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.     

Room-temperature exciton storage in elongated semiconductor nanocrystals

The excited state of colloidal nanoheterostructures consisting of a spherical CdSe nanocrystal with an epitaxially attached CdS rod can be perturbed effectively by electric fields. Field-induced fluorescence quenching coincides with a conversion of the excited state species from the bright exciton to a metastable trapped state (dark exciton) characterized by a power-law luminescence decay. The conversion is reversible so that up to 10% of quenched excitons recombine radiatively post turn-off of a 1 micro s field pulse, increasing the delayed luminescence by a factor of 80. Excitons can be stored for up to 10(5) times the natural lifetime, opening up applications in optical memory elements.     

Excitons and many-electron effects in the optical response of single-walled boron nitride nanotubes

We report first-principles calculations of the effects of quasiparticle self-energy and electron-hole interaction on the optical properties of single-walled boron nitride nanotubes. Excitonic effects are shown to be even more important in BN nanotubes than in carbon nanotubes. Electron-hole interactions give rise to complexes of bright (and dark) excitons, which qualitatively alter the optical response. Excitons with a binding energy larger than 2 eV are found in the BN nanotubes. Moreover, unlike the carbon nanotubes, theory predicts that these exciton states are comprised of coherent supposition of transitions from several different subband pairs, giving rise to novel behaviors.     

Observation of charged excitons in hole-doped carbon nanotubes using photoluminescence and absorption spectroscopy

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.     

Exciton lifetime in quantum well with vicinal high-density excitons

Radiative lifetime of an exciton in a GaAs quantum well (QW) is controlled by high-density excitons, which restrict the exciton coherence through scattering. In order to circumvent the phase space filling effect of high-density excitons, we have prepared a QW structure in such a way that a reservoir for high-density excitons is separated from the QW. The lifetime increases (up to 30%) with the exciton density in the reservoir and saturates at 1×10¹⁷/cm³. The upper bound lifetime is determined by the excitonic relative motion.     

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.     

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.     

Bose-einstein condensation of exciton polaritons in high-<Emphasis Type="Italic">Q</Emphasis> planar microcavities with GaAs quantum wells

Condensation of exciton polaritons in planar microcavities with GaAs/AlAs quantum wells in the active area has been studied. It has been found that an increase in the lifetime of polaritons up to ∼10–15 ps when the Q factor of a microcavity exceeds 7000 makes it possible to detect Bose-Einstein condensation of polaritons with a dominant (>90%) photon component. Condensation occurs under thermodynamically nonequilibrium conditions in lateral traps with diameters ∼10 μm formed due to long-range fluctuations of the polariton potential. The violet shift of the polariton emission line at the condensation threshold significantly exceeds the energy of the repulsive interaction between polaritons in the condensate. It has been shown that the shift is mainly due to a decrease in the oscillator strength of bright excitons in lateral traps, caused by the localization of photoexcited long-living dark excitons.     

Fluorescence dynamics and fine structure of dark excitons in semiconducting single-wall carbon nanotubes

Exact diagonalization results are reported for the bright and dark exciton structure of semiconducting single-wall carbon nanotubes in the framework of the Hubbard model combined with a small crystal approach for several values of the correlation coupling strength U/t. Our findings, in the low-intermediate correlation regime (1.5 < U/t < 2.1), show the presence of dark states above and below the first bright exciton |B> and can account for reported experimental values of deep triplet states below |B> and of a K-momentum singlet dark exciton above this state. In order to fit the temporal profile of the photoluminescence (PL) decay, a bottleneck mechanism is considered involving a few dark states, with the respective energy gaps correspondingly obtained in the above-mentioned correlation range. We find that a kinetic model with one dark state above and two below |B> is able to recover the observed biexponential features of the PL behaviour with a reasonable set of parameters. Within this model we attribute the long tail of the PL to a delayed luminescence process of the bright state caused by the nearby calculated dark states.     

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.     

Electron-electron interaction effects on the optical excitations of semiconducting single-walled carbon nanotubes

We report correlated-electron calculations of optically excited states in ten semiconducting single-walled carbon nanotubes with a wide range of diameters. Optical excitation occurs to excitons whose binding energies decrease with increasing nanotube diameter, and are smaller than the binding energy of an isolated strand of poly-(paraphenylene vinylene). The ratio of the energy of the second optical exciton polarized along the nanotube axis to that of the lowest exciton is smaller than the value predicted within single-particle theory. The experimentally observed weak photoluminescence is an intrinsic feature of semiconducting nanotubes.     

Phonon and electronic nonradiative decay mechanisms of excitons in carbon nanotubes

We investigate theoretically the rates of nonradiative decay of excited semiconducting nanotubes by a variety of decay mechanisms and compare them with experimental findings. We find that the multiphonon decay (MPD) of free excitons is too slow to be responsible for the experimentally observed lifetimes. However, MPD lifetimes of localized excitons could be 2-3 orders of magnitude shorter. We also propose a new decay mechanism that relies on a finite doping of nanotubes and involves exciton decay into an optical phonon and an intraband electron-hole pair. The resulting lifetime is in the range of 5 to 100 ps, even for a moderate doping level.     

