Hole Spin Dynamics Research Articles

A singlet-triplet hole-spin qubit in MOS silicon

Holes in silicon quantum dots are promising for spin qubit applications due to the strong intrinsic spin-orbit coupling. The spin-orbit coupling produces complex hole-spin dynamics, providing opportunities to further optimise spin qubits. Here, we demonstrate a singlet-triplet qubit using hole states in a planar metal-oxide-semiconductor double quantum dot. We demonstrate rapid qubit control with singlet-triplet oscillations up to 400 MHz. The qubit exhibits promising coherence, with a maximum dephasing time of 600 ns, which is enhanced to 1.3 μs using refocusing techniques. We investigate the magnetic field anisotropy of the eigenstates, and determine a magnetic field orientation to improve the qubit initialisation fidelity. These results present a step forward for spin qubit technology, by implementing a high quality singlet-triplet hole-spin qubit in planar architecture suitable for scaling up to 2D arrays of coupled qubits.

Coherent Carrier Spin Dynamics in FAPbBr3 Perovskite Crystals.

Coherent spin dynamics of electrons and holes are studied in hybrid organic-inorganic lead halide perovskite FAPbBr3 bulk single crystals using the time-resolved Kerr ellipticity technique at cryogenic temperatures. The Larmor spin precession of the carrier spins in a magnetic field is monitored to measure the Landé g-factors of electrons (+2.44) and holes (+0.41). These g-factors are highly isotropic. The measured spin dephasing times amount to a few nanoseconds, and the longitudinal hole spin relaxation time is 470 ns. The important role of the strong hyperfine interaction between carrier spins and nuclear spins is demonstrated via dynamic nuclear polarization. At low temperatures, electron and hole spin relaxation predominantly occurs via the hyperfine interaction, whose importance significantly decreases at temperatures above 12 K. We overview the spin dynamics in various lead halide perovskite crystals and polycrystalline films and conclude on their common features provided by charge carrier localization at cryogenic temperatures.

Temperature dependence of the electron and hole Landé g-factors in CsPbI3 nanocrystals embedded in a glass matrix.

The coherent spin dynamics of electrons and holes in CsPbI3 perovskite nanocrystals in a glass matrix are studied by the time-resolved Faraday ellipticity technique in magnetic fields up to 430 mT across a temperature range from 6 K to 120 K. The Landé g-factors and spin dephasing times are evaluated from the observed Larmor precession of electron and hole spins. The nanocrystal size in the three studied samples varies from about 8 to 16 nm, resulting in exciton transition varying from 1.69 to 1.78 eV at a temperature of 6 K, allowing us to study the corresponding energy dependence of the g-factors. The electron g-factor decreases with increasing confinement energy in the NCs as a result of NC size reduction, and also with increasing temperature. The hole g-factor shows the opposite trend. Model analysis shows that the variation of g-factors with NC size arises from the transition energy dependence of the g-factors, which becomes strongly renormalized by temperature.

Magnetic field control of light-induced spin accumulation in monolayer MoSe2

Semiconductor transition metal dichalcogenides (TMDs) have equivalent dynamics for their two spin/valley species. This arises from their energy-degenerated spin states, connected via time-reversal symmetry. When an out-of-plane magnetic field is applied, time-reversal symmetry is broken and the energies of the spin-polarized bands shift, resulting in different bandgaps and dynamics in the K and K valleys. Here, we use time-resolved Kerr rotation to study the magnetic field dependence of the spin dynamics in monolayer MoSe2. We show that the magnetic field can control the light-induced spin accumulation of the two valley states, with a small effect on the recombination lifetimes. We unveil that the magnetic field-dependent spin accumulation is in agreement with hole spin dynamics at the longer timescales, indicating that the electron spins have faster relaxation rates. We propose a rate equation model that suggests that lifting the energy-degeneracy of the valleys induces an ultrafast spin-flip toward the stabilization of the valley with the higher valence band energy. Our results provide an experimental insight into the ultrafast charge and spin dynamics in TMDs and a way to control it, which will be useful for the development of new spintronic and valleytronic applications.

