The usefulness of solid-state spins in quantum technologies depends on how long they can remain in a coherent superposition of quantum states. This Colloquium discusses how first-principles simulations can predict spin dynamics for different types of solid-state electron spins, helping design novel and improved platforms for quantum computing, networking, and sensing. We begin by outlining the necessary concepts of the noise affecting generic quantum systems. We then focus on recent advances in predicting spin-phonon relaxation of the spin-defect qubits. Next, we discuss cluster methods as a means of simulating quantum decoherence induced by spin-spin interactions, emphasizing the critical role of validation in ensuring the accuracy of these simulations. We highlight how validated cluster methods can be instrumental in interpreting recent experimental results and, more importantly, predicting the coherence properties of novel spin-based quantum platforms, guiding the development of next-generation quantum technologies.
The usefulness of solid-state spins in quantum technologies depends on how long they can remain in a coherent superposition of quantum states. This Colloquium discusses how first-principles simulations can predict spin dynamics for different types of solid-state electron spins, helping design novel and improved platforms for quantum computing, networking, and sensing. We begin by outlining the necessary concepts of the noise affecting generic quantum systems. We then focus on recent advances in predicting spin-phonon relaxation of the spin-defect qubits. Next, we discuss cluster methods as a means of simulating quantum decoherence induced by spin-spin interactions, emphasizing the critical role of validation in ensuring the accuracy of these simulations. We highlight how validated cluster methods can be instrumental in interpreting recent experimental results and, more importantly, predicting the coherence properties of novel spin-based quantum platforms, guiding the development of next-generation quantum technologies.
Predicting the quantum dynamics of promising solid-state and molecular quantum technology candidates remains a formidable challenge. Yet, accessing these dynamics is key to understanding and controlling decoherence mechanisms-a prerequisite for designing better qubits, sensors, and memories. We leverage a matrix product state representation to introduce a numerically exact and scalable method to achieve this goal. We demonstrate that our method accurately predicts coherence and population dynamics of spin networks across a wide range of parameter regimes, encompassing nuclear spin sensors and qubits in solid-state semiconductors and molecular magnets. Our method further predicts spin dynamics under the influence of repeated light pulses, which are commonly used to mitigate decoherence and perform quantum sensing experiments. Our method thus provides reliable results for moderately sized spin platforms spanning molecular magnets and solid-state spins that can guide the development of approximate but efficient quantum dynamics methods and enable principled inquiry into decoherence mechanisms.
This dissertation is a study of the decoherence of a solid-state spin qubit, either that of a localized electron spin or a donor nucleus, caused by a nuclear spin bath relevant to semiconductor quantum computer architectures. In the presence of an external magnetic field and at low temperatures, the dominant decoherence mechanism is the spectral diffusion of the qubit spin resonance frequency due to the temporally fluctuating random magnetic field associated with the dipolar interaction induced flip-flops of nuclear spin pairs. The qubit spin dephasing due to this random magnetic field depends intricately on the quantum dynamics of the nuclear spin bath, making the coupled decoherence problem difficult to solve. We provide a formally exact solution of this non-Markovian quantum decoherence problem which numerically calculates accurate spin decoherence at short times, of particular relevance in solid-state spin quantum computer architectures. A quantum cluster expansion method is motivated, developed, and tested for the spectral diffusion problem. The method is applicable to any ideal pulse sequence applied to the qubit. Dynamical decoupling sequences, which aim to prolong qubit coherence, are analyzed. In particular, concatenated dynamical decoupling sequences are shown to prolong not only the coherence time over the entire sequence but also the length of time between pulses necessary to maintain coherence. This is shown to result from successive low-order cancellations in applicable perturbative expansions with each level of concatenation. Each cancellation, however, will require the inclusion, in the cluster expansion, of increasingly large clusters to obtain the lowest-order results. These larger clusters in the lowest order often dominate decoherence and therefore invalidate, as being overly optimistic, the pair approximation as a means to study the effect of concatenated dynamical decoupling. We present numerical results from our cluster expansion technique for echoes of single (Hahn), concatenated, and periodic pulse sequences using realistic models of a localized electron in phosphorus doped Si and in a GaAs quantum dot and of a P donor nucleus in Si or GaAs. In the Si:P electron spin decoherence problem, we consider, along with spectral diffusion, the effects of anisotropic hyperfine (AHF) interactions and suggest a technique to suppress electron spin echo envelope modulations (ESEEM), an additional source of decoherence resulting from the AHF interactions. Our calculations for the Si:P Hahn echoes, including the effects of both anisotropic hyperfine interactions and spectral diffusion, are in excellent agreement with experimental results. Our calculations of concatenated pulse sequence echoes offer important predictions for the effectiveness of a promising strategy to preserve qubit coherence in semiconductor quantum computer architectures.
