Four-photon pressure-induced ionization of Xe by 351-nm radiation

The four-photon ionization of xenon gas at 351 nm is observed to be primarily pressure-induced. These observations indicate that the absorption occurs mainly through interaction with bound Xe₂ molecules. A three-photon near-resonance was found to enhance appreciably the cross-section for multiquantum ionization. The radiative lifetime of the resulting Xe¹₂ was determined to be τ_rad = 51 ns, implying only a partial mixing of the 0⁺_u and 1_u, 0^-_u states.     

Recombination dynamics of free and bound excitons in bulk GaN

We report new data on the transient photoluminescence behaviour of free and donor bound excitons in high quality bulk GaN material grown by HVPE. With 266 nm photoexcitation the no-phonon free exciton has a short decay time, about 100 ps at 2 K, assigned to nonradiative surface recombination. The LO replicas of the free exciton have a much longer decay at 2 K, about 1.4 ns, believed to be a lower bound for the bulk radiative lifetimes of the free excitons at 2 K. The donor bound exciton no-phonon lines exhibit a rather short (about 300 ps) nonexponential decay at 2 K, which appears to be dominated by a scattering process. The corresponding LO replicas and the two-electron transitions have a much longer decay. From the latter, the lower bound of the radiative lifetime of the O- and Si-bound excitons are 1800 ps and 1100 ps, respectively.     

Optical spectra in the region of exciton resonances in quantum wells and quantum dots of In0.3Ga0.7As/GaAs heterostructures

The transparency, reflection and luminescence spectra of In_0.3Ga_0.7As structures with 8 nm thickness and quantum wells limited by the barrier layer GaAs of a 9 nm (upper layer) and 100 nm (bottom layer) thickness had been studied in the region of photon energy 0.5–1.6 eV. Lines associated with the transitions hh,lh1-e1(1s,2s,3s), hh2,lh2-e2(1s,2s,3s), hh1,lh1-e2(1s) and hh3,lh3-e3(1s) had been revealed in reflection spectra. The shapes of the reflection and transparency lines had been calculated using a single oscillator model of dispersion relations and the Kramers–Kronig integrals. The binding energy of hh,lh1-e1 excitons, the effective mass m_hh^∗ and m_lh^∗ and the damping factor for the optical transitions to QW and QD had been determined. The lifetime of charge carriers on quantum dots varies in the range of 0.04–0.1 ps, while the radiative lifetime of excitons in quantum wells in the considered structure is around 2 ps.     

Short-living absorption and emission of CsI(Na)

This paper investigates the short-living absorption and the emission of CsI(Na) under a pulsed electron beam (Е_e=0.25 MeV, t_1/2=15 ns and W=0.003…0.16 J/cm²). The bands of singlet self-trapped excitons, as well as Na⁰ and V_k color centers have been detected in the transient absorption spectrum of CsI(Na). It has been found that the activator luminescence spectrum, peaking at 3.0 eV, fits a Gaussian (E_m=3.0 eV and FWHM=0.44±0.02 eV at 80 K) and remains the same at different time delays within 10⁻⁸-10⁻³ s. The decay kinetics of the 3.0 eV emission has one nanosecond exponential component and two microsecond ones with time constants 1.0 and 3.0 μs, which remain unchanged within 78-150 K. It is concluded that the activator emission is due to the radiative annihilation of sodium-perturbed two halide excitons from the non-relaxed singlet state. The pathways of such excitons creation are discussed.     

Lifetime of the Z1 centre in KC1:Sr

Data on the radiative lifetime τ(Z₁) of the relaxed excited state of the Z₁ centre in KC1:Sr in the 63–135 K range are reported for the first time [τ(Z₁)= 194 ± 10 nsec at 63 K]. The activation energy of deexcitation (ΔE = 0.132 ± 0.008 eV) for the luminescence process is in agreement with the value obtained by Paus from a quantum yield analysis.The results are discussed on the basis of an analogy with the F-centre behaviour.     

