit, we use the time-domain Prony fitting decomposition scheme to the bare-bath time correlation function (TCF) given by the bosonic fluctuation-dissipation theorem to generate the exponential decay basis (or pseudo modes) for DEOM construction. The accuracy and efficiency of this strategy have been explored by a variety of numerical results. We envision that this work provides new insights into extending the hierarchical equations of motion and DEOM approach to certain types of anharmonic environments with arbitrary TCF or spectral density.

Dephasing dynamics of a central spin interacting with a classical Ising spin bath

We study the effect of interaction between bath spins on central spin dynamics. For this end, we consider various types of interactions among the bath fluctuators. We give an analytical relation for the dephasing dynamics of a central spin homogeneously interacting with a bath of classically interacting spins in thermal equilibrium. The obtained exact relation for the central spin dynamics depends on the average of the number of bath spins N in the canonical ensemble. We find the relation of dephasing time with bath's temperature and strength of interaction between bath spins. We show that if the classically interacting bath is large enough, off-diagonal coherence will decay into Gaussian form. This Gaussian decay is valid for temperatures higher than critical temperature. Moreover, we analytically prove the equivalence of dephasing dynamics for central spin models with classical Ising spin bath and quantum flip-flop spin bath interactions. Therefore, the dephasing dynamics for central spin models with quantum spin bath interactions can be reproduced with much less expensive classical spin bath interaction model instead. Our results can be applied in a number of quantum systems used in quantum sensing such as color centers in solids or quantum dots manuscript.

Bath-Engineering Magnetic Order in Quantum Spin Chains: An Analytic Mapping Approach.

Dissipative processes can drive different magnetic orders in quantum spin chains. Using a nonperturbative analytic mapping framework, we systematically show how to structure different magnetic orders in spin systems by controlling the locality of the attached baths. Our mapping approach reveals analytically the impact of spin-bath couplings, leading to the suppression of spin splittings, bath dressing and mixing of spin-spin interactions, and emergence of nonlocal ferromagnetic interactions between spins coupled to the same bath, which become long ranged for a global bath. Our general mapping method can be readily applied to a variety of spin models: we demonstrate (i)a bath-induced transition from antiferromagnetic (AFM) to ferromagnetic ordering in a Heisenberg spin chain, (ii)AFM to extended Neel phase ordering within a transverse-field Ising chain with pairwise couplings to baths, and (iii)a quantum phase transition in the fully connected Ising model. Our method is nonperturbative in the system-bath coupling. It holds for a variety of non-Markovian baths and it can be readily applied towards studying bath-engineered phases in frustrated or topological materials.

Understanding Central Spin Decoherence Due to Interacting Dissipative Spin Baths.

We propose a new approach to simulate the decoherence of a central spin coupled to an interacting dissipative spin bath with cluster-correlation expansion techniques. We benchmark the approach on generic 1D and 2D spin baths and find excellent agreement with numerically exact simulations. Our calculations show a complex interplay between dissipation and coherent spin exchange, leading to increased central spin coherence in the presence of fast dissipation. Finally, we model near-surface nitrogen-vacancy centers in diamond and show that accounting for bath dissipation is crucial to understanding their decoherence. Our method can be applied to a variety of systems and provides a powerful tool to investigate spin dynamics in dissipative environments.

Generalized cluster correlation expansion theory for stimulated Raman adiabatic passage processes in the presence of a spin bath

Generalized cluster correlation expansion theory for stimulated Raman adiabatic passage processes in the presence of a spin bath

General framework for quantifying dissipation pathways in open quantum systems. I. Theoretical formulation.

We present a general and practical theoretical framework to investigate how energy is dissipated in open quantum system dynamics. This is performed by quantifying the contributions of individual bath components to the overall dissipation of the system. The framework is based on the Nakajima-Zwanzig projection operator technique, which allows us to express the rate of energy dissipation into a specific bath degree of freedom by using traces of operator products. The approach captures system-bath interactions to all orders, but is based on second-order perturbation theory on the off-diagonal subsystem's couplings and a Markovian description of the bath. The usefulness of our theory is demonstrated by applying it to various models of open quantum systems involving harmonic oscillators or spin baths and connecting the outcomes to existing results such as our previously reported formula derived for locally coupled harmonic baths [Kim and Franco, J. Chem. Phys. 154, 084109 (2021)]. We also prove that the dissipation calculated by our theory rigorously satisfies thermodynamic principles such as energy conservation and detailed balance. Overall, the strategy can be used to develop the theory and simulation of dissipation pathways to interpret and engineer the dynamics of open quantum systems.

Realization of robust quantum noise characterization in the presence of coherent errors

Complex quantum systems and their various applications are susceptible to noise of coherent and incoherent nature. Characterization of noise and its sources is an open, key challenge in quantum technology applications, especially in terms of distinguishing between inherent incoherent noise and systematic coherent errors. In this paper, we study a scheme of repeated sequential measurements that enables the characterization of incoherent errors by reducing the effects of coherent errors. We demonstrate this approach using a coherently controlled nitrogen vacancy in diamond, coupled to both a natural nuclear spin bath (non-Markovian) and to experimentally controlled relaxation through an optical pumping process (nearly Markovian). Our results show mitigation of coherent errors both for Markovian and non-Markovian incoherent noise profiles. We apply this scheme to the estimation of the dephasing time (T2*) due to incoherent noise. We observe an improved robustness against coherent errors in the estimation of dephasing time (T2*) compared to the standard (Ramsey) measurement.