Mode locking of hole spin coherences in CsPb(Cl, Br)3 perovskite nanocrystals

The spin physics of perovskite nanocrystals with confined electrons or holes is attracting increasing attention, both for fundamental studies and spintronic applications. Here, stable {{{{{{{rm{CsPb}}}}}}}}{({{{{{{{{rm{Cl}}}}}}}}}_{0.56}{{{{{{{{rm{Br}}}}}}}}}_{0.44})}_{3} lead halide perovskite nanocrystals embedded in a fluorophosphate glass matrix are studied by time-resolved optical spectroscopy to unravel the coherent spin dynamics of holes and their interaction with nuclear spins of the 207Pb isotope. We demonstrate the spin mode locking effect provided by the synchronization of the Larmor precession of single hole spins in each nanocrystal in the ensemble that are excited periodically by a laser in an external magnetic field. The mode locking is enhanced by nuclei-induced frequency focusing. An ensemble spin dephasing time {T}_{2}^{ * } of a nanosecond and a single hole spin coherence time of T2 = 13 ns are measured. The developed theoretical model accounting for the mode locking and nuclear focusing for randomly oriented nanocrystals with perovskite band structure describes the experimental data very well.

Relativistic time-dependent configuration-interaction singles method

In this work, a derivation and implementation of the relativistic time-dependent configuration interaction singles (RTDCIS) method is presented. Various observables for krypton and xenon atoms obtained by RTDCIS are compared with experimental data and alternative relativistic calculations. This includes energies of occupied orbitals in the Dirac-Fock ground state, Rydberg state energies, Fano resonances and photoionization cross sections. Diagrammatic many-body perturbation theory, based on the relativistic random phase approximation, is used as a benchmark with excellent agreement between RTDCIS reported at the Tamm-Dancoff level. Results from RTDCIS are computed in the length gauge, here the negative energy states can be omitted with acceptable loss of accuracy. A complex absorbing potential, that is used to remove photoelectrons far from the ion, is implemented as a scalar potential and validated for RTDCIS. The RTDCIS methodology presented here opens for future studies of strong-field processes, such as attosecond transient absorption and high-order harmonic generation, with electron and hole spin dynamics and other relativistic effects described by first principle via the Dirac equation.

Lead-Dominated Hyperfine Interaction Impacting the Carrier Spin Dynamics in Halide Perovskites.

The outstanding optical quality of lead halide perovskites inspires studies of their potential for the optical control of carrier spins as pursued in other materials. Entering largely uncharted territory, time-resolved pump-probe Kerr rotation is used to explore the coherent spin dynamics of electrons and holes in bulk formamidinium caesium lead iodine bromide (FA0.9 Cs0.1 PbI2.8 Br0.2 ) and to determine key parameters characterizing interactions of their spins, such as the g-factors and relaxation times. The demonstrated long spin dynamics and narrow g-factor distribution prove the perovskites as promising competitors for conventional semiconductors in spintronics. The dynamic nuclear polarization via spin-oriented holes is realized and the identification of the lead (207 Pb) isotope in optically detected nuclear magnetic resonance proves that the hole-nuclei interaction is dominated by the lead ions. A detailed theoretical analysis accounting for the specifics of the lead halide perovskite materials allows the evaluation of the underlying hyperfine interaction constants, both for electrons and holes. Recombination and spin dynamics evidence that at low temperatures, photogenerated electrons and holes are localized at different regions of the perovskite crystal, resulting in their long lifetimes up to 44μs. The findings form the base for the tailored development of spin-optoelectronic applications for the large family of lead halide perovskites and theirnanostructures.

Electron and Hole Spin Relaxation in CdSe Colloidal Nanoplatelets.

