Time-resolved Kerr Rotation Measurements Research Articles

Gate-controlled spin relaxation in bulk WSe2 flakes

We have studied the spin relaxation dynamics in both n- and p-type layered bulk WSe2 under a perpendicular electric field by employing time-resolved Kerr rotation and helicity-resolved transient reflection measurements. The experimental results reveal the efficient tuning of spin relaxation time from 3 ps to 46 ps by the external electric field at 10 K. The dependence of spin relaxation time on the external electric field is understood based on active interlayer hopping. These studies demonstrate the gate-tunable spin polarization and relaxation in bulk transition metal dichalcogenides (TMDCs), which are fundamentally important for understanding spin dynamics and the practical design of spintronic devices based on bulk TMDCs.

Unveiling Valley Lifetimes of Free Charge Carriers in Monolayer WSe2.

We report on nanosecond-long, gate-dependent valley lifetimes of free charge carriers in monolayer WSe2, unambiguously identified by the combination of time-resolved Kerr rotation and electrical transport measurements. While the valley polarization increases when tuning the Fermi level into the conduction or valence band, there is a strong decrease of the respective valley lifetime consistent with both electron-phonon and spin-orbit scattering. The longest lifetimes are seen for spin-polarized bound excitons in the band gap region. We explain our findings via two distinct, Fermi-level-dependent scattering channels of optically excited, valley-polarized bright trions either via dark or bound states. By electrostatic gating we demonstrate that the transition-metal dichalcogenide WSe2 can be tuned to be either an ideal host for long-lived localized spin states or allow for nanosecond valley lifetimes of free charge carriers (>10 ns).

Acceleration of the precession frequency for optically-oriented electron spins in ferromagnetic/semiconductor hybrids

Time-resolved Kerr rotation measurements were performed in InGaAs/GaAs quantum wells nearby a doped Mn delta layer. Our magneto-optical results show a typical time evolution of the optically-oriented electron spin in the quantum well. Surprisingly, this is strongly affected by the Mn spins, resulting in an increase of the spin precession frequency in time. This increase is attributed to the variation in the effective magnetic field induced by the dynamical relaxation of the Mn spins. Two processes are observed during electron spin precession: a quasi-instantaneous alignment of the Mn spins with photo-excited holes, followed by a slow alignment of Mn spins with the external transverse magnetic field. The first process leads to an equilibrium state imprinted in the initial precession frequency, which depends on pump power, while the second process promotes a linear frequency increase, with acceleration depending on temperature and external magnetic field. This observation yields new information about exchange process dynamics and on the possibility of constructing spin memories, which can rapidly respond to light while retaining information for a longer period.

Spin States Protected from Intrinsic Electron-Phonon Coupling Reaching 100 ns Lifetime at Room Temperature in MoSe2.

We present time-resolved Kerr rotation measurements, showing spin lifetimes of over 100 ns at room temperature in monolayer MoSe2. These long lifetimes are accompanied by an intriguing temperature-dependence of the Kerr amplitude, which increases with temperature up to 50 K and then abruptly switches sign. Using ab initio simulations, we explain the latter behavior in terms of the intrinsic electron-phonon coupling and the activation of transitions to secondary valleys. The phonon-assisted scattering of the photoexcited electron-hole pairs prepares a valley spin polarization within the first few ps after laser excitation. The sign of the total valley magnetization, and thus the Kerr amplitude, switches as a function of temperature, as conduction and valence band states exhibit different phonon-mediated intervalley scattering rates. However, the electron-phonon scattering on the ps time scale does not provide an explanation for the long spin lifetimes. Hence, we deduce that the initial spin polarization must be transferred into spin states, which are protected from the intrinsic electron-phonon coupling, and are most likely resident charge carriers, which are not part of the itinerant valence or conduction band states.

Optical control of spin-polarized photocurrent in topological insulator thin films

Dirac electrons in topological insulators (TIs) provide one possible avenue to achieve control of photocurrents and spin currents without the need to apply external fields by utilizing characteristic spin-momentum locking. However, for TI crystals with electrodes it is actually difficult to characterize the net flow of spin-polarized photocurrents because of the coexistence of surface carriers and bulk carriers generated by optical excitations. We demonstrate here that the net flow directions of spin-polarized photocurrents in TI polycrystalline thin films without electrodes can be precisely and intentionally controlled by the polarization of the excitation pulse alone, which is characterized by performing time-domain terahertz (THz) wave measurements and time-resolved magneto-optical Kerr rotation measurements that are non-contact methods. We show that the amplitudes of s-polarized THz waves radiated from photocurrents under right- and left-circularly polarized excitations are inverted relative to one another. Moreover, we observe the inversion of time-resolved magneto-optical Kerr rotation signals between the two excitations. Our results will open the way as innovative methods to control spin-polarized electrons in optoelectronic and spintronic TI devices without the need to apply external fields.