Lifetime measurements of the C1Π1 and B3Pi1 electronic states of InCl by laser induced fluorescence

The laser-induced fluorescence spectra of the InCl molecule over the range 266.5–287.0nm and 332.0–373.0nm are reported and assigned to C¹Π₁-X¹Σ⁺, B₃Π₁-X¹Σ⁺, or A³Π₀-X¹Σ⁺ transitions. It is the first time those radiative lifetimes of the C¹Π₁ and B³Π₁ states have been measured by laser-induced fluorescence. The collision-free fluorescence radiative lifetime τ₀ = 353(7)ns and a quenching rate constant k _Q = 1.985(0.010)x 10^-10 cm³ molecule^-1 s^-1 are proposed for B³Π₁ and τ₀ = 11(1)ns for C¹Π₁ states. From the radiative lifetime τ₀ and the Franck-Condon factors q_v″v′ for the v′ - v″ transitions, the electronic transition moments |R_e|² of the B³Π₁ and C¹Π₁ states have been obtained.     

Biexponential intersubband relaxation in n-modulation-doped quantum-well structures

Intersubband scattering in an n-modulation-doped GaAs/Al_0.31Ga_0.69As quantum-well structure is systematically investigated as a function of temperature and pump intensity. For the first time biexponential relaxation is observed during infrared bleaching experiments. The fast component with a time constant of ∼1 ps, which represents the depopulation of the first excited well subband, is found to dominate the signal more and more with decreasing temperature and pump intensity. The decay time of the slower component rises with decreasing temperature from τ₂=8 ps atT=300 K to τ₂=23 ps atT=10 K. This component is believed to be connected with a carrier transfer to the potential minima in the barrier layers. The intensity dependent excitation mechanism and the relaxation processes are discussed with the help of detailed numerical simulations.     

Exciton luminescence of YAlO<Subscript>3</Subscript> single crystals and single-crystal films

The paper reports on a study of exciton luminescence in single crystals (SCs) and single-crystal films (SCFs) of YAlO₃, which have substantially different concentrations of vacancy-type and substitutional defects, under excitation by synchrotron radiation near the fundamental absorption edge. The radiative annihilation of excitons in SCFs was shown to occur primarily at regular perovskite lattice sites and to be accompanied by luminescence in a band peaking at λ_max = 295 nm with τ = 5.2 ns. In contrast to SCFs, the radiative exciton decay in YAlO₃ SCs takes place predominantly near vacancy-type defects (F⁺ and F centers) and is accompanied by luminescence in the bands at λ_max = 350 nm (τ = 2.5 ns) and 440 nm (τ₁ = 1.9 ns, τ₂ = 30 ms). Photoexcitation in the 175-nm band of YAlO₃ SCs revealed photoconversion of the centers F → F⁺.     

Photoluminescence of F2+2 centres in additively coloured magnesium oxide

The principle luminescence bands excited in additively coloured MgO by radiation in the wavelength range 170–400 nm are observed at wavelengths of 520, 475, 441 and 375 nm. Polarised luminescence and uniaxial stress measurements on the 441 nm band, the radiative lifetime of 25 msec at 1.6 K and temperature dependence of luminescence intensities of the 375, 441 and 375 nm bands are consistent with the 441 nm band being due to ³B_1u → ¹A_g transitions of the F²⁺₂ centre.     

Ultrafast optical response in polydiacetylenes and polythiophenes

Ultrafast optical response in the films of poly(3-dodecylthiophene) (P3DT) and blue-and red-phase polydiacetylenes (PDA-4BCMU) has been investigated by femtosecond absorption and picosecond luminescence spectroscopies. Several nonlinear optical processes, i.e., hole burning, Raman gain, inverse Raman scattering, and induced-frequency shift, have been observed. The relaxation processes from photoexcited free excitons to self-trapped excitons (STEs) has been observed. The time constant is estimated as 140±40 fs in the blue-phase PDA-4BCMU and 100±50 fs in P3DT. The generated unthermalized STEs thermalize with the time constant of about 1 ps. The STEs in the blue-phase PDA-4BCMU decay exponentially with lifetime of 1.6±0.1 ps at 290 K and 2.1±0.2 ps at 10 K. The decay curves in the red-phase PDA-4BCMU and P3DT are not single exponential but can be fitted to biexponential functions with time constants of slightly shorter than 1 ps and about 5 ps. These two decay time constants correspond to relaxations to the ground state, respectively, from the free exciton and unthermalized STE and from the thermalized STE.     

