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.     

Intersubband exciton relaxation dynamics in single-walled carbon nanotubes

We study exciton (EX) dynamics in single-walled carbon nanotubes (SWNTs) included in polymethylmethacrylate by two-color pump-probe experiments with unprecedented temporal resolution. In the semiconducting SWNTs, we resolve the intersubband energy relaxation from the EX2 to the EX1 transition and find time constants of about 40 fs. The observation of a photoinduced absorption band strictly correlated to the photobleaching of the EX1 transition supports the excitonic model for primary excitations in SWNTs. We also detect in the time domain coherent oscillations due to the radial breathing modes at approximately 250 cm(-1).     

Multiphonon Raman scattering from individual single-walled carbon nanotubes

Combinations of up to 6 zone-edge and zone-center optical phonons are observed in the Raman spectra of individual single-walled carbon nanotubes (SWNTs). These multiphonon Raman modes exhibit distinct signatures of the one-dimensional nature of SWNTs and provide information on the phonon structure, exciton-phonon coupling, and excitonic transitions in nanotubes.     

Linear and nonlinear excitonic absorption in semiconducting quantum wires crystallized in a dielectric matrix

Spectra of linear and nonlinear absorption of GaAs and CdSe semiconducting quantum wires crystallized in a transparent dielectric matrix (inside chrysotile-asbestos nanotubes) have been measured. Their features are interpreted in terms of excitonic transitions and filling of the exciton phase space in the quantum wires. The theoretical model presented here has allowed us to calculate the energies of excitonic transitions that are in qualitative agreement with experimental data. The calculated exciton binding energies in quantum wires are a factor of several tens higher than in bulk semiconductors. The cause of this increase in the exciton binding energy is not only the size quantization, but also the “dielectric enhancement,” i.e., stronger attraction between electrons and holes owing to the large difference between permittivities of the semiconductor and dielectric matrix. Zh. éksp. Teor. Fiz. 114, 700–710 (August 1998)     

Structure Dependence of Excitonic Effects in Chiral Graphene Nanoribbons

We explore the excitonic effects in chiral graphene nanoribbons(cGNRs), whose edges are composed alternatively of armchair-edged and zigzag-edged segments. For cGNRs dominated by armchair edges, their energy gaps and exciton energies decrease with increasing chirality angles, and they, as functions of widths, oscillate with the period of three, while the exciton binding energies do not have such distinct oscillation. On the other hand,for cGNRs dominated by zigzag edges, all the energy gaps, exciton energies, and exciton binding energies show oscillation properties with their widths, due to the interactions between the edge states localized at the opposite zigzag edges. In addition, the triplet excitons are energy degenerate when the electrons are spin-unpolarized,while the degeneracy split when the electrons are spin-polarized. All the studied cGNRs show strong excitonic effects with the exciton binding energies of hundreds of meV.     

Resonant Raman scattering spectra in a ZnCdSe/ZnSe structure with a quantum well and open nanowires

Resonance Raman scattering (RS) spectra of a ZnCdSe/ZnSe sample containing a single quantum well and quantum well-based open nanowires were studied at T=300 K. The longitudinal optical (LO) phonons involved in the formation of the observed spectra of the quantum-well and nanowire regions differ noticeably in energy. The LO phonon energies in the structures under study were calculated taking into account the compositional effect (doping of Cd into ZnSe) and biaxial strain. When excited in the exciton resonance region, RS is shown to occur via free (extended) excitonic states with the involvement of LO phonons of the ZnCdSe strained layer with final wave vectors near the Brillouin zone center. When excited below the excitonic resonance in the ZnCdSe layer, resonance scattering via localized exciton states provides a noticeable contribution to the observed RS lines. Because of the finite size of a localized state, phonons with large wave vectors are involved in these scattering processes. The RS lines produced under excitation in the excitonic region of the thick barrier layers are due to scattering from the ZnSe barrier phonons.     

Resonance Raman scattering by excitonic polaritons in CuGaS2

Resonance Raman scattering by exciton polaritons in crystals of CuGaS₂ under excitation with the 4880 and 4765 Å lines of an Ar⁺ laser at 9 K is studied. Lines of one-and two-phonon scattering of excitonic polaritons are found and studied. It is shown that the 1LO and 2LO phonons are arranged in accordance with their energies as the Stokes shifts move farther away from the excitation energy.     