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 in Ferromagnet/10-nm-Thick N-Type GaAs Quantum Well Junctions

Spin dynamics in several different types of ferromagnetic metal (FM)/10-nm-thick n-type GaAs quantum well (QW) junctions is studied by means of time-resolved Kerr rotation measurements. Compared with the MnGa/in-situ doped 10-nm-thick n-type GaAs QW junction, the spin lifetime of the MnGa/modulation-doped 10-nm-thick n-type GaAs QW junction is shorter by a factor of 5, consistent with the D’yakonov–Perel’ spin relaxation mechanism. Meanwhile, compared with the spin lifetime of the MnAs/in-situ doped 10-nm-thick n-type GaAs QW junction, the MnGa/in-situ doped 10-nm-thick n-type GaAs QW junction is of a spin lifetime longer by a factor of 4.2. The later observation is well explained by the Rashba effect in the presence of structure inversion asymmetry, which acts directly on photo-excited electron spins. We demonstrate that MnGa-like FM/in-situ doped 10-nm-thick n-type GaAs QW junctions, which possess relatively low interfacial potential barriers, are able to provide long spin lifetimes.

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.

Temporal and spatial valley dynamics in two-dimensional semiconductors probed via Kerr rotation

Monolayer transition metal dichalcogenides (TMDCs) offer a tantalizing platform for control of both spin and valley degrees of freedom, which may enable future optoelectronic devices with enhanced and novel functionalities. Here, we investigate the valley dynamics of two prototypical members of TMDCs, namely $\mathrm{Mo}{\mathrm{S}}_{2}$ and $\mathrm{WS}{\mathrm{e}}_{2}$, using time-resolved Kerr rotation (TRKR) at temperatures from 10 K to 300 K. This pump-probe technique enables sub-picosecond temporal resolution, providing insight into ultrafast valley dynamics, which is inaccessible by polarized and time-resolved photoluminescence spectroscopy. Bi-exponential decay dynamics were observed for both materials at low temperatures, and the fast decay component indicated a rapid exciton valley depolarization time $(l10\phantom{\rule{0.16em}{0ex}}\mathrm{ps})$ due to strong Coulomb exchange interactions between the $K$ valleys. However, the slow decay components (several tens of picoseconds) were attributed to different origins in the two materials, which were further elucidated by temperature-dependent TRKR measurements. Moreover, the spatial dependence of the TRKR intensity across $\mathrm{Mo}{\mathrm{S}}_{2}$ monolayer flakes indicated a weaker valley polarization near the edges, which is likely associated with quenched excitons near the grain boundaries or a disordered edge region in chemical vapor deposition--grown monolayers. These temporal and spatial TRKR measurements reveal insight into the complex dynamics of valley excitonic states, which will be critical for valleytronic applications of monolayer TMDCs.

Long-Lived Hole Spin/Valley Polarization Probed by Kerr Rotation in Monolayer WSe2.

Time-resolved Kerr rotation and photoluminescence measurements are performed on MOCVD-grown monolayer tungsten diselenide (WSe2). We observe a surprisingly long-lived Kerr rotation signal (∼80 ns) at 10 K, which is attributed to spin/valley polarization of the resident holes. This polarization is robust to transverse magnetic field (up to 0.3 T). Wavelength-dependent measurements reveal that only excitation near the free exciton energy generates this long-lived spin/valley polarization.

Anisotropic spin dephasing of impurity-bound electron spins in ZnO

We investigate the electron spin dynamics of n-type c-axis oriented bulk zinc oxide (ZnO) by using time-resolved Kerr rotation and resonant spin amplification measurements. Calculating resonant spin amplification using an anisotropic spin dephasing model reveals that there are two species involved in the spin dynamics, which we attribute to conduction and impurity-bound electron spins, respectively. We find that the impurity-bound electron spin dephasing mechanism is strongly anisotropic due to anisotropic exchange interactions. The identification of the two spin species and their dephasing mechanisms is further supported by the temperature, power, and wavelength dependence of the spin coherence measurements.

Electron-nuclei spin coupling in GaAs—Free versus localized electrons

We report on an experimental evidence of a significantly different dynamic nuclear polarization (DNP) for localized and itinerant electrons in n-GaAs. Optically injected spin-polarized electrons are used to generate dynamic nuclear polarization via electron-nucleus hyperfine interaction. Using time resolved Kerr rotation measurements for probing the transient Overhauser field, the DNP time constants for itinerant and localized electrons are extracted to be 10 min and less than 1 min, respectively. This is attributed to a rapid DNP occurring in the vicinity of the donors followed by a delayed nuclear spin polarization in between the donor sites.

Comparison of measurement techniques for electron spin relaxation time in a GaAs/AlGaAs multiple quantum well

We compared the performance of three measurement techniques for electron spin relaxation time, i.e., polarization- and time-resolved photoluminescence (PTRPL) measurement, time-resolved reflectance (TRR) measurement, and time-resolved Kerr rotation measurement. With all three techniques similar electron spin relaxation times (0.83–1.2ns) were obtained in a (110) GaAs/AlGaAs multiple quantum well with excitation wavelengths near the heavy-hole exciton resonance at 77K. We extracted the spin-independent contribution of the Coulomb interaction which obscures TRR signals as an offset without limiting the excitation wavelength to heavy-hole exciton resonance, using the degree of electron spin polarization simultaneously obtained by the PTRPL measurement. It was found that the Coulomb interaction contribution is dominant in TRR signals over both heavy- and light-hole exciton resonances.