Solution-processed quantum-confined nanocrystals are important building blocks for scalable implementation of quantum information science. Extensive studies on colloidal quantum dots (QDs) have revealed subpicosecond hole spin relaxation, whereas the electron spin dynamics remains difficult to probe. Here we study electron and hole spin dynamics in CdSe colloidal nanoplatelets (also called quantum wells) of varying thicknesses using circularly polarized transient absorption spectroscopy at room temperature. The clear spectroscopic features of transition bands associated with heavy, light, and spin-orbit split-off holes enabled separate probes of electron and hole dynamics. The hole spin-flip occurred within ∼200 fs, arising from strong spin-orbit coupling in the valence band. The electron spin lifetime decreased from 6.2 to 2.2 ps as the platelet thickness is reduced from 6 to 4 monolayers, reflecting an exchange interaction between the electron and the hole and/or surface dangling bond spins enhanced by quantum confinement.

Spin dephasing of electrons and holes in isotopically purified ZnSe/(Zn,Mg)Se quantum wells

The coherent spin dynamics of resident electrons and holes in an isotopically purified ZnSe/(Zn,Mg)Se single quantum well is investigated in different regimes, requiring corresponding adaption of the applied time-resolved pump-probe Kerr rotation technique. The purification of the Zn and Se atom species in the crystal to the isotopes with zero nuclear spin is expected to lead to an extension of the spin dephasing times of resident carriers, due to the suppression of their interaction with the nuclear spins. Indeed, we find no indication of carrier-nuclear interaction in this sample and link the observed carrier spin relaxation to the spin-orbit interaction. Theoretical considerations support the experimental results.

Probing the Innermost Accretion Flow Geometry of Sgr A* with Event Horizon Telescope

Abstract Upcoming Event Horizon Telescope (EHT) observations will provide a unique opportunity to reveal the innermost region of the radiative inefficient accretion flow (RIAF) around the Galactic black hole, Sgr A*. Depending on the flow dynamics and accumulated magnetic flux, the innermost region of an RIAF could have a quasi-spherical or disk-like geometry. Here we present a phenomenological model to investigate the characteristics of the black hole shadow images with different flow geometries, together with the effect of black hole spin and flow dynamics. The resulting image consists in general of two major components: a crescent, which may surround the funnel region of the black hole or the black hole itself, and a photon ring, which may be partially luminous and overlapped with the crescent component. Compared to a quasi-spherical flow case, a disk-like flow in the vicinity of a black hole exhibits the following image features: (i) due to less material near the funnel region, the crescent structure has a smaller size, and (ii) due to the combination of emission from the flow beside and behind the black hole, the crescent structure has a more irregular shape, and a less smooth brightness distribution. How these features can result in different observables for EHT observations is discussed.

Asymmetric g Tensor in Low-Symmetry Two-Dimensional Hole Systems

The complex structure of the valence band in many semiconductors leads to multifaceted and unusual properties for spin-3/2 hole systems compared to typical spin-1/2 electron systems. In particular, two-dimensional hole systems show a highly anisotropic Zeeman spin splitting. We have investigated this anisotropy in GaAs/AlAs quantum well structures both experimentally and theoretically. By performing time-resolved Kerr rotation measurements, we found a non-diagonal tensor $g$ that manifests itself in unusual precessional motion as well as distinct dependencies of hole spin dynamics on the direction of the magnetic field $\vec{B}$. We quantify the individual components of the tensor $g$ for [113]-, [111]- and [110]-grown samples. We complement the experiments by a comprehensive theoretical study of Zeeman splitting in in-plane and out-of-plane fields $\vec{B}$. To this end, we develop a detailed multiband theory for the tensor $g$. Using perturbation theory, we derive transparent analytical expressions for the components of the tensor $g$ that we complement with accurate numerical calculations based on our theoretical framework. We obtain very good agreement between experiment and theory. Our study demonstrates that the tensor $g$ is neither symmetric nor antisymmetric. Opposite off-diagonal components can differ in size by up to an order of magnitude.

