Ultrafast magnetoacoustics in Galfenol nanostructures.

Phonons and magnons are prospective information carriers to substitute the transfer of charge in nanoscale communication devices. Our ability to manipulate them at the nanoscale and with ultimate speed is examined by ultrafast acoustics and femtosecond optomagnetism, which use ultrashort laser pulses for generation and detection of the corresponding coherent excitations. Ultrafast magnetoacoustics merges these research directions and focuses on the interaction of optically generated coherent phonons and magnons. In this review, we present ultrafast magnetoacoustic experiments with nanostructures based on the alloy (Fe,Ga) known as Galfenol. We demonstrate how broad we can manipulate the magnetic response on an optical excitation by controlling the spectrum of generated coherent phonons and their interaction with magnons. Resonant phonon pumping of magnons, formation of magnon polarons, driving of a magnetization wave by a guided phonon wavepacket are demonstrated. The presented experimental results have great application potential in emerging areas of modern nanoelectronics.

The squeezed dark nuclear spin state in lead halide perovskites.

Coherent many-body states are highly promising for robust quantum information processing. While far-reaching theoretical predictions have been made for various implementations, direct experimental evidence of their appealing properties can be challenging. Here, we demonstrate optical manipulation of the nuclear spin ensemble in the lead halide perovskite semiconductor FAPbBr3 (FA = formamidinium), targeting a long-postulated collective dark state that is insensitive to optical pumping after its build-up. Via optical orientation of localized hole spins we drive the nuclear many-body system into this entangled state, requiring a weak magnetic field of only a few milli-Tesla strength at cryogenic temperatures. During its fast establishment, the nuclear polarization along the optical axis remains small, while the transverse nuclear spin fluctuations are strongly reduced, corresponding to spin squeezing as evidenced by a strong violation of the generalized nuclear squeezing-inequality with ξs < 0.5. The dark state corresponds to an ~35-body entanglement between the nuclei. Dark nuclear spin states can be exploited to store quantum information benefiting from their long-lived many-body coherence and to perform quantum measurements with a precision beyond the standard limit.

Universal magnetic proximity effect in ferromagnet-semiconductor quantum well hybrid structures.

Hybrid ferromagnet-semiconductor systems possess new outstanding properties, which emerge when bringing magnetic and semiconductor materials into contact. In such structures, the long-range magnetic proximity effect couples the spin systems of the ferromagnet and semiconductor on distances exceeding the carrier wave function overlap. The effect is due to the effective p-d exchange interaction of acceptor-bound holes in the quantum well with d-electrons of the ferromagnet. This indirect interaction is established via the phononic Stark effect mediated by the chiral phonons. Here, we demonstrate that the long-range magnetic proximity effect is universal and observed in hybrid structures with diverse magnetic components and potential barriers of various thicknesses and compositions. We study hybrid structures consisting of a semimetal (magnetite Fe3O4) or dielectric (spinel NiFe2O4) ferromagnet and a CdTe quantum well separated by a nonmagnetic (Cd,Mg)Te barrier. The proximity effect is manifested in the circular polarization of the photoluminescence corresponding to the recombination of photoexcited electrons with holes bound to shallow acceptors in the quantum well induced by magnetite or spinel itself, in contrast to interface ferromagnet in case of metal-based hybrid systems. A nontrivial dynamics of the proximity effect is observed in the studied structures due to recombination-induced dynamic polarization of electrons in the quantum well. It enables the determination of the exchange constant Δexch ≈ 70 µeV in a magnetite-based structure. The universal origin of the long-range exchange interaction along with the possibility of its electrical control offers prospects for the development of low-voltage spintronic devices compatible with existing solid-state electronics.

Optical Orientation of Excitons in a Longitudinal Magnetic Field in Indirect-Band-Gap (In,Al)As/AlAs Quantum Dots with Type-I Band Alignment.

Exciton recombination and spin dynamics in (In,Al)As/AlAs quantum dots (QDs) with indirect band gap and type-I band alignment were studied. The negligible (less than 0.2 µeV) value of the anisotropic exchange interaction in these QDs prevents the mixing of the excitonic basis states and makes the formation of spin-polarized bright excitons possible under quasi-resonant, circularly polarized excitation. The recombination and spin dynamics of excitons are controlled by the hyperfine interaction between the electron and nuclear spins. A QD blockade by dark excitons was observed in the magnetic field, that eliminates the impact of nuclear spin fluctuations. A kinetic model which accounts for the population dynamics of the bright and dark exciton states as well as for the spin dynamics was developed to quantitatively describe the experimental data.