Sensing Coherent Nuclear Spin Dynamics with an Ensemble of Paramagnetic Nitrogen Spins

The unpolarized spin environment surrounding a central spin qubit is typically considered as an incoherent source of dephasing, however, precise characterization and control of the spin bath can yield a resource for storing and sensing with quantum states. In this work, we use nitrogen-vacancy (NV) centers in diamond to measure the coherence of optically dark paramagnetic nitrogen defects (P1 centers) and detect coherent interactions between the P1 centers and a local bath of 13C nuclear spins. The dipolar coupling between the P1 centers and 13C nuclear spins is identified by signature periodic collapses and revivals in the P1 spin coherence signal. We then demonstrate, using a range of dynamical decoupling protocols, that the probing NV centers and the P1 spins are coupled to independent ensembles of 13C nuclear spins. Our work illustrates how the optically dark P1 spins can be used to extract information from their local environment and offers new insight into the interactions within a many-body system. Published by the American Physical Society 2024

Adiabatically Manipulated Systems Interacting with Spin Baths beyond the Rotating Wave Approximation

The Stimulated Raman Adiabatic Passage (STIRAP) on a three-state system interacting with a spin bath is considered, focusing on the efficiency of the population transfer. Our analysis is based on the perturbation treatment of the interaction term evaluated beyond the Rotating Wave Approximation, thus focusing on the limit of weak system–bath coupling. The analytical expression of the correction to the efficiency and the consequent numerical analysis show that, in most of the cases, the effects of the environment are negligible, confirming the robustness of the population transfer.

Generation of genuine all-way entanglement in defect-nuclear spin systems through dynamical decoupling sequences

Multipartite entangled states are an essential resource for sensing, quantum error correction, and cryptography. Color centers in solids are one of the leading platforms for quantum networking due to the availability of a nuclear spin memory that can be entangled with the optically active electronic spin through dynamical decoupling sequences. Creating electron-nuclear entangled states in these systems is a difficult task as the always-on hyperfine interactions prohibit complete isolation of the target dynamics from the unwanted spin bath. While this emergent cross-talk can be alleviated by prolonging the entanglement generation, the gate durations quickly exceed coherence times. Here we show how to prepare high-quality GHZM-like states with minimal cross-talk. We introduce the M-tangling power of an evolution operator, which allows us to verify genuine all-way correlations. Using experimentally measured hyperfine parameters of an NV center spin in diamond coupled to carbon-13 lattice spins, we show how to use sequential or single-shot entangling operations to prepare GHZM-like states of up to M=10 qubits within time constraints that saturate bounds on M-way correlations. We study the entanglement of mixed electron-nuclear states and develop a non-unitary M-tangling power which additionally captures correlations arising from all unwanted nuclear spins. We further derive a non-unitary M-tangling power which incorporates the impact of electronic dephasing errors on the M-way correlations. Finally, we inspect the performance of our protocols in the presence of experimentally reported pulse errors, finding that XY decoupling sequences can lead to high-fidelity GHZ state preparation.

Detecting nitrogen-vacancy-hydrogen centers on the nanoscale using nitrogen-vacancy centers in diamond

In diamond, nitrogen defects like the substitutional nitrogen defect (Ns) or the nitrogen-vacancy-hydrogen complex (NVH) outnumber the nitrogen-vacancy (NV) defect by at least one order of magnitude creating a dense spin bath. While neutral Ns has an impact on the coherence of the NV spin state, the atomic structure of NVH reminds of a NV center decorated with a hydrogen atom. As a consequence, the formation of NVH centers could compete with that of NV centers possibly lowering the N-to-NV conversion efficiency in diamond grown with hydrogen-plasma-assisted chemical vapor deposition (CVD). Therefore, monitoring and controlling the spin bath is essential to produce and understand engineered diamond material with high NV concentrations for quantum applications. While the incorporation of Ns in diamond has been investigated on the nano- and mesoscale for years, studies concerning the influence of CVD parameters and the crystal orientation on the NVH formation have been restricted to bulk N-doped diamond providing high-enough spin numbers for electron paramagnetic resonance and optical absorption spectroscopy techniques. Here, we investigate submicron-thick (100)-diamond layers with nitrogen contents of (13.8±1.6)ppm and (16.7±3.6)ppm, and exploiting the NV centers in the layers as local nanosensors, we demonstrate the detection of NVH− centers using double electron-electron resonance (DEER). To determine the NVH− densities, we quantitatively fit the hyperfine structure of NVH− and confirm the results with the DEER method usually used for determining Ns0 densities. With our experiments, we access the spin bath composition on the nanoscale and enable a fast feedback loop in CVD recipe optimization with thin diamond layers instead of resource- and time-intensive bulk crystals. Furthermore, the quantification of NVH− plays a very important role for understanding the dynamics of vacancies and the incorporation of hydrogen into CVD diamond optimized for quantum technologies. Published by the American Physical Society 2024

Robust T2 estimation with balanced steady state free precession.

