Evidence for dark excitons in a single carbon nanotube due to the Aharonov-Bohm effect

We studied exciton structures and the Aharonov-Bohm effect in a single carbon nanotube using micro-photoluminescence (PL) spectroscopy under a magnetic field at low temperatures. A single sharp PL peak from the bright exciton state of a single carbon nanotube was observed under zero magnetic field, and the additional PL of dark exciton state appeared below the bright exciton peak under high magnetic fields. It was found that the split between the bright and dark exciton states is several millielectron volts at zero field. The tube diameter dependence of the splitting arises from the intervalley short-range Coulomb interaction.     

Coherent optical writing and reading of the exciton spin state in single quantum dots

We demonstrate a one-to-one correspondence between the polarization state of a light pulse tuned to neutral exciton resonances of single semiconductor quantum dots and the spin state of the exciton that it photogenerates. This is accomplished using two variably polarized and independently tuned picosecond laser pulses. The first "writes" the spin state of the resonantly excited exciton. The second is tuned to biexcitonic resonances, and its absorption is used to "read" the exciton spin state. The absorption of the second pulse depends on its polarization relative to the exciton spin direction. Changes in the exciton spin result in corresponding changes in the intensity of the photoluminescence from the biexciton lines which we monitor, obtaining thus a one-to-one mapping between any point on the Poincaré sphere of the light polarization to a point on the Bloch sphere of the exciton spin.     

Inversion of the exciton fine structure splitting in quantum dots

The fine structure splitting of exciton state was measured for a large number of single InAs quantum dots in GaAs. It is shown to decrease as the exciton confinement decreases, crucially passing through zero and changing sign. Degeneracy of the exciton spin states is an important step to producing entangled photons from the biexciton cascade. Thermal annealing reduces the exciton confinement and thereby increases the number of degenerate dots in a particular sample.     

Single molecule photobleaching probes the exciton wave function in a multichromophoric system

The exciton wave function of a trichromophoric system is investigated by means of single molecule spectroscopy at room temperature. Individual trimers exhibit superradiance and loss of vibronic structure in emission spectrum, features proving exciton delocalization. We identify two distinct photodegradation pathways for single trimers upon sequential photobleaching of the chromophores. The rate of each pathway is a measure for the contribution of the separate dyes to the collective excited state of the system, in this way probing the wave function of the delocalized exciton.     

Direct observation of dark exciton states in single carbon nanotubes

We have studied magneto-photoluminescence (PL) spectra of a single carbon nanotube at low temperatures. A single PL peak arising from optically allowed (bright) exciton state was observed under the zero-magnetic field, and an additional PL peak from optically forbidden (dark) exciton state was enhanced with increasing the magnetic field. Excitons populate in the lower dark state at low temperatures, and the optically forbidden transition is observed due to the Aharonov-Bohm effect.     

Shallow acceptor bound exciton and free exciton states in high-purity zinc telluride

We investigated excitons bound to shallow acceptors in high-purity ZnTe and measured excitation spectra of two-hole luminescence lines at 1.6 K using a tunable dye-laser. The electron-hole coupling in the bound exciton (BE) states appears to be very different for the various acceptors even for almost identical exciton localisation energies. Three different types of BE are reported. For the Li-acceptor BE we observe three sub-components separated by 0.22 and 0.17 meV and interpreted as J = $\text{1}\text{2}$, $\text{3}\text{2}$, $\text{5}\text{2}$ states. The Ag-acceptor BE exhibits a strong ground state and a weak excited state at 1.3 meV higher energy. For the as yet unidentified k-acceptor we observe a single BE level, degenerate with the Ag-acceptor BE ground state. Dips in the excitation spectra due to absorption into free exciton 1S, 2S, and 3S states yield an exciton Rydberg R₀ = 12.8±0.3 meV and a free exciton binding energy FE(1S) = 13.2±0.3 meV.     

Fine structure of excitons in self-assembled In0.60Ga0.40As quantum dots: Zeeman-interaction and exchange energy enhancement

The fine structure of the ground state exciton has been studied by magnetophotoluminescence spectroscopy of self-assembled In_0.60Ga_0.40As single quantum dots. This was realized by using lithography for fabricating mesa structures which contain only a single dot. Due to a dot geometry-induced symmetry breaking we are able to observe the dark exciton states in magnetic field besides the bright excitons. From the spin-splitting data values for the corresponding exciton g-factors are obtained. In addition, the electron–hole exchange energies are determined, which are compared to detailed numerical calculations.     

