Electron-hole Wavefunction Overlap Research Articles

Improving Lattice Rigidity and Charge Carrier Lifetime by Engineering Spacer Cation of Ruddlesden-Popper Perovskites: A Time-Domain Ab Initio Study.

First-principles quantum dynamics calculations show that charge carrier lifetimes, charge transport, and lattice stability are notably improved when BA (CH3(CH2)3NH3+) in BA2PbI4 is replaced with MTEA (CH3(CH2)2SNH3+). By suppressing atomic fluctuations, MTEA enhances the lattice stiffness and inhibits loss of coherence due to the S-S interaction. By delocalizing hole wave functions on the MTEA, particularly on the S atoms, while maintaining the electron wave functions largely unchanged compared to the BA2PbI4, MTEA serves to enhance charge transport and NA coupling while narrowing the bandgap by 0.18 eV. Overall, MTEA decreases NA coupling due to slow atomic motions against a large overlap of electron-hole wave functions, which suppresses nonradiative electron-hole recombination and prolongs carrier lifetime twice longer compared with BA2PbI4. This simulation presents a rational route to make high performance two-dimensional perovskite solar cells.

Drastic Effect of Sequential Deposition Resulting from Flux Directionality on the Luminescence Efficiency of Nanowire Shells.

Core-shell nanowire heterostructures form the basis for many innovative devices. When compound nanowire shells are grown by directional deposition techniques, the azimuthal position of the sources for the different constituents in the growth reactor, substrate rotation, and nanowire self-shadowing inevitably lead to sequential deposition. Here, we uncover for In0.15Ga0.85As/GaAs shell quantum wells grown by molecular beam epitaxy a drastic impact of this sequentiality on the luminescence efficiency. The photoluminescence intensity of shell quantum wells grown with a flux sequence corresponding to migration enhanced epitaxy, that is, when As and the group-III metals essentially do not impinge at the same time, is more than 2 orders of magnitude higher than for shell quantum wells prepared with substantially overlapping fluxes. Transmission electron microscopy does not reveal any extended defects explaining this difference. Our analysis of photoluminescence transients shows that co-deposition has two detrimental microscopic effects. First, a higher density of electrically active point defects leads to internal electric fields reducing the electron-hole wave function overlap. Second, more point defects form that act as nonradiative recombination centers. Our study demonstrates that the source arrangement of the growth reactor, which is of mere technical relevance for planar structures, can have drastic consequences for the material properties of nanowire shells. We expect that this finding holds good also for other alloy nanowire shells.

P-AlInN electron blocking layer for AlGaN-based deep-ultraviolet light-emitting diode

Commonly, the Al-rich AlGaN layer acts as electron blocking layer (EBL) to block the overflow of electrons from the active region in conventional AlGaN deep-ultraviolet (DUV) light-emitting diode (LED). However, the Al-rich AlGaN layer leads to the disadvantages of severe electron overflow and hole blocking effect. Herein, we proposed a new AlInN-based EBL to improve the optoelectronic characteristics of AlGaN-based DUV LED. The calculated results show that conventional (fixed Al composition) AlInN EBL has superior hole injection, reduced electron overflow, and lower electric field as compared to conventional AlGaN EBL. By using AlInN EBL, internal quantum efficiency (IQE) drop is reduced by 20%, and light output power improved by 165.30%. It was noticed that conventional AlInN EBL has a 28% IQE drop which can further be minimized by employing AlInN/AlInN superlattice EBL structure. It is found that superlattice EBL improved carrier distribution and reduced electric field resulting in a higher electron-hole wave-function overlap of 55% within multiple quantum wells (MQW) which elevate radiative recombination rate. AlInN superlattice EBL LED has drop-free 93% IQE, twice light output power, and spontaneous emission rate compared to conventional AlInN EBL LED.

Rational construction of staggered InGaN quantum wells for efficient yellow light-emitting diodes

High-efficiency InGaN-based yellow light-emitting diodes (LEDs) with high brightness are desirable for future high-resolution displays and lighting products. Here, we demonstrate efficient InGaN-based yellow (∼570 nm) LEDs with optimized three-layer staggered quantum wells (QWs) that are grown on patterned sapphire substrates. Numerical simulations show that the electron–hole wavefunction overlap of staggered InGaN QWs with high In content exhibits a 1.7-fold improvement over that of square InGaN QWs. At the same injection current, LEDs with staggered QWs exhibit lower forward voltages and narrower full widths at half maximum than LEDs with square QWs. The light output power and external quantum efficiency of a staggered QW LED are 10.2 mW and 30.8%, respectively, at 15 mA. We combine atomic probe tomography (APT), time-resolved photoluminescence (TRPL), and transmission electron microscopy (TEM) with energy-dispersive x-ray (EDX) mapping spectroscopy to shed light on the origin of enhanced device performance. APT results confirm the staggered In profile of our designed staggered QWs structure, and TRPL results reveal decreased defect-state carrier trapping in staggered QWs. Furthermore, TEM with EDX mapping spectroscopy supports the viewpoint that staggered QWs exhibit uniform elemental distribution and improved crystal quality. Together, these factors above contribute to enhanced LED performance. Our study shows that staggered InGaN QWs provide a promising strategy for the development of LEDs that are efficient in the long-wavelength region.

