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.     

Spin Physics of Excitons in Colloidal Nanocrystals

We present a review of spin-dependent properties of excitons in semiconductor colloidal nanocrystals. The photoluminescences (PL) properties of neutral and charged excitons (trions) are compared. The mechanisms and the polarization of radiative recombination of a “dark” (spin-forbidden) exciton that determines the low-temperature PL of colloidal nanocrystals are discussed in detail. The radiative recombination of a dark exciton becomes possible as a result of simultaneous flips of the surface spin and electron spin in a dark exciton that leads to admixture of bright exciton states. This recombination mechanism is effective in the case of a disordered state of the spin system and is suppressed if the polaron ferromagnetic state forms. The conditions and various mechanisms of formation of the spin polaron state and possibilities of its experimental detection are discussed. The experimental and theoretical studies of magnetic field-induced circular polarization of PL in ensembles of colloidal nanocrystals are reviewed.     

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.     

Temperature dependence of radiative recombination in CdSe quantum dots with enhanced confinement

We studied in details the recombination dynamics and its temperature dependence in epitaxially grown neutral CdSe/ZnSSe quantum dots with additional wide-band gap MgS barriers. Such design allows to preserve a very high quantum yield and track the radiative recombination dynamics up to room temperature. A fast initial decay of ∼0.6 ns followed by a slow decay with a time constant ∼30–50 ns is observed at low temperature T < 50 K. The fast decay gradually disappears with increasing temperature while the slow decay shortens and above 100 K predominantly a single-exponential decay is observed with a time constant ∼1.3 ns, which is weekly temperature dependent up to 300 K. To explain the experimental findings, a two-level model which includes bright and dark exciton states and a temperature dependent spin-flip between them is considered. According to the model, it is a thermal activation of the dark exciton to the bright state and its consequent radiative recombination that results in the long decay tail at low temperature. The doubling of the decay time at high temperatures manifests a thermal equilibrium between the dark and bright excitons.     

Direct observation of deep excitonic states in the photoluminescence spectra of single-walled carbon nanotubes

Low-energy, dark excitonic states have recently been predicted to lie below the first bright (E11) exciton in semiconducting single-walled carbon nanotubes [Phys. Rev. Lett. 93, 157402 (2004)10.1103/PhysRevLett.93.157402]. Decay into such deep excitonic states is implicated as a mechanism which reduces photoluminescence quantum yields. In this study we report the first direct observation of deep excitons in SWNTs. Photoluminescence (PL) microscopy of suspended semiconducting single-walled carbon nanotubes (SWNTs) reveals weak emission satellites redshifted by approximately 38-45 and approximately 100-130 meV relative to the main E11 PL emission peaks. Similar satellites, redshifted by 95-145 meV depending on nanotube species, were also found in PL measurements of ensembles of SWNTs in water-surfactant dispersions. The relative intensities of these deep exciton emission features depend on the nanotube surroundings.     

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.     

Direct observation of dark excitons in individual carbon nanotubes: inhomogeneity in the exchange splitting

We report the direct observation of spin-singlet dark excitons in individual single-walled carbon nanotubes through low-temperature micro-magneto-photoluminescence spectroscopy. A magnetic field (B) applied along the tube axis brightened the dark state, leading to the emergence of a new emission peak. The peak rapidly grew in intensity with increasing B at the expense of the originally dominated bright exciton peak and became dominant at B>3 T. This behavior, universally observed for more than 50 tubes of different chiralities, can be quantitatively modeled by incorporating the Aharonov-Bohm effect and intervalley Coulomb mixing. The directly measured dark-bright splitting values were 1-4 meV for tube diameters 1.0-1.3 nm. Scatter in the splitting value emphasizes the role of the local environment surrounding a nanotube in determining its excitonic fine structure.     

