Function Of Excitation Density Research Articles

Revealing the order parameter dynamics of 1T-TiSe_2 following optical excitation

The formation of a charge density wave state is characterized by an order parameter. The way it is established provides unique information on both the role that correlation plays in driving the charge density wave formation and the mechanism behind its formation. Here we use time and angle resolved photoelectron spectroscopy to optically perturb the charge-density phase in 1T-TiSe_2 and follow the recovery of its order parameter as a function of energy, momentum and excitation density. Our results reveal that two distinct orders contribute to the gap formation, a CDW order and pseudogap-like order, manifested by an overall robustness to optical excitation. A detailed analysis of the magnitude of the the gap as a function of excitation density and delay time reveals the excitonic long-range nature of the CDW gap and the short-range Jahn–Teller character of the pseudogap order. In contrast to the gap, the intensity of the folded Se_{4p}* band can only give access to the excitonic order. These results provide new information into the the long standing debate on the origin of the gap in TiSe_2 and place it in the same context of other quantum materials where a pseudogap phase appears to be a precursor of long-range order.

An all optical approach for comprehensive in-operando analysis of radiative and nonradiative recombination processes in GaAs double heterostructures

We demonstrate an all optical approach that can surprisingly offer the possibility of yielding much more information than one would expect, pertinent to the carrier recombination dynamics via both radiative and nonradiative processes when only one dominant deep defect level is present in a semiconductor material. By applying a band-defect state coupling model that explicitly treats the inter-band radiative recombination and Shockley–Read–Hall (SRH) recombination via the deep defect states on an equal footing for any defect center occupation fraction, and analyzing photoluminescence (PL) as a function of excitation density over a wide range of the excitation density (e.g., 5–6 orders in magnitude), in conjunction with Raman measurements of the LO-phonon plasmon (LOPP) coupled mode, nearly all of the key parameters relevant to the recombination processes can be obtained. They include internal quantum efficiency (IQE), minority and majority carrier density, inter-band radiative recombination rate (Wr), minority carrier nonradiative recombination rate (Wnr), defect center occupation fraction (f), defect center density (Nt), and minority and majority carrier capture cross-sections (σt and σtM). While some of this information is thought to be obtainable optically, such as IQE and the Wr/Wnr ratio, most of the other parameters are generally considered to be attainable only through electrical techniques, such as current-voltage (I-V) characteristics and deep level transient spectroscopy (DLTS). Following a procedure developed herein, this approach has been successfully applied to three GaAs double-heterostructures that exhibit two distinctly different nonradiative recombination characteristics. The method greatly enhances the usefulness of the simple PL technique to an unprecedented level, facilitating comprehensive material and device characterization without the need for any device processing.

Impact of Dark Excitons on the Population and Relaxation Kinetics of Two-Dimensional Biexcitons in [CH3(CH2)3NH3]2Pb1-xMnxBr4 (x = 0-0.09).

Two-dimensional (2D) semiconductors have emerged as an excellent platform for studying various excitonic matter under strong quantum and dielectric confinements. However, such effects can be seriously overestimated for Coulomb binding of two excitons to form a biexciton by a naive interpretation of the corresponding photoluminescence (PL) spectrum. By using 2D halide perovskite single crystals of [CH3(CH2)3NH3]2Pb1-xMnxBr4 (x = 0-0.09) as a model system, we investigated both population and relaxation kinetics of biexcitons as a function of excitation density, temperature, polarization, and Mn doping. We show that the biexciton is formed by binding of two dark excitons, which are partially bright, but they radiatively recombine to yield a bright exciton in the final state. This renders the spectral distance between the exciton peak and the biexciton peak as very different from the actual biexciton binding energy (ϕ) because of large bright-dark splitting. We show that Mn doping introduces paramagnetism to our 2D system and improves the biexciton stability as evidenced by increase in ϕ from 18.8 ± 0.7 to 20.0 ± 0.7 meV and the increase of the exciton-exciton capture coefficient C from 2.4 × 10-11 to 4.3 × 10-11cm2/ns within our doping range. The precisely determined ϕ values are significantly smaller than the previously reported ones, but they are consistent with the instability of the biexciton against thermal dissociation at room temperature. Our results demonstrate that electron-hole exchange interaction must be considered for precisely locating the biexciton level; therefore, the ϕ values should be reassessed for other 2D halide perovskites that even do not exhibit any dark exciton PL.