Analysis of InGaN-Delta-InN Quantum Wells on InGaN Substrates for Red Light Emitting Diodes and Lasers

Modern multi-color RGB micro-light emitting diode (μLED) displays and digital micro-mirror laser projectors often require the use of both III-V and III-Nitride material systems for different pixel/laser colors. This is due primarily to the conventionally low efficiencies of red emitters based on the InGaN materials system, which is used to create green and blue emitters for RGB displays. The main challenges for InGaN red emitters are the quantum confined stark effect (QCSE) and the difficulty of incorporating high In-content into the active region. In this work, InGaN/InGaN/delta-InN quantum wells (QWs) on InGaN substrates are proposed and demonstrated to show significant enhancement in electron-hole wavefunction overlap ( Γe_hh ) and spontaneous emission radiative recombination rate (Rsp) in the red emission regime. Analysis of InGaN/InGaN/delta-InN QWs with InGaN barriers emitting at 630 nm was performed using a self-consistent six-band $k \cdot p$ formalism. The Γe_hh was shown to increase by more than 230% compared to an InGaN/InGaN QW emitting at 630 nm, leading to significant increases in Rsp and internal quantum efficiency ( ηIQE ). With growth of InN monolayers on InGaN now readily achievable, this novel active region design could pave the way for high-efficiency, native red-emitting InGaN LEDs and lasers.

Long Wavelength InAs/InAsSb Infrared Superlattice Challenges: A Theoretical Investigation

InAs/InAsSb type-II superlattice focal plane arrays that demonstrate high operability and uniformity with cutoffs ranging from 5 μm to 13 μm have already been demonstrated. Compared to InAs/GaSb, the InAs/InAsSb superlattice is easier to grow and has longer minority carrier lifetimes, but requires a longer superlattice period to achieve long or very long wavelength cutoffs. A longer type-II superlattice period leads to smaller absorption coefficients and larger growth-direction hole conductivity effective masses. We explore by theoretical modeling some of the ideas aimed at addressing these challenges for the long and very long wavelength InAs/InAsSb superlattice. Increasing the Sb fraction in the InAsSb alloy can reduce the InAs/InAsSb superlattice period significantly, but this benefit can be negated by Sb segregation. Thin AlAsSb barrier layers can be inserted in InAs/InAsSb to form polytype W, M, and N superlattices in order to increase electron–hole wavefunction overlap for stronger optical absorption. However, this strategy can be unfavorable since the AlAsSb barriers increase the band gap, and thereby increase the superlattice period required to reach a given cutoff wavelength. Metamorphic growth on virtual substrates with larger lattice constants than GaSb can decrease the superlattice period needed to reach a specified cutoff wavelength, but this benefit should be weighed against the need for metamorphic buffer growth and the resulting higher defect density.

Correlation between performance and compositional grading in quantum well of deep UV-LED

A novel AlGaN/AlGaN multiple-quantum-wells light-emitting diode (LED) structure with linearly graded Al-content in the quantum well (QW) is thoroughly investigated in order to observe the effect on the electrical and optical performances of the devices. The results confirm that the polarization-shape across the active region highly depends on the concentration profile of aluminium, which eventually plays a critical role in determining the overall radiative recombination by promoting hole injection, as well as, improving the electron hole wave-function overlap. In order to correlate, two modified structures with variation in the compositional grading in the quantum well both along and opposite to the growth direction have been studied, and compared to a conventional structure. The outcomes reveal that the structure with Al composition grading in the QW which varies from 72 % to 76 % in the growth direction enhances the device performance.

Review—The Physics of Recombinations in III-Nitride Emitters

The physics of carrier recombinations in III-nitride light emitters are reviewed, with an emphasis on experimental investigations. After a discussion of various methods of measuring recombination dynamics, important results on recombination physics are examined. The radiative rate displays a complex behavior, influenced by Coulomb interaction and carrier screening. Non-radiative recombinations at low and high current are shown to scale with the overlap of electron-hole wavefunctions, similarly to the radiative rate, leading to a compensation effect which explains the high efficiency of III-nitride emitters. Finally, the droop current is decomposed into two contributions: the well-known Auger scattering, and a defect-assisted droop process, which is shown to play an important role in the green gap.

