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M. Bayer

Publications and source records attributed to M. Bayer.

At least 19 recordsLinked to original sources

Bragg-enhanced time-domain Brillouin scattering from a propagating acoustic grating

Generation and detection of coherent phonons in semiconductors by femtosecond optical pulses is a powerful tool for high-frequency acoustic control of their electronic properties. Here, we demonstrate a propagating one-dimensional acoustic grating in bulk semiconductors using above-band-gap excitation by a train of laser pulses with high repetition rate of 1 GHz. This approach enables shaping of the coherent acoustic phonon spectrum and leads to a significant enhancement of Brillouin light scattering at selected probe wavelengths in pump-probe configuration. We demonstrate this effect at a cryogenic temperature of 5 K in prototypical semiconductor systems, namely bulk crystalline GaAs and (Cd,Zn)Te, which serve as benchmark materials for the proposed method. The spectral dependence of the time-domain Brillouin light scattering amplitude exhibits resonant peaks at discrete probe wavelengths arising from Bragg reflection of the probe light by the propagating acoustic grating. A 10-30-fold resonant enhancement of the signal amplitude is observed for GaAs and (Cd,Zn)Te, determined by the finite spectral width of the probe pulse. With further spectral narrowing, enhancements of the order ~ 100-150 are expected, set by the number N of strain pulses in the acoustic grating within the sample and ultimately limited by the material parameters and sample thickness.

physics.optics

Scaling laws of electron and hole spin relaxation in indirect band gap (In,Al)As/AlAs quantum dots

We investigate the electron and heavy hole spin dynamics as a function of magnetic field in ensembles of indirect band gap (In,Al)As/AlAs quantum dots (QDs) with type-I band alignment. Employing a comprehensive model that accounts for both the exciton level quartet and the magnetic-field-driven redistribution of excitons between these states via spin relaxation processes, we extract the electron ($\tau_{se}$) and heavy hole ($\tau_{sh}$) spin relaxation times as a function of magnetic field for QDs of varying sizes. Our analysis reveals that both $\tau_{se}(B)$ and $\tau_{sh}(B)$ exhibit power-law scaling behavior, yet the scaling exponents for electrons and heavy holes show markedly different evolution with QD size. For QDs with a diameter of about 9 nm, we find $\tau_{se}(B)\propto B^{-5}$ and $\tau_{sh}(B)\propto B^{-3}$. Remarkably, increasing the QD diameter to about 16 nm results in a drastic change of the scaling laws, with both $\tau_{se}(B)$ and $\tau_{sh}(B)$ following a $\propto B^{-9}$ dependence. We discuss the underlying mechanisms responsible for this size-dependent transformation of the magnetic field scaling behavior of carrier spin relaxation.

cond-mat.mes-hall

Structural phase transitions in double perovskite crystals studied by Brillouin light scattering

Inorganic lead-free double perovskites represent particular interest as non-toxic and stable material platform for optoelectronic applications. Here, we employ Brillouin light scattering spectroscopy to investigate the elastic properties and structural phase transitions in single crystals of Cs2AgBiBr6 and Cs2AgBiCl6. A complete set of elastic constants is determined from the Brillouin scattering measurements performed along three different crystallographic directions. Both materials exhibit similar elastic constants and weak elastic anisotropy in the cubic phase. At low temperatures, the lifting of degeneracy of transverse acoustic phonon modes is attributed to a lowering of crystal symmetry. From the temperature dependence of the acoustic phonon frequencies, we determine the structural phase transition temperature of about 43 K for Cs2AgBiCl6, compared to 122 K for the cubic-to-tetragonal phase transition in Cs2AgBiBr6.

cond-mat.mtrl-sci

Spin dynamics of excitons and carriers in mixed-cation MA$_{x}$FA$_{1-x}$PbI$_{3}$ perovskite crystals: alloy fluctuations probed by optical orientation

Optical spin orientation measured by time-resolved photoluminescence provides a powerful tool to probe the spin dynamics of excitons and charge carriers in perovskite semiconductors. The impact of alloy fluctuations on the spin dynamics of mixed-cation \MAFAPI{} perovskite single crystals is studied here experimentally. The optical orientation is measured under nonresonant excitation for crystals with $x = 0.1$, $0.4$, and $0.8$ at cryogenic temperatures and compared with data on \MAPI{} crystals. The high degree of exciton optical orientation of $75-80$\% for $x = 0.1$ and $0.8$ reduces to about 60\% for $x = 0.4$. A similar trend is observed for the carrier spin optical orientation. This behavior is attributed to enhanced scattering of free excitons and carriers in the alloys with increased compositional and structural disorder. From the Larmor spin precession measured from spin dynamics in an external magnetic field applied in the Voigt geometry, the electron and hole $g$-factors are evaluated. Their dependence on the band gap energy in \MAFAPI{} crystals follows the universal trend previously established for lead halide perovskites.

