We report on the experimental evidence for a nanosecond time-scale spin memory based on nonradiative excitons. The effect manifests itself in magnetic-field-induced oscillations of the energy of the optically active (radiative) excitons. The oscillations detected by a spectrally-resolved pump-probe technique applied to a GaAs/AlGaAs quantum well structure in a transverse magnetic field persist over a time scale, which is orders of magnitude longer than the characteristic decoherence time in the system. The effect is attributed to the spin-dependent electron-electron exchange interaction of the optically active and inactive excitons. The spin relaxation time of the electrons belonging to nonradiative excitons appears to be much longer than the hole spin relaxation time.
We present a study of even parity Rydberg exciton states in cuprous oxide using time-resolved second harmonic generation (SHG). Excitonic states with principal quantum number n = 5 - 12 were excited by nanosecond pulses around 1143 nm. Using time-resolved single-photon counting, the coherently generated second harmonic was isolated both temporally and spectroscopically from inelastic emission due to lower-lying free and bound excitonic states, which included narrow resonances at 1.99 eV associated with an exceptional lifetime of 641 $\pm$ 7 $μ$s. The near transform-limited excitation bandwidth…
Excitonic properties of Ge$_2$H$_2$ and Sn$_2$H$_2$, also known as Xanes, are investigated within the effective mass model. A perpendicularly applied magnetic field induces a negative shift on the exciton center-of-mass kinetic energy that is approximately quadratic with its momentum, thus pushing down the exciton dispersion curve and flattening it. This can be interpreted as an increase in the effective mass of the magneto-exciton, tunable by the field intensity. Our results show that in low effective mass two-dimensional semiconductors, such as Xanes, the applied magnetic field allows one to…
The recent accessibility of high quality, charge neutral monolayer transition metal dichalcogenides with narrow exciton linewidths at the homogeneous limit provides an ideal platform to study excitonic many-body interactions. In particular, the possibility to manipulate coherent exciton-exciton interactions, which govern the ultrafast nonlinear optical response, by applying an external magnetic field has not been considered so far. We address this discrepancy by presenting a nonlinear microscopic theory in the coherent limit for optical excitations in the presence of out-of-plane, in-plane, an…
Distinct Magneto-Optical Response of Frenkel and Wannier Excitons in CrSBr
Wroclaw University of Science and Technology（弗罗茨瓦夫科技大学）；Laboratoire National des Champs Magnétiques Intenses, EMFL, CNRS UPR 3228, Université Grenoble Alpes, Université Toulouse, Université Toulouse 3, INSA-T（强磁场国家实验室）；King’s College London（伦敦国王学院）；University of Chemistry and Technology Prague（布拉格化工大学）
An anomalous magneto-optical spectrum is discovered for dipolar valley excitons in twisted double layer transition metal dichalcogenides (TMD), where in-plane magnetic field induces a sizable multiplet splitting of exciton states inside the light cone. Chiral dispersions of the split branches make possible efficient optical injection of unidirectional exciton current. We also find an analog effect with a modest heterostrain replacing the magnetic field for introducing large splitting and chiral dispersions in the light cone. Angular orientation of photo-injected exciton flow can be controlled …
In this paper we develop the excitonic theory of Kerr rotation angle in a two-dimensional (2D) transition metal dichalcogenide at zero magnetic field. The finite Kerr angle is induced by the interplay between spin-orbit splitting and proximity exchange coupling due to the presence of a ferromagnet. We compare the excitonic effect with the single particle theory approach. We show that the excitonic properties of the 2D material lead to a dramatic change in the frequency dependence of the optical response function. We also find that the excitonic corrections enhance the optical response by a fac…
Excitons in diluted magnetic semiconductors represent excellent probes for studying the magnetic properties of these materials. Various magneto-optical effects, which depend sensitively on the exchange interaction of the excitons with the localized spins of the magnetic ions can be used for probing. Here, we study core/shell CdSe/(Cd,Mn)S colloidal nanoplatelets hosting diluted magnetic semiconductor layers. The inclusion of the magnetic Mn$^{2+}$ ions is evidenced by three magneto-optical techniques using high magnetic fields up to 15 T: polarized photoluminescence, optically detected magneti…
Magnetic tunnel junctions operating in the superparamagnetic regime are promising devices in the field of probabilistic computing, which is suitable for applications like high-dimensional optimization or sampling problems. Further, random number generation is of interest in the field of cryptography. For such applications, a device's uncorrelated fluctuation time-scale can determine the effective system speed. It has been theoretically proposed that a magnetic tunnel junction designed to have only easy-plane anisotropy provides fluctuation rates determined by its easy-plane anisotropy field, a…
