We study theoretically the formation of the nuclear-spin polaron state in semiconductor nanosystems within the Lindblad equation approach. To this end, we derive a general Lindblad equation for the density operator that complies with the symmetry of the system Hamiltonian and address the nuclear-spin polaron formation for localized charge carriers subject to an arbitrarily anisotropic hyperfine interaction when optically cooling the nuclei. The steady-state solution of the density matrix for an anisotropic central spin model is presented as a function of the electron and nuclear spin bath temperature. Results for the electron-nuclear spin correlator as well as data for the nuclear spin distribution function serve as a measure of spin-entanglement. The features in both of them clearly indicate the formation of the nuclear polaron state at low temperatures where the crossover regime coincides with an enhancement of quantum fluctuations and agrees with the mean-field prediction of the critical temperature line. We can identify two distinct polaron states dependent upon the hyperfine anisotropy, which are separated by a quantum phase transition at the isotropic point. These states are reflected in the temporal spin autocorrelation functions accessible in experiment via spin-noise measurements.
We study theoretically the formation of the nuclear-spin polaron state in semiconductor nanosystems within the Lindblad equation approach. To this end, we derive a general Lindblad equation for the density operator that complies with the symmetry of the system Hamiltonian and address the nuclear-spin polaron formation for localized charge carriers subject to an arbitrarily anisotropic hyperfine interaction when optically cooling the nuclei. The steady-state solution of the density matrix for an anisotropic central spin model is presented as a function of the electron and nuclear spin bath temperature. Results for the electron-nuclear spin correlator as well as data for the nuclear spin distribution function serve as a measure of spin-entanglement. The features in both of them clearly indicate the formation of the nuclear polaron state at low temperatures where the crossover regime coincides with an enhancement of quantum fluctuations and agrees with the mean-field prediction of the critical temperature line. We can identify two distinct polaron states dependent upon the hyperfine anisotropy, which are separated by a quantum phase transition at the isotropic point. These states are reflected in the temporal spin autocorrelation functions accessible in experiment via spin-noise measurements.
The quantum Ising model is perhaps the simplest possible model of a quantum magnetic material. Despite its simplicity, its versatility and wide range of applications, from quantum computation, to combinatorial optimization, to biophysics, make it one of the most important models of modern physics. In this thesis, we develop a general framework for studying quantum Ising systems with an arbitrary single ion Hamiltonian, with emphasis on the effects of quantum fluctuations, and the quantum phase transition between paramagnetic and ferromagnetic states that occurs when a magnetic field is applied transverse to the easy axis of the system. The magnetic insulating crystal LiHoF₄ is a physical realization of the quantum Ising model, with the additional features that the dominant coupling between spins is the long range dipolar interaction, and each electronic spin is strongly coupled to a nuclear degree of freedom. These nuclear degrees of freedom constitute a spin bath environment acting on the system. In this thesis, we present an effective low temperature Hamiltonian for LiHoF₄ that incorporates both these features, and we analyze the effects of the nuclear spin bath on the system. We find the lowest energy crystal field excitation in the system is gapped at the quantum critical point by the presence of the nuclear spins, with spectral weight being transferred down to a lower energy electronuclear mode that fully softens to zero at the quantum critical point. Furthermore, we present a toy model, the spin half spin half model, that illustrates the effects of an anisotropic hyperfine interaction on a quantum Ising system. We find the critical transverse field is increased when the longitudinal hyperfine coupling is dominant, as well as an enhancement of both the longitudinal electronic susceptibility and an applied longitudinal field. In addition, we present a field theoretic formalism for incorporating the effects of fluctuations beyond the random phase approximation in general quantum Ising systems. We find that any regular on site interaction, such as a nuclear spin bath, does not fundamentally alter the critical properties of a quantum Ising system. This formalism is used to calculate corrections to the magnetization of LiHoF₄.
We use a one-dimensional tight binding model with an impurity site characterized by electron-vibration coupling, to describe electron transfer and localization at zero temperature, aiming to examine the process of polaron formation in this system. In particular we focus on comparing a semiclassical approach that describes nuclear motion in this many vibronic-states system on the Ehrenfest dynamics level to a numerically exact fully quantum calculation based on the Bonca-Trugman method [J. Bonča and S. A. Trugman, Phys. Rev. Lett. 75, 2566 (1995)]. In both approaches, thermal relaxation in the nuclear subspace is implemented in equivalent approximate ways: In the Ehrenfest calculation the uncoupled (to the electronic subsystem) motion of the classical (harmonic) oscillator is simply damped as would be implied by coupling to a Markovian zero temperature bath. In the quantum calculation, thermal relaxation is implemented by augmenting the Liouville equation for the oscillator density matrix with kinetic terms that account for the same relaxation. In both cases we calculate the probability to trap the electron by forming a polaron and the probability that it escapes to infinity. Comparing these calculations, we find that while both result in similar long time yields for these processes, the Ehrenfest-dynamics based calculation fails to account for the correct time scale for the polaron formation. This failure results, as usual, from the fact that at the early stage of polaron formation the classical nuclear dynamics takes place on an unphysical average potential surface that reflects the distributed electronic population in the system, while the quantum calculation accounts fully for correlations between the electronic and vibrational subsystems.