Photoluminescence spectra of nitrogen implanted GaSe crystals

GaSe single crystals were N-implanted along c-axis with ion beams of 10¹⁴ and 10¹⁶ ions/cm² doses having energy values of 60 and 100 keV. The photoluminescence (PL) spectra of undoped and N-implanted GaSe crystals were measured at different temperatures. The PL intensity was observed to decrease with increasing implantation dose while the FWHM of the exciton peaks increased. In heavily doped crystals, due to the interaction with the radiation induced disorders, the wave vector selection rules are satisfied and an indirect exciton PL band is observed 36 meV below the direct exciton states.     

电场调控下不对称耦合量子点中激子的发光特性

使用有效质量模型,从理论上对GaAs/A10.35Ga0.65As不对称耦合量子点在不同耦合强度下束缚态和反束缚态的能级分裂情况进行了详细分析,重点探讨了电子和空穴的耦合隧穿对量子点体系能级特征及激子发光强度的影响.研究发现:不对称耦合量子点在外电场作用下价带束缚态和反束缚态能级出现反交现象,反交处的能级分裂值和临界电...     

Role of bright and dark excitons in the temperature-dependent photoluminescence of carbon nanotubes

We report studies of the temperature dependence of the photoluminescence efficiency of single walled carbon nanotubes which demonstrate the role of bright and dark excitons. This is determined by the energy splitting of the excitons combined with 1-D excitonic properties. The splitting of the bright and dark singlet exciton states is found to be only a few meV and is very strongly diameter dependent for diameters in the range 0.8-1.2 nm. The luminescence intensities are also found to be strongly enhanced by magnetic fields at low temperatures due to mixing of the exciton states.     

K_2分子在强激光场下的量子调控:缀饰态选择性分布

利用含时量子波包法理论研究了分子在强激光场条件下的量子调控.选取K2分子的三态模型(基态|X〉、激发态|B〉和电离态|X+〉)作为研究对象.在强激光场的作用下,激发态|B〉缀饰成两个子态:|α〉态和|β〉态.分析K2分子电离后的光电子能谱,可以得到缀饰态|α〉和|β〉的能量和概率分布信息.同时,根据分子的缀饰态理论,提出了K2分子的缀饰态选择性分布方案.研究表明:调节激光场的强度可以实现对缀饰态能量的调控,改变激光场的波长可以实现对缀饰态概率的选择性分布.     

Time-resolved studies of single quantum dots in magnetic fields

We present time-resolved and time-integrated spectroscopy of single InAs quantum dots grown in a GaAs matrix. We observe a number of interesting features in the spectra, including the zero field splitting of exciton and biexciton lines due to quantum dot asymmetry. By the application of an in-plane magnetic field, the normally optically active and inactive exciton states become mixed, enabling us to optically probe the normally inaccessible ‘dark’ states. Time resolved measurements on the mixed states show decay times several times longer than the exciton lifetime at zero field, which we show to be consistent with a dark exciton lifetime orders of magnitude longer than that for bright exciton.     

Band-edge exciton fine structure of single CdSe/ZnS nanocrystals in external magnetic fields

We report a spectroscopic study of the two lowest-energy exciton levels of individual CdSe/ZnS nanocrystals under applied magnetic fields. Field-induced coupling between the bright and the dark excitonic states is directly observed in the low-temperature photoluminescence spectrum and decay and allows the determination of the angle between the nanocrystal c axis and the field. Orientation-dependent Zeeman splittings of the dark and bright exciton sublevels are measured and provide the corresponding exciton Landé factors, as well as spin-flip relaxation rates between Zeeman sublevels.     

Fine structure of highly charged excitons in semiconductor quantum dots

An exciton in a symmetric semiconductor quantum dot has two possible states, one dark and one bright, split in energy by the electron-hole exchange interaction. We demonstrate that for a doubly charged exciton, there are also two states split by the electron-hole exchange, but both states are now bright. We also uncover a fine structure in the emission from the triply charged exciton. By measuring these splittings, and also those from the singly charged and doubly charged biexcitons, all on the same quantum dot, we show how the various electron-hole exchange energies can be measured without having to break the symmetry of the dot.     

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.     