cond-mat.mtrl-sci

Optical cooling of nuclear spins in GaAs/(Al,Ga)As quantum wells at subkelvin temperatures: Evidence of the dynamic self-polarization of nuclear spins

We investigate the dynamic polarization of nuclear spins in a nominally undoped GaAs/Al$_{0.35}$Ga$_{0.65}$As quantum well using two complementary experimental approaches: time-resolved Kerr rotation and optical orientation measurements of photoluminescence. Using the first technique, we measure a remarkably large Overhauser field of 3.1 T in a geometry close to the Faraday configuration for a 19.7 nm wide quantum well at a temperature of 1.6 K. A nuclear spin temperature of 6.4 $\mu$K is measured at an external magnetic field of 0.006 T following an adiabatic sweep from 0.6 T. Despite the quadrupole-induced nuclear spin splitting inherent to nanostructures, the nuclear spin system is found to follow the predictions of spin temperature theory. Using the optical orientation of the photoluminescence, we investigated nuclear spin dynamics at millikelvin temperatures down to 300 mK. At a temperature of 500 mK, an Overhauser field of 160 mT is generated in an oblique but nearly Voigt magnetic field using low optical power to avoid heating. The nuclear polarization build-up time is of 150 s, consistent with earlier reports at higher temperatures, where hyperfine scattering on free photoexcited electrons governs relaxation. At 500 mK, the onset of dynamic self-polarization of nuclear spins is observed, which becomes more pronounced as the lattice temperature is further reduced to 300 mK. The estimated nuclear spin temperature in the dynamic self-polarization regime can be as low as 200 nK.

cond-mat.mes-hall

Immobile and mobile excitations of three-spin interactions on the diamond chain

We present a solvable one-dimensional spin-1/2 model on the diamond chain featuring three-spin interactions, which displays both, mobile excitations driving a second-order phase transition between an ordered and a $\mathbb{Z}_2$-symmetry broken phase, as well as non-trivial fully immobile excitations. The model is motivated by the physics of fracton excitations, which only possess mobility in a reduced dimension compared to the full model. We provide an exact mapping of this model to an arbitrary number of independent transverse-field Ising chain segments with open boundary conditions. The number and lengths of these segments correspond directly to the number of immobile excitations and their respective distances from one another. Furthermore, we demonstrate that multiple immobile excitations exhibit Casimir-like forces between them, resulting in a non-trivial spectrum.

cond-mat.str-el

Quantum beats of exciton-polarons in CsPbI3 perovskite nanocrystals

Exciton-phonon interactions govern the energy level spectrum and thus the optical response in semiconductors. In this respect, lead-halide perovskite nanocrystals represent a unique system, for which the interaction with optical phonons is particularly strong, giving rise to a ladder of multiple exciton states which can be optically excited with femtosecond pulses. We establish a new regime of coherent exciton-polaron dynamics with exceptionally long coherence times (T2 ~300 ps) in an ensemble of CsPbI3 nanocrystals embedded in a glass matrix. Using transient two-pulse photon echo at 2 K temperature, we observe quantum beats between the exciton-polaron states. Within a four-level model, we directly quantify the exciton-phonon coupling strength through the Huang-Rhys factors of 0.05-0.1 and 0.02-0.04 for low-energy optical phonons with energies of 3.2 and 5.1 meV, respectively. The pronounced size dependence of both coupling strengths and phonon lifetimes offers a path to tune the optical transitions between polaron states and to tailor the coherent optical dynamics in perovskite semiconductors for solid-state quantum technologies.