Spin dynamics and magneto-optical response in charge-neutral tunnel-coupled quantum dots

We model the electron and hole spin dynamics in an undoped double quantum dot structure, considering the carrier tunneling between quantum dots. Taking the presence of an additional in-plane or tilted magnetic field into account, we enable the simulation of magneto-optical experiments, like the time-resolved Kerr rotation measurement, which are currently performed on such structures to probe the temporal spin dynamics. With our model, we reproduce the experimentally observed effect of the extension of the spin polarization lifetime caused by spatial charge separation, which may occur in structures of this type. Moreover, we provide a number of qualitative predictions concerning the necessary conditions for observation of this effect as well as about possible channels of its suppression, including the spin–orbit coupling, which leads to tunneling of carriers accompanied by a spin flip. We also consider the impact of the magnetic field tilting, which results in an interesting spin polarization dynamics.

Spin flips in generic black hole binaries

We study the spin dynamics of individual black holes in a binary system. In particular we focus on the polar precession of spins and the possibility of a complete flip of spins with respect to the orbital plane. We perform a full numerical simulation that displays these characteristics. We evolve equal mass binary spinning black holes for $t=20,000M$ from an initial proper separation of $d=25M$ down to merger after 48.5 orbits. We compute the gravitational radiation from this system and compare it to 3.5 post-Newtonian generated waveforms finding close agreement. We then further use 3.5 post-Newtonian evolutions to show the extension of this spin {flip-flop} phenomenon to unequal mass binaries. We also provide analytic expressions to approximate the maximum {flip-flop} angle and frequency in terms of the binary spins and mass ratio parameters at a given orbital radius. Finally we discuss the effect this spin {flip-flop} would have on accreting matter and other potential observational effects.

Hole-spin dynamics and holeg-factor anisotropy in coupled quantum well systems

Due to its $p$-like character, the valence band in GaAs-based heterostructures offers rich and complex spin-dependent phenomena. One manifestation is the large anisotropy of Zeeman spin splitting. Using undoped, coupled quantum wells (QWs), we examine this anisotropy by comparing the hole-spin dynamics for high- and low-symmetry crystallographic orientations of the QWs. We directly measure the hole $g$ factor via time-resolved Kerr rotation, and for the low-symmetry crystallographic orientations (110) and ($113a$), we observe a large in-plane anisotropy of the hole $g$ factor, in good agreement with our theoretical calculations. Using resonant spin amplification, we also observe an anisotropy of the hole-spin dephasing in the (110)-grown structure, indicating that crystal symmetry may be used to control hole-spin dynamics.

Hole dynamics and spin currents after ionization in strong circularly polarized laser fields

We apply the time-dependent analytical R-matrix theory to develop a movie of hole motion in a Kr atom upon ionization by strong circularly polarized field. We find rich hole dynamics, ranging from rotation to swinging motion. The motion of the hole depends on the final energy and the spin of the photoelectron and can be controlled by the laser frequency and intensity. Crucially, hole rotation is a purely non-adiabatic effect, completely missing in the framework of quasistatic (adiabatic) tunneling theories. We explore the possibility to use hole rotation as a clock for measuring ionization time. Analyzing the relationship between the relative phases in different ionization channels we show that in the case of short-range electron-core interaction the hole is always initially aligned along the instantaneous direction of the laser field, signifying zero delays in ionization. Finally, we show that strong-field ionization in circular fields creates spin currents (i.e. different flow of spin-up and spin-down density in space) in the ions. This phenomenon is intimately related to the production of spin-polarized electrons in strong laser fields Barth and Smirnova (2013 Phys. Rev. A 88 013401). We demonstrate that rich spin dynamics of electrons and holes produced during strong field ionization can occur in typical experimental conditions and does not require relativistic intensities or strong magnetic fields.

Two-colour spin noise spectroscopy and fluctuation correlations reveal homogeneous linewidths within quantum-dot ensembles.

