Intrinsic Spin Fluctuations Reveal the Dynamical Response Function of Holes Coupled to Nuclear Spin Baths in (In,Ga)As Quantum Dots

Spin inertia measurements are a novel experimental tool to study long-time spin relaxation processes in semiconductor nanostructures. We develop a theory of the spin inertia effect for resident electrons and holes localized in quantum dots. We consider the spin orientation by short optical pulses with arbitrary pulse area and detuning from the trion resonance. The interaction with an external longitudinal magnetic field and the hyperfine interaction with the nuclear spin bath is considered in both the ground and excited (trion) states of the quantum dots. We analyze how the spin inertia signal depends on the magnetic field (polarization recovery) and on the modulation frequency of the helicity of the pump pulses as well as on their power and detuning. In particular, we elaborate how approaching the saturation limit of the spin polarization influences the measurements. The quantitative description of spin inertia measurements will enable the determination of the parameters of spin dynamics such as the spin relaxation times in the ground and excited states and the parameters of the hyperfine interaction. Finally, we predict the emergence of resonant spin amplification due to the transverse components of the nuclear spin fluctuations, which manifests itself as oscillations of the spin polarization as a function of the longitudinal magnetic field.

Interaction with nuclear spins leads to decoherence and information loss in solid-state electron-spin qubits. One particular, ineradicable source of electron decoherence arises from decoherence of the nuclear spin bath, driven by nuclear–nuclear dipolar interactions. Owing to its many-body nature nuclear decoherence is difficult to predict, especially for an important class of strained nanostructures where nuclear quadrupolar effects have a significant but largely unknown impact. Here, we report direct measurement of nuclear spin bath coherence in individual self-assembled InGaAs/GaAs quantum dots: spin-echo coherence times in the range 1.2–4.5 ms are found. Based on these values, we demonstrate that strain-induced quadrupolar interactions make nuclear spin fluctuations much slower compared with lattice-matched GaAs/AlGaAs structures. Our findings demonstrate that quadrupolar effects can potentially be used to engineer optically active III-V semiconductor spin-qubits with a nearly noise-free nuclear spin bath, previously achievable only in nuclear spin-0 semiconductors, where qubit network interconnection and scaling are challenging.

We investigate theoretically the spin echo signal of an electron localized in a quantum dot and interacting with a bath of nuclear spins. We consider the regime of very low magnetic fields (corresponding to fields as low as a militesla in realistic GaAs and InGaAs dots). We use both the exact numerical simulations and the analytical theory employing the effective pure dephasing Hamiltonian. The comparison shows that the latter approach describes very well the spin echo decay at magnetic fields larger than the typical Overhauser field, and that the timescale at which this theory works is larger than previously expected. The numerical simulations are also done for very low values of electron spin splitting at which the effective Hamiltonian based theory fails quantitatively. Interestingly, the qualitative difference in the spin echo decay between the cases of a homonuclear and a heteronuclear bath (i.e. bath containing nuclear isotopes having different Zeeman energies), predicted previously using the effective Hamiltonian approach, is still visible at very low fields outside the regime of applicability of the analytical theory. We have found that the spin echo signal for a homonuclear bath oscillates with a frequency corresponding to the Zeeman splitting of the single nuclear isotope present in the bath. The physics behind this feature is similar to that of the electron spin echo envelope modulation (ESEEM). While purely isotropic hyperfine interactions are present in our system, the tilting of the electron precession axis at low fields may explain this result.

In double quantum dots, the exchange interaction between two electron spins renormalizes the excitation energy of pair flips in the nuclear spin bath, which in turn modifies the non-Markovian bath dynamics. As the energy renormalization varies with the static Overhauser field mismatch between the quantum dots, the electron singlet-triplet decoherence resulting from the bath dynamics depends on sampling of nuclear spin states from an ensemble, leading to the transition from superexponential decoherence in single-sample dynamics to power-law decay under ensemble averaging. In contrast, the decoherence of a single electron spin in one dot is essentially the same for different choices of the nuclear spin configuration.