Exciton states in wurtzite InGaN/GaN quantum wells: Strong built-in electric field and interface optical-phonon effects

Considering the strong built-in electric field (BEF) effects and large exciton–phonon interactions, we investigate the exciton states confined in an InGaN/GaN single quantum well (QW) by using the Lee–Low–Pines variational method. We find that the exciton state modification caused by the exciton–phonon interactions is remarkable. The exciton energy shift due to exciton–phonon interactions increases monotonically if the well width increases. With increasing the In fraction, the exciton energy shift firstly increases to a maximum, then decreases. The BEF has a significant influence on the exciton states in a QW with large well width. The physical reasons have been analyzed in detail. Good agreement for the zero-phonon peak energies and the Huang–Rhys factor has been obtained between our numerical results and the corresponding experimental measurements.     

Nonradiative heterofusion of excitons in doped organic molecular crystals

The nonradiative heterofusion of a host exciton with a guest molecule electronic excitation resulting in a higher electronic neutral single excited state is examined theoretically in the doped organic molecular crystals. The heterofusion process is treated as a nonradiative spontaneous multi-lattice phonon transition of the crystal from the electronic double excited initial state to the electronic single excited final state under the action of the interaction between the host molecules and the guest molecule. Two heterofusion channels are considered: the first one resulting in a higher electronic excited state of the guest molecule and the second one resulting in a higher host exciton state. The corresponding rate constants are calculated and discussed within the framework of the first order time dependent perturbation theory.     

Phonon-assisted decoherence in the production of polarization-entangled photons in a single semiconductor quantum dot

We theoretically investigate the production of polarization-entangled photons through the biexciton cascade decay in a single semiconductor quantum dot. In the intermediate state the entanglement is encoded in the polarizations of the first emitted photon and the exciton, where the exciton state can be effectively "measured" by the solid-state environment through the formation of a lattice distortion. We show that the resulting loss of entanglement becomes drastically enhanced if the phonons contributing to the lattice distortion are subject to elastic scatterings at the device boundaries, which might constitute a serious limitation for quantum-dot based entangled-photon devices.     

Coherent control in a single semiconductor quantum dot exhibiting excitonic and biexcitonic features

We have developed a simplified theoretical model to analyze the phenomenon of coherent control in a single semiconductor quantum dot excited by a pair of optical pulses. The first pulse populates a biexciton state by two-photon absorption while the second pulse generates population in the exciton state via deexcitation from the biexciton state. We have used density-matrix analysis for a 3-level system to calculate the time dependent biexciton and exciton state populations. The usual 9×9 matrix has been reduced to a 6×6 matrix. The time variation of the population in each state and it’s dependence on the pulse delay manifest coherent control. Numerical estimates made for In_0.5Ga_0.5As/GaAs single quantum dots qualitatively agree with the recent experimental results. PACS 78.67.Hc; 42.50.Md; 78.55.Cr     

Oxygen-related band gap state in single crystal rubrene

A molecular exciton signature is established and investigated under different ambient conditions in rubrene single crystals. An oxygen-related band gap state is found to form in the ambient atmosphere. This state acts as an acceptor center and assists in the fast dissociation of excitons, resulting in a higher dark and photoconductivity of oxidized rubrene. The band gap state produces a well-defined photoluminescence band at an energy 0.25 eV below the energy of the 0-0 molecular exciton transition. Two-photon excitation spectroscopy shows that the states are concentrated near the surface of naturally oxidized rubrene.     

Surface-enhanced emission from single semiconductor nanocrystals

The fluorescence behavior of single CdSe(ZnS) core-shell nanocrystal (NC) quantum dots is dramatically affected by electromagnetic interactions with a rough metal film. Observed changes include a fivefold increase in the observed fluorescence intensity of single NCs, a striking reduction in their fluorescence blinking behavior, complete conversion of the emission polarization to linear, and single NC exciton lifetimes that are >10(3) times faster. The enhanced excited state decay process for NCs coupled to rough metal substrates effectively competes with the Auger relaxation process, allowing us to observe both charged and neutral exciton emission from these NC quantum dots.     

Probing the spin state of a single magnetic ion in an individual quantum dot

The magnetic state of a single magnetic ion (Mn2+) embedded in an individual quantum dot is optically probed using microspectroscopy. The fine structure of a confined exciton in the exchange field of a single Mn2+ ion (S=5/2) is analyzed in detail. The exciton-Mn2+ exchange interaction shifts the energy of the exciton depending on the Mn2+ spin component and six emission lines are observed at zero magnetic field. Magneto-optic measurements reveal that the emission intensities in both circular polarizations are controlled by the Mn2+ spin distribution imposed by the exchange interaction with the exciton, the magnetic field, and an effective manganese temperature which depends on both the lattice temperature and the density of photocreated carriers. Under magnetic field, the electron-Mn interaction induces a mixing of the bright and dark exciton states.     