Quantum decoherence induced by defects remains a major limitation for solid-state quantum technologies, yet predicting decoherence in realistic materials remains computationally challenging. Complex defect populations are often approximated as homogeneous spin baths, obscuring the role of defect-specific electronic structure and spin dynamics. Here, we develop a predictive framework for decoherence in diamond by combining first-principles electronic-structure calculations, quantum many-body spin-bath simulations, and experimental validation. The framework incorporates defect-resolved spin Hamiltonians and heterogeneous spin baths containing multiple paramagnetic defect species. Using diamond nitrogen-vacancy ensembles as a model platform, we investigate mixed nitrogen-, vacancy-, and hydrogen-related defect environments. We show that decoherence depends not only on defect density but also on defect identity and bath composition, whose distinct electronic structures, hyperfine interactions, and spin dynamics produce different coherence behavior. Heterogeneous defect populations can either suppress or enhance decoherence, producing trends unexplained by homogeneous-bath models. Magnetic-field-dependent Hahn-echo measurements on samples with different defect concentrations validate the framework. The calculations reproduce the observed coherence times and stretched-exponential decay behavior across a broad magnetic-field range and identify vacancy-related defects as critical contributors beyond the conventionally assumed P1 spin bath. By linking atomistic defect properties to quantum coherence, our framework provides a predictive route for identifying hidden defect environments and optimizing decoherence in defect-based quantum materials.
Solid state based quantum information processing is focused on physical implementation of all necessary elements of quantum computation and quantum information in solid state systems, mainly due to their scalability compared to e.g. optical systems. Among many proposals to realize these types of devices, such as quantum dots as charge qubits or Josephson junction circuits, we study here one of the most promising candidates, i.e., the spin of an electron confined to a quantum dot as a qubit. Experimentally, it has been shown that the relaxation rate of this two level system can be pushed above few seconds in low magnetic fields. Moreover, using spin echo techniques, \nthe spin dephasing time can be maximized up to milliseconds with the current technology. This long spin decay time is one of the main reasons that make this system desirable for quantum computation and quantum information purposes. \nWe reexamined the recent measurement based proposal called one-way quantum computation which exploits entanglement and local measurements as tools to perform quantum computation on N qubits. Although it was suggested in the original work to entangle the qubits via the nearest neighbor Ising interaction, we investigated how one can generate the so-called cluster states with the Heisenberg interaction. We extended our method to include more general forms of Heisenberg interaction such as asymmetric coupling of adjacent qubits. These forms of couplings, rather than Ising interaction, are more encountered in solid state devices, and therefore make it possible to perform one-way quantum computation with electron spins in quantum dots coupled via exchange interaction to their adjacent spins. \n \nChapters II, III, and IV of my thesis are devoted to the study of the spin-orbit interaction in heterostructure quantum dots and its effect on the spin dynamics. We observed that one can actually use spin-orbit interaction to manipulate the spin state of an electron on time scales much smaller than the spin dephasing time. Specifically, in chapter II, we studied the effect of a nearby functioning quantum point contact (QPC) on the relaxation of the electron spin and show that the charge fluctuations in QPC lead to spin relaxation of the confined electron in the presence of spin-orbit interactiom and an applied magnetic field. We also addressed the relation of this rate to the microscopic parameters of the system and found some geometrical dependence