Recombination rates in green-yellow InGaN-based multiple quantum wells with AlGaN interlayers

The recombination rates in InGaN/AlGaN/GaN multiple quantum wells (MQWs) emitting in the green-yellow and grown with different Al compositions in the AlGaN interlayer (IL) are shown. By transforming measurements on radiative efficiency, absorption, and differential carrier lifetime, the radiative and nonradiative rates are determined. The IL Al composition controls lattice relaxation of the MQWs, as determined by X-ray reciprocal space mapping, and, therefore, defect formation. For the most pseudomorphic MQWs, the Shockley-Read-Hall (SRH) A coefficient is minimized and is similar to reports at shorter (blue and green) wavelengths. It is an order of magnitude smaller than a conventional InGaN/GaN MQW and is the most significant factor behind the improvement in radiative efficiency using the IL. The radiative B coefficient is also reduced and a minimum for the most pseudomorphic MQWs due to a reduction in the electron-hole wavefunction overlap. However, the decrease in A is more significant and leads to an overall improvement in the radiative efficiency. These recombination rate measurements confirm that if the SRH recombination is controlled, then the severe reduction of radiative recombination with an increased emitting wavelength is one of the main challenges in realizing high efficiency, long-wavelength InGaN-based MQW emitters operating at low to moderate current densities.

Compensation between radiative and Auger recombinations in III-nitrides: The scaling law of separated-wavefunction recombinations

The magnitude of radiative and Auger recombinations in polar InGaN quantum wells is studied. Lifetime measurements show that these two processes are related by a power law as the electron-hole wavefunction overlap varies, leading to a near-compensation of their relative contributions. Theoretical investigation reveals that, in systems with wavefunction separation, recombination rates are controlled by the spatial tails of decaying wavefunctions. Such recombinations observe a general power law whose exponent is determined only by the ratio of the carriers' effective masses. These findings explain why III-nitride emitters remain efficient despite significant wavefunction separation.

Type-II AlInN/ZnGeN2 quantum wells for ultraviolet laser diodes

We propose a type-II AlInN/ZnGeN2 quantum well (QW) structure serving as the active region for ultraviolet (UV) laser diodes. A remarkably low threshold current density can be achieved using the type-II AlInN/ZnGeN2 QW structure, providing a pathway for the realization of electrically-driven nitride-based semiconductor UV laser diodes. ZnGeN2 has both a very similar lattice constant and bandgap to GaN. Its large band offsets with GaN enable the potential of serving as a hole confinement layer to increase the electron-hole wavefunction overlap in the active region. In this study, we investigate the spontaneous emission and gain properties of type-II AlInN/ZnGeN2 QWs with different ZnGeN2 layer thicknesses. Our findings show that the use of ZnGeN2 layers in the active region provides a significant improvement in hole carrier confinement, which results in ∼5 times enhancement of the electron-hole wave function overlap. Such an enhancement provides the ability to achieve a significant increase (∼6 times) in the spontaneous emission rate and material gain, along with a remarkable reduction in threshold carrier density compared to the conventional AlGaN-based QW design, which is essential for practical UV laser diodes.

Enhanced Performance of an AlGaN-Based Deep-Ultraviolet LED Having Graded Quantum Well Structure

AlGaN-based deep ultraviolet light-emitting diodes (DUV LEDs) suffer from severe quantum confined Stark effect (QCSE) due to the strong polarization field in the quantum wells (QWs) grown on c -plane substrates. In this paper, we propose a novel DUV LED structure embedded with graded QWs in which the Al composition was linearly changed to screen the QCSE. A significant increase of the internal quantum efficiency and thus an enhancement of the light output power by nearly 67% can be achieved, attributing to the improvement of the electron-hole wave function overlap (Гe-hh) to 58.6% in the Increased-Al-composition graded QWs, as compared to the QW without grading (Гe-hh = 40.4%) and reverse grading (Гe-hh = 33.6%). Further investigations show that the grading profile of the Al composition in the QWs, including either linearly increases or decreases along the growth direction and the thickness of graded QWs, determine the polarization electrical field in the QWs and as a result, significantly affecting the performance of the devices. In the end, a careful optimization of the graded QWs is called. The proposed structure with such unique graded QWs provides us an effective solution to suppress the QCSE effect in the pursuit of high-performance DUV emitters.