Energy-transfer upconversion and excited-state absorption in KGdxLuyEr1-x-y(WO4)2 waveguide amplifiers

We perform a systematic spectroscopic study in channel waveguides of potassium gadolinium lutetium double tungstate doped with different Er3+ concentrations. Transition cross sections of ground-state absorption (GSA) and excited-state absorption (ESA), as well as stimulated emission (SE) at the pump wavelength around 980 nm are determined. ESA is directly measured by the pump-probe technique. Evaluation of GSA and ESA spectra indicates that ESA may be diminished by an appropriate choice of pump wavelength near 980 nm. Besides, GSA and SE at the signal wavelength around 1.5 µm are measured and the wavelength-dependent gain cross section as a function of excitation density is determined. Non-exponential luminescence decay curves from the 4I13/2 and 4I11/2 levels are analyzed and the probabilities of the energy-transfer-upconversion (ETU) processes (4I13/2, 4I13/2) → (4I15/2, 4I9/2) and (4I11/2, 4I11/2) → (4I15/2, 4F7/2) are quantified. Despite the large interionic distance between neighboring rare-earth sites in potassium double tungstates, the probability of ETU is comparatively large because of the large cross sections of the involved transitions. A rate-equation analysis of the influence of ETU and ESA on gain at ∼1.5 µm is performed, revealing that ETU from the 4I13/2 amplifier level strongly limits the gain when the doping concentration increases above ∼6at.%. The calculated maximum achievable internal net gain per unit length amounts to ∼15 dB/cm for an optimized Er3+ concentration of ∼4 × 1020 cm−3 and a launched pump power of 300 mW at a pump wavelength of 984.5 nm, in reasonable agreement with recent experimental results.

Charge trapping and coalescence dynamics in few layer MoS2

The optoelectronic properties of a material are determined by the processes following light-matter interaction. Here we use femtosecond optical spectroscopy to systematically study photoexcited carrier relaxation in few-layer MoS2 flakes as a function of excitation density and sample thickness. We find bimolecular coalescence of charges into indirect excitons as the dominant relaxation process in two- to three-layer flakes while thicker flakes show a much higher density of defects, which efficiently trap charges before they can coalesce.

Two-dimensional double-quantum spectroscopy: peak shapes as a sensitive probe of carrier interactions in quantum wells

We identify carrier scattering at densities below which it has previously been observed in semiconductor quantum wells. These effects are evident in the peakshapes of 2D double-quantum spectra, which change as a function of excitation density. At high excitation densities ($\geq 10^{9}$ carriers/,cm$^{-2}$) we observe untilted peaks similar to those reported in previous experiments. At low excitation densities (<$10^{8}$ carriers cm$^{-2}$) we observe narrower, tilted peaks. Using a simple simulation, we show that tilted peak-shapes are expected in double-quantum spectra when inhomogeneous broadening is much larger than homogeneous broadening, and that fast pure-decoherence of the double-quantum coherence can obscure this peak tilt. These results show that carrier interactions are important at lower densities than previously expected, and that the `natural' double-quantum peakshapes are hidden by carrier interactions at the excitation densities typically used. Furthermore, these results demonstrate that analysis of 2D peak-shapes in double-quantum spectroscopy provides an incisive tool for identifying interactions at low excitation density.

Kinetic Monte Carlo Simulations of Scintillation Processes in NaI(Tl)

Developing a comprehensive understanding of the processes that govern the scintillation behavior of inorganic scintillators provides a pathway to optimize current scintillators and allows for the science-driven search for new scintillator materials. Recent experimental data on the excitation density dependence of the light yield of inorganic scintillators presents an opportunity to incorporate parameterized interactions between excitations in scintillation models and thus enable more realistic simulations of the nonproportionality of inorganic scintillators. Therefore, a kinetic Monte Carlo (KMC) model of elementary scintillation processes in NaI(Tl) is developed in this paper to simulate the kinetics of scintillation for a range of temperatures and Tl concentrations as well as the scintillation efficiency as a function of excitation density. The ability of the KMC model to reproduce available experimental data allows for elucidating the elementary processes that give rise to the kinetics and efficiency of scintillation observed experimentally for a range of conditions.

