Light-induced Transient Grating Technique Research Articles

Evaluation of ambipolar diffusion coefficient in AlxGa1−xN semiconductor

Numerical approach to account for the influence of randomly fluctuating potential on carrier mobility in compound semiconductors with compositional disorder is developed and exploited for calculating the heavy hole-defined ambipolar diffusion coefficient in AlxGa1-xN layers. The rates of inelastic heavy hole-phonon scattering were obtained by integrating the quasi-classical hole-phonon scattering rates for the virtual crystal over the semiclassical confining potential obtained by using the local landscape method. The calculated dependence of the heavy-hole diffusion coefficient on the aluminum content in AlxGa1-xN crystal in a wide compositional range (x = 0 – 1) evidences a substantial influence of localization on the diffusivity of nonequilibrium carriers and is in a good quantitative correspondence with the experimental data obtained in this work by using the light-induced transient grating technique. The adopted Monte Carlo simulation technique also enables diffusivity calculations in other multicomponent compounds (e.g., high-In-content InGaN) and their structures, in particular, those for LEDs and µ-LEDs.

Stimulated emission threshold in thick GaN epilayers: interplay between charge carrier and photon dynamics

Room-temperature luminescence properties of a dense electron-hole plasma were studied in a set of GaN epilayers with thickness varying from 2 to 25 µm. The stimulated emission threshold was measured by photoluminescence and light-induced transient grating techniques under short-pulse excitation. Both techniques revealed the stimulated emission threshold increase with layer thickness despite the reduction of defect density. Numerical modeling of photoexcited carrier dynamics showed the different roles of carrier and photon populations. The stimulated emission threshold is mainly determined by the photon dynamics with weak influence of nonradiative carrier recombination. Increasing layer thickness results in the decreasing overlap of the gain layer with the optical mode, which reduces the transfer of energy from carriers to photons.

Photoluminescence efficiency of Al-rich AlGaN heterostructures in a wide range of photoexcitation densities over temperatures up to 550 K

Time-resolved photoluminescence and light-induced transient grating techniques were applied for temperature and excitation dependent internal quantum efficiency and carrier diffusion investigation in silicon-doped epilayer and AlxGa1-xN MQWs (x > 0.6). Decrease of photoluminescence efficiency at high excitations correlated with increase of diffusion coefficient as well as nonradiative recombination rate, indicating excitation and temperature dependent localized exciton density reduction. Excitation-dependent lifetime decrease was less pronounced than the corresponding drop of the time-integrated photoluminescence efficiency dominated by thermal dissociation of excitons. At lowest excitations excitons were found captured to vacancy complexes. With increase of excitation exciton ionization appeared, leading to enhanced nonradiative recombination of holes on aluminum vacancies and simultaneous droop of PL efficiency due to saturated bimolecular free carrier plasma recombination. At initial recombination stages and high excitations diffusive recombination on dislocations was also revealed. Modelling provided free exciton binding energies of 104, 140 meV in the MQWs and in the layer; exciton localization energies in 12-35 meV range; localized exciton lifetimes in 2-4 ns range; free exciton and carrier radiative recombination rate coefficients of rex = (0.6 0.2)109(T/300)-1 1/s and Brad = (7 1)10-10(T/300)-3/2 cm3/s, respectively. Vacancy complex capture cross section for excitons was determined to be = (2 1)10-16(300/T)2 cm2. Electron and hole capture cross sections to aluminum vacancy were modeled (1.5 1)10-13 cm2 and (7 1)10-13 cm2, respectively. Dislocation Coulomb radius for free carrier recombination was found to be 12-15 nm.

Carrier recombination processes in Fe-doped GaN studied by optical pump–probe techniques

We applied time-resolved free carrier absorption and light-induced transient grating techniques for monitoring carrier dynamics in lightly Fe-doped GaN bulk crystals. Comparison of measured decay times at single- and two-photon carrier photoexcitation with those reported for higher Fe doping revealed two different branches of lifetime dependence on iron density. A deeper insight was reached by using different wavelengths for probing carrier dynamics, which enabled discrimination of electron and hole capture processes by Fe ions. The capture cross section for holes, σh = (4 ± 1) × 10−15 cm2 for the Fe2+* state (5E → 4T2 transition) was determined to be ten times larger than that for electrons, σe = (4 ± 1) × 10−16 cm2 for the Fe3+* state (4T1 → 3T1 transition). Thermal activation of the [Fe2+(5T2),hVB] complex, where hVB is a free hole, required an energy of 315 meV. Light-induced transient grating decay revealed decreasing diffusivity of electrons with Fe doping due to initial carrier capture to Fe3+ states. Simultaneous measurements of carrier diffusion coefficient and lifetime at low excitation conditions (3 × 1017 cm−3) revealed a decrease of bipolar diffusion length from 2 μm in the undoped GaN down to 0.08 μm in the Fe-doped samples at 300 K.

