We present a full configuration interaction study of the spontaneous recombination of neutral and singly charged excitons (trions) in semiconductor quantum dots, from weak to strong coupling regimes. We find that the enhancement of the recombination rate of neutral excitons with increasing dot size is suppressed for negative trions, and even reversed for positive trions. Our findings agree with recent comprehensive photoluminescence experiments in self-assembled quantum dots [P. Dalgarno et al. Phys. Rev. B {\bf 77}, 245311 (2008)] and confirm the major role played by correlations in the valence band.The effect of the temperature on the photoluminescence spectrum and that of the ratio between the electron and hole wavefunction lengthscales are also described.
We studied the excitation density dependence of photoluminescence (PL) spectra of excitons and trions (charged excitons) in hole-doped single-walled carbon nanotubes. We found that the PL intensity of trions exhibited a strong nonlinear saturation behavior as the excitation density increased, whereas that of excitons exhibited a weak sublinear behavior. The strong PL saturation of trions is attributed to depletion of doped holes that are captured by excitons in the formation processes. Moreover, the effective radiative lifetime of a trion was evaluated to be approximately 20 ns.
We report the first observation of trions (charged excitons), three-particle bound states consisting of one electron and two holes, in hole-doped carbon nanotubes at room temperature. When p-type dopants are added to carbon nanotube solutions, the photoluminescence and absorption peaks of the trions appear far below the E11 bright exciton peak, regardless of the dopant species. The unexpectedly large energy separation between the bright excitons and the trions is attributed to the strong electron-hole exchange interaction in carbon nanotubes.
We study spatial photoluminescence characteristics of neutral and charged excitons across extended monolayer MoS$_2$ synthesized by chemical vapor deposition. Using two-dimensional hyperspectral photoluminescence mapping at cryogenic temperatures we identify regions with increased emission from charged excitons associated with both spin-orbit split valence subbands. Such regions are attributed to unintentional doping at defect sites with excess charge that bind neutral excitons to form defect-pinned trions. Our findings imply comparable timescales for the formation, relaxation, and radiative d…
Monolayer molybdenum disulfide (MoS$_2$) has emerged as an excellent 2D model system because of its two inequivalent, direct-gap valleys that lead to exotic bound and excited states. Here we focus on one such bound state, the negatively charged trion. Unlike excitons, trions can radiatively decay with non-zero momentum by kicking out an electron, resulting in an asymmetric trion photoluminescence (PL) peak with a long low-energy tail. As a consequence, the peak position does not correspond to the zero momentum trion energy. By including the trion's long tail in our analysis we are able to accu…
So far in the literature the terms "charged exciton" and "trion" are often confused with each other and mostly considered as the same. In this work we show this is not the case in 2D quantum dots with a parabolic confinement. By using the unrestricted Hartree-Fock method the energy and binding energy of both charged excitons and trions in 2D parabolic quantum dots are calculated in dependence on the confinements of charge carriers in quantum dot. It is shown that the binding energies of the charged exciton and the trion behave differently in regard to the ratios of the confinements between the…
We demonstrate that the temperature and doping dependencies of the photoluminescence (PL) spectra of a doped MoS2 monolayer have several peculiar characteristics defined by trion radiative decay. While only zero-momentum exciton states are coupled to light, radiative recombination of non-zero momentum trions is also allowed. This leads to an asymmetric broadening of the trion spectral peak and redshift of the emitted light with increasing temperature. The lowest energy trion state is dark, which is manifested by the sharply non-monotonic temperature dependence of the PL intensity. Our calculat…
Charge doping in transition metal dichalcogenide is currently a subject of high importance for future electronic and optoelectronic applications. Here we demonstrate chemical doping in CVD grown monolayer (1L) of WS2 by a few commonly used laboratory solvents by investigating the room temperature photoluminescence (PL). The appearance of distinct trionic emission in the PL spectra and quenched PL intensities suggest n-type doping in WS2. The temperature-dependent PL spectra of the doped 1L-WS2 reveal significant enhancement of trion emission intensity over the excitonic emission at low tempera…
We investigate, within the envelope function approximation, the low-energy states of trions in graphene quantum dots. The presence of valley pseudospin in graphene as an electron degree of freedom apart from spin adds convolution to the interplay between exchange symmetry and the electron-electron interaction in the trion, leading to new states of trions as well as a low energy trion spectrum different from those in semiconductors. Due to the involvement of valley pseudospin, it is found that the low-energy spectrum is nearly degenerate and consists of states all characterized by having an ant…