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 [Formula: see text] 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 [Formula: see text] 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.

The Landé factors of electrons and holes in lead halide perovskites: universal dependence on the band gap.

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 (MAPbI3, MAPb(Br0.5Cl0.5)3, MAPb(Br0.05Cl0.95)3, FAPbBr3, FA0.9Cs0.1PbI2.8Br0.2, MA=methylammonium and FA=formamidinium) and all-inorganic (CsPbBr3) lead halide perovskites, determined by pump-probe Kerr rotation and spin-flip Raman scattering in magnetic fields up to 10 T at cryogenic temperatures. Further, we use first-principles density functional theory (DFT) calculations in combination with tight-binding and k ⋅ p approaches to calculate microscopically the Landé factors. The results demonstrate their universal dependence on the band gap energy across the different perovskite material classes, which can be summarized in a universal semi-phenomenological expression, in good agreement with experiment.

Stimulated Resonant Spin Amplification Reveals Millisecond Electron Spin Coherence Time of Rare-Earth Ions in Solids.

The inhomogeneity of an electron spin ensemble as well as fluctuating environment acting upon individual spins drastically shorten the spin coherence time T_{2} and hinder coherent spin manipulation. We show that this problem can be solved by the simultaneous application of a radio frequency (rf) field, which stimulates coherent spin precession decoupled from an inhomogeneous environment, and periodic optical pulses, which amplify this precession. The resulting resonance, taking place when the rf field frequency approaches the laser pulse repetition frequency, has a width determined by the spin coherence time T_{2} that is free from the effects of inhomogeneity and slow nuclear spin fluctuations. We measure a 50-Hz-narrow electron spin resonance and milliseconds-long T_{2} for electrons in the ground state of Ce^{3+} ions in the yttrium aluminum garnet (YAG) lattice at low temperatures, while the inhomogeneous spin dephasing time T_{2}^{*} is only 25 ns. This study paves the way to coherent optical manipulation in spin systems decoupled from their inhomogeneous environment.

Dynamic Polarization of Electron Spins Interacting with Nuclei in Semiconductor Nanostructures.

We suggest a new spin orientation mechanism for localized electrons: dynamic electron spin polarization provided by nuclear spin fluctuations. The detrimental effect of nuclear spin fluctuations can be harnessed and employed to provide angular momentum for the electrons via the hyperfine interaction in a weak magnetic field. For this, the sample is illuminated by an unpolarized light, which directly polarizes neither the electrons nor the nuclei. We predict that, for the electrons bound in localized excitons, 100% spin polarization can be reached in longitudinal magnetic fields of a few millitesla. The proof of principle experiment is performed on momentum-indirect excitons in (In,Al)As/AlAs quantum dots, where in a magnetic field of 17 mT the electron spin polarization of 30% is measured.

Optical detection of electron spin dynamics driven by fast variations of a magnetic field: a simple method to measure [Formula: see text], [Formula: see text], and [Formula: see text] in semiconductors.

We develop a simple method for measuring the electron spin relaxation times [Formula: see text], [Formula: see text] and [Formula: see text] in semiconductors and demonstrate its exemplary application to n-type GaAs. Using an abrupt variation of the magnetic field acting on electron spins, we detect the spin evolution by measuring the Faraday rotation of a short laser pulse. Depending on the magnetic field orientation, this allows us to measure either the longitudinal spin relaxation time [Formula: see text] or the inhomogeneous transverse spin dephasing time [Formula: see text]. In order to determine the homogeneous spin coherence time [Formula: see text], we apply a pulse of an oscillating radiofrequency (rf) field resonant with the Larmor frequency and detect the subsequent decay of the spin precession. The amplitude of the rf-driven spin precession is significantly enhanced upon additional optical pumping along the magnetic field.

Low voltage control of exchange coupling in a ferromagnet-semiconductor quantum well hybrid structure.