Extreme radiation resistance in InN

Carrier dynamics were studied in InN, which is a promising material for radiation-resistant optoelectronic devices. InN epilayers with different background electron densities were prepared by metal-organic chemical vapor deposition and irradiated with protons. Application of the light-induced transient grating technique in the sub-picosecond domain allowed to study the carrier lifetime and diffusion coefficient as a function of the total carrier density (intrinsic, photoexcited, and irradiation-induced). The dominance of the direct Auger process in carrier recombination was revealed. The irradiation of InN by protons, such as those encountered in space applications, decreases the carrier lifetime while simultaneously increasing the diffusion coefficient (up to 190 cm2/s at the highest total carrier density studied). As a result, the average carrier diffusion length does not decrease below ∼140 nm, and exceeds the light absorption depth of InN. The lifetime damage factor was determined, and the lifetime dependence on the displacement damage dose was measured. The radiation resistance of InN surpasses that of GaAs, InGaAs, and InGaN. InN-based photovoltaic devices may work for long space missions.

Diffusion Enhancement in Highly Excited MAPbI3 Perovskite Layers with Additives.

Carrier mobility is one of the crucial parameters determining the electronic device performance. We apply the light-induced transient grating technique to measure independently the carrier diffusion coefficient and lifetime, and to reveal the impact of additives on carrier transport properties in wet-cast CH3NH3PbI3 (MAPbI3) perovskite films. We use the high excitation regime, where diffusion length of carriers is controlled purely by carrier diffusion and not by the lifetime. We demonstrate a four-fold increase in diffusion coefficient due to the reduction of localization center density by additives; however, the density dependence analysis shows the dominance of localization-limited diffusion regime. The presented approach allows us to estimate the limits of technological improvement-carrier diffusion coefficient in wet-cast layers can be expected to be enhanced by up to one order of magnitude.

Direct Auger recombination and density-dependent hole diffusion in InN

Indium nitride has a good potential for infrared optoelectronics, yet it suffers from fast nonradiative recombination, the true origin of which has not been established with certainty. The diffusion length of free carriers at high densities is not well investigated either. Here, we study carrier recombination and diffusion using the light-induced transient grating technique in InN epilayers grown by pulsed MOCVD on c-plane sapphire. We show that direct Auger recombination governs the lifetime of carriers at densities above ~1018 cm−3. The measured Auger recombination coefficient is (8 ± 1) × 10−29 cm−3. At carrier densities above ~5 × 1019 cm−3, we observe the saturation of Auger recombination rate due to phase space filling. The diffusion coefficient of holes scales linearly with carrier density, increasing from 1 cm2/s in low-doped layers at low excitations and up to ~40 cm2/s at highest carrier densities. The resulting carrier diffusion length remains within 100–300 nm range, which is comparable to the light absorption depth. This feature is required for efficient carrier extraction in bipolar devices, thus suggesting MOCVD-grown InN as the material fit for photovoltaic and photonic applications.

Two Regimes of Carrier Diffusion in Vapor-Deposited Lead-Halide Perovskites

Metal halide perovskites are attractive materials for the realization of cheap and effective solar cells, thin film transistors, and light emitters. Carrier diffusion at high excitations, however, is poorly addressed in perovskites, even though it governs the diffusion length and determines the efficiency of photonic devices. To fully understand the dependence of diffusion length on carrier density, we performed direct and independent measurements of the carrier diffusion coefficient and recombination rate in several methylammonium lead-halide perovskite layers by applying the light-induced transient grating technique. We demonstrate the existence of two distinct carrier diffusion regimes within the density range of 1018–1020 cm–3. In the perovskite films of high compositional quality, diffusion is governed by a bandlike transport of free carriers. The diffusivity is high (0.28–0.7 cm2/s) in these samples, even at low carrier density, and further increases with excitation due to carrier degeneracy. The op...