We study the Stark effect for an exciton confined in a pair of vertically coupled quantum dots. A single-band approximation for the hole and a parabolic lateral confinement potential are adopted which allows for the separation of the lateral center-of-mass motion and consequently for an exact numerical solution of the Schrödinger equation. We show that for intermediate tunnel coupling the external electric field leads to the dissociation of the exciton via an avoided crossing of bright and dark exciton energy levels which results in an atypical form of the Stark shift. The electric-field-induc…
Transition metal dichalcogenide (TMD) monolayers are two-dimensional semiconductors with two valleys in their band structure that can be selectively addressed using circularly polarized light. Their photoluminescence spectrum is characterized by neutral and charged excitons (trions) that form a chemical equilibrium governed by the net charge density. Here, we use chemical doping to drive the conversion of excitons into trions in $\text{WS}_{2}$ monolayers at room temperature, and study the resulting valley polarization via photoluminescence measurements under valley-selective optical excitatio…
A new generalised group-theoretical approach, based on master Maxwell-pseudospin equations, is proposed to explain recently observed enhanced circular dichroism in the excited state emission from p-doped quantum dot ensembles under resonant circularly polarised excitation into hot trion states, herein referred to as "spin-filtering effect". The theory agrees remarkably well with polarised time-resolved photoluminescence experiments, yielding largely unknown inter- and intra-shell spin relaxation time scales. This approach allows to predict optimum pulse parameters for control of spin dynamics,…
Single-layer WS$_2$ is a direct-gap semiconductor showing strong excitonic photoluminescence features in the visible spectral range. Here, we present temperature-dependent photoluminescence measurements on mechanically exfoliated single-layer WS$_2$, revealing the existence of neutral and charged excitons at low temperatures as well as at room temperature. By applying a gate voltage, we can electrically control the ratio of excitons and trions and assert a residual n-type doping of our samples. At high excitation densities and low temperatures, an additional peak at energies below the trion do…
Magneto-optical parameters of trions in novel large and symmetric InP-based quantum dots, uncommon for molecular beam epitaxy grown nanostructures, with emission in the third telecom window, are measured in Voigt and Faraday configurations of external magnetic field. The diamagnetic coefficients are found to be in the range of 1.5-4 μeV/{\T^2}, and 8-15 μeV/{\T^2}, respectively out of plane and in plane of the dots. The determined values of diamagnetic shifts are related to the anisotropy of dot sizes. Trion g-factors are measured to be relatively small, in the range of 0.3-0.7 and 0.5-1.3, in…
We study Rabi rotations arising in intensity-dependent photon echoes from an ensemble of self-assembled InGaAs quantum dots. To achieve a uniform distribution of intensities within the excited ensemble, we introduce flattop intensity profiles of picosecond laser pulses. This allows us to overcome the damping of Rabi rotations imposed by the spatial inhomogeneity of Rabi frequencies by a Gaussian laser profile. Using photon echo polarimetry, we distinguish between the coherent optical responses from exciton and trion ensembles. Here, we demonstrate that a photo-induced charging of the quantum d…
We discuss, from a theoretical point of view, the four wave mixing spectroscopy on an ensemble of p-doped quantum dots in a magnetic field slightly tilted from the in-plane configuration. We describe the system evolution in the density matrix formalism. In the limit of coherent ultrafast optical driving, we obtain analytical formulas for the single system dynamics and for the response of an inhomogeneously broadened ensemble. The results are compared to the previously studied time-resolved Kerr rotation spectroscopy on the same system. We show that the Kerr rotation and four wave mixing spectr…
A computational model is presented to calculate the ground state energy of neutral and charged excitons confined in semiconductor quantum dots. The model is based on the variational Quantum Monte Carlo method and effective mass Hamiltonians. Through an iterative Newton-Rhapson process, minimizing the local energy, and (optional) parallelization of random walkers, fast and accurate estimates of both confinement and Coulomb binding energies can be obtained in standard desktop computers. To illustrate the reach of the model, we provide Fortran programs and illustrative calculations for colloidal …