Optical traps for dark excitons

We propose a mechanism for optical trapping of dark excitons by linearly polarized unabsorbed standing waves, with a potential depth of the order of a few meV. Since this trapping, based on carrier exchanges with virtual excitons coupled to unabsorbed photons, equally acts on bright and dark states, Bose-Einstein condensation of excitons--which occurs in dark states--must appear as dark spots in a cloud of bright excitons, at the trap potential minima, when the temperature decreases.     

Charged and neutral biexciton–exciton cascade in a single quantum dot within a photonic bandgap

We investigate the recombination dynamics of positively charged and neutral biexcitons and excitons in a single InAs/GaAs quantum dot (QD) within a two-dimensional (2D) photonic bandgap (PBG). The 2D PBG makes the exciton lifetime four times longer and enhances photon-extraction efficiency compared to those without the PBG. Photon cross-correlation measurements demonstrate the cascade emissions of both charged and neutral biexcitons–excitons from the same QD. In the charged case, a hole in the p-shell relaxes into the s-shell between the cascade, and the corresponding transition is confirmed based on the spin configuration. The long exciton lifetime with the PBG helps us to reveal the spin dynamics that did not clearly appear in intrinsic 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.     

WS_2与WSe_2单层膜中的A激子及其自旋动力学特性研究

单层过渡金属硫化物由于其特有的激子效应以及强自旋-谷耦合性质,在光电子学及谷电子学等方面有着很广阔的应用前景.利用超快时间分辨光谱,本文系统地比较了两类钨基单层硫化物(WS_2和WSe_2)的A-激子动力学和谷自旋弛豫特性.实验结果表明, WS_2单层膜的A-激子弛豫表现为双指数过程,而对于WSe_2,其A-激子衰减表现为三指数过程,且激子的寿命远长于前者. WS_2谷自旋极化弛豫表现为单指数衰减,其寿命约0.35 ps,主要由电子-空穴交换作用所主导.而对于WSe_2,谷自旋弛豫表现出双指数弛豫特性:一个寿命为0.5 ps的快过程和一个寿命为28 ps的慢过程.快过程的弛豫来源于电子-空穴交换作用,而慢过程则由于自旋晶格散射形成暗激子的过程.通过调谐抽运光波长,进一步证实WSe_2较WS_2更容易形成暗激子.     

Lifetime of quasiparticles in a hybrid electron-exciton system

The lifetimes (damping) of one-body and collective excitations in a hybrid system consisting of spatially separated layers of a two-dimensional electron gas and a gas of indirect excitons have been calculated at zero temperature in the presence of the Bose-Einstein condensate of excitons. It has been shown that the electron-exciton interaction leads to a considerable shortening of the lifetime of electrons as compared to the electron-electron interaction and to the appearance of a nonzero (linear in the wave vector) damping of plasmons. The interaction of the exciton Bose gas with the electron layer induces damping of Bogoliubov phonons in the exciton Bose gas, which is, however, much lower than their intrinsic (Belyaev) damping.     

Photoluminescence of “dark” excitons in CdMnTe quantum well, embedded in a microcavity

A diluted magnetic semiconductor (DMS) quantum well (QW) microcavity operating in the limit of the strong coupling regime is studied by magnetoptical experiments. The interest of DMS QW relies on the possibility to vary the excitonic resonance over a wide range of energies by applying an external magnetic field, typically about 30 meV for 5 T in our sample. In particular, the anticrossing between the QW exciton and the cavity mode can be tuned by the external field. We observe the anticrossing and formation of exciton polaritons in magneto-reflectivity experiments. In contrast, magneto-luminescence exhibits purely excitonic character. Under resonant excitation conditions an additional emission line is observed at the energy of the dark exciton. The creation of dark excitons is made possible due to heavy hole–light hole mixing in the QW. The emission at this energy could be due to a combined spin flip of an electron and a bright exciton recombination.     

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.     

Radiative dark–bright instability and the critical Casimir effect in DQW exciton condensates

It is already well known that radiative interband interaction in the excitonic normal liquid in semiconducting double quantum wells is responsible for a negligible splitting between the energies of the dark and bright excitons enabling us to consider a four fold spin degeneracy. This has also lead many workers to naively consider the same degeneracy in studying the condensate. On the other hand, the non-perturbative aspects of this interaction in the condensed phase, e.g. its consequences on the order parameter and the dark–bright mixture in the ground state have not been explored. In this work, we demonstrate that the ground state concentrations of the dark and the bright exciton condensates are dramatically different beyond a sharp interband coupling threshold where the contribution of the bright component in the ground state vanishes. This shows that the effect of the radiative interband interaction on the condensate is nonperturbative.We also observe in the free energy a discontinuous derivative with respect to the layer separation at the entrance to the condensed phase, indicating a strong critical Casimir force. An estimate of its strength shows that it is measurable. Measuring the Casimir force is challenging, but at the same time it has a conclusive power about the presence of the long sought for condensed phase.