Ultrafast non-linear optical signal from a single quantum dot: exciton and biexciton effects

We present results on both the intensity and phase-dynamics of the transient non-linear optical response of a single quantum dot (SQD). The time evolution of the Four Wave Mixing (FWM) signal on a subpicosecond time scale is dominated by biexciton effects. In particular, for the cross-polarized excitation case a biexciton bound state is found. In this latter case, mean-field results are shown to give a poor description of the non-linear optical signal at small times. By properly treating exciton-exciton effects in a SQD, coherent oscillations in the FWM signal are clearly demonstrated. These oscillations, with a period corresponding to the inverse of the biexciton binding energy, are correlated with the phase dynamics of the system's polarization giving clear signatures of non-Markovian effects in the ultrafast regime.Comment: 10 pages, 3 figure

Reducing decoherence of the confined exciton state in a quantum dot by pulse-sequence control

We study the phonon-induced dephasing of the exciton state in a quantum dot excited by a sequence of ultra-short pulses. We show that the multiple-pulse control leads to a considerable improvement of the coherence of the optically excited state. For a fixed control time window, the optimized pulsed control often leads to a higher degree of coherence than the control by a smooth single Gaussian pulse. The reduction of dephasing is considerable already for 2-3 pulses.Comment: Final version (moderate changes

Experimental imaging and atomistic modeling of electron and hole quasiparticle wave functions in InAs/GaAs quantum dots

We present experimental magnetotunneling results and atomistic pseudopotential calculations of quasiparticle electron and hole wave functions of self-assembled InAs/GaAs quantum dots. The combination of a predictive theory along with the experimental results allows us to gain direct insight into the quantum states. We monitor the effects of (i) correlations, (ii) atomistic symmetry and (iii) piezoelectricity on the confined carriers and (iv) observe a peculiar charging sequence of holes that violates the Aufbau principle.Comment: Submitted to Physical Review B. A version of this paper with figures can be found at http://www.sst.nrel.gov/nano_pub/mts_preprint.pd

Full configuration interaction approach to the few-electron problem in artificial atoms

We present a new high-performance configuration interaction code optimally designed for the calculation of the lowest energy eigenstates of a few electrons in semiconductor quantum dots (also called artificial atoms) in the strong interaction regime. The implementation relies on a single-particle representation, but it is independent of the choice of the single-particle basis and, therefore, of the details of the device and configuration of external fields. Assuming no truncation of the Fock space of Slater determinants generated from the chosen single-particle basis, the code may tackle regimes where Coulomb interaction very effectively mixes many determinants. Typical strongly correlated systems lead to very large diagonalization problems; in our implementation, the secular equation is reduced to its minimal rank by exploiting the symmetry of the effective-mass interacting Hamiltonian, including square total spin. The resulting Hamiltonian is diagonalized via parallel implementation of the Lanczos algorithm. The code gives access to both wave functions and energies of first excited states. Excellent code scalability in a parallel environment is demonstrated; accuracy is tested for the case of up to eight electrons confined in a two-dimensional harmonic trap as the density is progressively diluted and correlation becomes dominant. Comparison with previous Quantum Monte Carlo simulations in the Wigner regime demonstrates power and flexibility of the method.Comment: RevTeX 4.0, 18 pages, 6 tables, 9 postscript b/w figures. Final version with new material. Section 6 on the excitation spectrum has been added. Some material has been moved to two appendices, which appear in the EPAPS web depository in the published versio

Tight-Binding model for semiconductor nanostructures

An empirical $s_cp^3_a$ tight-binding (TB) model is applied to the investigation of electronic states in semiconductor quantum dots. A basis set of three $p$-orbitals at the anions and one $s$-orbital at the cations is chosen. Matrix elements up to the second nearest neighbors and the spin-orbit coupling are included in our TB-model. The parametrization is chosen so that the effective masses, the spin-orbit-splitting and the gap energy of the bulk CdSe and ZnSe are reproduced. Within this reduced $s_cp_a^3$ TB-basis the valence (p-) bands are excellently reproduced and the conduction (s-) band is well reproduced close to the $\Gamma$-point, i.e. near to the band gap. In terms of this model much larger systems can be described than within a (more realistic) $sp^3s^*$-basis. The quantum dot is modelled by using the (bulk) TB-parameters for the particular material at those sites occupied by atoms of this material. Within this TB-model we study pyramidal-shaped CdSe quantum dots embedded in a ZnSe matrix and free spherical CdSe quantum dots (nanocrystals). Strain-effects are included by using an appropriate model strain field. Within the TB-model, the strain-effects can be artifically switched off to investigate the infuence of strain on the bound electronic states and, in particular, their spatial orientation. The theoretical results for spherical nanocrystals are compared with data from tunneling spectroscopy and optical experiments. Furthermore the influence of the spin-orbit coupling is investigated

