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.
View Article and Find Full Text PDFThe atomic doping of open-shell nanographenes enables precise tuning of their electronic and magnetic states, which is crucial for their promising potential applications in optoelectronics and spintronics. Among this intriguing class of molecules, triangulenes stand out with their size-dependent electronic properties and spin states, which can also be influenced by the presence of dopant atoms and functional groups. However, the occurrence of Jahn-Teller distortions in such systems can have a crucial impact on their total spin and requires further theoretical and experimental investigation.
View Article and Find Full Text PDFWe present here a theory of Majorana excitons, photo-excited conduction electron-valence band hole pairs, interacting with Majorana Fermions in a Kitaev chain of semiconductor quantum dots embedded in a nanowire. Using analytical tools and exact diagonalization methods, we identify the presence of Majorana zero modes in the nanowire absorption spectra.
View Article and Find Full Text PDFWe predict the existence of spontaneous spin and valley symmetry-broken states of interacting massive Dirac Fermions in a gated bilayer graphene quantum dot based on the exact diagonalization of the many-body Hamiltonian. The dot is defined by a vertical electric field and lateral gates, and its single-particle (SP) energies, wave functions, and Coulomb matrix elements are computed by using the atomistic tight-binding model. The effect of the Coulomb interaction is measured by the ratio of Coulomb elements to the SP level spacing.
View Article and Find Full Text PDFWe present a theory of excitons in gated bilayer graphene (BLG) quantum dots (QDs). Electrical gating of BLG opens an energy gap, turning this material into an electrically tunable semiconductor. Unlike in laterally gated semiconductor QDs, where electrons are attracted and holes repelled, we show here that lateral structuring of metallic gates results in a gated lateral QD confining both electrons and holes.
View Article and Find Full Text PDFWe present here a theory of the electronic properties of quasi two-dimensional quantum dots made of topological insulators. The topological insulator is described by either eight band k→·p→ Hamiltonian or by a four-band k→·p→ Bernevig-Hughes-Zhang (BHZ) Hamiltonian. The trivial versus topological properties of the BHZ Hamiltonian are characterized by the different topologies that arise when mapping the in-plane wavevectors through the BHZ Hamiltonian onto a Bloch sphere.
View Article and Find Full Text PDFAtomically thin semiconductors from the transition metal dichalcogenide family are materials in which the optical response is dominated by strongly bound excitonic complexes. Here, we present a theory of excitons in two-dimensional semiconductors using a tight-binding model of the electronic structure. In the first part, we review extensive literature on 2D van der Waals materials, with particular focus on their optical response from both experimental and theoretical points of view.
View Article and Find Full Text PDFHigh-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 SiO/Si substrates. Here, we describe different van der Waals heterostructures based on uncapped single-layer MoS 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.
View Article and Find Full Text PDFSemiconductor quantum rings are topological structures that support fascinating phenomena such as the Aharonov-Bohm effect and persistent current, which are of high relevance in the research of quantum information devices. The annular shape of quantum rings distinguishes them from other low-dimensional materials, and enables topologically induced properties such as geometry-dependent spin manipulation and emission. While optical transition dipole moments (TDMs) in zero to two-dimensional optical emitters have been well investigated, those in quantum rings remain obscure despite their utmost relevance to the quantum photonic applications of quantum rings.
View Article and Find Full Text PDFJ Phys Condens Matter
July 2019
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.
View Article and Find Full Text PDFPhoton 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 WS, with energy gain up to 150 meV.
View Article and Find Full Text PDFWe show here how to create macroscopic quantum states in a semiconductor device: a chain of InAs quantum dots embedded in an InP nanowire. Filling the nanowire with 4 electrons per dot creates a synthetic spin-one chain, with four-fold degenerate topological ground state protected by a Haldane gap. The four states correspond to two spin-½ quasiparticles localised at the ends of the macroscopic wire.