of the spin relaxation time on the orientation of the QPC on the substrate. Moreover, we showed in chapters III and IV that the spin-orbit interaction can play a positive role, in order to rotate the spin around the Bloch sphere. We considered different mechanisms, particularly, Electron Dipole Spin Resonance (EDSR) and holonomic unitary gates in quantum dots. We verified that these mechanisms of spin manipulation can be realized in solid state systems with the state of the art semiconductor technologies. \n \nChapter V of the thesis covers a slightly different topic and focuses on the role of the Coulomb interaction in electronic transport. There, we reviewed the non-analytic corrections to the Fermi liquid behavior and their consequences on the momentum occupation number of the electrons in a two dimensional electron gas (2DEG). As an example, we calculated the tunneling rate from an interacting electron reservoir onto a quantum dot and compared our result to the corresponding case for electron tunneling between bilayer 2DEGs. Moreover, within RPA approximation, we found that the electron-plasmon coupling leads to a quadratic frequency dependence of the electron self-energy at low frequencies at the Fermi surface. This correction suppresses the same order corrections due to the particle-hole bubble. \n \n \n
Interacting spin systems in solids underpin a wide range of quantum technologies, from quantum sensors and single-photon sources to spin-defect-based quantum registers and processors. We develop a quantum-computer-aided framework for simulating such devices using a general many-body electron-spin-resonance Hamiltonian that incorporates zero-field splitting, the Zeeman effect, hyperfine interactions, dipole-dipole spin-spin interactions, and electron-phonon decoherence. Within this framework, we combine Gray-encoded qudit-to-qubit mappings, qubit-wise commuting aggregation, and a multi-reference selected quantum Krylov fast-forwarding hybrid algorithm, aiming to access extended-time dynamics within the constraints of NISQ and early fault-tolerant hardware. Numerical simulations demonstrate the computation of operationally useful quantities including autocorrelation functions up to ∼100 ns, together with microwave absorption spectra and the ℓ1-norm of coherence, achieving 18-30% reductions in gate counts and circuit depth for Trotterized time-evolution circuits compared to unoptimized implementations. Using the nitrogen vacancy center in diamond as a testbed, we benchmark the framework against classical simulations and identify the reference-state selection in sQKFF as the primary factor governing accuracy at fixed hardware cost. This methodology provides a flexible blueprint for using quantum computers to design, compare, and optimize solid-state spin-qubit technologies under experimentally realistic conditions.
The interaction of solid-state qubits with environmental degrees of freedom strongly affects the qubit dynamics, and leads to decoherence. In quantum information processing with solid-state qubits, decoherence significantly limits the performances of such devices. Therefore, it is necessary to fully understand the mechanisms that lead to decoherence. In this review, we discuss how decoherence affects two of the most successful realizations of solid-state qubits, namely, spin qubits and superconducting qubits. In the former, the qubit is encoded in the spin 1/2 of the electron, and it is implemented by confining the electron spin in a semiconductor quantum dot. Superconducting devices show quantum behaviour at low temperatures, and the qubit is encoded in the two lowest energy levels of a superconducting circuit. The electron spin in a quantum dot has two main decoherence channels, a (Markovian) phonon-assisted relaxation channel, due to the presence of a spin–orbit interaction, and a (non-Markovian) spin bath constituted by the spins of the nuclei in the quantum dot that interact with the electron spin via the hyperfine interaction. In a superconducting qubit, decoherence takes place as a result of fluctuations in the control parameters, such as bias currents, applied flux and bias voltages, and via losses in the dissipative circuit elements.