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Krzysztof Gawarecki

Publications and source records attributed to Krzysztof Gawarecki.

At least 19 recordsLinked to original sources

Strain tunability of electron and hole g-factors in CsPb$X_3$: bulk and nanocrystals

In this paper, we theoretically study the electron and hole $g$-factors in inorganic lead-halide perovskites for the reference cubic phase. We employ an 18-band $k \cdot p$ model and determine its parameters using target band structures obtained from DFT calculations. We use the linear response theory to calculate the $g$-factors and investigate their dependence on external strain. We then perform real-space calculations of the electron and hole $g$-factors in perovskite nanocrystals. We show that the bulk $g$-factors can be tuned over a wide range by external strain. In some cases, strain can be used to tune the $g$-factor through zero. By contrast, the carrier $g$-factors in CsPb$X_3$ nanocrystals are considerably less sensitive to strain due to quantum confinement.

cond-mat.mtrl-sci↗

Tunable g-Factors of Hybridized Orbitals in a Quantum Dot Molecule

The ability to control the $g$-factors of orbital spin states in optically active quantum dot molecules (QDMs) is a prerequisite for the high-fidelity generation of multi-photonic cluster states with higher-dimensional entanglement structure. Protocols that rely on two coupled spins require knowledge of the $g$-factor and its dependence on external control parameters. Mismatches in the $g$-factor between tunnel-coupled dots introduce unwanted dephasing of coupled spin-states, making precise characterization and voltage control essential. Here, we measure the gate voltage dependence of the electron and hole $g$-factors of negatively charged trions $X^{-}$ in a single InGaAs QDM using polarization-resolved magneto-photoluminescence spectroscopy. The electron $g$-factor exhibits a pronounced step-like change at the tunneling resonance, shifting from $g_\mathrm{e} = -0.336\pm 0.008$ to $g_\mathrm{e} = -0.389\pm 0.003$, providing a direct spectroscopic fingerprint of molecular orbital formation and a shift of the wavefunction localization from the lower to the upper dot. In contrast, the hole $g$-factor remains nearly constant at $g_\mathrm{h} \approx 0.094 \pm 0.007$, exhibiting a weak modulation near the anticrossing voltages attributed to Coulomb-mediated deformation of the wavefunction by the tunneling electron. Our results are quantitatively reproduced by an eight-band $\mathbf{k}{\cdot}\mathbf{p}$ model, establishing electric-field control of the trion $g$-factors as a practical tool for independently tuning the Zeeman splitting of individual dots and opening new pathways towards the deterministic generation of two-dimensional photonic cluster states.

cond-mat.mes-hall↗

Emission dynamics in zincblende InAsxP1-x quantum dots in InP nanowires: influence of quantum dot size, composition and nanowire geometry

Hereby, we present an experimental and theoretical investigation of emission dynamics in zincblende InAsxP1-x quantum dots (QDs) embedded in InP nanowires (NWs) grown via vapour-liquid-solid mechanism by chemical beam epitaxy, using Au nanoparticles as a nucleation catalyst. By measuring time-resolved photoluminescence from an ensemble of QD-NWs it was possible to determine the exciton lifetime dependence on QD composition and height. Changes in the InP shell thickness surrounding the InP NW stem with a QD, brought additional insight into the influence of photonic environment on the carrier dynamics. High-resolution transmission electron microscopy, combined with energy-dispersive X-ray spectroscopy, provided actual structural parameters. The experimentally obtained lifetimes were interpreted in the light of results of 8 band kp calculations combined with configuration-interaction model to take into account the Coulomb interactions and finite-difference time domain photonic simulations to include the effect of optical confinement. The full understanding of the experimental results required considering both, the changes in the QD potential and the Purcell effect, the latter leading to spontaneous emission inhibition in the case of NWs with thin InP shell.

cond-mat.mes-hall↗

Ultra-slow orbital and spin dynamics in an electrically tunable quantum dot molecule