Tuning of exciton states in a magnetic quantum ring

The exciton states in a CdTe quantum ring subjected to an external magnetic field containing a single magnetic impurity are investigated. We have used the multiband approximation which includes the heavy hole–light hole coupling effects. The electron–hole spin interactions and the s, p–d interactions between the electron, the hole and the magnetic impurity are also included. The exciton energy levels and optical transitions are evaluated using the exact diagonalization scheme. We show that due to the spin interactions it is possible to change the bright exciton state into the dark state and vice versa with the help of a magnetic field. We propose a new route to experimentally estimate the s, p–d spin interaction constants.     

Radiative life time of an exciton confined in a strained GaN/Ga1-xAlxN cylindrical dot: built-in electric field effects

The binding energy of an exciton in a wurtzite GaN/GaAlN strained cylindrical quantum dot is investigated theoretically.The strong built-in electric field due to the spontaneous and piezoelectric polarizations of a GaN/GaAlN quantum dot is included.Numerical calculations are performed using a variational procedure within the single band effective mass approximation.Valence-band anisotropy is included in our theoretical model by using different hole masses in different spatial directions.The exciton oscillator strength and the exciton lifetime for radiative recombination each as a function of dot radius have been computed.The result elucidates that the strong built-in electric field influences the oscillator strength and the recombination life time of the exciton.It is observed that the ground state exciton binding energy and the interband emission energy increase when the cylindrical quantum dot height or radius is decreased,and that the exciton binding energy,the oscillator strength and the radiative lifetime each as a function of structural parameters (height and radius) sensitively depend on the strong built-in electric field.The obtained results are useful for the design of some opto-photoelectronic devices.     

Eigenstate symmetry probed by biexciton transitions in a single quantum dot

The eigenstate symmetry in CdSe/ZnSe single quantum dots (SQDs) has been studied by low-temperature magnetoluminescence spectroscopy. Regarding both, the fine structure splitting and the polarization properties of the biexciton transition, the influence of exchange and Zeeman interaction on the eigenstate symmetry of the final state of recombination, the ground state of the single exciton, is investigated.     

Exciton fine structure splitting of single InGaAs self-assembled quantum dots

We show how the resonant absorption of the ground state neutral exciton confined in a single InGaAs self-assembled quantum dot can be directly observed in an optical transmission experiment. A spectrum of the differential transmitted intensity is obtained by sweeping the exciton energy into resonance with laser photons exploiting the voltage induced Stark-shift. We describe the details of this experimental technique and some example results which exploit the 1 μeV spectral resolution. In addition to the fine structure splitting of the neutral exciton and an upper bound on the homogeneous linewidth at 4.2 K, we also determine the transition electric dipole moment.     

Effects of excitation spectral width on decay profile of weakly confined excitons

We report the effect due to a simultaneous excitation of several exciton states on the radiative decay profiles on the basis of the nonlocal response of weakly confined excitons in GaAs thin films. In the case of excitation of single exciton state, the transient grating signal has two decay components. The fast decay component comes from nonlocal response, and the long-lived component is attributed to free exciton decay. With an increase of excitation spectral width, the nonlocal component becomes small in comparison with the long-lived component, and disappears under irradiation of a femtosecond-pulse laser with broader spectral width. The transient grating spectra clearly indicates the contribution of the weakly confined excitons to the signal, and the exciton line width hardly changes by excitation spectral width. From these results, we concluded that the change of decay profile is attributed not to the many-body effect but to the effect of simultaneous excitation of several exciton states.     

Interferometric spectroscopy for excitons in InP single quantum dots

Dynamical dephasing processes of an exciton and a charged exciton in single InP quantum dots were studied by using interferometric spectroscopy. Interferometric spectroscopy enabled us to observe with high sensitivity the dephasing of exciton or other exciton complexes in single quantum dots. In order to observe the dephasing of the exciton or exciton complexes, emitted single-photons generated from single InP quantum dots were detected through the Michelson interferometer. The contrast of the interferometric signal due to the exciton and the charged exciton shows non-exponential decay under band-to-band excitation for the GaInP matrix. The band-to-band excitation generates carriers trapped in the matrix and the trapped carriers modulate the energy of the quantum dots because of the quantum-confined Stark effect. Therefore the non-exponential decays are caused by energy fluctuation due to the trap carriers in the long timescale.