The origin of the variation of photoluminescence (PL) spectra of monolayer tungsten disulfide (WS2) is investigated systematically. Dependence of the PL spectrum on the excitation power show that the relatively sharp component corresponds to excitons whereas the broader component at slightly lower energy corresponds to negatively charged trions. PL imaging and second harmonic generation measurements show that the trion signals are suppressed more than the exciton signals near the edges, thereby relatively enhancing the excitonic feature in the PL spectrum and that such relative enhancement of …
We report an out-of-plane magnetic field induced large photoluminescence enhancement in WS${}_2$ flakes at $4$ K, in contrast to the photoluminescence enhancement provided by in-plane field in general. Two mechanisms for the enhancement are proposed. One is a larger overlap of electron and hole caused by the magnetic field induced confinement. The other is that the energy difference between $Λ$ and K valleys is reduced by magnetic field, and thus enhancing the corresponding indirect-transition trions. Meanwhile, the Landé g factor of the trion is measured as $-0.8$, whose absolute value is muc…
Magneto photoluminescence and excitation spectroscopy are used to probe the excited state spectrum of negatively charged trions in a InGaAs quantum dot. A single dot optical charging device allows us to selectively prepare specific few (1e, 2e) electron states and stabilize hot trions against decay via electron tunnelling from excited orbital states. The spin structure of the excited state results in the formation of metastable trions with strong optical activity that are directly observed in luminescence. Excitation spectroscopy is employed to map the excited singlet and triplet states of the…
We study the impact of a free carrier reservoir on the optical properties of excitonic and trionic complexes in a MoSe$_2$ monolayer at cryogenic temperatures. By applying photodoping via a non-resonant pump laser the electron density can be controlled in our sample and in turn the exciton and trion densities can be tuned. We find a significant increase of the trion binding energy in the presence of an induced electron gas both in power- and in time-resolved photoluminescence spectra. This behaviour is reproduced within the original variational approach that takes into account both screening a…
This paper has been updated by the author to: arXiv:1012.0060v1 [cond-mat.mes-hall], titled "Collective Nuclear Stabilization by Optically Excited Hole in Quantum Dot"
We present a detailed investigation into the optical characteristics of individual InAs quantum dots (QDs) grown by metalorganic chemical vapor deposition, with low temperature emission in the telecoms window around 1300 nm. Using micro-photoluminescence (PL) spectroscopy we have identified neutral, positively charged, and negatively charged exciton and biexciton states. Temperature-dependent measurements reveal dot-charging effects due to differences in carrier diffusivity. We observe a pronounced linearly polarized splitting of the neutral exciton and biexciton lines (~250 ueV) resulting fro…
Atomically thin materials, like semiconducting transition metal dichalcogenides, are highly sensitive to the environment. This opens up an opportunity to externally control their properties by changing their surroundings. In this work, high-quality van der Waals heterostructures assembled from hBN-encapsulated monolayer MoS$_2$ are studied with the aid of photoluminescence, photoluminescence excitation, and reflectance contrast experiments. We demonstrate that carrier concentration in MoS$_2$ monolayers, arising from charge transfer from impurities in the substrate, can be significantly tuned …
We have analyzed the energetics of decay of the X^- trion (exciton + electron) on the assumption that the exciton and trion are independent excitations of a single two-dimensional semiconducting quantum well. For the first time, it has been shown that in filling a well with electrons from a selective donor-doped matrix, the binding energy of the trion (of the electron with the exciton) increases linearly with a shift of the Fermi level into the depth of the c band. This agrees with the well-known experimental data on the low-temperature radiative decay (photoluminescence) of trions in the hete…
Photoluminescence spectroscopy measurements are performed on suspended carbon nanotubes in a field-effect configuration, and the gate voltage dependence of photoluminescence spectra are compared for the pristine and the molecularly adsorbed states of the nanotubes. We quantify the molecular screening effect on the trion binding energies by determining the energy separation between the bright exciton and the trion emission energies for the two states. The voltage dependence shows narrower voltage regions of constant photoluminescence intensity for the adsorbed states, consistent with a reductio…
High-resolution spectral hole burning (SHB) in coherent nondegenerate differential transmission spectroscopy discloses spin-trion dynamics in an ensemble of negatively charged quantum dots. In the Voigt geometry, stimulated Raman spin coherence gives rise to Stokes and anti-Stokes sidebands on top of the trion spectral hole. The prominent feature of an extremely narrow spike at zero detuning arises from spin population pulsation dynamics. These SHB features confirm coherent electron spin dynamics in charged dots, and the linewidths reveal spin spectral diffusion processes.
