Spin Decoherence Research Articles

Toward exact predictions of spin-phonon relaxation times: An ab initio implementation of open quantum systems theory.

Spin-phonon coupling is the main driver of spin relaxation and decoherence in solid-state semiconductors at finite temperature. Controlling this interaction is a central problem for many disciplines, ranging from magnetic resonance to quantum technologies. Spin relaxation theories have been developed for almost a century but often use a phenomenological description of phonons and their coupling to spin, resulting in a nonpredictive tool and hindering our detailed understanding of spin dynamics. Here, we combine time-local master equations up to the fourth order with advanced electronic structure methods and perform predictions of spin-phonon relaxation time for a series of solid-state coordination compounds based on both transition metals and lanthanide Kramers ions. The agreement between experiments and simulations demonstrates that an accurate, universal, and fully ab initio implementation of spin relaxation theory is possible, thus paving the way to a systematic study of spin-phonon relaxation in solid-state materials.

Mechanism of Electron Spin Decoherence in a Partially Deuterated Glassy Matrix.

Long electron spin coherence lifetimes are essential for applications in quantum information science and electron paramagnetic resonance, for instance, for nanoscale distance measurements in biomolecular systems using double electron-electron resonance. We experimentally investigate the decoherence dynamics under the Hahn echo sequence of the organic radical d18-TEMPO in a variably deuterated frozen water:glycerol matrix. The coherence time (phase memory time) TM scales with proton concentration as [1H]-0.65. For selectively deuterated matrices, decoherence is accelerated in the presence of proton clustering, that is, substantial short-range density in the proton-proton radial distribution functions (<3 Å). Simulations using molecular dynamics and many-body spin quantum dynamics show excellent agreement with experiment and show that geminal proton pairs such as CH2 and OH2 groups are major decoherence drivers. This provides a predictive tool for designing molecular systems with long electron spin coherence times.

Protected two-qubit entangling gate with mechanical driven continuous dynamical decoupling

In this work, we propose a high-fidelity phonon-mediated entangling gate in a hybrid mechanical system based on two silicon-vacancy color centers in diamond. In order to suppress the influence of the spin decoherence on the entangling gate, we use a continuous dynamical decoupling approach to create new dressed spin states, which are less sensitive to environmental fluctuations and exhibit an extended spin dephasing time. The effective spin–spin Hamiltonian modified by the mechanical driving field and the corresponding master equation are derived in the dispersive regime. We show that in the presence of the mechanical driving field, the effective spin–spin coupling can be highly controlled. By calculating the entangling gate fidelity in the dressed basis, we find that once the mechanical field is turned on, the gate fidelity can be significantly improved. In particular, under an optimized spin-phonon detuning and a stronger Rabi frequency of the mechanical driving field, the two-qubit gate is capable of reaching fidelity exceeding 0.99. Moreover, by employing appropriate driving modulation, we show that a high-fidelity full quantum gate can be also realized, in which the initial and final spin states are on a bare basis. Our work provides a promising scheme for realizing high-fidelity quantum information processing.

Selective nuclear-spin interaction based on a dissipatively stabilized nitrogen-vacancy center

Current typical methods to realize nuclear-nuclear quantum gates require a sequence of electronnuclear quantum gates by using dynamical decoupling techniques, which are implemented at low temperature because of short decoherence and relaxation time of the NV spin at room temperature. This limitation could be overcome by using periodical resets of an NV spin as a mediator of interaction between two nuclear spins [Chen, Schwarz, and Plenio, 119, 010801 (2017)]. However, this method works under stringent coupling strengths condition, which makes it not applicable to heteronuclear quantum gate operations. Here we develop this scheme by using radio-frequency (RF) fields to control different nuclear spin species. Periodical resets of the NV center protect the nuclear spins from decoherence and relaxation of the NV spin. RF control provides probability to have highly selective and high fidelity quantum gates between heteronuclear spins as well as detecting nuclear spins by using a nuclear spin sensor under ambient conditions.

Coherence properties of a spin in a squeezed resonator

A promising venue for hybrid quantum computation involves the strong coupling between impurity spins and superconducting resonators. One strategy to control and enhance this coupling is to prepare the resonator in a non-classical state, such as a squeezed state. In this work, we theoretically study the effects of these states on the coherence properties of the spin. We develop an analytic approach based on the Schrieffer-Wolf transformation that allows us to quantitatively predict the coupling and the dephasing rate of the spin, and we numerically confirm its validity. We find that squeezing can enhance the coupling between the resonator and the spin. However, at the same time, it amplifies the photon noise and enhances the spin decoherence. Our work demonstrates a major impediment in using squeezing to reach the strong-coupling limit.