Magnetoreflectance of the Γ6 – Γ8 exciton ground state in cubic ZnSe

Magnetoreflectance measurements on the ground state of the Γ₆ – Γ₈ free exciton in cubic ZnSe in magnetic fields up to 18 T are reported. The splitting between the |1, ±1〉 states was derived from the measured difference spectrum between σ⁺ and σ^--polarized reflectance in Faraday configuration. The splitting between the two states corresponding to |2, 0〉 and |1, 0〉 at B = 0 was determined by means of a lineshape analysis. We derive an electron g-factor g = 1.48 ± 0.25, in reasonable agreement with existing k · p calculations, and obtain an effective hole g-value $\text{K}\text{?}\text{= -0.26±0.06}$. In addition, we find an upper limit for the short range electron-hole spin exchange energy Δ ? 0.1 meV, which is considerably smaller than values, which is considerably smaller than values reported in the literature, but agrees with recent results on ZnTe obtained by uniaxial stress and also magnetoreflectance measurements.     

Resonant exciton trapping at impurity states in silver bromide

Excitation spectra near the indirect exciton edge of AgBr at 1.8K are reported for several luminescence lines from weakly localized excitons. Excitation below the exciton absorption threshold reveals several excited bound exciton states the energetic positions of which are determined. For excitation above the threshold, strong energy dependent structure is observed. It is interpreted in terms of resonant trapping of free excitons in both ground and excited bound exciton states associated with emission of LO(Γ), long wavelength acoustic and intervalley TA(X) and LA(X) phonons as well as combinations and overtones of these. From measurements in doped crystals two bound exciton systems are found to be correlated with Cd²⁺ and Ca²⁺, respectively.     

Optical anisotropy and the direction of polarization of exciton emissions in a semiconductor quantum dot:Effect of heavy-and light-hole mixing

The dependence of the directions of polarization of exciton emissions, fine structure splittings(FSS), and polarization anisotropy on the light-and heavy-hole(LH–HH) mixing in semiconductor quantum dots(QDs) is investigated using a mesoscopic model. In general, all QDs have a four-fold exciton ground state. Two exciton states have directions of polarization in the growth-plane, while the other two are along the growth direction of the QD. The LH–HH mixing does affect the FSS and polarization anisotropy of bright exciton states in the growth-plane in the low symmetry QDs(e.g., C_(2V),C_S, C_1), while it has no effect on the FSS and polarization anisotropy in high symmetry QDs(e.g., C_(3V), D_(2d)). When the hole ground state is pure HH or LH, the bright exciton states in the growth-plane are normal to each other. The LH–HH mixing affects the relative intensities and directions of bright exciton states in the growth-plane of the QD. The polarization anisotropy of exciton emissions in the growth-plane of the QD is independent of the phase angle of LH–HH mixing but strongly depends on the magnitude of LH–HH mixing in low symmetry QDs.     

Energy of K-momentum dark excitons in carbon nanotubes by optical spectroscopy

Phonon sideband optical spectroscopy determines the energy of the dark K-momentum exciton for (6,5) carbon nanotubes. One-phonon sidebands appear in absorption and emission, split by two zone-boundary (K-point) phonons. Their average energy locates the E11 K-momentum exciton 36 meV above the E11 bright level, higher than available theoretical estimates. A model for exciton-phonon coupling shows the absorbance sideband depends sensitively on the K-momentum exciton effective mass and has minimal contributions from zone-center phonons, which dominate the Raman spectra of carbon nanotubes.     

Electronic structure of ZnO wurtzite quantum wires

The electronic structure and optical properties of ZnO wurtzite quantum wires with radius R≥3 nm are studied in the framework of six-band effective-mass envelope function theory. The hole effective-mass parameters of ZnO wurtzite material are calculated by the empirical pseudopotential method. It is found that the electron states are either two-fold or four-fold degenerate. There is a dark exciton effect when the radius R of the ZnO quantum wires is in the range of [3,19.1] nm (dark range in our model). The dark ranges of other wurtzite semiconductor quantum wires are calculated for comparison. The dark range becomes smaller when the |Δ_so| is larger, which also happens in the quantum-dot systems. The linear polarization factor of ZnO quantum wires is larger when the temperature is higher.