Voltage control of ferromagnetism on the nanometer scale is highly appealing for the development of novel electronic devices with low power consumption, high operation speed, reliable reversibility and compatibility with semiconductor technology. Hybrid structures based on the assembly of ferromagnetic and semiconducting building blocks are expected to show magnetic order as a ferromagnet and to be electrically tunable as a semiconductor. Here, we demonstrate the electrical control of the exchange coupling in a hybrid consisting of a ferromagnetic Co layer and a semiconductor CdTe quantum well, separated by a thin non-magnetic (Cd,Mg)Te barrier. The electric field controls the phononic ac Stark effect-the indirect exchange mechanism that is mediated by elliptically polarized phonons emitted from the ferromagnet. The effective magnetic field of the exchange interaction reaches up to 2.5 Tesla and can be turned on and off by application of 1V bias across the heterostructure.

Polarimetry of photon echo on charged and neutral excitons in semiconductor quantum wells.

Coherent optical spectroscopy such as four-wave mixing and photon echo generation deliver rich information on the energy levels involved in optical transitions through the analysis of polarization of the coherent response. In semiconductors, it can be applied to distinguish between different exciton complexes, which is a highly non-trivial problem in optical spectroscopy. We develop a simple approach based on photon echo polarimetry, in which polar plots of the photon echo amplitude are measured as function of the angle φ between the linear polarizations of the two exciting pulses. The rosette-like polar plots reveal a distinct difference between the neutral and charged exciton (trion) optical transitions in semiconductor nanostructures. We demonstrate this experimentally by photon echo polarimetry of a CdTe/(Cd, Mg)Te quantum well. The echoes of the trion and donor-bound exciton are linearly polarized at the angle 2φ with respect to the first pulse polarization and their amplitudes are weakly dependent on φ. While on the exciton the photon echo is co-polarized with the second exciting pulse and its amplitude scales as cosφ.

Discretization of the total magnetic field by the nuclear spin bath in fluorine-doped ZnSe.

The coherent spin dynamics of fluorine donor-bound electrons in ZnSe induced by pulsed optical excitation is studied in a perpendicular applied magnetic field. The Larmor precession frequency serves as a measure for the total magnetic field exerted onto the electron spins and, surprisingly, does not increase linearly with the applied field, but shows a step-like behavior with pronounced plateaus, given by multiples of the laser repetition rate. This discretization occurs by a feedback mechanism in which the electron spins polarize the nuclear spins, which in turn generate a local Overhauser field adjusting the total magnetic field accordingly. Varying the optical excitation power, we can control the plateaus, in agreement with our theoretical model. From this model, we trace the observed discretization to the optically induced Stark field, which causes the dynamic nuclear polarization.

Generation of spin waves by a train of fs-laser pulses: a novel approach for tuning magnon wavelength.

Currently spin waves are considered for computation and data processing as an alternative to charge currents. Generation of spin waves by ultrashort laser pulses provides several important advances with respect to conventional approaches using microwaves. In particular, focused laser spot works as a point source for spin waves and allows for directional control of spin waves and switching between their different types. For further progress in this direction it is important to manipulate with the spectrum of the optically generated spin waves. Here we tackle this problem by launching spin waves by a sequence of femtosecond laser pulses with pulse interval much shorter than the relaxation time of the magnetization oscillations. This leads to the cumulative phenomenon and allows us to generate magnons in a specific narrow range of wavenumbers. The wavelength of spin waves can be tuned from 15 µm to hundreds of microns by sweeping the external magnetic field by only 10 Oe or by slight variation of the pulse repetition rate. Our findings expand the capabilities of the optical spin pump-probe technique and provide a new method for the spin wave generation and control.

Zn-VI quasiparticle gaps and optical spectra from many-body calculations.

The electronic band structures of hexagonal ZnO and cubic ZnS, ZnSe, and ZnTe compounds are determined within hybrid-density-functional theory and quasiparticle calculations. It is found that the band-edge energies calculated on the [Formula: see text] (Zn chalcogenides) or GW (ZnO) level of theory agree well with experiment, while fully self-consistent QSGW calculations are required for the correct description of the Zn 3d bands. The quasiparticle band structures are used to calculate the linear response and second-harmonic-generation (SHG) spectra of the Zn-VI compounds. Excitonic effects in the optical absorption are accounted for within the Bethe-Salpeter approach. The calculated spectra are discussed in the context of previous experimental data and present SHG measurements for ZnO.

Picosecond Control of Quantum Dot Laser Emission by Coherent Phonons.