Photomodification of carrier lifetime and diffusivity in AlGaN epitaxial layers

Nonradiative recombination rate and diffusivity of nonequilibrium carriers were modified by intense laser pulses in AlGaN epilayers with Al content ranging from 16 to 71%. The epilayers were examined before and after the photomodification using light-induced transient grating and photoluminescence spectroscopy techniques. The photomodification resulted in (i) enhancement of the nonradiative recombination rate and (ii) large changes of the diffusion coefficient of the nonequilibrium carriers, without imposing any macroscopic structural damage to the epilayers. The photomodification effect on the recombination rate was stronger in the layers with higher Al content indicating the involvement of the Al atoms in this process. The carrier diffusivity exhibited a rapid initial increase as a consequence of the photomodification followed by a slow decline, as the photomodification duration was increased. The enhancement of the diffusion coefficient of up to 2.4 times was accompanied by 13% decrease in the carrier lifetime.

Nonradiative Recombination, Carrier Localization, and Emission Efficiency of AlGaN Epilayers with Different Al Content

The interplay between nonradiative recombination and carrier localization in AlxGa1−xN epilayers (0.11 < x < 0.78) was studied using the photoluminescence (PL) and light-induced transient grating (LITG) techniques. The carrier localization conditions were estimated from the temperature dependence of the PL band peak position. The room-temperature carrier lifetimes estimated by LITG were limited by the competition between the carrier localization and nonradiative recombination. Strong carrier localization was shown to be insufficient to achieve high internal quantum efficiency in AlGaN epilayers.

Dynamics of nonequilibrium carrier decay in AlGaN epitaxial layers with high aluminum content

Carrier dynamics in high-Al-content AlGaN epilayers with different dislocation densities from 5 × 10(8) cm(-2) to 5 × 10(9) cm(-2) is studied by comparing the photoluminescence decay with the decay of carrier density. The carrier density decay was investigated using the light-induced transient grating technique. This comparison shows that the luminescence at the nonequilibrium carrier densities expected in operating light-emitting diodes depends on the recombination of free carriers and the localized exciton-like electron-hole pairs and localization-delocalization processes. In addition, a fraction of the nonequilibrium carriers is captured by the deep capture centers with extremely long lifetimes. These carriers have an insignificant contribution to the band-to-band radiative recombination. This capture is an important factor in decreasing the emission efficiency.

Photoluminescence features and carrier dynamics in InGaN heterostructures with wide staircase interlayers and differently shaped quantum wells

We present a comprehensive study of photoexcited carrier dynamics in differently grown InGaN/InGaN multiple quantum well (MQW) structures, modified by insertion of a wide interlayer structure and subsequent growth of differently shaped quantum wells (rectangular, triangular, trapezoidal). This approach of strain management allowed the reduction of dislocation density due to gradually increasing In content in the interlayer and shaping the smooth quantum well/barrier interfaces. A set of c-oriented MQW structures emitting at 470 nm were grown at Vilnius University, Institute of Applied Research, using a closed coupled showerhead type MOCVD reactor. Photoluminescence (PL) spectra of MQW structures were analysed combining continuous wave and pulsed PL measurements. Reactive ion etching of the structures enabled discrimination of PL signals originated in the InGaN interlayer structure, underlying quantum wells, and quantum barriers, thus providing growth-related conditions for enhanced carrier localization in the wells. Time-resolved PL and differential transmission kinetics provided carrier lifetimes and their spectral distribution, being the longest in triangular-shape QWs which exhibited the highest PL intensity. The light-induced transient grating (LITG) technique was used to determine the spatially averaged carrier lifetime in the entire heterostructure, in this way unravelling the electronic quality of the LED internal structure at conditions similar to device performance. LITG decay rates at low and high excitation energy densities revealed increasing with photoexcitation nonradiative recombination rate in the triangular and trapezoidal wells.