Self-trapped excitons in LiB3O5 and Li2B4O7 lithium borates: Time-resolved low-temperature luminescence VUV spectroscopy

Results are reported of a coordinated investigation of the dynamics of electronic excitations in LiB₃O₅ and Li₂B₄O₇ crystals by low-temperature luminescence VUV spectroscopy performed with subnano-second resolution under synchrotron photoexcitation. Data on the photoluminescence (PL) decay kinetics, time-resolved PL and PL excitation spectra, and reflectance spectra obtained at 295 and 9.6 K are reported for the first time; the PL of the borates in the 3.5-eV region caused by radiative annihilation of self-trapped excitons (STE) has been established to have an intrinsic nature; the σ and π STE luminescence bands originating from singlet and triplet radiative transitions have been isolated; the shift of the STE σ band relative to the π band has been interpreted; the LBO recombination luminescence band has been isolated; and the creation and decay channels of relaxed and unrelaxed excitons in lithium borates are discussed.     

Two-photon correlations of luminescence at the Bose-Einstein condensation of dipolar excitons

Correlations of the luminescence intensity (the second-order correlation function g ⁽²⁾(τ)), where τ is the delay time between the photons detected in pairs) under the conditions of the Bose-Einstein condensation (BEC) of dipolar excitons has been studied in a temperature range of 0.45–4.2 K. Photoexcited dipolar excitons have been accumulated in a lateral trap in a GaAs/AlGaAs Schottky diode with a 25-nm wide single quantum well with an electric bias applied across the heterolayers. Two-photon correlations have been measured with the use of a two-beam intensity interferometer with a time resolution of }~0.4 ns according to the well-known classical Hanbury-Brown-Twiss scheme. The photon bunching has been observed at the onset of Bose-Einstein condensation manifested by the appearance of a narrow exciton condensate line in the luminescence spectrum at an increase in the optical pumping (the line width near the threshold is ?200 μeV). At the same time, the two-photon correlation function itself obeys the super-Poisson distribution, g ⁽²⁾(τ) > 1, at time scale τ_c ? 1 ns of the system coherence. The photon bunching is absent at a pumping level substantially below the condensation threshold. The effect of bunching also decreases at pumping significantly above the threshold, when the narrow exciton condensate line starts to dominate in the luminescence spectra, and finally disappears with the further increase in the optical excitation. In this region, the distribution of pair photon correlations is a Poisson distribution manifesting the united quantum coherent state of the exciton condensate. Under the same conditions, the first-order spatial correlation function g ⁽¹⁾(r) determined from the interference pattern of the luminescence signals from the spatially separated parts of the condensate at constant pumping remains noticeable at distances of no less than 4 μm. The discovered effect of photon bunching is very sensitive to temperature and decreases by several times with a temperature increase in the range of 0.45–4.2 K. Assuming that the luminescence of the dipolar excitons directly reflects the coherence properties of the gas of interacting excitons, the discovered photon bunching at the onset of condensation, where the fluctuations of the exciton density and, consequently, of the luminescence intensity are most significant, indicates a phase transition in the interacting Bose gas of excitons, which is an independent way of detecting the Bose-Einstein condensation of excitons.     

Low-temperature luminescence and thermally stimulated luminescence of BeO: Mg single crystals

Luminescence and thermally stimulated luminescence (TL) of BeO: Mg crystals are studied at T = 6–380 K. The TL glow curves and the spectra of luminescence (1.2–6.5 eV), luminescence excitation, and reflection (3.7–20 eV) are obtained. It is found that the introduction of an isovalent magnesium impurity into BeO leads to the appearance of three new broad luminescence bands at 6.2–6.3, 4.3–4.4, and 1.9–2.6 eV. The first two are attributed to the radiative annihilation of a relaxed near-impurity (Mg) exciton, the excited state of which is formed as a result of energy transfer by free excitons. The impurity VUV and UV bands are compared with those for the intrinsic luminescence of BeO caused by the radiative annihilation of self-trapped excitons (STE) of two kinds: the band at 6.2–6.3 eV of BeO: Mg is compared with the band at 6.7 eV (STE₁) of BeO, and the band at 4.3–4.4 eV is compared with the band at 4.9 eV (STE²) of BeO. In the visible region, the luminescence spectrum is due to a superposition of intracenter transitions in an impurity complex including a magnesium ion. The manifestation of X-ray-induced luminescence bands at T = 6 K in BeO: Mg indicates their excitation during band-to-band transitions and in recombination processes. The energy characteristics of the impurity states in BeO: Mg are determined; the effect of the isovalent impurity on the fluctuation rearrangement of the BeO: Mg structure in the thermal transformation region of STE₁ → STE₂ is revealed.     