View Article and Find Full Text PDFIt has previously been found that Auger processes can lead to femtosecond carrier trapping in quantum dots, limiting their performance in optoelectronic applications that rely on radiative recombination. Using atomistic simulations, we investigate whether a shell can protect carriers from Auger-assisted trapping. For these studies we investigate CdSe/CdS core-shell quantum dots having total diameters reaching up to 10 nm.
View Article and Find Full Text PDFColloidal quantum dots (CQDs) feature a low degeneracy of electronic states at the band edges compared with the corresponding bulk material, as well as a narrow emission linewidth. Unfortunately for potential laser applications, this degeneracy is incompletely lifted in the valence band, spreading the hole population among several states at room temperature. This leads to increased optical gain thresholds, demanding high photoexcitation levels to achieve population inversion (more electrons in excited states than in ground states-the condition for optical gain).
View Article and Find Full Text PDFThe 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.
View Article and Find Full Text PDFWe design quasi-type-II CdSe/CdS core-shell colloidal quantum dots (CQDs) exhibiting a suppressed Auger recombination rate. We do so using fully atomistic tight-binding wave functions and microscopic Coulomb interactions. The recombination rate as a function of the core and shell size and shape is tested against experiments.
View Article and Find Full Text PDFWe present transient absorption measurements and microscopic theory of biexciton binding in triangular colloidal graphene quantum dots consisting of 168 sp(2)-hybridized C atoms. We observe optical transitions from the lowest orbitally dark singlet exciton states to states below the energy of an unbound dark+bright singlet-exciton pair. Through microscopic calculations of the low-energy exciton and biexciton states via tight-binding, Hartree-Fock, and configuration interaction methods, the spectra reveal a biexciton consisting primarily of a dark-bright singlet-pair bound by ∼0.
View Article and Find Full Text PDFMaterials 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.
View Article and Find Full Text PDFWe present a theory of electronic properties of HgTe quantum dot and propose a strain sensor based on a strain-driven transition from a HgTe quantum dot with inverted bandstructure and robust topologically protected quantum edge states to a normal state without edge states in the energy gap. The presence or absence of edge states leads to large on/off ratio of conductivity across the quantum dot, tunable by adjusting the number of conduction channels in the source-drain voltage window. The electronic properties of a HgTe quantum dot as a function of size and applied strain are described using eight-band k · p Luttinger and Bir-Pikus Hamiltonians, with surface states identified with chirality of Luttinger spinors and obtained through extensive numerical diagonalization of the Hamiltonian.
View Article and Find Full Text PDFWe review the recent progress in theory and experiments with lateral triple quantum dots with controlled electron numbers down to one electron in each dot. The theory covers electronic and spin properties as a function of topology, number of electrons, gate voltage and external magnetic field. The orbital Hund's rules and Nagaoka ferromagnetism, magnetic frustration and chirality, interplay of quantum interference and electron-electron interactions and geometrical phases are described and related to charging and transport spectroscopy.
View Article and Find Full Text PDFControlling electron spins strongly coupled to magnetic and nuclear spins in solid state systems is an important challenge in the field of spintronics and quantum computation. We show here that electron droplets with no net spin in semiconductor quantum dots strongly coupled with magnetic ion or nuclear spin systems break down at low temperature and form a nontrivial antiferromagnetic spatially ordered spin texture of magnetopolarons. The spatially ordered combined electron-magnetic ion spin texture, associated with spontaneous symmetry breaking in the parity of electronic charge and spin densities and magnetization of magnetic ions, emerges from an ab initio density functional approach to the electronic system coupled with mean-field approximation for the magnetic or nuclear spin system.
View Article and Find Full Text PDFWe 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.
View Article and Find Full Text PDFRadio frequency identification (RFID) is a form of wireless communication that is used to identify assets and people. RFID has significant benefits to the medical environment. However, serious security threats are present in RFID systems that must be addressed in a medical environment.
View Article and Find Full Text PDFWe 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.
View Article and Find Full Text PDFCoherent 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.
View Article and Find Full Text PDF