Excitons and their constituent charge carriers play the central role in electroluminescence mechanisms determining the ultimate performance of organic optoelectronic devices. The involved processes and their dynamics are often studied with time-resolved techniques limited by spatial averaging that obscures the properties of individual electron-hole pairs. Here we overcome this limit and characterize single charge and exciton dynamics at the nanoscale by using time-resolved scanning tunnelling microscopy-induced luminescence (TR-STML) stimulated with nanosecond voltage pulses. We use isolated d…
We investigate theoretically the magnetoplasmon (cyclotron) resonance in a hybrid system consisting of spatially separated two-dimensional layers of electron and dipolar exciton gases coupled via the Coulomb forces. We study the dynamics of this system under the action of weak alternating external electromagnetic field in the presence of uniform magnetic field, perpendicular to the layers. We reveal that the electromagnetic power absorption exhibits a double-resonance spectrum. We show that the first resonance is associated with the conventional well-studied magnetoplasmon excitations of the e…
Magnetic tuning of the bound exciton states and corresponding giant Zeeman splitting (GZS) between σ^{+} and σ^{-} excitonic transitions in CdTe/Cd_{1-x}Mn_{x}Te quantum ring has been investigated in the Faraday configuration for various concentrations of Mn^{2+} ions, using the variational technique in the effective mass approximation. The sp-d exchange interaction between the localized magnetic impurity ions and the delocalized charge carriers has been accounted via mean-field theory with the inclusion of a modified Brillouin function. The enhancement of the GZS, and in turn, the effective g…
Detailed theoretical study of the magneto-optical properties of weakly confining GaAs/AlGaAs quantum dots is provided. We focus on the diamagnetic coefficient and the $g$-factor of the neutral and the charged excitonic states, respectively, and their evolution with various dot sizes for the magnetic fields applied along $[001]$ direction. For the calculations we utilize the combination of ${\bf k}\cdot{\bf p}$ and the configuration interaction methods. We decompose the theory into four levels of precision,~i.e., (i) single-particle electron and hole states, (ii) non-interacting electron-hole p…
We report on the experimental and theoretical investigation of magnetic-field-induced second harmonic generation (SHG) and two-photon absorption (TPA) of excited exciton states ($n \geq 3$) of the yellow series in Cu$_2$O. In this centrosymmetric material, SHG can occur due to constructive interplay of electric dipole and electric quadrupole/magnetic dipole transitions for light propagating along the low-symmetry directions [111] or [112]. By application of a magnetic field in Voigt configuration, SHG gets also allowed for excitation along the [110]-axis and even the high-symmetry cubic direct…
Monolayer transition metal dichalcogenides host a variety of optically excited quasiparticles species that stem from two-dimensional confinement combined with relatively large carrier effective masses and reduced dielectric screening. The magnetic response of these quasiparticles gives information on their spin and valley configurations, nuanced carrier interactions, and insight into the underlying band structure. Recently, there have been several reports of 2$s$/3$s$ charged excitons in TMDs, but very little is still known about their response to external magnetic fields. Using photoluminesce…
The results of magneto-optical spectroscopy investigations of excitons in a CVD grown monolayer of WSe2 encapsulated in hexagonal boron nitride are presented. The emission linewidth for the 1s state is of 4:7 meV, close to the narrowest emissions observed in monolayers exfoliated from bulk material. The 2s excitonic state is also observed at higher energies in the photoluminescence spectrum. Magneto-optical spectroscopy allows for the determination of the g-factors and of the spatial extent of the excitonic wave functions associated with these emissions. Our work establishes CVD grown monolaye…
The magneto-optical response of monolayer transition metal dichalcogenides (TMDs), including excitonic effects, is studied using a nanoribbon geometry. We compute the diagonal optical conductivity and the Hall conductivity. Comparing the excitonic optical Hall conductivity to results obtained in the independent particle approximation, we find an increase in the amplitude corresponding to one order of magnitude when excitonic effects are included. The Hall conductivities are used to calculate Faraday rotation spectra for MoS2 and WSe2. Finally, we have also calculated the diamagnetic shift of t…
