The band structure of type-I (In,Al)As/AlAs quantum dots with band gap energy exceeding 1.63 eV is indirect in momentum space, leading to long-lived exciton states with potential applications in quantum information. Optical access to these excitons is provided by mixing of the $Γ$- and X-conduction band valleys, from which control of their spin states can be gained. This access is used here for studying the exciton spin-level structure by resonant spin-flip Raman scattering, allowing us to accurately measure the anisotropic hole and isotropic electron $g$ factors. The spin-flip mechanisms for the indirect exciton and its constituents as well as the underlying optical selection rules are determined. The spin-flip intensity is a reliable measure of the strength of $Γ$-X-valley mixing, as evidenced by both experiment and theory.
CdSe colloidal nanoplatelets are studied by spin-flip Raman scattering in magnetic fields up to 5 T. We find pronounced Raman lines shifted from the excitation laser energy by an electron Zeeman splitting. Their polarization selection rules correspond to those expected for scattering mediated by excitons interacting with resident electrons. Surprisingly, Raman signals shifted by twice the electron Zeeman splitting are also observed. The theoretical analysis and experimental dependencies show that the mechanism responsible for the double flip involves two resident electrons interacting with a p…
Spin-flip Raman scattering of electrons and heavy-holes is studied for resonant excitation of neutral and charged excitons in a CdTe/Cd$_{0.63}$Mg$_{0.37}$Te quantum well. The spin-flip scattering is characterized by its dependence on the incident and scattered light polarization as well as on the magnetic field strength and orientation. Model schemes of electric-dipole allowed spin-flip Raman processes in the exciton complexes are compared to the experimental observations, from which we find that lowering of the exciton symmetry, time of carrier spin relaxation, and mixing between electron st…
High-resolution spectral hole burning (SHB) in coherent nondegenerate differential transmission spectroscopy discloses spin-trion dynamics in an ensemble of negatively charged quantum dots. In the Voigt geometry, stimulated Raman spin coherence gives rise to Stokes and anti-Stokes sidebands on top of the trion spectral hole. The prominent feature of an extremely narrow spike at zero detuning arises from spin population pulsation dynamics. These SHB features confirm coherent electron spin dynamics in charged dots, and the linewidths reveal spin spectral diffusion processes.
A theory of electron spin-flip Raman scattering (SFRS) is presented that describes the Raman spectral signals shifted by both single and twice the electron Zeeman energy under nearly resonant excitation of the heavy hole excitons in semiconductor nanoplatelets. We analyze the spin structure of photoexcited intermediate states, derive compound matrix elements of the spin-flip scattering and obtain polarization properties of the one- and two-electron SFRS common for all the intermediate states. We show that, in the resonant scattering process under consideration, the complexes "exciton plus loca…
The class of Ruddlesden-Popper type (PEA)$_2$PbI$_4$ perovskites comprises two-dimensional (2D) structures whose optical properties are determined by excitons with a large binding energy of about 260 meV. It complements the family of other 2D semiconductor materials by having the band structure typical for lead halide perovskites, that can be considered as inverted compared to conventional III-V and II-VI semiconductors. Accordingly, novel spin phenomena can be expected for them. Spin-flip Raman scattering is used here to measure the Zeeman splitting of electrons and holes in a magnetic field …
We report the observation of tens of minor lines of the combinational spin-flip Raman scattering in a CdTe:Mn quantum well by means of the high-resolution optical spectroscopy. Classification of this manifold leads to four characteristic values of energy, that correspond to four different types of pair clusters of Mn ions: the nearest, second, third etc. neighbors. All the four energies show up in a single experiment with a very high precision, providing experimental grounds for a deeper understanding of the d-d exchange interactions in a diluted magnetic semiconductor and demonstrating the ca…
The discovery of 2-dimensional (2D) materials, such as CrI3, that retain magnetic ordering at monolayer thickness has resulted in a surge of research in 2D magnetism from both pure and applied perspectives. Here, we report a magneto-Raman spectroscopy study on multilayered CrI3, focusing on two new features in the spectra which appear at temperatures below the magnetic ordering temperature and were previously assigned to high frequency magnons. We observe a striking evolution of the Raman spectra with increasing magnetic field in which clear, sudden changes in intensities of the modes are attr…
We show theoretically that stimulated spin flip Raman scattering can be used to inject spin currents in doped semiconductors with spin split bands. A pure spin current, where oppositely oriented spins move in opposite directions, can be injected in zincblende crystals and structures. The calculated spin current should be detectable by pump-probe optical spectroscopy and anomalous Hall effect measurement.