Tunnel-coupled optically active quantum dot molecules (QDMs), have the potential to operate as spin-photon-interfaces with coupled spins that interact with two different photon frequencies at the same time. A prerequisite is to deterministically prepare two (electron or hole) spins in the QDM and be able to electrically tune the orbital state couplings. Here, we demonstrate the sequential optical charging of a single QDM with two electron spins while simultaneously maintaining the ability to widely tune orbital couplings using static electric fields and optically drive the system for quantum light generation. We optically prepare one- and two-spin states, initialize via optical pumping and explore orbital and spin relaxation dynamics for one and two-spin states as a function of the energy detuning and hybridization of orbital states. For two-spin states, remarkably long S-T relaxation times are observed extending beyond $\sim 100μs$ with strong dependence on the relative energy of ground and excited two-spin states. Qualitative agreement is observed with $\mathbf{k \cdot p}$ calculations of phonon-mediated spin-relaxation. Our results provide new quantitative understanding of the dynamics of one and two-spin states and confirm their suitability of QDMs for creating multidimensional photonic cluster states by exploiting tunable spin-spin exchange couplings at zero magnetic fields combined with optical driving.

cond-mat.mes-hall↗

Light-hole states and hyperfine interaction in electrically-defined Ge/GeSn quantum dots

We theoretically investigate hole spins confined in a gate-defined quantum dot (QD) embedded in GeSn/Ge/GeSn quantum well (QW) structure. Owing to the tensile strain in the Ge layer, the system effectively realizes a light-hole qubit. We systematically study how various morphological parameters influence the energy spectrum, g-factors, and the hyperfine coupling to the nuclear spin bath. The simulations are carried out using a realistic, fully atomic sp$^3$d$^5$s$^*$ tight-binding model. We also perform complementary DFT calculations of wave functions near the atomic cores and use them to parameterize the hyperfine-interaction Hamiltonian. We evaluate the Overhauser field fluctuations and demonstrate that the strength of the hyperfine coupling for the lowest hole doublet crucially depends on the Sn content in the barrier. We highlight the conduction-valence band mixing, which leads to considerable $s$-type admixtures to the hole states, providing the dominant channel of hyperfine coupling due to the Fermi contact interaction.

cond-mat.mes-hall↗

Modeling the g-factors, hyperfine interaction and optical properties of semiconductor QDs: the atomistic and eight-band $k \cdot p$ approaches

We present a detailed comparative study of two important theoretical approaches: atomistic sp$^3$d$^5$s$^*$ tight-binding and continuum eight-band $k \cdot p$ methods, for modeling the spin and optical properties of quantum dots (QDs). Our investigation spans key physical observables, including single-particle energy levels, g-factors, exciton radiative lifetimes, and hyperfine-induced Overhauser field fluctuations. We perform our calculations for self-assembled InGaAs/GaAs QD systems as representative case studies. While both methods yield qualitatively consistent trends, quantitative discrepancies arise due to different treatment of atomistic details, strain effects, and confinement. We introduce targeted corrections to the eight-band $k \cdot p$ framework, including a modified deformation potential scheme and adjusted remote-band contributions, to improve agreement with atomistic results, especially for electron g-factors and single-particle energies. Furthermore, we validate the eight-band implementation of hyperfine interactions by benchmarking it against the tight-binding model, showing reasonable convergence for both electrons and holes. Our results establish criteria for selecting the appropriate modeling framework based on the desired physical accuracy and computational efficiency in spin-optical studies of semiconductor QDs.

cond-mat.mes-hall↗

Resonant and Anti-resonant Exciton-Phonon Coupling in Quantum Dot Molecules

Optically active quantum dot molecules (QDMs) can host multi-spin quantum states with the potential for the deterministic generation of photonic graph states with tailored entanglement structures. Their usefulness for the generation of such non-classical states of light is determined by orbital and spin decoherence mechanisms, particularly phonon-mediated processes dominant at energy scales up to a few millielectronvolts. Here, we directly measure the spectral function of orbital phonon relaxation in a QDM and benchmark our findings against microscopic kp theory. Our results reveal phonon-mediated relaxation rates exhibiting pronounced resonances and anti-resonances, with rates ranging from several ten ns$^{-1}$ to tens of $μ$s$^{-1}$. Comparison with a kinetic model reveals the voltage (energy) dependent phonon coupling strength and fully explains the interplay between phonon-assisted relaxation and radiative recombination. These anti-resonances can be leveraged to increase the lifetime of energetically unfavorable charge configurations needed for realizing efficient spin-photon interfaces and multi-dimensional cluster states.

cond-mat.mes-hall↗

Electronic and spectral properties of Ge1-xSnx quantum dots: an atomistic study

In this paper, we study theoretically the electron and spectral properties of Ge1-xSnx systems, including alloys, cubic- and spherical quantum dots. The single-particle electron and hole states are calculated within the sp3d5s* tight-binding approach and used in further modeling of the optical properties. We systematically study the interplay of Sn-driven indirect-direct band-gap transition and the quantum confinement effect in systems of reduced dimensionality. We demonstrate the regime of sizes and composition, where the ground state in Ge1-xSnx quantum dot is optically active. Finally, we calculate absorbance spectra in experimentally-relevant colloidal quantum dots and demonstrate a satisfactory agreement with experimental data.