Zero-field magnetometry using hyperfine-biased nitrogen-vacancy centers near diamond surfaces

Shallow nitrogen-vacancy (NV) centers in diamond are promising for nanomagnetometry, for they can be placed proximate to targets. To study the intrinsic magnetic properties, zero-field magnetometry is desirable. However, for shallow NV centers under zero field, the strain near diamond surfaces would cause level anticrossing between the spin states, leading to clock transitions whose frequencies are insensitive to magnetic signals. Furthermore, the charge noises from the surfaces would induce extra spin decoherence and hence reduce the magnetic sensitivity. Here, we demonstrate that the relatively strong hyperfine coupling (130 MHz) from a first-shell $^{13}\mathrm{C}$ nuclear spin can provide an effective bias field to an NV center spin so that the clock-transition condition is broken and the charge noises are suppressed. The hyperfine bias enhances the dc magnetic sensitivity by a factor of 22 in our setup. With the charge noises suppressed by the strong hyperfine field, the ac magnetometry under zero field also reaches the limit set by decoherence due to the nuclear spin bath. In addition, the 130 MHz splitting of the NV center spin transitions allows relaxometry of magnetic noises simultaneously at two well-separated frequencies (\ensuremath{\sim}2.870 \ifmmode\pm\else\textpm\fi{} 0.065 GHz), providing (low-resolution) spectral information of high-frequency noises under zero field. The hyperfine-bias-enhanced zero-field magnetometry can be combined with dynamical decoupling to enhance single-molecule magnetic resonance spectroscopy and to improve the frequency resolution in nanoscale magnetic resonance imaging.

Optimized microwave sensing in broad frequency range by a fiber diamond probe

Diamond based quantum sensing is a fast-emerging field with both scientific and technological importance. The nitrogen-vacancy (NV) center, a crystal defect in diamond, is a unique model system for microwave sensing application due to its excellent photo-stability, long spin coherence time in ambient conditions. In this work, we systematically optimized the measurement parameters for microwave sensing. The system noise is analyzed, and 1/f noise is suppressed by introducing a differential algorithm. The gain of avalanche photodiode and the gating window of the pulsed fluorescence is optimized to further suppress the noise floor. The decoherence of spin is characterized by varying the duration of the laser and microwave. The minimal detectable power on a standard microstrip is characterized with sampling time down to 1 ms, showing flat frequency dependence. The results have important implications toward fast measurement of broadband microwave power, especially in the field of IC testing and radar signal processing under intense electromagnetic interference.

Ampere Field Fluctuation from Acoustic Phonons as a Possible Source of Spin Decoherence

Ampere Field Fluctuation from Acoustic Phonons as a Possible Source of Spin Decoherence

Spin manipulation and decoherence in a quantum dot mediated by a synthetic spin–orbit coupling of broken T-symmetry

The electrical control of a spin qubit in a quantum dot (QD) relies on spin–orbit coupling (SOC), which could be either intrinsic to the underlying crystal lattice or heterostructure, or extrinsic via, for example, a micro-magnet. In experiments, micromagnets have been used as a synthetic SOC to enable strong coupling of a spin qubit in quantum dots with electric fields. Here we study theoretically the spin relaxation, pure dephasing, spin manipulation, and spin–photon coupling of an electron in a QD due to the synthetic SOC induced spin–orbit mixing. We find qualitative difference in the spin dynamics in the presence of a synthetic SOC compared with the case of the intrinsic SOC. Specifically, spin relaxation due to the synthetic SOC and deformation potential phonon emission (or Johnson noise) shows (or B 0) dependence with the magnetic field, which is in contrast with the (or ) dependence in the case of the intrinsic SOC. Moreover, charge noise induces fast spin dephasing to the first order of the synthetic SOC, which is in sharp contrast with the negligible spin pure dephasing in the case of the intrinsic SOC. These qualitative differences are attributed to the broken time-reversal symmetry (T-symmetry) of the synthetic SOC. An SOC with broken T-symmetry (such as the synthetic SOC from a micro-magnet) eliminates the ‘Van Vleck cancellation’ and causes a finite longitudinal spin–electric coupling that allows the longitudinal coupling between spin and electric field, and in turn allows spin pure dephasing. Finally, through proper choice of magnetic field orientation, the electric-dipole spin resonance via the synthetic SOC can be improved with potential applications in spin-based quantum computing.

Decoupling of Spin Decoherence Paths near Zero Magnetic Field.