We propose a novel acoustic cavity design where we confine a mechanical mode by adiabatically changing the acoustic properties of a GaAs/AlAs superlattice. By means of high resolution Raman scattering measurements, we experimentally demonstrate the presence of a confined acoustic mode at a resonance frequency around 350 GHz. We observe an excellent agreement between the experimental data and numerical simulations based on a photoelastic model. We demonstrate that the spatial profile of the confined mode can be tuned by changing the magnitude of the adiabatic deformation, leading to strong vari…
We present theoretical aspects of spin polarized two dimensional electron gas (SP2DEG) which can be achieved in doped semimagnetic quantum wells. This original model system has been recently studied by magneto Raman scattering experiments has given a new access to spin resolved excitations and spectrum of the SP2DEG. Starting from the Diluted Magnetic Semiconductor (DMS) Hamiltonian in presence of the Coulomb interaction between conduction electrons, we define the conditions to reach such a SP2DEG. The equilibrium state is studied at low temperature; in particular a theory for the degree of sp…
We have measured dispersions of spin-flip waves and spin-flip single-particle excitations of a spin polarized two-dimensional electron gas in a CdMnTe quantum well using resonant Raman scattering. We find the energy of the spin-flip wave to be below the spin-flip single particle excitation continuum, a contradiction to the theory of spin waves in diluted magnetic semiconductors put forth in [Phys. Rev. B 70, 045205 (2004)]. We show that the inclusion of terms accounting for the Coulomb interaction between carriers in the spin wave propagator leads to an agreement with our experimental results.…
Solid state quantum emitters have shown strong potential for applications in quantum information, but spectral inhomogeneity of these emitters poses a significant challenge. We address this issue in a cavity-quantum dot system by demonstrating cavity-stimulated Raman spin flip emission. This process avoids populating the excited state of the emitter and generates a photon that is Raman shifted from the laser and enhanced by the cavity. The emission is spectrally narrow and tunable over a range of at least 125 GHz, which is two orders of magnitude greater than the natural linewidth. We obtain t…
Ramsey interferometry provides a natural way to determine the coherence time of most qubit systems. Recent experiments on quantum dots however, demonstrated that dynamical nuclear spin polarization can strongly influence the measurement process, making it difficult to extract the $T_2^*$ coherence time using optical Ramsey pulses. Here, we demonstrate an alternative method for spin coherence measurement that is based on first-order coherence of photons generated in spin-flip Raman scattering. We show that if a quantum emitter is driven by a weak monochromatic laser, Raman coherence is determin…
Electron dynamics in quantum dots manifests itself in spin-flip spectra through electric dipole spin resonance (EDSR). Near a neutrality point separating two different singlet charged states of a double quantum dot, charge dynamics inside a $2\times2$ singlet manifold can be described by a 1/2-pseudospin. In this region, charge dynamics is highly nonlinear and strongly influenced by flopping its soft pseudospin mode. As a result, the responses to external driving include first and second harmonics of the driving frequency and their Raman satellites shifted by the pseudospin frequency. In EDSR …
The Zeeman-split spin states of a single quantum dot can be used together with its optical trion transitions to form a spin-photon interface between a stationary (the spin) and a flying (the photon) quantum bit. Besides long coherence times of the spin state itself, the limiting decoherence mechanisms of the trion states are of central importance. We investigate here in time-resolved resonance fluorescence the electron and trion dynamics in a single self-assembled quantum dot in an applied magnetic field of up to $B = 10\,$T. The quantum dot is only weakly coupled to an electron reservoir with…
We report on optical orientation of Mn^2+ in bulk GaAs under application of weak longitudinal magnetic field (B <= 100 mT). The manganese spin polarization of 25% is directly evaluated using spin flip Raman scattering spectroscopy. The dynamical polarization of Mn^2+ occurs due to s-d exchange interaction with optically oriented conduction band electrons. Time-resolved photoluminescence uncovers nontrivial electron spin dynamics where the oriented Mn^2+ ions tend to stabilize the electron spin.