cond-mat.mes-hall

Antiferromagnetic nonreciprocity of light emission in CuB$_2$O$_4$

Nonreciprocity of light emission, when the radiation intensity differs for two opposite propagation directions, is a rare phenomenon in solids because it requires a violation of the crystal symmetry with respect to time-reversal. Such violation via time-reversal symmetry breaking can occur either due to an applied magnetic field or due to a magnetic ordering. We perform a detailed theoretical and experimental study of the photoluminescence (PL) nonreciprocity in the noncentrosymmetric tetragonal antiferromagnet CuB$_2$O$_4$, where this effect reaches 80\% below the N\'eel phase transition temperature of $T_N = 20$~K. The effect is observed for three sets of extremely narrow exciton and exciton-magnon PL lines, associated with Frenkel excitons on the Cu$^{2+}$ ions in the magnetic $4b$ subsystem. A strong manifestation of the nonreciprocity of emission is found in certain geometries for the commensurate antiferromagnetic phase, as well as in other phases with incommensurate spin ordering. In accordance with the magnetic symmetry of CuB$_2$O$_4$, the nonreciprocity of emission is observed for light propagation along certain directions within the easy (001) plane. A rigorous quantum-mechanical analysis of the wave functions of the initial and final states of the Cu$^{2+}$ ions responsible for the PL is performed for various experimental geometries of the crystallographic axes and the applied magnetic field. The analysis confirms that the nonreciprocity of emission from Frenkel excitons in CuB$_2$O$_4$ is due to the interference of magnetic-dipole and electric-dipole transitions of antiferromagnetically ordered $4b$ spins of the Cu$^{2+}$ ions, in good agreement with the experimental data.

cond-mat.mtrl-sci

Coherence of dipole-forbidden Rydberg excitons in Cu$_2$O measured by polarization- and time-resolved multi-photon spectroscopy

Quantum applications of solid state systems base upon generation and control of coherent electronic excitations. Prominent examples are exciton states in semiconductors excitable by photons. The high oscillator strength of electric-dipole (ED) allowed exciton states favors their efficient coherent generation, but limits also their lifetime. ED-forbidden exciton states with long recombination times might maintain long-lived coherence, especially in highly-quality crystals with suppressed exciton scattering. Here, we propose a multi-photon technique combining two-photon excitation with difference frequency generation (2PE-DFG) for time-resolved measurements of exciton coherence. The technique utilizes polarization tomography for state-selective control in both the pump and probe processes. Its potential is demonstrated by measuring the coherent dynamics of the ED-forbidden $S$ and $D$ excitons in Cu$_2$O crystals. The excited states of the Rydberg excitons with principal quantum number $n=2$, $3$, and $4$ have short dephasing times of a few picoseconds, limited by their relaxation to lower lying states. The dephasing time reaches 3 ns for the $1S$ state. In an external magnetic field up to 10 T, the $1S$ exciton splits into a triplet so that quantum beats are observed after coherent excitation, for which three distinct regimes are found depending on the chosen polarization tomography scheme. These results establish the 2PE-DFG technique as a powerful tool to assess the coherent dynamics of ED-forbidden excitons.

cond-mat.mtrl-sci

Nonreciprocal magnetic-field-induced second harmonic generation of exciton polaritons in ZnSe

We report on the optical second harmonic generation (SHG) on the 1S exciton-polariton resonance in bulk ZnSe that is subject to an external magnetic field applied perpendicular to the light wave vector $\mathbf k$ (Voigt geometry). For the symmetry allowed geometry with the $\mathbf{k}\parallel[111]$ crystal axes, the nonreciprocal dependence of the SHG intensity on the magnetic field direction is found. It is explained by an interference of the crystallographic and magnetic-field-induced SHG signals. Relative phases of these signals are evaluated from the rotational anisotropy diagrams. Phenomenological and microscopic models of the effect are developed. To the best of our knowledge, this is the first experimental observation of the nonreciprocal SHG in semiconductor crystals, and the first one for exciton-polaritons.

cond-mat.mes-hall

Magnetic field induced exciton spin dynamics in indirect band gap (In,Al)As/AlAs quantum dots

The exciton recombination and spin dynamics are investigated both experimentally and theoretically in an ensemble of indirect band gap (In,Al)As/AlAs quantum dots (QDs) with type-I band alignment. The magnetic-field-induced circular polarization of the time-integrated photoluminescence changes sign across the emission spectrum with a width reflecting the QD size. It is negative on the low energy side, i.e. for emission from large QDs, but positive on the high energy side, i.e. for emission from small QDs. However, the exciton g factor, measured by spin-flip Raman scattering, is positive across the whole QD ensemble. The magnetic-field-induced circular polarization of the photoluminescence dynamics is studied as function of the magnetic field strength and direction. The dynamics are non-monotonic over a time range up to milliseconds. The time dependence of the photoluminescence circular polarization degree and sign strongly depends on the emission energy and changes with magnetic field orientation. The observed nonmonotonic behavior is provided by the interplay of bright and dark exciton states, contributing to the emission. The experiment is interpreted using a kinetic theory, which accounts for the dynamics of the spin states in the exciton level quartet in longitudinal and tilted magnetic fields, the radiative recombination processes, and the redistribution of the excitons between these states as result of spin relaxation. The model allows us to evaluate the electron and heavy hole spin relaxation times in QDs with different sizes.