Multiplication of anion and cation electronic excitations in luminescent wide-gap ionic crystals

The spectra of intrinsic luminescence excitation by synchrotron radiation (6–32 eV) at 8 K have been analyzed for NaCl, KCl, RbCl, KBr, RbBr, CsBr, MgO, CaO and YalO₃ crystals. In all crystalsv (except MgO and CaO) the process of multiplication of electronic excitations (MEE) causes a sharp increase of the intensity of self-trapped exciton emission, but leads (in KBr and NaCl) to the decrease of intra-band luminescence efficiency. The analysis of the intensity ratio spectra for two components of exciton emission allows us to separate the process of secondary exciton creation by hot photolectrons (NaCl, KBr, YAlO₃). The threshold energies of excitonic and electron-hole mechanisms of MEE are compared for a number of alkali halides.     

Resonant Raman Scattering by excitonic polaritons in semiconductors

We report results on Resonant Raman Scattering (RRS) mediated by excitonic polaritons in a high-purity semiconductor (CdTe) at low temperatures. For the first time ingoing and outgoing resonances at the n = 1, 2, 3 exciton states are detected on the one and two LO-phonon RRS. The transformation at resonance of sharp Raman peaks into well-thermalized exciton luminescence bands is observed for every ingoing, outgoing or intermediate state resonance.     

Exciton binding energy and the optical absorption coefficient in a strained CdxZn1−xO/ZnO quantum dot

Numerical calculations of the excitonic absorption spectra in a strained Cd_xZn_1?xO/ZnO quantum dot are investigated for various Cd contents. We calculate the quantized energies of the exciton as a function of dot radius for various confinement potentials and thereby the interband emission energy is computed considering the internal electric field induced by the spontaneous and piezoelectric polarizations. The optical absorption as a function of photon energy for different dot radii is discussed. Decrease of exciton binding energy and the corresponding optical band gap with the Cd concentration imply that the confinement of carriers decreases with composition x. The main results show that the confined energies and the transition energies between the excited levels are significant for smaller dots. Non-linearity band gap with the increase in Cd content is observed for smaller dots in the strong confinement region and the magnitude of the absorption spectra increases for the transitions between the higher excited levels.     

Interband optical absorption in a strained CdxZn1−xO/ZnO quantum dot

Numerical calculations of the excitonic absorption spectra in a strained Cd_xZn_1−xO/ZnO quantum dot are investigated for various Cd contents. We calculate the quantized energies of the exciton as a function of dot radius for various confinement potentials and thereby the interband emission energy is computed considering the internal electric field induced by the spontaneous and piezoelectric polarizations. The optical absorption as a function of photon energy for different dot radii is discussed. Decrease of exciton binding energy and the corresponding optical band gap with the Cd concentration imply that the confinement of carriers decreases with composition x. The main results show that the confined energies and the transition energies between the excited levels are significant for smaller dots. Non-linearity band gap with the increase in Cd content is observed for smaller dots in the strong confinement region and the magnitude of the absorption spectra increases for the transitions between the higher excited levels.     

Exciton States and Linear Optical Spectra of Semiconducting Carbon Nanotubes under Uniaxial Strain

Considering the exciton effect, the linear optical spectra of semiconducting single-walled carbon nanotubes （SWNTs） under uniaxial strain are theoretically studied by using the standard formulae of Orr and Ward [Mol. Phys. 20（1971）513]. It is found that due to the wrapping effect existing in the semiconducting zigzag tubes, the excitation energies of the linear optical spectra show two different kinds of variations with increasing uniaxial strain, among which one decreases such as tube （11,0）, and the other increases firstly and then decreases such as tube （10,0）. These variations of the linear optical spectra are consistent with the changes of the exciton binding energies or the （quasi）continuum edge of these SWNTs calculated in our previous work, which can be used as a supplemented tool to detect the deformation degree of an SWNT under uniaxial strain.     

Strain-modulated excitonic gaps in mono-and bi-layer MoSe_2

Photoluminescence(PL) and Raman spectra under uniaxial strain were measured in mono- and bi-layer MoSe_2 to comparatively investigate the evolution of excitonic gaps and Raman phonons with strain. We observed that the strain dependence of excitonic gaps shows a nearly linear behavior in both flakes. One percent of strain increase gives a reduction of ~42 meV(~35 me V) in A-exciton gap in monolayer(bilayer) MoSe_2. The PL width remains little changed in monolayer MoSe_2 while it increases rapidly with strain in the bilayer case. We have made detailed discussions on the observed strain-modulated results and compared the difference between monolayer and bilayer cases. The hybridization between 4d orbits of Mo and 4p orbits of Se, which is controlled by the Se–Mo–Se bond angle under strain, can be employed to consistently explain the observations. The study may shed light into exciton physics in few-layer MoSe_2 and provides a basis for their applications.     