Picosecond time-resolved luminescence of localized excitons in CdS1-xSex

We present time-resolved luminescence results on CdS_0.36Se_0.64 which give a new insight on the kinetics of excitons localized by alloy potential fluctuations. By exciting in the localized exciton band with detection close to the exciting wavelength we obtain the lifetime across the band. Below the exciting laser energy two processes contribute to luminescence: transfer of localized excitons by tunnel effect assisted by acoustical phonons, and luminescence (assisted by acoustical phonons) of all the states excited at time t = 0 either directly or through their acoustical absorption wing. The time behavior of luminescence with respect to the detuning from the exciting energy helps to discriminate between those two contributions. Furthermore it shows that intermediate long-living states are involved in the exciton relaxation process.     

Blue luminescence from the InGaN multiple quantum wells

We have fabricated very high-quality In_0.13Ga_0.87N/GaN multiple quantum wells with thickness as small as on (0 0 0 1) sapphire substrate using metal organic chemical vapour deposition (MOCVD). We have investigated these ultra-thin multiple quantum wells by continuous wave (cw) and time resolved spectroscopy in the picosecond time scales in a wide range of temperatures from 10 K to 290 K. In the luminescence spectrum at 10 K we observed a broad peak at 3.134 eV which was attributed to the quantum wells emission of InGaN. The full-width at half-maximum of this peak was 129 meV at 10 K and the broadening at low temperatures which was mostly inhomogeneous was thought to be due to compositional fluctuations and interfacial disorder in the alloy. The ultra narrow width of the quantum well was found to have a very profound effect in increasing the emission linewidth. We also observed an intense and narrow peak at 3.471 eV due to the GaN barrier. The temperature dependence of the luminescence was studied. The peak positions and intensities of the different peaks were obtained after a careful Lorentzian analysis. The activation energy of the InGaN quantum well emission peak was estimated as 69 meV. The lifetime of the quantum well emission was found to be 720 ps at 10 K. The results were explained by considering the localization of the excitons due to potential fluctuations. At higher temperatures the non-radiative recombination was found to be very dominant.     

Trapping and self-trapping in ytterbium-doped oxides with charge transfer luminescence

Temperature dependence of the charge transfer luminescence (CTL) of Yb-doped yttrium aluminum garnet Y₃Al₅O₁₂-Yb (YAG-Yb) and Yb-doped lutetium aluminum perovskite LuAlO₃-Yb (LuAP-Yb) crystals under X-ray excitation and their thermostimulated luminescence are investigated in the temperature range 30-350 K and compared to those of undoped crystals. Simulation using a set of kinetic equations describing the processes of creation of excitons, electron-hole pairs, their trapping and self-trapping, radiative relaxation and quenching is presented for the systems under investigation to analyze qualitatively two different types of experimentally observed temperature dependences: CTL yield decline with the temperature decrease below 110 K as in case of YAG-Yb and constant yield in the same temperature range as in case of LuAP-Yb.     

Electronic excitations and defects in nanostructural Al<Subscript>2</Subscript>O<Subscript>3</Subscript>