Relationships Between Strain and Recombination in Intermediate Growth Stages of GaN

Using metalorganic chemical vapor deposition, we heteroepitaxially grew undoped gallium nitride epilayers on sapphire. Assessing the epilayers at different growth stages, we investigated changes in epilayer strain and the lifetime of minority nonequilibrium charge carriers. The in-plane compressive strain was evaluated by x-ray diffraction and bandgap photoluminescence. The epilayer thickness ranged from 200 nm (islets) to 3.5 μm (continuous structure). The carrier lifetimes, measured using a light-induced transient grating technique, revealed a correlation between strain and the density of edge-type threading dislocations. This dislocation density was 109 cm−2 to 1011 cm−2, corresponding to the dominant mechanism for nonradiative carrier recombination. How the carrier lifetime depended on the growth stage differed between the surface and interfacial measurements. On the surface side, the carrier lifetime increased monotonically up to ~500 ps with thickness; on the interface side, the lifetime changed little with thickness, except in the thickest sample, where the carrier lifetime increased with thickness. We attributed this behavior to defect healing aided by long-term annealing, leading to mutual lateral motion and annihilation of mixed threading dislocations.

Application of excite-probe techniques for determination of surface, bulk and nonlinear recombination rates in cubic SiC

Non-equilibrium carrier dynamics was studied in a free-standing 160 μm thick 3C-SiC wafer using time-resolved differential transmittivity (DT), differential reflectivity (DR), and light induced transient grating (LITG) techniques. To enable investigation of carrier recombination and diffusion features in the middle part of the wafer, a wedge-shaped strip was prepared by polishing out the most-defective part of the wafer on the substrate side. Measurements of DT and DR decay kinetics on both sides of the wedged sample and their numerical fitting provided bulk lifetimes of 180 ns in the middle part and 60 ns in the edge part (∼50 μm thick subsurface region). On the as-grown side, the surface recombination velocity was equal to 3 × 103 cm/s. Carrier diffusivity, determined by LITG technique, and recombination rate were found injection-dependent. The low-injection value of diffusion length, LD = 8 μm, was found the longest in the middle part of the wafer, while at high injections it decreased to 1 μm due to an impact of Auger recombination with a coefficient, C = (4 ± 1) × 10−32 cm6/s. The 2.7 times lower diffusion length value in the edge part was explained by an impact of point defects to the carrier lifetime and diffusivity.

Temperature- and excitation-dependent carrier diffusivity and recombination rate in 4H-SiC

Time-resolved optical ‘pump-probe’ techniques were applied to monitor carrier dynamics in CVD-grown 4H-SiC for investigation of carrier diffusivity and recombination rate over a wide temperature (80–800 K) and excitation (1016–1019 cm−3) range. The light-induced transient grating technique provided the dependence of ambipolar diffusion coefficient on nonequilibrium carrier density at various temperatures, attributable to bandgap renormalization at low excitation levels and to plasma degeneracy at high ones. The free carrier absorption technique allowed us to monitor carrier lifetimes at various excitation levels and revealed its essential decrease from microseconds to a few nanoseconds. The latter effect was attributed to phonon-assisted Auger recombination with a temperature-independent, unscreened coefficient, C0 = (5 ± 1) × 10−31 cm6 s−1, which was Coulomb-enhanced at low excitations (up to C300 K ∼ 10−30 cm6 s−1 at 1018 cm3) but gradually decreased with increasing excitation due to screening of the carrier–polar optical phonon interaction. The measurements provided an ambipolar diffusion length of ∼30 µm which was almost temperature independent at low excitations (up to ΔN = 1017 cm−3) but decreased to 1 µm at high excitations, mainly due to the impact of nonlinear recombination.

Injection-Activated Defect-Governed Recombination Rate in InN

Excess carrier dynamics was investigated by free-carrier absorption and light-induced transient grating techniques in InN layers with residual electron density varying from n0=1.4×1018 to 4.7×1018 cm-3 in a wide excitation range (up to 1020 cm-3). Carrier lifetime τ decreased with injected carrier density ΔN≥n0 and followed the same inverse relationship as on residual electron density τ∝[B(n0+ΔN)]-1, thus confirming defect-related recombination mechanism. Its nonradiative origin was verified by τ(T) measurements and ascribed to injection-enhanced nonlinear recombination via defect-assisted Auger recombination with CTAAR= B/NT=(4.5±2)×10-28 cm6/s, assuming the defect density NT being equal to electron density. Oxygen or hydrogen impurities are proposed as possible candidates for traps assisting in Auger process.

