Time, momentum, and energy resolved pump-probe tunneling spectroscopy of two-dimensional electron systems.

Real-time probing of electrons can uncover intricate relaxation mechanisms and many-body interactions in strongly correlated materials. Here, we introduce time, momentum, and energy resolved pump-probe tunneling spectroscopy (Tr-MERTS). The method allows the injection of electrons at a particular energy and observation of their subsequent decay in energy-momentum space. Using Tr-MERTS, we visualize electronic decay processes, with lifetimes from tens of nanoseconds to tens of microseconds, in Landau levels formed in a GaAs quantum well. Although most observed features agree with simple energy-relaxation, we discovered a splitting in the nonequilibrium energy spectrum in the vicinity of a ferromagnetic state. An exact diagonalization study suggests that the splitting arises from a maximally spin-polarized state with higher energy than a conventional equilibrium skyrmion. Furthermore, we observe time-dependent relaxation of the splitting, which we attribute to single-flipped spins forming skyrmions. These results establish Tr-MERTS as a powerful tool for studying the properties of a 2DES beyond equilibrium.

Probing negatively charged and neutral excitons in MoS2/hBN and hBN/MoS2/hBN van der Waals heterostructures.

High-quality van der Waals heterostructures assembled from hBN-encapsulated monolayer transition metal dichalcogenides enable observations of subtle optical and spin-valley properties whose identification was beyond the reach of structures exfoliated directly on standard SiO2/Si substrates. Here, we describe different van der Waals heterostructures based on uncapped single-layer MoS2 stacked onto hBN layers of different thicknesses and hBN-encapsulated monolayers. Depending on the doping level, they reveal the fine structure of excitonic complexes, i.e. neutral and charged excitons. In the emission spectra of a particular MoS2/hBN heterostructure without an hBN cap we resolve two trion peaks, T1 and T2, energetically split by about 10 meV, resembling the pair of singlet and triplet trion peaks (T S and T T ) in tungsten-based materials. The existence of these trion features suggests that monolayer MoS2 has a dark excitonic ground state, despite having a 'bright' single-particle arrangement of spin-polarized conduction bands. In addition, we show that the effective excitonic g-factor significantly depends on the electron concentration and reaches the lowest value of -2.47 for hBN-encapsulated structures, which reveals a nearly neutral doping regime. In the uncapped MoS2 structures, the excitonic g-factor varies from -1.15 to -1.39 depending on the thickness of the bottom hBN layer and decreases as a function of rising temperature.

Oscillations of the bandgap with size in armchair and zigzag graphene quantum dots.

We determine here the evolution of the bandgap energy with size in graphene quantum dots (GQDs). We find oscillatory behaviour of the bandgap and explain its origin in terms of armchair and zigzag edges. The electronic energy spectra of GQDs are computed using both the tight binding model and ab initio density functional methods. The results of the tight binding model are analyzed by dividing zigzag graphene quantum dots into concentric rings. For each ring, the energy spectra, the wave functions and the bandgap are obtained analytically. The effect of inter-ring tunneling on the energy gap is determined. The growth of zigzag terminated GQD into armchair GQD is shown to be associated with the addition of a one-dimensional Lieb lattice of carbon atoms with a shell of energy levels in the middle of the energy gap of the inner zigzag terminated GQD. This introduces a different structure of the energy levels at the bottom of the conduction and top of the valence band in zigzag and armchair GQD which manifests itself in the oscillation of the energy gap with increasing size. The evolution of the bandgap with the number of carbon atoms is compared with the notion of confined Dirac Fermions and tested against ab initio calculations of Kohn-Sham and TD-DFT energy gaps.

Room temperature multi-phonon upconversion photoluminescence in monolayer semiconductor WS2.

Photon upconversion is an anti-Stokes process in which an absorption of a photon leads to a reemission of a photon at an energy higher than the excitation energy. The upconversion photoemission has been already demonstrated in rare earth atoms in glasses, semiconductor quantum wells, nanobelts, carbon nanotubes and atomically thin semiconductors. Here, we demonstrate a room temperature upconversion photoluminescence process in a monolayer semiconductor WS2, with energy gain up to 150 meV. We attribute this process to transitions involving trions and many phonons and free exciton complexes. These results are very promising for energy harvesting, laser refrigeration and optoelectronics at the nanoscale.

Manipulation of a Nuclear Spin by a Magnetic Domain Wall in a Quantum Hall Ferromagnet.