cond-mat.mes-hall↗

Material gain and eight-band k.p description for selected perovskites

In this work, we present a ready-to-use symmetry invariant expansion form of the eight-band k.p Hamiltonian for inorganic and organic metal halide perovskites (CsPbX$_3$ and MAPbX$_3$ with $X = \{$Cl, Br, I$\}$). We use the k.p model to calculate the electronic band structures for perovskite materials of cubic and pseudo-cubic phase. In order to find respective parameters, the band structures of considered materials were obtained within state-of-the-art density functional theory and used next as targets to adjust the k.p bands and determine the values of k.p parameters. The calculated band structures were used to obtain the material gain for bulk crystals (CsPbCl$_3$, CsPbBr$_3$, CsPbI$_3$, MAPbCl$_3$, MAPbBr$_3$ and MAPbI$_3$) which is compared with the material gain in well-established III-V semiconductors. It was found that for these perovskites a positive material gain appears at lower carrier density than for the reference materials (GaAs and InP). We demonstrate that from the point of view of the electronic band structure, the studied perovskites are very promising gain medium for lasers.

cond-mat.mtrl-sci↗

Controlled Coherent Coupling in a Quantum Dot Molecule Revealed by Ultrafast Four-Wave Mixing Spectroscopy

Semiconductor quantum dot molecules are considered as promising candidates for quantum technological applications due to their wide tunability of optical properties and coverage of different energy scales associated with charge and spin physics. While previous works have studied the tunnel-coupling of the different excitonic charge complexes shared by the two quantum dots by conventional optical spectroscopy, we here report on the first demonstration of a coherently controlled inter-dot tunnel-coupling focusing on the quantum coherence of the optically active trion transitions. We employ ultrafast four-wave mixing spectroscopy to resonantly generate a quantum coherence in one trion complex, transfer it to and probe it in another trion configuration. With the help of theoretical modelling on different levels of complexity we give an instructive explanation of the underlying coupling mechanism and dynamical processes.

cond-mat.mes-hall↗

Structural symmetry-breaking to explain radiative Auger transitions in self-assembled quantum dots

The optical spectrum of a quantum dot is typically dominated by the fundamental transition between the lowest-energy configurations. However, the radiative Auger process can result in additional red-shifted emission lines. The origin of these lines is a combination of Coulomb interaction and symmetry-breaking in the quantum dot. In this paper, we present measurements of such radiative Auger lines for a range of InGaAs/GaAs self-assembled quantum dots and use a tight-binding model with a configuration interaction approach to explain their appearance. Introducing a composition fluctuation cluster in the dot, our calculations show excellent agreement with measurements. We relate our findings to group theory explaining the origin of the additional emission lines. Our model and results give insight into the interplay between the symmetry breaking in a quantum dot and the position and strength of the radiative Auger lines.

cond-mat.mes-hall↗

Invariant expansion of the 30-band k.p model and its parameters for III-V compounds

In this work we derive a ready-to-use symmetry invariant expansion of the full-zone 30-band k.p Hamiltonian for the Td point group. In order to find respective parameters, the band structures of III-V materials were calculated within a state-of-the-art Density Functional Theory (DFT) approach and used next as targets to adjust the k.p bands. A satisfactory agreement of the k.p model with the DFT band structures, for all the tested zinc blende III-V semiconductors, has been achieved. Values of many of the parameters have not been known so far. We also compare the fitted k.p parameters with the values calculated using momentum matrix elements obtained directly from the DFT.

cond-mat.mes-hall↗

Tunneling-related electron spin relaxation in self-assembled quantum-dot molecules