Spectral distribution of excitation-dependent recombination rate in an In0.13Ga0.87N epilayer

Time-resolved optical techniques of photoluminescence (PL), light-induced transient grating (LITG), and differential transmission spectroscopy were used to investigate carrier dynamics in a single 50-nm thick In0.13Ga0.97N epilayer at high photoexcitation levels. Data in wide spectral, temporal, excitation, and temperature ranges revealed novel features in spectral distribution of recombination rates as follows: at low injection levels, an inverse correlation of carrier lifetime increasing with temperature and diffusivity decreasing with temperature confirmed a mechanism of diffusion-limited nonradiative recombination at extended defects. Carrier dynamics in the spectral region below the absorption edge but ∼70 meV above the PL band revealed a recombination rate that increased with excitation, while recombination rate in PL emission band (420–430 nm) decreased after saturation of trapping centers. Monitoring of spectrally integrated carrier dynamics by LITG technique allowed us to ascribe the enhanced recombination rate to bimolecular recombination and determine its coefficient B = 7 × 10−11 cm3/s. Complementary measurements unveiled the cause of PL efficiency saturation at injection levels above 5 × 1018 cm−3, attributable to bandgap renormalization in the extended states above the PL emission band, which encumbers carrier transfer from high-to-low energy states. As the degree of localization, and therefore, the total number of band tail states is expected to increase with In content, their impact to dependence of PL efficiency on excitation density could even be stronger for higher In compositions. These results provided insight that spectrally resolved carrier generation-recombination rates are excitation-dependent and would play a critical role in saturation of internal quantum efficiency in InGaN alloys used in light emitters, such as light emitting diodes.

Carrier Diffusivity in Highly Excited Bulk SiC, GaN, and Diamond Crystals by Optical Probes

Optical monitoring of diffusivity in wide bandgap semiconductors was performed by using a picosecond light-induced transient grating technique. The bandgap renormalization and carrier-carrier scattering manifested itself at room temperature as two-fold decrease of the ambipolar diffusion coefficient Da in cubic SiC and 5-fold decrease of Da in diamond at excess carrier density N &gt; 1017 cm-3, while for GaN the impact was observed only at T 19 cm-3, the plasma degeneracy led to enhanced Da values in SiC and GaN and compensated the diffusivity decrease in diamond.

Carrier dynamics in bulk GaN

Carrier dynamics in hydride vapor phase epitaxy grown bulk GaN with very low density of dislocations, 5–8 × 105 cm−2, have been investigated by time-resolved photoluminescence (PL), free carrier absorption, and light-induced transient grating techniques in the carrier density range of 1015 to ∼1019 cm−3 under single and two photon excitation. For two-photon carrier injection to the bulk (527 nm excitation), diffusivity dependence on the excess carrier density revealed a transfer from minority to ambipolar carrier transport with the ambipolar diffusion coefficient Da saturating at 1.6 cm2/s at room temperature. An extremely long lifetime value of 40 ns, corresponding to an ambipolar diffusion length of 2.5 μm, was measured at 300 K. A nearly linear increase of carrier lifetime with temperature in the 80–800 K range and gradual decrease of D pointed out a prevailing mechanism of diffusion-governed nonradiative recombination due to carrier diffusive flow to plausibly the grain boundaries. Under single photon excitation (266 and 351 nm), subnanosecond transients of PL decay and their numerical modeling revealed fast processes of vertical carrier diffusion, surface recombination, and reabsorption of emission, which mask access to pure radiative decay.

High-excitation luminescence properties of m-plane GaN grown on LiAlO 2 substrates

Optically induced carrier dynamics was investigated in highly excited m-plane GaN films grown by metalorganic vapor phase epitaxy (MOVPE) on LiAlO 2 substrates and compared to a c-plane GaN reference. Photoluminescence (PL) spectra showing spontaneous and stimulated emission (SE) were investigated at room temperature in both backscattering and lateral geometries, the latter using two different orientations of the excitation stripe with respect to the m-plane GaN c-axis. A lower SE threshold was observed for the m-plane GaN film, which may be attributed to a different defect structure and in-plane strain. The threshold in the m-plane GaN layer is the lowest when using stripe excitation along [0 0 0 1], which is caused by a structural anisotropy in the film. The maximum degree of polarization for SE and spontaneous emission in the m-plane GaN film was found to be 0.47 and 0.23, respectively. The light-induced transient grating technique (LITG) provides carrier lifetimes of 40 and 380 ps for the m-plane and c-plane orientation, respectively, and reveals SE threshold values comparable to the ones obtained by PL.