Toward Ultra-Low Efficiency Droop in C-Plane Polar InGaN Light-Emitting Diodes by Reducing Carrier Density with a Wide InGaN Last Quantum Well

We demonstrate an ultra-low efficiency droop in c-plane polar InGaN blue light-emitting diodes (LEDs) by reducing the carrier density using a wide InGaN last quantum well (LQW). It is found that the LEDs with a 5.2 nm thick LQW show a negligible efficiency droop, with an external quantum efficiency (EQE) reducing from a peak value of 38.8% to 36.4% at 100 A/cm2 and the onset-droop current density is raised from 3 A/cm2 to 40 A/cm2 as the LQW thickness increases from 3.0 nm to 5.2 nm. The analysis based on the ABC model indicates that small efficiency droop is caused by the reduced carrier density using a wide LQW. The peak efficiency is reduced with a wide LQW, which is caused by the reduction of the electron-hole wavefunction overlap and the deterioration of the crystal quality of the InGaN layer. This study suggests that the application of the InGaN LEDs with a wide LQW can be a promising and simple remedy for achieving high efficiency at a high current density.

On intrinsic Stokes shift in wide GaN/AlGaN polar quantum wells

The interpretation of electromodulated reflectance (ER) spectra of polar quantum wells (QWs) is difficult even for homogeneous structures because of the built-in electric field. In this work we compare the room temperature contactless ER and photoluminescence (PL) spectra of polar GaN/AlGaN QWs with the effective-mass band structure calculations. We show that the emission from the ground state transition is observed in PL but the ER is dominated by transitions between excited states. This effect results from the polarization-induced built-in electric field in QW that breaks the selection rules that apply to square-like QWs, allowing many optical transitions which cannot be separately distinguished in the ER spectrum. We develop the guidelines for the identification of optical transitions observed in PL and ER spectra. We conclude that an intrinsic Stokes shift, i.e., a shift between emission and absorption, is present even for homogeneous GaN/AlGaN QWs with large width, where the electron–hole wavefunction overlap for the fundamental transition is weak.

Electronic and optical properties of polar, semi- and non-polar InGaN QDs: the role of second-order piezoelectric effects

In this work, we study the impact of second-order piezoelectricity on total built-in field, electronic and optical properties of InGaN/GaN quantum dots grown along different crystallographic directions. The calculations are carried out in the frame of a symmetry-adapted k · p model. Special attention is paid to the impact of Coulomb effects (excitonic effects) on the results. Overall our calculations reveal that for a c-plane system with 20% In, Coulomb effects and second-order piezoelectric effects are of secondary importance for the electron hole wave function overlap. For the semi- and non-polar systems, we find that Coulomb effects are essential to achieve an accurate description of their electron and hole wave function overlap. This stems from the observation that in the here studied systems the built-in field is strongly reduced compared to the c-plane dot. Overall, our calculations reveal that second-order piezoelectricity significantly affects the results in the non-polar case, resulting for instance in a noticeably larger oscillator strength and therefore shorter radiative lifetimes compared to the studied semi-polar system. The here calculated radiative lifetimes of the semi- and non-polar structures are in good agreement with reported experimental literature data.

Design of InGaN-ZnSnN2 quantum wells for high-efficiency amber light emitting diodes

InGaN-ZnSnN2 based quantum wells (QWs) structure is proposed and studied as an active region for high efficiency amber (λ ∼ 600 nm) light emitting diodes (LEDs), which remains a great challenge in pure InGaN based LEDs. In the proposed InGaN-ZnSnN2 QW heterostructure, the thin ZnSnN2 layer serves as a confinement layer for the hole wavefunction utilizing the large band offset at the InGaN-ZnSnN2 interface in the valence band. The barrier layer is composed of GaN or AlGaN/GaN in which the thin AlGaN layer is used for a better confinement of the electron wavefunction in the conduction band. Utilizing the properties of band offsets between ZnSnN2 and InGaN, the design of InGaN-ZnSnN2 QW allows us to use much lower In-content (∼10%) to reach peak emission wavelength at 600 nm, which is unachievable in conventional InGaN QW LEDs. Furthermore, the electron-hole wavefunction overlap (Γe-h) for the InGaN-ZnSnN2 QW design is significantly increased to 60% vs. 8% from that of the conventional InGaN QW emitting at the same wavelength. The tremendous enhancement in electron-hole wavefunction overlap results in ∼225× increase in the spontaneous emission radiative recombination rate of the proposed QW as compared to that of the conventional one using much higher In-content. The InGaN-ZnSnN2 QW structure design provides a promising route to achieve high efficiency amber LEDs.