'Spin noise spectroscopy' is an optical technique for probing electron and hole spin dynamics that is based on detecting their intrinsic fluctuations while in thermal equilibrium. Here we show that fluctuation correlations can be further exploited in multi-probe noise studies to reveal information that in general cannot be accessed by conventional linear optical spectroscopy, such as the underlying homogeneous linewidths of individual constituents within inhomogeneously broadened systems. This is demonstrated in singly charged (In,Ga)As quantum-dot ensembles using two weak probe lasers: When the lasers have similar wavelengths, they probe the same quantum dots in the ensemble and show correlated spin fluctuations. In contrast, mutually detuned probe lasers measure different subsets of quantum dots, giving uncorrelated fluctuations. The noise correlation versus laser detuning directly reveals the quantum dot homogeneous linewidth even in the presence of a strong inhomogeneous broadening. Such noise-based correlation techniques are not limited to semiconductor spin systems, but are applicable to any system with measurable intrinsic fluctuations.

Strong hyperfine-induced modulation of an optically driven hole spin in an InAs quantum dot

Compared to electrons, holes in InAs quantum dots have a significantly weaker hyperfine interaction that leads to less dephasing from nuclear spins. Thus many recent studies have suggested that nuclear spins are unimportant for hole spin dynamics compared to electric field fluctuations. We show that the hole hyperfine interaction can have a strong effect on hole spin coherence measurements through a nuclear feedback effect. The nuclear polarization is generated through a unique process that is dependent on the anisotropy of the hole hyperfine interaction and the coherent precession of nuclear spins, giving rise to strong modulation at the nuclear precession frequency.

Hole spin dynamics and valence‐band spin excitations in two‐dimensional hole systems

AbstractIn recent years, the spin dynamics and spin–orbit interaction in GaAs‐based two‐dimensional hole systems (2DHS) have created a lot of attention. This is due to the complex structure of the valence band, with its p‐like character, which leads to strong spin–orbit coupling. In this paper, we review our recent studies on hole spin dynamics and valence‐band spin excitations in GaAs‐based, p‐modulation‐doped quantum wells (QWs). In 2DHS with low carrier concentration, we demonstrate that maximizing the heavy‐hole–light‐hole band splitting by changing the QW width leads to long hole spin dephasing times at low temperatures. Different mechanisms for initializing a resident hole spin polarization by optical excitation are presented. To accurately determine hole spin dynamics parameters, the resonant spin amplification technique is utilized. The strong anisotropy of the hole g factor, and electrical g factor control are investigated, using this technique. In highly doped 2DHS, we use resonant inelastic light scattering (RILS) to study the spin splitting of the valence band. We observe a low‐energy spin‐density excitation (SDE), which is a measure of the spin splitting of the hole ground state. By varying the laser energy in the RILS experiment, we can resonantly probe the k dependence of the spin splitting. The spectral shape of the SDE depends on the orientation of the light polarizations relative to the crystal axes and reflects the in‐plane anisotropy of the valence‐band spin splitting.

Spin dynamics inp-doped semiconductor nanostructures subject to a magnetic field tilted from the Voigt geometry

We develop a theoretical description of the spin dynamics of resident holes in a p-doped semiconductor quantum well (QW) subject to a magnetic field tilted from the Voigt geometry. We find the expressions for the signals measured in time-resolved Faraday rotation (TRFR) and resonant spin amplification (RSA) experiments and study their behavior for a range of system parameters. We find that an inversion of the RSA peaks can occur for long hole spin dephasing times and tilted magnetic fields. We verify the validity of our theoretical findings by performing a series of TRFR and RSA experiments on a p-modulation doped GaAs/Al_{0.3}Ga_{0.7}As single QW and showing that our model can reproduce experimentally observed signals.

Spin-Echo Dynamics of a Heavy Hole in a Quantum Dot

We develop a theory for the spin-echo dynamics of a heavy hole in a quantum dot, accounting for both hyperfine- and electric-field-induced fluctuations. We show that a moderate applied magnetic field can drive this system to a motional-averaging regime, making the hyperfine interaction ineffective as a decoherence source. Furthermore, we show that decay of the spin-echo envelope is highly sensitive to the geometry. In particular, we find a specific choice of initialization and π-pulse axes which can be used to study intrinsic hyperfine-induced hole-spin dynamics, even in systems with substantial electric-field-induced dephasing. These results point the way to designed hole-spin qubits as a robust and long-lived alternative to electron spins.