A time-resolved cathodo-and photoluminescence study of nanostructural modifications of Al₂O₃ (powders and ceramics) excited by heavy-current electron beams, as well as by pulsed synchrotron radiation, is reported. It was found that Al₂O₃ nanopowders probed before and after Fe⁺ ion irradiation have the same phase composition (the γ-phase/δ-phase ratio is equal to 1), an average grain size equal to ～17 nm, and practically the same set of broad cathodoluminescence (CL) bands peaking at 2.4, 3.2, and 3.8 eV. It was established that Al₂O₃ nanopowders exhibit fast photoluminescence (PL) (a band at 3.2 eV), whose decay kinetics is described by two exponential stages (τ₁ = 0.5 ns, τ₂ = 5.5 ns). Three bands, at 5.24, 6.13, and 7.44 eV, were isolated in the excitation spectrum of the fast PL. Two alternate models of PL centers were considered, according to which the 3.2-eV luminescence either originates from radiative relaxation of the P^? centers (anion-cation vacancy pairs) or is due to the formation of surface analogs of the F⁺ center (F _S ⁺ -type centers). In addition to the fast luminescence, nano-Al₂O₃ was found to produce slow luminescence in the form of a broad band peaking at 3.5 eV. The excitation spectrum of the 3.5-eV luminescence obtained at T = 13 K exhibits two doublet bands with maxima at 7.8 and 8.3 eV. An analysis of the luminescent properties of nanostructural and single-crystal Al₂O₃ suggests that the slow luminescence of nanopowders at 3.5 eV is due to radiative annihilation of excitons localized near structural defects.     

Temperature dependent time-resolved exciton luminescence in GaAs/AlGaAs quantum wires and dots

Transient photoluminescence of GaAs/AlGaAs quantum wires and quantum dots formed by strain confinement is studied as a function of temperature. At low temperature, luminescent decay times of the wires and dots correspond to the radiative decay times of localized excitons. The radiative decay time can be either longer or shorter than that of the host quantum well, depending on the size of the wires and dots. For small wires and dots (∼ 100 nm stressor), the exciton radiative recombination rate increases due to lateral confinement. Exciton localization due to the fluctuation of quantum well thickness plays an important role in the temperature dependence of luminescent decay time and exciton transfer in quantum wire and dot structures up to at least ∼ 80 K. Lateral exciton transfer in quantum wire and dot structures formed by laterally patterning quantum wells strongly affects the dynamics of wire and dot luminescence. The relaxation time of hot excitons increases with the depth of strain confinement, but we find no convincing evidence that it is significantly slower in quasi 1-D or 0-D systems than in quantum wells.     

Multicomponent Rayleigh scattering from guanidine hydrochloride solutions

We present results of Brillouin light scattering studies of lysozyme and guanidine hydrochloride solutions in the temperature range 290–350 K. The Brillouin spectra of 6 M guanidine hydrochloride have been found to contain an additional component in Rayleigh scattering that manifests itself as a broad quasi‐elastic scattering line centered at the unshifted frequency and described by a Lorentz function (i.e. a Debye relaxor with relaxation time τ₁ ~ 25 ps at room temperature). The temperature dependence of τ₁ is described by the Arrhenius law with activation energy E_a = 0.11 ± 0.01 eV and prefactor τ₀= 0.33 ± 0.03 ps. The Brillouin spectra of lysozyme denatured by 6 M guanidine hydrochloride exhibit a more complicated structure of the additional contribution into Rayleigh scattering, which is fitted best of all by a sum of two Lorentzians centered at the unshifted frequency (with relaxation times τ₁ ~ 19 ps and τ₂ ~ 180 ps at 339 K). Possible origins of the quasi‐elastic scattering are discussed. Copyright © 2012 John Wiley & Sons, Ltd.     

Creation of excitons and defects in a CsI crystal during pulsed electron irradiation

Data presented on the influence of the temperature in the range 80–650 K on the spectral kinetics of the luminescence and transient absorption of unactivated CsI crystals under irradiation by pulsed electron beams (〈E〉=0.25 MeV, t _1/2=15 ns, j=20 A/cm²). The structure of the short-wavelength part of the transient absorption spectra at T=80–350 K exhibits features, suggesting that the nuclear subsystem of self-trapped excitons (STE’s) transforms repeatedly during their lifetime until their radiative annihilation at T⩾80 K, alternately occupying di-and trihalide ionic configurations. It is established that a temperature-induced increase in the yield of radiation defects, as well as F and H color centers, and quenching of the UV luminescence in CsI occur in the same temperature region (above 350 K) and are characterized by identical thermal activation energies (∼0.22 eV). It is postulated that the STE’s in a CsI crystal can have a trihalide ionic core with either an on-center or off-center configuration; the high-temperature luminescence of CsI crystals is associated with the radiative annihilation of an off-center STE with the structure (I⁻(I⁰I⁻ e ⁻))*. Fiz. Tverd. Tela (St. Petersburg) 40, 640–644 (April 1998)