High excitation carrier density recombination dynamics of InGaN/GaN quantum well structures: Possible relevance to efficiency droop

We report on the optical properties of InGaN/GaN quantum well structures measured at 10 K as a function of excitation density. At high excitation power densities we observe a component in the spectra that decays more rapidly than the localised carrier emission observed for low excitation power densities. We attribute this component to recombination involving weakly localised or delocalised carriers. At the high excitation power densities there is a reduction in the recombination internal quantum efficiency, so called efficiency droop. These observations are compatible with the model whereby efficiency droop is explained in terms of the non radiative loss of delocalised carriers.

Dark Carriers, Trapping, and Activation Control of Carrier Recombination in Neat P3HT and P3HT:PCBM Blends

Using flash photolysis, time-resolved microwave conductivity we report the sub-200 ns photoconductivity transients for neat poly(3-hexylthiophene), P3HT, and four associated blends containing 1%, 5%, 20%, and 50%, by weight, of the soluble fullerene, [6,6]-phenyl-c61-butyric acid methyl ester, PCBM. We propose a detailed kinetic scheme that when solved numerically is consistent with all the data recorded as a function of excitation density and that describes the fate of mobile and trapped carriers in the system. In the neat polymer, mobile holes are the only contributor to the photoconductance transients, which decay according to first-order kinetics at all light intensities due to the presence of a large concentration of dark carriers present in the polymer. The signal decays with a characteristic rate constant (∼1 × 107 s–1) that describes the re-equilibration of trapped and mobile holes. In all four blends, the microwave absorption contains a significant contribution due to electrons in the PCBM clusters, even at the lowest blend ratio of 1%. The magnitude of the second-order rate coefficient, γb, for carrier recombination in all four blends (3.25 × 10–12 cm3 s–1 < γb < 10 × 10–12 cm3 s–1), and also that identified for the neat polymer, corresponds to a slow process that is not limited by diffusion but is activation controlled.

Tunable two-photon pumped lasing from alloyed semiconductor nanoribbons

Single-crystal ZnS1−xSexnanoribbons with various compositions were synthesized through an Au-catalyzed vapor transport method. Under two-photon pumping with an 800 nm femtosecond pulsed laser, the spontaneous emission peak of the ternary nanoribbons undergoes a gradual red-shift from 422 to 464 nm with the increase of Se content. When the pump energy densities are increased above the thresholds, the nanoribbons exhibit a tunable upconverted laser emission accompanied by a dramatic decrease in spectral linewidth as a set of sharp peaks on the corresponding wavelengths of each sample, featuring the occurrence of stimulated emission. Two components appear in the fluorescence lifetimes, which indicate that the ZnS1−xSexnanoribbons have two different recombination centers. Both lifetime components decrease with the increase of pump energy, further confirming the occurrence of stimulated emission. The two-photon pumped lasing behavior was also observed from single nanoribbons, in which the photoluminescence (PL) spectra are composed of multimode of lasing. The distinct modes show gain competition and pronounced shifts as a function of excitation density.

Ga(AsSb)/GaAs/(AlGa)As heterostructures: additional hole‐confinement due to quantum islands

AbstractFormation of self‐organized Ga(AsSb) quantum‐islands during growth is shown to occur in a series of Ga(AsSb)/GaAs/(AlGa)As heterostructures, resulting in an in‐plane hole confinement of several hundred meV. The shape of the in‐plane confinement potential is nearly parabolic and thus yields almost equidistant hole energy levels. Transmission electronmicroscopy reveals that the quantum islands (QIs) are 100 nm in diameter and exhibit an inplane variation of the Sb concentration of more than 30%, which is the origin of the confinement. Up to seven bound hole states are observed in the photoluminescence spectra. Time‐resolved photoluminescence data are shown as function of excitation density. The influence of size and density of such structures as well as the mechanisms of growth are discussed. (© 2009 WILEY‐VCH Verlag GmbH &amp; Co. KGaA, Weinheim)