We demonstrate a method to quantify and manipulate nuclear spin decoherence mechanisms that are active in zero to ultralow magnetic fields. These include (i) nonadiabatic switching of spin quantization axis due to residual background fields and (ii) scalar pathways due to through-bond couplings between 1H and heteronuclear spin species, such as 2H used partially as an isotopic substitute for 1H. Under conditions of free evolution, scalar relaxation due to 2H can significantly limit nuclear spin polarization lifetimes and thus the scope of magnetic resonance procedures near zero field. It is shown that robust trains of pulsed dc magnetic fields that apply π flip angles to one or multiple spin species may switch the effective symmetry of the nuclear spin Hamiltonian, imposing decoupled or coupled dynamic regimes on demand. The method should broaden the spectrum of hyperpolarized biomedical contrast-agent compounds and hyperpolarization procedures that are used near zero field.

Electrical control of the g tensor of the first hole in a silicon MOS quantum dot

Single holes confined in semiconductor quantum dots are a promising platform for spin qubit technology, due to the electrical tunability of the $g$-factor of holes. However, the underlying mechanisms that enable electric spin control remain unclear due to the complexity of hole spin states. Here, we study the underlying hole spin physics of the first hole in a silicon planar MOS quantum dot. We show that non-uniform electrode-induced strain produces nanometre-scale variations in the HH-LH splitting. Importantly, we find that this \RR{non-uniform strain causes} the HH-LH splitting to vary by up to 50\% across the active region of the quantum dot. We show that local electric fields can be used to displace the hole relative to the non-uniform strain profile, allowing a new mechanism for electric modulation of the hole g-tensor. Using this mechanism we demonstrate tuning of the hole $g$-factor by up to 500\%. In addition, we observe a \RR{potential} sweet spot where d$g_{(1\overline{1}0)}$/d$V$ = 0, offering a configuration to suppress spin decoherence caused by electrical noise. These results open a path towards a previously unexplored technology: engineering of \RR{non-uniform} strains to optimise spin-based devices.

Moiré Tuning of Spin Excitations: Individual Fe Atoms on MoS_{2}/Au(111).

Magnetic adatoms on properly designed surfaces constitute exquisite systems for addressing, controlling, and manipulating single quantum spins. Here, we show that monolayers of MoS_{2} on a Au(111) surface provide a versatile platform for controllably tuning the coupling between adatom spins and substrate electrons. Even for equivalent adsorption sites with respect to the atomic MoS_{2} lattice, we observe that Fe adatoms exhibit behaviors ranging from pure spin excitations, characteristic of negligible exchange and dominant single-ion anisotropy, to a fully developed Kondo resonance, indicating strong exchange and negligible single-ion anisotropy. This tunability emerges from a moiré structure of MoS_{2} on Au(111) in conjunction with pronounced many-body renormalizations. We also find striking spectral variations in the immediate vicinity of the Fe atoms, which we explain by quantum interference reflecting the formation of Fe-S hybrid states despite the nominally inert nature of the substrate. Our work establishes monolayer MoS_{2} as a tuning layer for adjusting the quantum spin properties over an extraordinarily broad parameter range. The considerable variability can be exploited for quantum spin manipulations.

Clock transitions guard against spin decoherence in singlet fission.

Short coherence times present a primary obstacle in quantum computing and sensing applications. In atomic systems, clock transitions (CTs), formed from avoided crossings in an applied Zeeman field, can substantially increase coherence times. We show how CTs can dampen intrinsic and extrinsic sources of quantum noise in molecules. Conical intersections between two periodic potentials form CTs in electron paramagnetic resonance experiments of the spin-polarized singlet fission photoproduct. We report on a pair of CTs for a two-chromophore molecule in terms of the Zeeman field strength, molecular orientation relative to the field, and molecular geometry.

Ab initio ultrafast spin dynamics in solids

Spin relaxation and decoherence is at the heart of spintronics and spin-based quantum information science. Currently, theoretical approaches that can accurately predict spin relaxation of general solids including necessary scattering pathways and capable for ns to ms simulation time are urgently needed. We present a first-principles real-time density-matrix approach based on Lindblad dynamics to simulate ultrafast spin dynamics for general solid-state systems. Through the complete first-principles descriptions of pump, probe and scattering processes including electron-phonon, electron-impurity and electron-electron scatterings with self-consistent electronic spin-orbit couplings, our method can directly simulate the ultrafast pump-probe measurements for coupled spin and electron dynamics over ns at any temperatures and doping levels. We first apply this method to a prototypical system GaAs and obtain excellent agreement with experiments. We find that the relative contributions of different scattering mechanisms and phonon modes differ considerably between spin and carrier relaxation processes. In sharp contrast to previous work based on model Hamiltonians, we point out that the electron-electron scattering is negligible at room temperature but becomes dominant at low temperatures for spin relaxation in n-type GaAs. We further examine ultrafast dynamics in novel spin-valleytronic materials - monolayer and bilayer WSe2 with realistic defects. We find that spin relaxation is highly sensitive to local symmetry and chemical bonds around defects. Our work provides a predictive computational platform for spin dynamics in solids, which has unprecedented potentials for designing new materials ideal for spintronics and quantum information technology.