Determination of strain relaxation in InGaN/GaN nanowalls from quantum confinement and exciton binding energy dependent photoluminescence peak

GaN based nanostructures are being increasingly used to improve the performance of various devices including light emitting diodes and lasers. It is important to determine the strain relaxation in these structures for device design and better prediction of device characteristics and performance. We have determined the strain relaxation in InGaN/GaN nanowalls from quantum confinement and exciton binding energy dependent photoluminescence peak. We have further determined the strain relaxation as a function of nanowall dimension. With a decrease in nanowall dimension, the lateral quantum confinement and exciton binding energy increase and the InGaN layer becomes partially strain relaxed which decreases the piezoelectric polarization field. The reduced polarization field decreases quantum confined Stark effect along the c-axis and increases electron-hole wave-function overlap which further increases the exciton binding energy. The strong dependency of the exciton binding energy on strain is used to determine the strain relaxation in these nanostructures. An analytical model based on fractional dimension for GaN/InGaN/GaN heterostructures along with self-consistent simulation of Schrodinger and Poisson equations are used to theoretically correlate them. The larger effective mass of GaN along with smaller perturbation allows the fractional dimensional model to accurately describe our system without requiring first principle calculations.

Surface Charges on CdSe-Dot/CdS-Rod Nanocrystals: Measuring and Modeling the Diffusion of Exciton-Fluorescence Rates and Energies.

By performing spectroscopic single-particle measurements at cryogenic temperatures over the course of hours, we study both the spectral diffusion as well as the diffusion of the decay rates of the fluorescence emission of core/shell CdSe/CdS dot/rod nanoparticles. A special analysis of the measurements allows for a correlation of data for single neutral excitons only, undisturbed by the possible emission of other excitonic complexes. We find a nearly linear dependency of the fluorescence decay rate on the emission energy. The experimental data are compared to self-consistent model calculations within the effective-mass approximation, in which migrating point charges set onto the surface of the nanoparticles have been assumed to cause the temporal changes of optical properties. These calculations reveal a nearly linear relationship between the squared electron-hole wave function overlap, which is linked to the experimentally determined fluorescence rate, and the exciton emission energy. Within our model, single migrating surface charges are not sufficient to fully explain the measured rather broad ranges of emission rates and energies, while two-and in particular negative-surface charges close to the core of the DR induce large enough shifts. Importantly, for our nanoparticle system, the surface charges more strongly affect the hole wave function than the electron wave function and both wave functions are still localized within the dot-like core of the nanoparticle, showing that the type-I character of the band alignment between core and shell is preserved.

Strong Size Dependency on the Carrier and Photon Dynamics in InGaN/GaN Single Nanowalls Determined Using Photoluminescence and Ultrafast Transient Absorption Spectroscopy.

Here, we have demonstrated strong size dependency of quasi-equilibrium and nonequilibrium carrier and photon dynamics in InGaN/GaN single nanowalls using photoluminescence and transient absorption spectroscopy. We demonstrate that two-dimensional carrier confinement, strain relaxation, and modified density of states lead to a reduced Stokes shift, smaller full width at half-maxima, increased exciton binding energy, and reduced nonradiative recombination. The ultrafast transient spectroscopy shows that carrier capture is a two-step process dominated by optical phonons and carrier-carrier scattering in succession. The carrier capture is a strongly size-dependent process and becomes slower due to modulation of the density of available states for progressively decreasing nanowall sizes. The slowest process is the electron-hole recombination, which is also extremely size-dependent and the rate increases by almost an order of magnitude in comparison to that of quantum-well structures. Electron-hole wave function overlap and modified density of states are among the key aspects in determining all the properties of these structures.

Significant internal quantum efficiency enhancement of GaN/AlGaN multiple quantum wells emitting at ~350 nm via step quantum well structure design

Significant internal quantum efficiency (IQE) enhancement of GaN/AlGaN multiple quantum wells (MQWs) emitting at ~350 nm was achieved via a step quantum well (QW) structure design. The MQW structures were grown on AlGaN/AlN/sapphire templates by metal-organic chemical vapor deposition (MOCVD). High resolution x-ray diffraction (HR-XRD) and scanning transmission electron microscopy (STEM) were performed, showing sharp interface of the MQWs. Weak beam dark field imaging was conducted, indicating a similar dislocation density of the investigated MQWs samples. The IQE of GaN/AlGaN MQWs was estimated by temperature dependent photoluminescence (TDPL). An IQE enhancement of about two times was observed for the GaN/AlGaN step QW structure, compared with conventional QW structure. Based on the theoretical calculation, this IQE enhancement was attributed to the suppressed polarization-induced field, and thus the improved electron–hole wave-function overlap in the step QW.