Excitonic effects play a particularly important role in the optoelectronic behavior of two-dimensional (2D) semiconductors. To facilitate the interpretation of experimental photoabsorption and photoluminescence spectra we provide statistically exact diffusion quantum Monte Carlo binding-energy data for Mott-Wannier models of excitons, trions, and biexcitons in 2D semiconductors. We also provide contact pair densities to allow a description of contact (exchange) interactions between charge carriers using first-order perturbation theory. Our data indicate that the binding energy of a trion is ge…
Optical interband transitions in monolayer transition metal dichalcogenides such as WSe2 and MoS2 are governed by chiral selection rules. This allows efficient optical initialization of an electron in a specific K-valley in momentum space. Here we probe the valley dynamics in monolayer WSe2 by monitoring the emission and polarization dynamics of the well separated neutral excitons (bound electron hole pairs) and charged excitons (trions) in photoluminescence. The neutral exciton photoluminescence intensity decay time is about 4ps, whereas the trion emission occurs over several tens of ps. The …
Strong Coulomb interactions in single-layer transition metal dichalcogenides (TMDs) result in the emergence of strongly bound excitons, trions and biexcitons. These excitonic complexes possess the valley degree of freedom, which can be exploited for quantum optoelectronics. However, in contrast to the good understanding of the exciton and trion properties, the binding energy of the biexciton remains elusive, with theoretical calculations and experimental studies reporting discrepant results. In this work, we resolve the conflict by employing low-temperature photoluminescence spectroscopy to id…
The spin dynamics of positively (X$^{+}$) and negatively (X$^{-}$) charged excitons in InP/In$_{0.48}$Ga$_{0.52}$P quantum dots subject to a magnetic field is studied. We find that a characteristic feature of the system under study is the presence of nuclear quadrupole interaction, which leads to stabilization of the nuclear and electron spins in a quantum dot in zero external magnetic field. In detail, the nuclear quadrupole interaction leads to pinning of the Overhauser field along the quadrupole axis, which is close to the growth axis of the heterostructure. The nuclear effects are observed…
We analyze the lineshape of the quasiparticle photoluminescence of monolayer and bilayer molybdenum ditelluride in temperature- and excitation intensity-dependent experiments. We confirm the existence of a negatively charged trion in the bilayer based on its emission characteristics and find hints for a coexistence of intra- and interlayer trions with a few meV splitting in energy. From the lineshape analysis of exciton and trion emission we extract values for exciton and trion deformation potentials as well as acoustical and optical phonon-limited mobilities in MoTe2, with the mobilities show…
We study nuclear spin polarization in the quantum Hall regime through the optically pumped electron spin polarization in the lowest Landau level. The nuclear spin polarization is measured as a nuclear magnetic field $B_N$ by means of the sensitive resistive detection. We find the dependence of $B_N$ on filling factor unmonotonous. The comprehensive measurements of $B_N$ with the help of the circularly polarized photoluminescence measurements indicate the participation of the photo-excited complexes i.e., the exciton and trion (charged exciton), in nuclear spin polarization. On the basis of a n…
A theory of photoluminescence in semiconductor quantum dots is developed which relies on two key ingredients. First, it takes into account non-adiabaticity of the exciton-phonon system. Second, it includes the multimode dielectric model of LO-phonons and of the electron-phonon interaction in confined systems. The role of non-adiabaticity is shown to be of paramount importance in spherical quantum dots, where the lowest one-exciton state can be degenerate or quasi-degenerate. For various quantum dot structures, the calculated intensities of phonon satellites as a function of temperature, excita…
We present a comprehensive photoluminescence study of exchange interaction in self-assembled CdTe/ZnTe quantum dots. We exploit the presence of multiple charge states in the photoluminescence spectra of single quantum dots to analyze simultaneously fine structure of different excitonic transitions, including recombination of neutral exciton/biexciton, doubly charged negative exciton and negatively charged biexciton. We demonstrate that the fine structure results from electron-hole exchange interaction and that spin Hamiltonians with effective exchange constants $δ_i$ can provide a good descrip…