Hole confinement in quantum islands in Ga(AsSb)∕GaAs∕(AlGa)As heterostructures

Formation of self-organized Ga(AsSb) quantum islands during growth is shown to occur in a series of Ga(AsSb)∕GaAs∕(AlGa)As heterostructures, resulting in an in-plane hole confinement of several hundred meV. The shape of the in-plane confinement potential is nearly parabolic and, thus, yields almost equidistant hole energy levels. Transmission electron microscopy reveals that the quantum islands are 100nm in diameter and exhibit an in-plane variation of the Sb concentration of more than 30%. Up to seven bound hole states are observed in the photoluminescence spectra. Time-resolved photoluminescence data are shown as function of excitation density, lattice temperature, and excitation photon energy and reveal fast carrier capture into, and relaxation within, the quantum islands. The advantages of such structures as active laser material are discussed.

Excitation density dependence of the photoluminescence from CdxHg1-xTe multiple quantum wells

A study of the photoluminescence from a four-period CdxHg1-xTe multiple quantum well structure at 11 K as a function of excitation density is presented. High-resolution X-ray diffraction and transmission electron microscopy revealed that the quantum well structure is of high quality. This was supported by the narrow photoluminescence peak originating in the ground state electron - heavy hole transition, with a full width at half maximum of only 7.4 meV for an excitation density of 1.3 W/cm2. When the excitation density was increased from 1.3 to 23.4 W/cm2, the peak position was shifted toward higher energy by 2.6 meV and the full width at half maximum increased from 7.4 to 10.9 meV.

Lasing dynamics in single ZnO nanorods

We study the lasing dynamics of individual ZnO nanorods by time-resolved mu-photoluminescence. The distinct laser modes show gain competition and pronounced shifts as a function of excitation density. This behavior can be understood in terms of many-particle effects within an inverted electron-hole plasma and of the calculated mode spectra of the particular nanorod, whose geometry is known from electron microscope investigations.

Behaviour of scintillators under XUV free electron laser radiation

Free electron lasers (FEL) are new generation accelerator-based short wavelength light sources providing high pulse intensity and femtosecond pulse duration, which enable investigation of interaction of elementary excitations in solids under extreme conditions. Using the FLASH facility of HASYLAB at DESY (Hamburg, Germany), we investigated the response of different materials with scintillating properties based on intrinsic emissions to the 25.6 and 13.8 nm FEL radiation by means of time-resolved luminescence spectroscopy. FLASH delivered single pulses of 25 fs duration having energy per pulse up to 30 μJ resulting in power densities of ∼10 12 W/cm 2 on crystals. As a function of excitation density we observed the shortening of lifetime and non-exponential behaviour of emission decays in CaWO 4, while the emission spectra recorded are comparable to those obtained at conventional excitation sources.

Saturation of the ultrafast laser-induced demagnetization in nickel

We study the loss of magneto-optic contrast in nickel, in response to excitation by a short laser pulse, as a function of excitation density. Our measurements in the picosecond and subpicosecond regime show saturation of the contrast loss at high excitation densities. We conclude that spin relaxation is incomplete on this time scale, and explain the loss of magneto-optic contrast and its saturation in terms of a collapse of the Stoner gap due to band filling effects.

Cathodoluminescence imaging and spectroscopy of excited states in InAs self-assembled quantum dots