Cs3Cu2I5晶体薄膜吸收谱的研究

本文测定了Ｃｓ３Ｃｕ２ Ｉ５ 晶体薄膜在室温及液氮温度下的吸收谱,并依此计算出该材料的激子参数,即激子束缚能ΔＥ（１）ｅｘ ＝ （０．５３±０．０７）ｅＶ,激子半径ａｅｘ ＝ ０．３２６ ｎｍ ,禁带宽度Ｅｇ ＝ （５．００±０．０７）ｅＶ。在谱分析的基础上,论证了Ｃｓ３Ｃｕ２Ｉ５ 的电子和激子激发定域在该晶体的ＣｕＩ亚晶格之中,同时,揭示了在低温下Ｃｓｘ Ｃｕ１－ ｘ Ｉ系列化合物的第一激子峰位置随其摩尔组分变化的规律。     

Excitonic absorption and Urbach's tail in bismuth sulfide single crystals

The absorption coefficient of bismuth sulfide single crystals has been measured through more than four orders of magnitude and in the range of energies from 1.25 to 1.70 eV. A detailed study as a function of temperature has been carried out from 29 to 300 K. An Urbach tail for low values of absorption has been found. This tail and its temperature evolution fit the expression for ionic materials. An excitonic region appears at low temperature and the shape of the exciton peak is Gaussian, which corresponds to a strong exciton-phonon coupling. The exciton binding energy is estimated (28±3 meV) and then the energy gap at 29 K is obtained (E _g =1.523±0.003 eV). The fundamental electronic transition has been found to be a strongly anisotropic allowed direct transition. From reflectivity measurements a localized level at 1.361 eV at 29 K has been found. The change of the gap with temperature is interpreted through an electron-phonon mechanism.     

Polaron effects on excitons in parabolic quantum wells: fractional-dimension variational approach

Polaron effects on excitons in parabolic quantum wells are studied theoretically by using a variational approach with the so-called fractional dimension model. The numerical results for the exciton binding energies and longitudinal-optical phonon contributions in GaAs/Al_0.3Ga_0.7As parabolic quantum well structures are obtained as functions of the well width. It is shown that the exciton binding energies are obviously reduced by the electron (hole)-phonon interaction and the polaron effects are un-negligible. The results demonstrate that the fractional-dimension variational theory is effectual in the investigations of excitonic polaron problems in parabolic quantum wells.     

Optical properties and temperature dependence of critical transitions in ZnSe

The dielectric function of ZnSe has been deduced from ellipsometric measurements between 20 K and 380 K. is analysed around each critical point with the standard critical point model. The variations of the different parameters characterising each transition with temperature are presented and analysed. The temperature coefficients of the energies of the critical transitions are given. is essentially governed by the Coulomb interaction near the fundamental gap. Thanks to the high binding energy of the exciton and the low spectral width of the ellipsometer, the fundamental state of the exciton is found completely separated from the first excited states and the continuum at low temperature. In return the strong transition E₁ near the L points of the Brillouin zone can be described equally well with a 2D or an excitonic transition. Received 5 February 1999 and Received in final form 15 June 1999     

Excitons and electron-hole plasma in quasi-two-dimensional systems

A theoretical study of many-body effects in quasi-two-dimensional electron-hole systems is presented. The renormalized single-particle energies and the exciton binding energy are calculated as functions of the carrier density and temperature. A simple model for the nonlinear excitonic absorption and refraction is proposed.     

Strong excitonic effect in organic–inorganic hybrid crystals

We investigate the optical properties of the hybrid crystal ZnTe(C₂H₈N₂)_0.5 from first principles. The excitonic effect is included by solving the Bethe–Salpeter equation for the two-particle Green's function. The inorganic ZnTe acts as optical active layer and the excitonic wave function is confined within it by C₂H₈N₂ layers. Due to the confinement of electronic states, electron–hole interaction within ZnTe layers is enhanced and the absorption spectra are thus changed drastically. The exciton binding energies are 0.54 and 0.42 eV for α and β structures, respectively. The calculated quasiparticle gap of the β structure is 3.68 eV.     

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.