We theoretically examine the magnetoluminescence from a trion and a biexciton in a type-II semiconductor quantum dot, in which holes are confined inside the quantum dot and electrons are in a ring-shaped region surrounding the quantum dot. First, we show that two electrons in the trion and biexciton are strongly correlated to each other, forming a Wigner molecule: Since the relative motion of electrons is frozen, they behave as a composite particle whose mass and charge are twice those of a single electron. As a result, the energy of the trion and biexciton oscillates as a function of magnetic…
Spin-forbidden intravalley dark exciton in tungsten-based transition metal dichalcogenides (TMDCs), owing to its unique spin texture and long lifetime, has attracted intense research interest. Here, we show that we can control the dark exciton electrostatically by dressing it with one free electron or free hole, forming the dark trions. The existence of the dark trions is suggested by the unique magneto-photoluminescence spectroscopy pattern of the boron nitride (BN) encapsulated monolayer WSe2 device at low temperature. The unambiguous evidence of the dark trions is further obtained by direct…
We present here an atomistic theory of the electronic and optical properties of hexagonal InAsP quantum dots in InP nanowires in the wurtzite phase. These self-assembled quantum dots are unique in that their heights, shapes, and diameters are well known. Using a combined valence-force-field, tight-binding, and configuration-interaction approach we perform atomistic calculations of single-particle states and excitonic, biexcitonic and trion complexes as well as emission spectra as a function of the quantum dot height, diameter and As versus P concentration. The atomistic tight-binding parameter…
Physical implementations of large-scale quantum processors based on solid-state platforms benefit from realizations of quantum bits positioned in regular arrays. Self-assembled quantum dots are well-established as promising candidates for quantum optics and quantum information processing, but they are randomly positioned. Site-controlled quantum dots, on the other hand, are grown in pre-defined locations, but have not yet been sufficiently developed to be used as a platform for quantum information processing. In this letter we demonstrate all-optical ultrafast complete coherent control of a qu…
e study theoretically, the photoluminescence properties of a single quantum dot in a microcavity under incoherent excitation. We propose a microscopic quantum statistical approach providing a Lindblad (thus completely positive) description of pumping and decay mechanisms of the quantum dot and of the cavity mode. Our analytical results show that strong coupling (SC) and linewidths are largely independent on the pumping intensity (until saturation effects come into play), in contrast to previous theoretical findings. We shall show the reliable predicting character of our theoretical framework i…
We report on resonant optical spectroscopy of self-assembled InGaAs quantum dots in which the number of electrons can accurately be tuned to N=0,1,2 by an external gate voltage. Polarization, wave vector and magnetic field dependent measurements enable us to clearly distinguish between resonant Raman and resonant photoluminescence processes. The Raman spectra for N=1 and 2 electrons considerably differ from each other. In particular, for N=2, the quantum-dot He, the spectra exhibit both singlet and triplet transitions reflecting the elementary many-particle interaction. Also the resonant photo…
Photoluminescence of graphene quantum dots (GQDs) of shungite, attributed to individual fragments of reduced graphene oxide (rGO), has been studied for the frozen rGO colloidal dispersions in water, carbon tetrachloride, and toluene. Morphological study shows a steady trend of GQDs to form fractals and a drastic change in the colloids fractal structure caused by solvent was reliably established. Spectral study reveals a dual character of emitting centers: individual GQDs are responsible for the spectra position while fractal structure of GQD colloids provides high broadening of the spectra due…
We investigate adsorption effects of copper phthalocyanine molecules on excitons and trions in air-suspended carbon nanotubes. Using photoluminescence excitation spectroscopy, we observe that exciton energy redshifts gradually with the molecular deposition thickness. The trion emission is also observed at large deposition amounts, which indicates charge transfer between the phthalocyanine molecules and carbon nanotubes. Analysis of the spectra for individual tubes reveal a correlation between the exciton-trion energy separation and the exciton emission energy, showing that the many-body intera…