We report millisecond-range spin memory of resident electrons in an ensemble of InP quantum dots (QDs) under a small magnetic field of 0.1 T applied along the optical excitation axis at temperatures up to about 5 K. A pump-probe photoluminescence (PL) technique is used for optical-orientation of electron spins by the pump pulses and for study of spin relaxation over the long time scale by measuring the degree of circular polarization of the probe PL as a function of pump-probe delay. Dependence of spin decay rate on temperature and magnetic field suggests two-phonon processes as the dominant spin relaxation mechanism in these QDs at low temperatures.

Central spin models describe a variety of quantum systems in which a spin-1/2 qubit interacts with a bath of surrounding spins, as realized in quantum dots and defect centers in diamond. We show that the fully anisotropic central spin Hamiltonian with (XX) Heisenberg interactions is integrable. Building on the class of integrable Richardson-Gaudin models, we derive an extensive set of conserved quantities and obtain the exact eigenstates using the Bethe ansatz. These states divide into two exponentially large classes: bright states, where the qubit is entangled with the bath, and dark states, where it is not. We discuss how dark states limit qubit-assisted spin bath polarization and provide a robust long-lived quantum memory for qubit states.

Towards modeling spatiotemporal processes in metal–organic frameworks

Transition metal dichalcogenide (TMD)-based quantum dots (QDs) have proven to be a successful and promising device for physically implementing electron spin-valley based qubits. Although the electron spin in a TMDs monolayer semiconductor QD can be isolated and controlled with high precision, decoherence occurs due to unavoidable coupling with the surrounding environment, such as nuclear spin environments. In this paper, using an exact master equation (ME) of spin qubit dynamics coupled to a nuclear spin bath in terms of hyperfine interaction (HI), we have investigated the controllability of dynamics processes with varying degrees of non-Markovianity. In large magnetic fields, we show that pure spin or valley qubits can be created. We calculate the loss of fidelity due to the Overhauser field of HI in a wide range of nuclear spin. In this context, we prove that this field restricts the decoherence process of the central electron spin, which can regain its coherence. Finally, we discuss how the coherence of the spin qubit remains robust for large .

Photoluminescence (PL) intermittency characteristics are examined for single quantum dots (QDs) in a CdSe QD sample synthesized at a slow rate at 75 degrees C. Although the PL quantum efficiency was relatively low ( approximately 0.25), we noticed that the PL intensity of single CdSe QDs fluctuated on a subsecond time scale with short-lived "on" and "off" states. The subsecond PL intensity fluctuations of CdSe QDs are different from "on" and "off" PL blinking generally observed for QDs fluctuating on a millisecond to minute time scale. We characterized single QDs by identifying polarized excitations, topographic imaging using atomic force microscopy (AFM), and transmission electron microscopy (TEM). From analysis of the PL intensity trajectories from >100 single CdSe QDs, the average intermittency time was 213 ms. From the PL quantum efficiency, slow growth of QDs, intensity trajectory analyses, and previous reports relating surface trap states and PL properties of QDs, we attribute the subsecond PL intensity fluctuations of single CdSe QDs and short-lived "on" and "off" states to a high-density distribution of homogeneous surface trap states.

The intermediate-band assisted hot-carrier solar cell (IB-HCSC) concept has been proposed in order to assist the extraction of hot carriers from an absorber that has an intermediate band (IB). In this study, we used a heterostructure based on ten layers of In(Ga)As quantum dots (QDs) embedded in an Al0.2Ga0.8As single-junction solar cell designed for an intermediate band solar cell (IBSC). QD-IBSCs have proven to be limited by the thermal escape of photo-carriers from QDs at room temperature. In such cases, fundamental improvements in conversion efficiency are only possible if carriers in the IB are not in thermal equilibrium with either conduction or valence bands. Additionally, the IB-HCSC concept provides a high-efficiency limit and enables us to work with all relaxation mechanisms (thermalization, carrier-carrier scattering, and thermal radiation). Under high irradiation, we confirmed the emergence of a hot carrier population in the QDs, limited mostly by thermionic emission, which assists the IBSC by providing a thermoelectric gain in voltage without hindering the possibility of sequential two-photon absorption. Absolute intensity calibrated photoluminescence spectroscopy indicated that the triggering mechanism happens when the QD ensemble is estimated to have a high carrier concentration that behaves as a metal-like IB. Experimental results suggested that the hot carrier effect also occurred in other solar cells based on quantum heterostructures and directions for improvements of hot-carrier assisted QD-IBSCs are proposed for further efficiency gain in optimized device architectures.