The manipulation of a nuclear spin by an electron spin requires the energy to flip the electron spin to be vanishingly small. This can be realized in a many electron system with degenerate ground states of opposite spin polarization in different Landau levels. We present here a microscopic theory of a domain wall between spin unpolarized and spin polarized quantum Hall ferromagnet states at filling factor two with the Zeeman energy comparable to the cyclotron energy. We determine the energies and many-body wave functions of the electronic quantum Hall droplet with up to N = 80 electrons as a function of the total spin, angular momentum, cyclotron and Zeeman energies from the spin singlet ν = 2 phase, through an intermediate polarization state exhibiting a domain wall to the fully spin-polarized phase involving the lowest and the second Landau levels. We demonstrate that the energy needed to flip one electron spin in a domain wall becomes comparable to the energy needed to flip the nuclear spin. The orthogonality of orbital electronic states is overcome by the many-electron character of the domain - the movement of the domain wall relative to the position of the nuclear spin enables the manipulation of the nuclear spin by electrical means.

Magnetoluminescence and valley polarized state of a two-dimensional electron gas in WS2 monolayers.

Materials often exhibit fundamentally new phenomena in reduced dimensions that potentially lead to novel applications. This is true for single-layer, two-dimensional semiconductor crystals of transition-metal dichalcogenides, MX2 (M = Mo, W and X = S, Se). They exhibit direct bandgaps with energies in the visible region at the two non-equivalent valleys in the Brillouin zone. This makes them suitable for optoelectronic applications that range from light-emitting diodes to light harvesting and light sensors, and to valleytronics. Here, we report the results of a magnetoluminescence study of WS2 single-layer crystals in which the strong spin-orbit interaction additionally locks the valley and spin degrees of freedom. The recombination of the negatively charged exciton in the presence of a two-dimensional electron gas (2DEG) is found to be circularly polarized at zero magnetic field despite being excited with unpolarized light, which indicates that the existence of a valley polarized 2DEG is caused by valley and spin locking and strong electron-electron interactions.

Quantum interference in exciton-Mn spin interactions in a CdTe semiconductor quantum dot.

We show theoretically and experimentally the existence of a new quantum-interference effect between the electron-hole interactions and the scattering by a single Mn impurity. The theoretical model, including electron-valence-hole correlations, the short- and long-range exchange interaction of a Mn ion with the heavy hole and with electron and anisotropy of the quantum dot, is compared with photoluminescence spectroscopy of CdTe dots with single magnetic ions. We show how the design of the electronic levels of a quantum dot enables the design of an exciton, control of the quantum interference, and hence engineering of light-Mn interaction.

Antibonding ground states in InAs quantum-dot molecules.

Coherent tunneling between two InAs quantum dots forms delocalized molecular states. Using magnetophotoluminescence spectroscopy we show that when holes tunnel through a thin barrier, the lowest energy molecular state has bonding orbital character. However, as the thickness of the barrier increases, the molecular ground state changes character from a bonding orbital to an antibonding orbital, confirming recent theoretical predictions. We explain how the spin-orbit interaction causes this counterintuitive reversal by using a four-band k.p model and atomistic calculations that account for strain.

Magnetism and correlations in fractionally filled degenerate shells of graphene quantum dots.

We show that the ground state and magnetization of the macroscopically degenerate shell of electronic states in triangular gated graphene quantum dots depends on the filling fraction of the shell. The effect of degeneracy, finite size, and electron-electron interactions are treated nonperturbatively using a combination of density functional theory, tight-binding, Hartree-Fock and configuration interaction methods. We show that electronic correlations play a crucial role in determining the nature of the ground state as a function of filling fraction of the degenerate shell at the Fermi level. We find that the half-filled charge neutral shell leads to full spin polarization but this magnetic moment can be completely destroyed by adding a single electron.

Spin-selective Aharonov-Bohm oscillations in a lateral triple quantum dot.

We present a theory of spin-selective Aharonov-Bohm oscillations in a lateral triple quantum dot. We show that to understand the Aharonov-Bohm (AB) effect in an interacting electron system within a triple quantum dot molecule (TQD) where the dots lie in a ring configuration requires one to not only consider electron charge but also spin. Using a Hubbard model supported by microscopic calculations we show that, by localizing a single electron spin in one of the dots, the current through the TQD molecule depends not only on the flux but also on the relative orientation of the spin of the incoming and localized electrons. AB oscillations are predicted only for the spin singlet electron complex resulting in a magnetic field tunable "spin valve."

Intershell exchange and sequential electrically injected spin populations of InAs quantum-dot shell states.

We report sequential spin population of individual shell states of self-assembled InAs quantum dots controlled by a spin-polarized current from an Fe contact, and determine the s-p and p-d intershell exchange energies. We resolve excitonic features in the electroluminescence (EL) spectra associated with individual quantum levels. In contrast with simple models of shell occupation, the EL circular polarization exhibits maxima shifted with respect to the intensity peaks. Calculations show that this is due to intershell exchange. Exchange energies for the s-p and p-d shells are 7+/-2 and 13.5+/-1 meV, respectively.

Direct observation of polarons in electron populated quantum dots by resonant Raman scattering.