cond-mat.mes-hall

The effect of doping layers position on the heterojunction sharpness in (In,Al)As/AlAs quantum dots

Effect of doped layer placed in structures with indirect band-gap (In,Al)As/AlAs quantum dots (QDs) on heterointerface sharpness is investigated. We demonstrate that growth of n (p) doped layer below QDs sheet leads to pronounced deceleration (acceleration) for dynamics of exciton recombination (which is very sensitive to heterointeface structure in these QDs) in compare with the undoped structure. Opposite, the placing of the same doped layers above the QDs sheet does not effect on the exciton recombination dynamic at all. The experimental data are explained by increase (decrease) charged vacancy formation rate in the cation sublattice, that result in QD/matrix interface bluring (sharping), with the increases in the electron (hole) concentration at this heterointerface formation. The thicknesses of the diffuse layer on QD/matrix heterointerface estimated is in range from 0 up to 5 in the lattice constant depending on doped layer placing.

cond-mat.mes-hall

A Pristine-UNIONS view on the Galaxy: Kinematics of the distant spur feature of the Sagittarius stream traced by Blue Horizontal Branch stars

Providing a detailed picture of the Sagittarius (Sgr) stream offers important constraints on the build-up of the Galactic halo as well as its gravitational potential at large radii. While several attempts have been made to model the structure of the Sgr stream, no model has yet been able to match all the features observed for the stream. Moreover, for several of these features, observational characterisation of their properties is rather limited, particularly at large distances. The aim of this work is to investigate the kinematics of the Sgr stream outermost spur feature using blue horizontal branch (BHB) stars. Candidate BHB stars were selected by combining two approaches; one capitalising on Pan-STARRS1 3$\Pi$ griz and u photometry taken as part of UNIONS, the other using Pristine Survey CaHK and SDSS ugr photometry. Follow-up optical spectra are obtained using ESO/VLT/FORS2 to confirm their BHB nature and obtain line-of-sight (LOS) velocities. Of our 25 candidates, 20 stars can be confirmed as bona fide BHB stars. Their LOS velocities, together with the 3D positions of these stars qualitatively match well with Sgr model predictions and trace the outer apocentre of the trailing arm and its spur feature very nicely. The quantitative offsets that are found between our data and the different models can be used to provide information about the Galactic gravitational potential at large distances. We present a first, tentative, analysis in this direction, showing that the model of Vasiliev et al. (2021) would provide better agreement with our observations if the enclosed mass of the Milky Way within 100 kpc were lowered to $(5.3\!\pm\!0.4)\!\times\!10^{11}$ M$_\odot$ (versus $(5.6\!\pm\!0.4)\!\times\!10^{11}$ M$_\odot$). Our selection of BHB stars provides a new view on the outermost structure in 3D positions and LOS velocities of the Sgr debris.

astro-ph.GA

Hole spin coherence in InAs/InAlGaAs self-assembled quantum dots emitting at telecom wavelengths

We report measurements of the longitudinal and transverse spin relaxation times of holes in an ensemble of self-assembled InAs/InAlGaAs quantum dots (QDs), emitting in the telecom spectral range. The spin coherence of a single carrier is determined using spin mode-locking in the inhomogeneous ensemble of QDs. Modeling the signal allows us to extract the hole spin coherence time to be in the range of T$_2 = 0.02-0.4$ $\mu$s. The longitudinal spin relaxation time T$_1 = 0.5$ $\mu$s is measured using the spin inertia method.

cond-mat.mes-hall

Continuous time crystal in an electron-nuclear spin system: stability and melting of periodic auto-oscillations

Crystals spontaneously break the continuous translation symmetry in space, despite the invariance of the underlying energy function. This has triggered suggestions of time crystals analogously lifting translational invariance in time. Originally suggested for closed thermodynamic systems in equilibrium, no-go theorems prevent the existence of time crystals. Proposals for open systems out of equilibrium led to the observation of discrete time crystals subject to external periodic driving to which they respond with a sub-harmonic response. A continuous time crystal is an autonomous system that develops periodic auto-oscillations when exposed to a continuous, time-independent driving, as recently demonstrated for the density in an atomic Bose-Einstein condensate with a crystal lifetime of a few ms. Here we demonstrate an ultra-robust continuous time crystal in the nonlinear electron-nuclear spin system of a tailored semiconductor with a coherence time exceeding hours. Varying the experimental parameters reveals huge stability ranges of this time crystal, but allows one also to enter chaotic regimes, where aperiodic behavior appears corresponding to melting of the crystal. This novel phase of matter opens the possibility to study systems with nonlinear interactions in an unprecedented way.