Enhanced Parameter Estimation with Periodically Driven Quantum Probe.

I propose a quantum metrology protocol for measuring frequencies and weak forces based on a periodic modulating quantum Jahn–Teller system composed of a single spin and two bosonic modes. I show that, in the first order of the frequency drive, the time-independent effective Hamiltonian describes spin-dependent interaction between the two bosonic modes. In the limit of high-frequency drive and low bosonic frequency, the quantum Jahn–Teller system exhibits critical behavior which can be used for high-precision quantum estimation. A major advantage of the scheme is the robustness of the system against spin decoherence, which allows it to perform parameter estimation with measurement time not limited by spin dephasing.

Magnetic-Gradient-Free Two-Axis Control of a Valley Spin Qubit in SixGe1−x

Spins in SiGe quantum dots are promising candidates for quantum bits but are also challenging due to the valley degeneracy which could potentially cause spin decoherence and weak spin-orbital coupling. In this work we demonstrate that valley states can serve as an asset that enables two-axis control of a singlet-triplet qubit formed in a double quantum dot without the application of a magnetic field gradient. We measure the valley spectrum in each dot using magnetic field spectroscopy of Zeeman split triplet states. The interdot transition between ground states requires an electron to flip between valleys, which in turn provides a g-factor difference $\Delta g$ between two dots. This $\Delta g$ serves as an effective magnetic field gradient and allows for qubit rotations with a rate that increases linearly with an external magnetic field. We measured several interdot transitions and found that this valley introduced $\Delta g$ is universal and electrically tunable. This could potentially simplify scaling up quantum information processing in the SiGe platform by removing the requirement for magnetic field gradients which are difficult to engineer.

Spatially Resolved Decoherence of Donor Spins in Silicon Strained by a Metallic Electrode

By taking advantage of how strain gradients affect spin energy levels, experiments provide a spatial map of spin coherence times of donor atoms in silicon---necessary information for many quantum-based applications.

Quantum spin mixing in Dirac materials

The spin of the electron is nowadays replacing the charge as basic carrier of information not only in spintronics applications, but also in the emerging field of quantum information. Topological quantum materials, where spin-momentum locking is believed to lead to particularly long spin lifetimes, are regarded as a promising platform for such applications. However, spin-orbit coupling, that is essential to all topological matter, at the same time gives rise to spin mixing and decoherence as a major obstacle for quantum computing. Here, we give experimental evidence that hot-spots of spin-mixing and spin-conserving contributions of the spin-orbit operator coexist in an archetypal topological Dirac metal, and that these hot spots can have a strongly anisotropic distribution of their respective wave vectors with respect to the spin quantization direction. Our results can be understood within a theory that takes into account the decomposition of the spin-orbit Hamiltonian into spin-conserving and spin-flip terms, contributing to a better understanding of quantum decoherence in topological materials, in general.

Gravitational decoherence: A nonrelativistic spin 1/2 fermionic model

In a previous work [L. Asprea, G. Gasbarri, and A. Bassi, Gravitational decoherence: A general nonrelativistic model, Phys. Rev. D 103, 104041 (2021).] we derived a quantum master equation for the dynamics of a scalar bosonic particle interacting with a weak, stochastic and classical gravitational field. As standard matter is made of fermions, such an equation should be suitably extended to describe more relevant experimental situations. Here we derive a nonrelativistic model for the gravitational decoherence of spin 1/2 particles. We enrich the treatment by also considering a coupling with an external classical electromagnetic field. We comment on the differences with the scalar bosonic model and we describe the regimes in which they become negligible.

Influence of Spin Decoherence on the Yield of Photodriven Quantum Teleportation in Molecular Triads.

The evolution of spin coherences due to spin-selective recombination in the system with three unpaired electrons is discussed. It is shown that in the case of bidirectional kinetics, the decoherence processes can significantly change the quantum yield of the products. This enables one to discriminate between approaches that model spin-selective recombination but predict different decoherence rates. The rigid donor-acceptor-radical molecular triad is suggested to study the decay rate of singlet-triplet coherence. A modification of the photodriven quantum teleportation protocol is proposed to measure the quantum yields of the monoradical products.