The time evolution of spin states of two electrons interacting with a nuclear spin bath in a quantum dot system is studied. The hyperfine interaction between the electrons and the nuclear spins is modeled by an isotropic Heisenberg interaction, and the interaction between the electron spins by Heisenberg exchange. Depending on the extent of the overlap between the spatial wave functions of the electrons, there are two physically different cases, namely, the two qubits either interact with the same set of nuclear spins or they see different nuclear spin environments. In the two cases, the decoherence of the two-qubit state is studied analytically. We have identified a class of two-qubit states that have a rich dynamics when the exchange interaction between the qubits becomes large in comparison to the hyperfine interaction strengths. The decoherence time scale is determined as a function of the bath-spin distribution and the polarizations of the initial two-qubit state. States with large decoherence times are identified by performing a minimization over all the two-qubit pure states.
Dynamic nuclear polarization (DNP) is one of the most promising techniques towards a new generation of Magnetic Resonance Imaging (MRI). The idea is to use the Nuclear Magnetic Resonance (NMR) in other nuclei rather than the traditional hydrogen, such as carbon. For the carbon signal to be detected, one needs to enhance its spin polarization. In thermal equilibrium — at low temperature and high magnetic field — electron spins are far more polarized than any system of nuclear spins, which is due to their smaller mass. With the DNP technique we bring the system out-of-equilibrium irradiating it with microwaves. This triggers polarization transfer from the electron spins to the nuclear ones. During my Ph.D, I have studied both analytically and numerically the competition between the dipolar interactions among electron spins (which can be tuned experimentally) and the disorder naturally present in the sample. I proposed two models to study DNP: a Heisenberg spin-chain and a system free-fermions in the Anderson model. Two different regimes were found : For strongly interacting electron spins, the out-of-equilibrium steady state displays an effective thermodynamic behavior characterised by a very low spin temperature. In the weakly interacting regime, it is not possible to define a spin temperature, and it is associated to a many-body localized phase (or an Anderson-localized phase). My research was focused on the properties of the two phases with respect to the performance of DNP, and I found it to be optimal at the transition between the two. This is a very important result that has been verified by recent experiments carried in École Normale Supérieure de Paris.
Spins localized in semiconductor nanostructures have been intensively investigated for quantum spintronics. These include the spin of single electron localized by quantum dots or impurities, and spins of the lattice nuclei. These localized spins can be exploited as carriers of quantum information, while in some circumstances they also play the role of deleterious noise sources for other quantum objects through their couplings. Quantum control of the spins in semiconductor nanostructures is therefore of central interest for quantum applications. In this thesis, we address several problems related to the quantum control of electron or hole spin and nuclear spins in semiconductor quantum dots and impurity centers. The first problem studied is the control of nuclear spin bath for a hole spin qubit in III-V semiconductor quantum dot. In quantum dots formed on III-V compounds, the direct band gap of the host material allows ultrafast optical addressability of a single electron or hole spin qubit. However, nonzero nuclear spins of group III and group V elements result in a large statistical fluctuation in the Zeeman splitting of the spin qubit which then dephases in nanosecond time scale. We present a novel feedback scheme to suppress the statistical fluctuation of the nuclear spin field for enhancing the coherence time of the hole spin qubit. We also find positive feedback control which can amplify the magnitude of the nuclear field, so that a bimodal distribution can develop, realizing a quantum environment that can not be described by a single temperature. The second problem addressed here is the control of donor spin qubits in silicon architecture which have ultra-long quantum coherence time. We developed the quantum control scheme to realize the quantum metrology of magnetic field gradient, based on the celebrated Kane’s architecture for quantum computation. The scheme can also be generalized to calibrate the locations of the donors. In the third part of the thesis, we investigate a novel type of quantum dot formed in a new class of two-dimensional semiconductors, monolayer transition metal dichalcogenides (TMDs), which exhibit interesting spin and pseudospin physics. This novel quantum dot system may offer new opportunity for quantum spintronics in the ultimate 2D limit, and we investigate here the valley pseudospin as a possible quantum bit carrier. A main finding is that, contrary to the intuition, the lateral confinement by the quantum dot potential does not lead to noticeable valley hybridization, and therefore the valley pseudospin in monolayer TMDs QD can well inherit the valley physics such as the valley optical selection rules from the 2D bulk which implies a variety of quantum control possibilities.
Identification of the I10 Donor in ZnO as a Sn--Li Complex with Large Hyperfine Interaction
Donor impurities in wide direct band gap semiconductors provide a promising platform for spin--photon quantum technologies by combining a donor spin qubit with optically addressable transitions. In ZnO, the shallow donor with the largest reported binding energy has long been associated with the I10 bound exciton line, but its microscopic origin has remained unresolved. Here we demonstrate the controlled formation and identification of this donor as a Sn--Li complex through a combination of ion implantation, annealing, optical spectroscopy, and first-principles calculations. Resonant two-laser coherent population trapping measurements reveal an electron--119Sn hyperfine interaction of 392±15\,MHz, establishing a coupled electron--spin--1/2, nuclear--spin--1/2 system with one of the largest hyperfine couplings reported for shallow donors in semiconductors. Density functional theory calculations show that a nearest-neighbor SnZn--LiZn complex has favorable formation energetics, donor character with the electron localized on Sn, and an extrapolated hyperfine interaction consistent with experiment. The large donor binding energy and excited-state structure indicate enhanced thermal robustness of the optical transition relative to conventional group--III donors, while the strong hyperfine interaction enables fast electron--nuclear spin control and prospects for direct nuclear--spin--photon interfaces. We further observe efficient optically induced nuclear spin polarization, highlighting a path toward nuclear spin initialization. More broadly, our results reveal how a donor--acceptor complex can access previously unexplored regimes of shallow donor physics, extending the design space of quantum defects beyond isolated substitutional dopants.