Radiative corrections to the excitonic molecule state in GaAs microcavities

The optical properties of excitonic molecules (XXs) in GaAs-based quantum well microcavities (MCs) are studied, both theoretically and experimentally. We show that the radiative corrections to the XX state, the Lamb shift $\Delta^{\rm MC}_{\rm XX}$ and radiative width $\Gamma^{\rm MC}_{\rm XX}$, are large, about $10-30$ of the molecule binding energy $\epsilon_{\rm XX}$, and definitely cannot be neglected. The optics of excitonic molecules is dominated by the in-plane resonant dissociation of the molecules into outgoing 1$\lambda$-mode and 0$\lambda$-mode cavity polaritons. The later decay channel, ``excitonic molecule $\to$ 0$\lambda$-mode polariton + 0$\lambda$-mode polariton'', deals with the short-wavelength MC polaritons invisible in standard optical experiments, i.e., refers to ``hidden'' optics of microcavities. By using transient four-wave mixing and pump-probe spectroscopies, we infer that the radiative width, associated with excitonic molecules of the binding energy $\epsilon_{\rm XX} \simeq 0.9-1.1$ meV, is $\Gamma^{\rm MC}_{\rm XX} \simeq 0.2-0.3$ meV in the microcavities and $\Gamma^{\rm QW}_{\rm XX} \simeq 0.1$ meV in a reference GaAs single quantum well (QW). We show that for our high-quality quasi-two-dimensional nanostructures the $T_2 = 2 T_1$ limit, relevant to the XX states, holds at temperatures below 10 K, and that the bipolariton model of excitonic molecules explains quantitatively and self-consistently the measured XX radiative widths. We also find and characterize two critical points in the dependence of the radiative corrections against the microcavity detuning, and propose to use the critical points for high-precision measurements of the molecule bindingenergy and microcavity Rabi splitting.Comment: 16 pages, 11 figures, accepted for publication in Phys. Rev.

Excitons, biexcitons, and phonons in ultrathin CdSe/ZnSe quantum structures

The optical properties of CdSe nanostructures grown by migration-enhanced epitaxy of CdSe on ZnSe are studied by time-, energy-, and temperature-dependent photoluminescence and excitation spectroscopy, as well as by polarization-dependent four-wave mixing and two-photon absorption experiments. The nanostructures consist of a coherently strained Zn1−xCdxSe/ZnSe quantum well with embedded islands of higher Cd content with sizes of a few nanometer due to strain-induced CdSe accumulation. The local increase in CdSe concentration results in a strong localization of the excitonic wave function, in an increase in radiative lifetime, and a decrease of the dephasing rate. Local LO-phonon modes caused by the strong modulation of the Cd concentration profile are found in phonon-assisted relaxation processes. Confined biexcitons with large binding energies between 20 and 24 meV are observed, indicating the important role of biexcitons even at room temperature

Ultralong Dephasing Time in InGaAs Quantum Dots

We measure a dephasing time of several hundred picoseconds at low temperature in the groundstate transition of strongly confined InGaAs quantum dots, using a highly sensitive four-wave mixing technique. Between 7 and 100 K the polarization decay has two distinct components resulting in a non-Lorentzian line shape with a lifetime-limited zero-phonon line and a broadband from elastic excitonacoustic phonon interactions

Relaxation and dephasing of multiexcitons in semiconductor quantum dots

We measure the dephasing time of ground-state excitonic transitions in InGaAs quantum dots under electrical injection in the temperature range from 10 to 70 K. Electrical injection into the barrier region results in a pure dephasing of the excitonic transitions. Once the injected carriers fill the electronic ground state, the biexciton to exciton transition is probed and a correlation of the exciton and biexciton phonon scattering mechanisms is found. Additional filling of the excited states creates multiexcitons that show a fast dephasing due to population relaxation

Resonant hyper-Raman scattering in spherical quantum dots

A theoretical model of resonant hyper-Raman scattering by an ensemble of spherical semiconductor quantum dots has been developed. The electronic intermediate states are described as Wannier-Mott excitons in the framework of the envelope function approximation. The optical polar vibrational modes of the nanocrystallites (vibrons) and their interaction with the electronic system are analized with the help of a continuum model satisfying both the mechanical and electrostatic matching conditions at the interface. An explicit expression for the hyper-Raman scattering efficiency is derived, which is valid for incident two-photon energy close to the exciton resonances. The dipole selection rules for optical transitions and Fr\"ohlich-like exciton-lattice interaction are derived: It is shown that only exciton states with total angular momentum $L=0,1$ and vibrational modes with angular momentum $l_p=1$ contribute to the hyper-Raman scattering process. The associated exciton energies, wavefunctions, and vibron frequencies have been obtained for spherical CdSe zincblende-type nanocrystals, and the corresponding hyper-Raman scattering spectrum and resonance profile are calculated. Their dependence on the dot radius and the influence of the size distribution on them are also discussed.Comment: 12 pages REVTeX (two columns), 2 tables, 8 figure