To develop a novel signal representation for balanced steady state free precession (bSSFP) displaying its T2 independence on B1 and on magnetization transfer (MT) effects. A signal model for bSSFP is developed that shows only an explicit dependence (up to a scaling factor) on E2 (and, therefore, T2) and a novel parameter c (with implicit dependence on the flip angle and E1). Moreover, it is shown that MT effects, entering the bSSFP signal via a binary spin bath model, can be captured by a redefinition of T1 and, therefore, leading to modification of E1, resulting in the same signal model. Various sets of phase-cycled bSSFP brain scans (different flip angles, different TR, different RF pulse durations, and different number of phase cycles) were recorded at 3 T. The parameters T2 (E2) and c were estimated using a variable projection (VARPRO) method and Monte-Carlo simulations were performed to assess T2 estimation precision. Initial experiments confirmed the expected independence of T2 on various protocol settings, such as TR, the flip angle, B1 field inhomogeneity, and the RF pulse duration. Any variation (within the explored range) appears to directly affect the estimation of the parameter c only-in agreement with theory. BSSFP theory predicts an extraordinary feature that all MT and B1-related variational aspects do not enter T2 estimation, making it a potentially robust methodology for T2 quantification, pending validation against existing standards.

Nuclear Spin-Depleted, Isotopically Enriched 70 Ge/28 Si70 Ge Quantum Wells.

The p-symmetry of the hole wavefunction is associated with a weaker hyperfine interaction, which makes hole spin qubits attractive candidates to implement quantum processors. However, recent studies demonstrate that hole qubits are still very sensitive to nuclear spin bath, thus highlighting the need for nuclear spin-free germanium (Ge) qubits to suppress this decoherence channel. Herein, this work demonstrates the epitaxial growth of 73 Ge- and 29 Si-depleted, isotopically enriched 70 Ge/silicon-germanium (SiGe) quantum wells. The growth is achieved by reduced pressure chemical vapor deposition using isotopically purified monogermane 70 GeH4 and monosilane 28 SiH4 with an isotopic purity higher than 99.9% and 99.99%, respectively. The quantum wells consist of a series of 70 Ge/SiGe heterostructures grown on Si wafers. The isotopic purity is investigated using atom probe tomography (APT) following an analytical procedure addressing the discrepancies caused by the overlap of isotope peaks in mass spectra. The nuclear spin background is found to be sensitive to the growth conditions with the lowest concentration of 73 Ge and 29 Si is below 0.01% in the Ge well and SiGe barriers. The measured average distance between nuclear spins reaches 3-4 nm in 70 Ge/28 Si70 Ge, which is an order of magnitude larger than in natural Ge/SiGe heterostructures.The spread of the hole wavefunction and the residual nuclear spin background in APT voluminals comparable to the size of realistic quantum dots are also discussed.

Extending Spin Dephasing Time of Perfectly Aligned Nitrogen‐Vacancy Centers by Mitigating Stress Distribution on Highly Misoriented Chemical‐Vapor‐Deposition Diamond

AbstractExtending the spin‐dephasing time (T2*) of perfectly aligned nitrogen‐vacancy (NV) centers in large‐volume chemical vapor deposition (CVD) diamonds leads to enhanced DC magnetic sensitivity. However, T2* of the NV centers is significantly reduced by the stress distribution in the diamond film as its thickness increases. To overcome this issue, they developed a method to mitigate the stress distribution in the CVD diamond films, leading to a T2* extension of the ensemble NV centers. CVD diamond films of ≈60 µm thickness with perfectly aligned NV centers are formed on (111) diamond substrates with misorientation angles of 2.0°, 3.7°, 5.0°, and 10.0°. The study found that T2* of the ensemble of NV centers increased to approach its value limited only by the electron and nuclear spin bath with increasing the misorientation angle. Microscopic stress imaging revealed that the stress distribution is highly inhomogeneous along the depth direction in the CVD diamond film at low misorientation angles, whereas the inhomogeneity is largely suppressed on highly misoriented substrates. The reduced stress distribution possibly originates from the reduction of the dislocation density in the CVD diamond. This study provides an important method for synthesizing high‐quality diamond materials for use in highly sensitive quantum sensors.

Adiabatic Manipulation of a System Interacting with a Spin Bath

The Stimulated Raman Adiabatic Passage, a very efficient technique for manipulating a quantum system based on the adiabatic theorem, is analyzed in the case where the manipulated physical system is interacting with a spin bath. The exploitation of the rotating wave approximation allows for the identification of a constant of motion, which simplifies both the analytical and the numerical treatment, which allows for evaluating the total unitary evolution of the system and bath. The efficiency of the population transfer process is investigated in several regimes, including the weak and strong coupling with the environment and the off-resonance. The formation of appropriate Zeno subspaces explains the lowering of the efficiency in the strong damping regime.