A picosecond acoustic pulse can be used to control the lasing emission from semiconductor nanostructures by shifting their electronic transitions. When the active medium, here an ensemble of (In,Ga)As quantum dots, is shifted into or out of resonance with the cavity mode, a large enhancement or suppression of the lasing emission can dynamically be achieved. Most interesting, even in the case when gain medium and cavity mode are in resonance, we observe an enhancement of the lasing due to shaking by coherent phonons. In order to understand the interactions of the nonlinearly coupled photon-exciton-phonon subsystems, we develop a semiclassical model and find an excellent agreement between theory and experiment.

Direct Measurements of Magnetic Polarons in Cd1-xMnxSe Nanocrystals from Resonant Photoluminescence.

In semiconductors, quantum confinement can greatly enhance the interaction between band carriers (electrons and holes) and dopant atoms. One manifestation of this enhancement is the increased stability of exciton magnetic polarons in magnetically doped nanostructures. In the limit of very strong 0D confinement that is realized in colloidal semiconductor nanocrystals, a single exciton can exert an effective exchange field Bex on the embedded magnetic dopants that exceeds several tesla. Here we use the very sensitive method of resonant photoluminescence (PL) to directly measure the presence and properties of exciton magnetic polarons in colloidal Cd1-xMnxSe nanocrystals. Despite small Mn2+ concentrations (x = 0.4-1.6%), large polaron binding energies up to ∼26 meV are observed at low temperatures via the substantial Stokes shift between the pump laser and the resonant PL maximum, indicating nearly complete alignment of all Mn2+ spins by Bex. Temperature and magnetic field-dependent studies reveal that Bex ≈ 10 T in these nanocrystals, in good agreement with theoretical estimates. Further, the emission line widths provide direct insight into the statistical fluctuations of the Mn2+ spins. These resonant PL studies provide detailed insight into collective magnetic phenomena, especially in lightly doped nanocrystals where conventional techniques such as nonresonant PL or time-resolved PL provide ambiguous results.

Picosecond acoustics in semiconductor optoelectronic nanostructures.

We overview the results of three recently performed experiments, where the picosecond acoustic technique was applied to semiconductor devices with quantum wells or quantum dots embedded in an optical microcavity. In these experiments, high amplitude picosecond strain pulses are injected into such a device and the resulting changes in the response of the optical resonance are monitored. First, in quantum well devices we observe the generation of THz sidebands in optical reflectivity near the polariton resonance. Second, for certain conditions we detect the destruction and recurrence of excitons by acoustic shock waves on picosecond time scales. Third, in a vertical cavity surface emitting laser with a quantum dot layer the injection of the picosecond strain pulses induces the giant increase of the laser output. All these effects are governed by nonadiabatic processes in the interaction between a strain pulse and the electronic quantum confined states. Their observation became possible due to the possibility of generating very short strain pulses with sufficiently high amplitude.

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.

Lasing from active optomechanical resonators.

Planar microcavities with distributed Bragg reflectors (DBRs) host, besides confined optical modes, also mechanical resonances due to stop bands in the phonon dispersion relation of the DBRs. These resonances have frequencies in the 10- to 100-GHz range, depending on the resonator's optical wavelength, with quality factors exceeding 1,000. The interaction of photons and phonons in such optomechanical systems can be drastically enhanced, opening a new route towards the manipulation of light. Here we implemented active semiconducting layers into the microcavity to obtain a vertical-cavity surface-emitting laser (VCSEL). Thereby, three resonant excitations--photons, phonons and electrons--can interact strongly with each other providing modulation of the VCSEL laser emission: a picosecond strain pulse injected into the VCSEL excites long-living mechanical resonances therein. As a result, modulation of the lasing intensity at frequencies up to 40 GHz is observed. From these findings, prospective applications of active optomechanical resonators integrated into nanophotonic circuits may emerge.

Coherent coupling of excitons and trions in a photoexcited CdTe/CdMgTe quantum well.

We present zero-, one-, and two-quantum two-dimensional coherent spectra of excitons and trions in a CdTe/(Cd,Mg)Te quantum well. The set of spectra provides a unique and comprehensive picture of the coherent nonlinear optical response. Distinct peaks in the spectra are manifestations of exciton-exciton and exciton-trion coherent coupling. Excellent agreement using density matrix calculations highlights the essential role of many-body effects on the coupling. Strong exciton-trion coherent interactions open up the possibility for novel conditional control schemes in coherent optoelectronics.