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…
Quantum spin fluctuations provide a unique way to study spin dynamics without system perturbation. Here we put forward an optical resonance shift spin noise spectroscopy as a powerful tool to measure the spin noise of various systems from magnetic impurities in solids to free atoms and molecules. The quantum spin fluctuations in these systems can shift the optical resonances by more than the homogeneous linewidth and produce huge Faraday rotation noise. We demonstrate, that the resonance shift spin noise spectroscopy gives access to the high order spin correlators, which contain complete infor…
The spin of an electron in a self-assembled InAs/GaAs quantum dot molecule is optically prepared and measured through the trion triplet states. A longitudinal magnetic field is used to tune two of the trion states into resonance, forming a superposition state through asymmetric spin exchange. As a result, spin-flip Raman transitions can be used for optical spin initialization, while separate trion states enable cycling transitions for non-destructive measurement. With two-laser transmission spectroscopy we demonstrate both operations simultaneously, something not previously accomplished in a s…
We report on the direct measurement of the electron spin splitting and the accompanying nuclear Overhauser (OH) field, and thus the underlying nuclear spin polarization (NSP) and fluctuation bandwidth, in a single InAs quantum dot under resonant excitation conditions with unprecedented spectral resolution. The electron spin splitting is measured directly via resonant spin-flip single photon Raman scattering detected by superconducting nanowires to generate excitation-emission energy maps. The observed two-dimensional maps reveal an OH field that has a non-linear dependence on excitation freque…
Two promising architectures for solid-state quantum information processing are electron spins in semiconductor quantum dots and the collective electromagnetic modes of superconducting circuits. In some aspects, these two platforms are dual to one another: superconducting qubits are more easily coupled but are relatively large among quantum devices $(\sim\mathrm{mm})$, while electrostatically-confined electron spins are spatially compact ($\sim \mathrm{μm}$) but more complex to link. Here we combine beneficial aspects of both platforms in the Andreev spin qubit: the spin degree of freedom of an…
Theory of spin noise in low dimensional systems and bulk semiconductors is reviewed. Spin noise is usually detected by optical means, continuously measuring the rotation angle of the polarization plane of the probe beam passing through the sample. Spin noise spectra yield rich information about the spin properties of the system including, for example, $g$-factors of the charge carriers, spin relaxation times, parameters of the hyperfine interaction, spin-orbit interaction constants, frequencies and widths of the optical resonances. The review describes basic models of spin noise, methods of it…
Photoluminescence spectra of a (001)-Cd0.99Mn0.01Te quantum well were taken with linear-polarization resolution and using an in-plane magnetic field. Because the quantum well contained a two-dimensional electron gas, the spectra consisted of several features. Since the quantum well layer was formed by a diluted magnetic semiconductor, the spectra showed pronounced polarization-dependent transformations when the in-plane magnetic field was applied. In the magnetic field, a 90-degrees rotation of the sample about the surface normal axis resulted in a clearly different spectrum, meaning that the …
In coherent control, electromagnetic vacuum fluctuations usually cause coherence loss through irreversible spontaneous emission. However, since the dissipation via emission is essentially due to correlation of the fluctuations, when emission ends in a superposition of multiple final states, correlation between different pathways may build up if the "which-way" information is not fully resolved (i.e., the emission spectrum is broader than the transition energy range). Such correlation can be exploited for spin-flip control in a $Λ$-type three-level system, which manifests itself as an all-optic…
We address spin properties and spin dynamics of carriers and charged excitons in CdSe/CdS colloidal nanoplatelets with thick shells. Magneto-optical studies are performed by time-resolved and polarization-resolved photoluminescence, spin-flip Raman scattering and picosecond pump-probe Faraday rotation in magnetic fields up to 30 T. We show that at low temperatures the nanoplatelets are negatively charged so that their photoluminescence is dominated by radiative recombination of negatively charged excitons (trions). Electron g-factor of 1.68 is measured and heavy-hole g-factor varying with incr…
We propose a scheme to perform single-shot quantum non-demolition (QND) readout of the spin of an electron trapped in a semiconductor quantum dot (QD). Our proposal relies on the interaction of the QD electron spin with optically excited, quantum well (QW) microcavity exciton-polaritons. The spin-dependent Coulomb exchange interaction between the QD electron and cavity polaritons causes the phase and intensity response of left circularly polarized light to be different to that of the right circularly polarized light, in such a way that the QD electron's spin can be inferred from the response t…
The Landé or $g$-factors of charge carriers are decisive for the spin-dependent phenomena in solids and provide also information about the underlying electronic band structure. We present a comprehensive set of experimental data for values and anisotropies of the electron and hole Landé factors in hybrid organic-inorganic (MAPbI$_3$, MAPb(Br$_{0.5}$Cl$_{0.5}$)$_3$, MAPb(Br$_{0.05}$Cl$_{0.95}$)$_3$, FAPbBr$_3$, FA$_{0.9}$Cs$_{0.1}$PbI$_{2.8}$Br$_{0.2}$) and all-inorganic (CsPbBr$_3$) lead halide perovskites, determined by pump-probe Kerr rotation and spin-flip Raman scattering in magnetic field…
Several logical qubits and quantum gates have been proposed for semiconductor quantum dots controlled by voltages applied to top gates. The different schemes can be difficult to compare meaningfully. Here we develop a theoretical framework to evaluate disparate qubit-gating schemes on an equal footing. We apply the procedure to two types of double-dot qubits: the singlet-triplet (ST) and the semiconducting quantum dot hybrid qubit. We investigate three quantum gates that flip the qubit state: a DC pulsed gate, an AC gate based on logical qubit resonance (LQR), and a gate-like process known as …
Since the well-known PT symmetry has its fundamental significance and implication in physics, where PT denotes the combined operation of space-inversion P and time-reversal T, it is extremely important and intriguing to completely classify exotic PT-invariant topological metals and to physically realize them. Here we, for the first time, establish a rigorous classification of topological metals that are protected by the PT symmetry using KO-theory. As a physically realistic example, a PT-invariant nodal loop (NL) model in a 3D Brillouin zone is constructed, whose topological stability is revea…