We study theoretically spin relaxation during phonon-assisted tunneling of a single electron in self-assembled InAs/GaAs quantum-dot molecules formed by vertically stacked dots. We find that the spin-flip tunneling rate may be as high as 1% of the spin-conserving one. By studying the dependence of spin relaxation rate on external fields, we show that the process is active at a considerable rate even without the magnetic field, and scales with the latter differently than the relaxation in a Zeeman doublet. Utilizing a multiband $\boldsymbol{k}\cdot\boldsymbol{p}$ theory, we selectively investigate the impact of various spin-mixing terms in the electron energy and carrier-phonon interaction Hamiltonians. As a result, we identify the main contribution to come from the Dresselhaus spin-orbit interaction, which is responsible for the zero-field effect. At magnetic fields above $\sim$ 15 T, this is surpassed by other contributions due to the structural shear strain. We also study the impact of the sample morphology and determine that the misalignment of the dots may enhance relaxation rate by over an order of magnitude. Finally, via virtual tunneling at nonzero temperature, the process in question also affects stationary electrons in tunnel-coupled structures and provides a Zeeman-doublet spin relaxation channel even without the magnetic field.

cond-mat.mes-hall↗

Phonon-assisted carrier tunneling in coupled quantum dot systems with hyperfine-induced spin flip

We calculate the rates of phonon-assisted hyperfine spin flips during electron and hole tunneling between quantum dots in a self-assembled quantum dot molecule. We show that the hyperfine process dominates over the spin-orbit-induced spin relaxation in magnetic fields up to a few Tesla for electrons, while for holes this cross-over takes place at field magnitudes of a fraction of Tesla, upon the assumption of a large $d$-shell admixture to the valence band state, resulting in a strong transverse hyperfine coupling. The interplay of the two spin-flip mechanisms leads to a minimum of the spin-flip probability, which is in principle experimentally measurable and can be used as a test for the presence of substantial transverse hyperfine couplings in the valence band.

cond-mat.mes-hall↗

Electron g-factor in nanostructures: continuum media and atomistic approach

We report studies of $k$-dependent Landé $g$-factor, performed by both continuous media approximation k.p method, and atomistic tight-binding sp$^3$d$^5$s$^*$ approach. We propose an effective, mesoscopic model for InAs that we are able to successfully compare with atomistic calculations, for both very small and very large nanostructures, with a number of atoms reaching over 60 million. Finally, for nanostructure dimensions corresponding to near-zero $g$-factor we report electron spin states anti-crossing as a function of system size, despite no shape-anisotropy nor strain effects included, and merely due to breaking of atomistic symmetry of cation/anion planes constituting the system.

cond-mat.mes-hall↗

Phonon-assisted relaxation between triplet and singlet states in a self-assembled double quantum dot

We study theoretically phonon-induced spin dynamics of two electrons confined in a self-assembled double quantum dot. We calculate the transition rates and time evolution of occupations for the spin-triplet and spin-singlet states. We characterize the relative importance of various relaxation channels as a function of the electric and magnetic fields. The simulations are based on a model combining the eight-band k.p method and configuration-interaction approach. We show that the electron g-factor mismatch between the Zeeman doublets localized on different dots opens a relatively fast triplet-singlet relaxation channel. We also demonstrate, that the relaxation near the triplet-singlet anticrossing is slowed down up to several orders of magnitude due to vanishing of some relaxation channels.

cond-mat.mes-hall↗

Hole spin-flip transitions in a self-assembled quantum dot

In this work, we investigate hole spin-flip transitions in a single self-assembled InGaAs/GaAs quantum dot. We find the hole wave functions using the 8-band $kp$ model and calculate phonon-assisted spin relaxation rates for the ground-state Zeeman doublet. We systematically study the importance of various admixture- and direct spin-phonon mechanisms giving rise to the transition rates. We show that the biaxial and shear strain constitute dominant spin-admixture coupling mechanisms. Then, we demonstrate that hole spin lifetime can be increased if a quantum dot is covered by a strain-reducing layer. Finally, we show that the spin relaxation can be described by an effective model.

cond-mat.mes-hall↗

Interplay between emission wavelength and s-p splitting in MOCVD-grown InGaAs/GaAs quantum dots emitting above 1.3 μm

The electronic structure of strain-engineered single InGaAs/GaAs quantum dots emitting in the telecommunication O band is probed experimentally by photoluminescence excitation spectroscopy. Observed resonances can be attributed to p-shell states of individual quantum dots. The determined energy difference between s-shell and p-shell shows an inverse dependence on the emission energy. The experimental data are compared with the results of confined states calculations, where the impact of the size and composition in the investigated structures is simulated within the 8-band $\mathbf{k}\cdot\mathbf{p}$ model. On this basis, the experimental observation is attributed mainly to changes in indium content within individual quantum dots, indicating a way of engineering and selecting a desired quantum dot, whose electronic structure is the most suitable for a given nanophotonic application.

cond-mat.mes-hall↗