The general problem of the pairing of strongly interacting elementary excitations producing new quasiparticles such as polarons arises in many areas of solid state physics. Recent interest in polaron formation in semiconductor quantum dots has been motivated by the need to understand the physical nature of the carrier relaxation processes and their role in quantum-dot based devices. We report on the direct observation of polarons in InAs/GaAs self-assembled quantum dots populated by few electrons where the polarons are strongly coupled modes of quantum dot phonons and electron intersublevel transitions. The degree of coupling is varied in a systematic way in a set of samples having electron intersublevel spacing changing from larger to smaller than the longitudinal optical phonon energy. The signature of polarons is evidenced clearly by the observation of a large (12-20 meV) anticrossing for both InAs and GaAs-like quantum dot phonons using resonant Raman spectroscopy.

Remanent zero field spin splitting of self-assembled quantum dots in a paramagnetic host.

We report on the observation of a finite spin splitting at zero magnetic field in resonant tunneling experiments on CdSe self-assembled quantum dots in a (Zn,Be,Mn)Se barrier. This is remarkable since bulk II-VI dilute magnetic semiconductors are paramagnets. Our experiment may be viewed as tunneling through a single magnetic polaron, where the carriers contained inside the dot act to mediate an effective ferromagnetic interaction between Mn ions in their vicinity. The effect is observable up to relatively high temperatures, which we tentatively ascribe to a feedback mechanism with the electrical current, previously predicted theoretically.

Stability diagram of a few-electron triple dot.

Individual and coupled quantum dots containing one or two electrons have been realized and are regarded as components for future quantum information circuits. In this Letter we map out experimentally the stability diagram of the few-electron triple dot system, the electron configuration map as a function of the external tuning parameters, and reveal experimentally for the first time the existence of quadruple points, a signature of the three dots being in resonance. In the vicinity of these quadruple points we observe a duplication of charge transfer transitions related to charge and spin reconfigurations triggered by changes in the total electron occupation number. The experimental results are largely reproduced by equivalent circuit analysis and Hubbard models. Our results are relevant for future quantum mechanical engineering applications within both quantum information and quantum cellular automata architectures.

Excitonic energy shell structure of self-assembled InGaAs/GaAs quantum dots.

Performing optical spectroscopy of highly homogeneous quantum dot arrays in ultrahigh magnetic fields, an unprecedently well resolved Fock-Darwin spectrum is observed. The existence of up to four degenerate electronic shells is demonstrated where the magnetic field lifts the initial degeneracies, which reappear when levels with different angular momenta come into resonance. The resulting level shifting and crossing pattern also show evidence of many-body effects such as the mixing of configurations and exciton condensation at the resonances.

Spin-blockade spectroscopy of a two-level artificial molecule.

Coulomb- and spin-blockade spectroscopy investigations have been performed on an electrostatically defined "artificial molecule" connected to spin polarized leads. The molecule is first effectively reduced to a two-level system by placing both constituent atoms at a specific location of the level spectrum. The spin sensitivity of the conductance enables us to identify the electronic spin states of the two-level molecule. We find in addition that the magnetic field induces variations in the tunnel coupling between the two atoms. The lateral nature of the device is evoked to explain this behavior.

Optical detection of the Aharonov-Bohm effect on a charged particle in a nanoscale quantum ring.

We study spectroscopically the current produced by a charged particle moving in a nanosize semiconductor quantum ring subject to a perpendicular magnetic field. Several Aharonov-Bohm oscillations are observed in the emission of a charged exciton confined in a single ring structure. The magnetic field period of the oscillations correlates well with the size of the rings.

Fine structure of excitons in InAs/GaAs coupled auantum dots: a sensitive test of electronic coupling.

Exciton fine structure in InAs/GaAs coupled quantum dots has been studied by photoluminescence spectroscopy in magnetic fields up to 8 T. Pronounced anticrossings and mixings of optically bright and dark states as functions of magnetic field are seen. A theoretical treatment of the mixing of the excitonic states has been developed, and it traces observed features to structural asymmetries. These results provide direct evidence for coherent coupling of excitons in quantum dot molecules.

Exciton dephasing in quantum dot molecules.

We have measured the exciton dephasing time in InAs/GaAs quantum dot molecules having different interdot barrier thicknesses in the temperature range from 5 to 60 K, using a highly sensitive four-wave mixing heterodyne technique. At 5 K dephasing times of several hundred picoseconds are found. Moreover, a systematic dependence of the dephasing dynamics on the barrier thickness is observed. These results show how the quantum-mechanical coupling of the electronic wave functions in the molecules affects both the exciton radiative lifetime and the exciton-acoustic phonon interaction.

Collapse of the spin-singlet phase in quantum dots.

We present experimental and theoretical results on a new regime in quantum dots in which the filling factor two-singlet state is replaced by new spin polarized phases. We make use of spin blockade spectroscopy to identify the transition to this new regime as a function of the number of electrons. The key experimental observation is a reversal of the phase in the systematic oscillation of the amplitude of Coulomb blockade peaks as the number of electrons is increased above a critical number. It is found theoretically that correlations are crucial to the existence of the new phases.