We have examined state filling and thermal activation of carriers in buried InAs self-assembled quantum dots (SAQDs) with excitation-dependent cathodoluminescence (CL) imaging and spectroscopy. The InAs SAQDs were formed during molecular-beam epitaxial growth of InAs on undoped planar GaAs (001). The intensities of the ground- and excited-state transitions were analyzed as a function of temperature and excitation density to study the thermal activation and reemission of carriers. The thermal activation energies associated with the thermal quenching of the luminescence were measured for ground- and excited-state transitions of the SAQDs, as a function of excitation density. By comparing these activation energies with the ground- and excited-state transition energies, we have considered various processes that describe the reemission of carriers. Thermal quenching of the intensity of the QD ground- and first excited-state transitions at low excitations in the ∼230–300-K temperature range is attributed to dissociation of excitons from the QD states into the InAs wetting layer. At high excitations, much lower activation energies of the ground and excited states are obtained, suggesting that thermal reemission of single holes from QD states into the GaAs matrix is responsible for the observed temperature dependence of the QD luminescence in the ∼230–300-K temperature range. The dependence of the CL intensity of the ground-and first excited-state transition on excitation density was shown to be linear at all temperatures at low-excitation density. This result can be understood by considering that carriers escape and are recaptured as excitons or correlated electron–hole pairs. At sufficiently high excitations, state-filling and spatial smearing effects are observed together with a sublinear dependence of the CL intensity on excitation. Successive filling of the ground and excited states in adjacent groups of QDs that possess different size distributions is assumed to be the cause of the spatial smearing.

Charge Recombination in CuPc/PTCDA Thin Films

The recombination kinetics of photogenerated charge carriers in perylene-3, 4, 9, 10-tetracarboxylic dianhydride (PTCDA) and copper phthalocyanine (CuPc) thin films grown by organic molecular beam deposition have been studied using transient absorption spectroscopy. Optical excitation is observed to generate long-lived polaron states, which exhibit power law recombination dynamics on time scales from microseconds to milliseconds. Studies as a function of excitation density and temperature, and comparison between heterostructures and PTCDA single layers, all indicate that this power law behavior results from trapping of PTCDA- polarons in localized states, with an estimated trap state density of approximately 6 x 10(17) polarons cm(-3). This recombination behavior is found to be remarkably similar to that previously observed for polymer/fullerene blends, suggesting that it may be generic to a range of semiconducting materials.

Strong near-infrared photoluminescence and absorption from Si/Si1−xGex type-II multiple quantum wells on bulk crystal SiGe substrates

We report a study of photoluminescence (PL) and optical absorption in high-quality tensile-strained Si type-II multiple quantum wells (QWs) grown on bulk crystal SiGe substrates by using low-temperature ultrahigh-vacuum chemical vapor deposition. Detailed PL experiments, as a function of excitation density together with applied uniaxial stress, were performed to study the band alignment and to help elucidate the origin of the observed PL peaks. Spatially direct and indirect transitions of the Si QWs and an intense broad subgap PL were observed. With increasing excitation power, the PL lines of Si QWs shift to lower energies, whereas the broad PL shifts to higher energy. The applied [110] compressive stress results in a redshift of the substrate PL lines, as expected, but a blueshift of both the Si QW PL and the broad PL lines. The optical absorption data also show strong absorption in the near-infrared region where the broad PL was observed. Near the absorption edge (Eg), the energy dependence obeys a square law rather than a square root law, suggesting that Eg is associated with a quasi-direct transition. The Eg value deduced according to the square law agrees well with the broad PL peak energy provided that temperature-dependent Eg, excitonic binding energy, and exciton localization energy, as well as quantum confinement are considered.

Exciton localization and quantum efficiency—A comparative cathodoluminescence study of (In,Ga)N/GaN and GaN/(Al,Ga)N quantum wells

We study the quantum efficiency (η) and transition energy (Et) as a function of excitation density and temperature in (In,Ga)N/GaN multiple quantum wells (MQWs) fabricated by molecular-beam epitaxy (MBE) and metal-organic chemical-vapor deposition (MOCVD), as well as in an MBE-grown GaN/(Al,Ga)N MQW. A method based on cathodoluminescence spectroscopy is proposed to be suitable for a reproducible measurement of the power dependence of η and Et. The experimental results are fit to a recently developed model allowing for a distinction of localization and electric-field effects for η and Et, as well as for the extraction of the localization energy, density of localization centers, and radiative recombination rate of localized excitons. In the (In,Ga)N/GaN MQWs grown by MBE and MOCVD, we found a value of the localization energy of 34 and 100 meV, respectively. In the MBE-grown GaN/(Al,Ga)N MQW, the exciton recombination is dominated by quasifree excitons even at low temperatures.