cond-mat.mes-hall

Spin-Flip Raman Scattering on Electrons and Holes in Two-Dimensional (PEA)$_2$PbI$_4$ Perovskites

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 up to 10 T. From the recorded data, the electron and hole Land\'e factors ($g$-factors) are evaluated, their signs are determined, and their anisotropies are measured. The electron $g$-factor value changes from $+2.11$ out-of-plane to $+2.50$ in-plane, while the hole $g$-factor ranges between $-0.13$ and $-0.51$. The spin flips of the resident carriers are arranged via their interaction with photogenerated excitons. Also the double spin-flip process, where a resident electron and a resident hole interact with the same exciton, is observed showing a cumulative Raman shift. Dynamic nuclear spin polarization induced by spin-polarized holes is detected in corresponding changes of the hole Zeeman splitting. An Overhauser field of the polarized nuclei acting on the holes as large as $0.6$ T can be achieved.

cond-mat.mes-hall

Temporal sorting of optical multi-wave-mixing processes in semiconductor quantum dots

Coherent control of ensembles of light emitters by means of multi-wave mixing processes is key for the realization of high capacity optical quantum memories and information processing devices. In this context, semiconductor quantum dots placed in optical microcavities represent excellent candidates to explore strong light-matter interactions beyond the limits of perturbative non-linear optics and control the unitary evolution of optically driven quantum systems. In this work, we demonstrate that a sequence of two optical picosecond pulses can be used to establish coherent control over the phase evolution of the ensemble of trions in (In,Ga)As quantum dots independent of their initial quantum state. Our approach is based on coherent transfer between degenerate multi-wave-mixing signals in the strong field limit where Rabi rotations in multi-level systems take place. In particular, we use the two-pulse photon echo sequence to uncover the coherent dynamics of the trion ensemble, whereas the areas of two additional control pulses serve as tuning knobs for adjusting the magnitude and timing of the coherent emission. Furthermore, we make use of the spin degeneracy of ground and excited state of trions to control the polarization state of the emitted signal. Surprisingly, we reveal that the use of optical control pulses, whose durations are comparable to the dephasing time of the ensemble, lifts the temporal degeneracy between wave-mixing processes of different order. This phenomenon is manifested in a significant modification of the temporal shape of the coherent optical response for strong optical fields. Lifting the temporal degeneracy allows to smoothly trace the transition from the perturbative to the regime of Rabi rotations and opens up new possibilities for the optical investigation of complex energy level structures in so far unexplored material systems.

cond-mat.mes-hall

Weak dispersion of exciton Land\'e factor with band gap energy in lead halide perovskites: Approximate compensation of the electron and hole dependences

The photovoltaic and optoelectronic properties of lead halide perovskite semiconductors are controlled by excitons, so that investigation of their fundamental properties is of critical importance. The exciton Land\'e or g-factor g_X is the key parameter, determining the exciton Zeeman spin splitting in magnetic fields. The exciton, electron and hole carrier g-factors provide information on the band structure, including its anisotropy, and the parameters contributing to the electron and hole effective masses. We measure g_X by reflectivity in magnetic fields up to 60 T for lead halide perovskite crystals. The materials band gap energies at a liquid helium temperature vary widely across the visible spectral range from 1.520 up to 3.213 eV in hybrid organic-inorganic and fully inorganic perovskites with different cations and halogens: FA_{0.9}Cs_{0.1}PbI_{2.8}Br_{0.2], MAPbI_{3}, FAPbBr_{3}, CsPbBr_{3}, and MAPb(Br_{0.05}Cl_{0.95})_{3}. We find the exciton g-factors to be nearly constant, ranging from +2.3 to +2.7. Thus, the strong dependences of the electron and hole g-factors on the band gap roughly compensate each other when combining to the exciton g-factor. The same is true for the anisotropies of the carrier g-factors, resulting in a nearly isotropic exciton g-factor. The experimental data are compared favorably with model calculation results.

cond-mat.mes-hall