WSe$_2$ monolayers with variable doping are an ideal system to study two-dimensional excitonic complexes. Here, we find that the strongest photoluminescence from bright neutral excitons occurs at moderate $p$-doping levels, owing to a rapid decrease of signal from positive dark trions and a slow increase of signal from positive bright trions with growing $p$-concentrations. We explain our observations with a qualitative model, in which the scattering rate of bright excitons into dark complexes is enhanced by exciton localization, while the scattering rate into positive bright trions increases …
Transition-metal dichalcogenides can be easily produced as atomically thin sheets, exhibiting the possibility to optically polarize and read out the valley pseudospin of extremely stable excitonic quasiparticles present in these 2D semiconductors. Here, we investigate a monolayer of tungsten disulphide in high magnetic fields up to 30\,T via photoluminescence spectroscopy at low temperatures. The valley degeneracy is lifted for all optical features, particularly for excitons, singlet and triplet trions, for which we determine the g factor separately. While the observation of a diamagnetic shif…
Design, epitaxial growth, and resonant spectroscopy of CdSe Quantum Dots (QDs) embedded in an innovative (Zn,Cd)Se barrier are presented. The (Zn,Cd)Se barrier enables shifting of QDs energy emission down to 1.87 eV, that is below the energy of Mn$^{2+}$ ions internal transition (2.1 eV). This opens a perspective for implementation of epitaxial CdSe QDs doped with several Mn ions as, e. g., the light sources in high quantum yield magnetooptical devices. Polarization resolved Photoluminescence Excitation measurements of individual QDs reveal sharp ($Γ<$ 150 $μ$eV) maxima and transfer of optical…
A trion magnetic polaron formed by the exchange interaction of a positively charged exciton (trion) with localized spins of Mn$^{2+}$ ions is found experimentally in a 4\,nm wide Cd$_{0.98}$Mn$_{0.02}$Te/Cd$_{0.78}$Mn$_{0.02}$Mg$_{0.2}$Te quantum well containing resident holes. The experiment is performed at a temperature of 1.6 K using resonant excitation of the trion with circularly polarized light. The trion is formed from a resident hole, which is in a hole magnetic polaron state, and a photogenerated electron-hole pair. The dynamical evolution from the hole magnetic polaron to the trion m…
Effect of spin-dependent tunneling and intervalley scattering in magnetic-semiconductor van der Waals heterostructures on exciton and trion polarization
We present a comprehensive experimental and theoretical studies of photoluminescence of single CdMnTe quantum dots with Mn content x ranging from 0.01 to 0.2. We distinguish three stages of the equilibration of the exciton-Mn ion spin system and show that the intermediate stage, in which the exciton spin is relaxed, while the total equilibrium is not attained, gives rise to a specific asymmetric shape of the photoluminescence spectrum. From an excellent agreement between the measured and calculated spectra we are able to evaluate the exciton localization volume, number of paramagnetic Mn ions,…
Layered transition-metal dichalcogenides have attracted great interest in the last few years. Thinned down to the monolayer limit they change from an indirect band structure to a direct band gap in the visible region. Due to the monolayer thickness the inversion symmetry of the crystal is broken and spin and valley are coupled to each other. The degeneracy between the two equivalent valleys, K and K', respectively, can be lifted by applying an external magnetic field. Here, we present photoluminescence measurements of CVD-grown tungsten disulphide (WS${_2}$) monolayers at temperatures of 2 K. …
Vertically stacked van der Waals heterostructures constitute a promising platform for providing tailored band alignment with enhanced excitonic systems. Here we report observations of neutral and charged interlayer excitons in trilayer WSe2-MoSe2-WSe2 van der Waals heterostructures and their dynamics. The addition of a WSe2 layer in the trilayer leads to significantly higher photoluminescence quantum yields and tunable spectral resonance compared to its bilayer heterostructures at cryogenic temperatures. The observed enhancement in the photoluminescence quantum yield is due to significantly la…