Coherence of an electron spin in quantum dots generated by a resonant optical pulse with elliptic polarization

We have experimentally observed the spin polarization process of single electrons in InP/InGaP quantum dots by time-resolved Kerr rotation measurements. It is found that the inversion of the spin polarization direction occurs with the variation of the intensity of the optical pulse. The spin coherence lifetime abruptly changes on the occurrence of the inversion. We have reproduced the inversion in numerical simulations using the density operator of the electron–trion four-level system, assuming a small deviation of the optical pulse from circular polarization. The change of the spin lifetime is attributed to the qualitative change of the four-level system in the electric polarization state.

Coherent heteroepitaxy of Bi2Se3 on GaAs (111)B

We report the heteroepitaxy of single crystal thin films of Bi2Se3 on the (111)B surface of GaAs by molecular beam epitaxy. We find that Bi2Se3 grows highly c-axis oriented, with an atomically sharp interface with the GaAs substrate. By optimizing the growth of a very thin GaAs buffer layer before growing the Bi2Se3, we demonstrate the growth of thin films with atomically flat terraces over hundreds of nanometers. Initial time-resolved Kerr rotation measurements herald opportunities for probing coherent spin dynamics at the interface between a candidate topological insulator and a large class of GaAs-based heterostructures.

Ultrafast Kerr rotations and zero-field dephasing time of electron spins in InAs/GaAs quantum disks

Time-resolved Kerr rotation (TRKR) measurements based on pump-probe arrangement were carried out at 5 K on the monolayer fluctuation induced InAs/GaAs quantum disks grown on GaAs substrate without external magnetic field. The lineshape of TRKR signals shows an unusual dependence on the excitation wavelength, especially antisymmetric step-shaped structures appearing when the excitation wavelength was resonantly scanned over the heavy- and light-hole subbands. Moreover, these step structures possess an almost identical decay time of ∼ 40 ps which is believed to be the characteristic spin dephasing time of electrons in the extremely narrow InAs/GaAs quantum disks.

Skyrmion Effect on the Relaxation of Spin Waves in a Quantum Hall Ferromagnet

Spin relaxation of two-dimensional electrons in a GaAs/AlGaAs quantum well was studied by time-resolved Kerr rotation measurements using a two-color pump and probe technique. In quantum Hall ferromagnets, the spin-wave relaxation is strongly influenced by the photogenerated Skyrmion and anti-Skyrmion pairs. By tuning the pump and probe lights to the lowest optical transition, an intrinsic filling factor dependence of spin relaxation is obtained without photogeneration of Skyrmions. The relaxation time of the spin wave presents a sharp peak at odd filling factors, accompanied by dips on both sides of it. The peculiar filling factor dependence of the spin-wave relaxation around quantum Hall ferromagnets can be explained by the interaction between the spin wave and Skyrmion. Observation of a similar feature around ν=1, 3, and 5 may suggest the existence of Skyrmions around higher odd filling factors.

Gate voltage dependence of nuclear spin relaxation in an impurity-doped semiconductor quantum well

We investigated the gate voltage dependence of the nuclear spin relaxation in a Schottky-gated n-GaAs/AlGaAs (110) quantum well by the time-resolved Kerr rotation measurement combined with the nuclear magnetic resonance technique. The Fermi contact hyperfine interaction is enhanced by decreasing the background electron density, as the electrons become localized at impurity site. The energy relaxation time T1 and the decay time of the Rabi oscillation T2Rabi can be controlled by more than a factor of 10 and a factor of ∼2, respectively.

Anisotropic electron spin relaxation in bulk GaN

Electron spin dynamics in n-type c-oriented wurtzite GaN epilayers is studied by time-resolved Kerr-rotation measurements at T=80 K. The electron spin lifetime shows a sudden increase if an external magnetic field is applied in the sample plane. This enhancement is explained by anisotropic Dyakonov–Perel spin relaxation in bulk GaN as a direct consequence of the anisotropy of spin-orbit coupling in semiconductors with wurtzite structure.

Spin dynamics of electrons in the first excited subband of a high-mobility low-density two-dimensional electron system

We report on time-resolved Kerr rotation measurements of spin coherence of electrons in the first excited subband of a high-mobility low-density two-dimensional electron system in a GaAs/Al0.35Ga0.65As heterostructure. While the transverse spin lifetime (T2*) of electrons decreases monotonically with increasing magnetic field, it has a non-monotonic dependence on the temperature, with a peak value of 596 ps at 36 K, indicating the effect of inter-subband electron-electron scattering on the electron spin relaxation. The spin lifetime may be long enough for potential device application with electrons in excited subbands.