A huge effort is underway to develop semiconductor nanostructures as low-noise hosts for qubits. The main source of dephasing of an electron spin qubit in a GaAs-based system is the nuclear spin bath. A hole spin may circumvent the nuclear spin noise. In principle, the nuclear spins can be switched off for a pure heavy-hole spin. In practice, it is unknown to what extent this ideal limit can be achieved. A major hindrance is that p-type devices are often far too noisy. We investigate here a single hole spin in an InGaAs quantum dot embedded in a new generation of low-noise p-type device. We measure the hole Zeeman energy in a transverse magnetic field with 10 neV resolution by dark-state spectroscopy as we create a large transverse nuclear spin polarization. The hole hyperfine interaction is highly anisotropic: the transverse coupling is <1% of the longitudinal coupling. For unpolarized, randomly fluctuating nuclei, the ideal heavy-hole limit is achieved down to nanoelectronvolt energies; equivalently dephasing times up to a microsecond. The combination of large and strong optical dipole makes the single hole spin in a GaAs-based device an attractive quantum platform.

Ultrafast phenomena on the nanoscale

We propose a dynamic quantum sensing scheme by using a quantum many-spin\nsystem composed of a central spin interacting with many surrounding spins.\nStarting from a generalized Ising ring model, we investigate the error\npropagation formula of the central spin and it indicates that Heisenberg\nscaling can be reached while the probe state only needs to be a product state.\nParticularly, we derive an analytical form of the dynamic quantum Fisher\ninformation in a limit case, which explicitly exhibits the Heisenberg scaling.\nBy comparing with numerical results, we demonstrate that the general case can\nbe well approximated by the analytical result when the coupling strength among\nthe surrounding spins is much weaker than the coupling strength between the\ncentral and surrounding spins. This analytic result guides us to find the\nappropriate probe state and the proper measurement time, to achieve the\nHeisenberg scaling in realistic situations. Furthermore, we investigate various\neffects which are important in practical quantum systems, including the central\nspin Zeeman term, the anisotropy of the hyperfine interaction and the\ninhomogeneity of the hyperfine coupling strength. Our result indicates that the\ndynamic quantum-enhanced sensing scheme seems feasible in realistic quantum\ncentral spin systems, like semiconductor quantum dots.\n

We develop an explicit description of a time-dependent response of fermionic\ncondensates to perturbations. The dynamics of Cooper pairs at times shorter\nthan the energy relaxation time can be described by the BCS model. We obtain a\ngeneral explicit solution for the dynamics of the BCS model. We also solve a\nclosely related dynamical problem - the central spin model, which describes a\nlocalized spin coupled to a "spin bath". Here, we focus on presenting the\nsolution and describing its general properties, but also mention some\napplications, e.g. to nonstationary pairing in cold Fermi gases and to the\nissue of electron spin decoherence in quantum dots. A typical dynamics of the\nBCS and central spin models is quasi-periodic with a large number of\nfrequencies and stable under small perturbations. We show that for certain\nspecial initial conditions the number of frequencies decreases and the solution\nsimplifies. In particular, periodic solutions correspond to the ground state\nand excitations of the BCS model.\n

This paper analyzes the observed phenomenology of the fluorescence time trace of collections of quantum dots (QDs) in terms of the model parameters that characterize the fluorescence blinking statistics of single QDs. We demonstrate that the non-universal dynamics that appear in fluorescence time traces of collections of QDs at short time scales are related to the universal dynamics that appear at longer time scales. We explore how the extent of time separation between the short and long dynamics affects the transition region and the dynamics at longer time scales. We suggest a methodology to extract single QD statistical model parameters from experimental fluorescence time traces of collections of QDs. We explore theoretical time traces and their experimental analogs for three different cases that span the diverse nonuniversal dynamics that appear at short time scales.