Excitonic Gain Research Articles

Optical Gain Spectrum and Confinement Factor of a Monolayer Semiconductor in an Ultrahigh-Quality Cavity.

Two-dimensional (2D) semiconductors have attracted great attention as a novel class of gain materials for low-threshold, on-chip coherent light sources. Despite several experimental reports on lasing, the underlying gain mechanism of 2D materials remains elusive due to a lack of key information, including modal gain and the confinement factor. Here, we demonstrate a novel approach to directly determine the absorption coefficient of monolayer WS2 by characterizing the whispering gallery modes in a van der Waals microdisk cavity. By exploiting the cavity's high intrinsic quality factor of 2.5 × 104, the absorption coefficient spectrum and confinement factor are experimentally resolved with unprecedented accuracy. The excitonic gain reduces the WS2 absorption coefficient by 2 × 104 cm-1 at room temperature, and the experimental confinement factor is found to agree with the theoretical prediction. These results are essential for unveiling the gain mechanism in emergent, low-threshold 2D-semiconductor-based laser devices.

Excitonic processes and lasing in ZnO thin films and micro/nanostructures

Low dimensional ZnO-based materials have drawn much attention for the past few decades due to their unique electronic and optical properties and potential applications in optoelectronic devices. In this Tutorial, we will cover the past and the latest developments in ZnO thin films and micro/nanostructures in terms of excitonic and related lasing processes. First, we give a brief overview of structural and band properties of ZnO along with the linear optical and excitonic properties. Second, we introduce a feedback mechanism for lasing in various forms of ZnO, ranging from nanoparticles to nanowires, nanodisks, and thin films. As for the feedback mechanism, detailed descriptions are given to random lasing, Fabry–Pérot lasing, and whispering gallery mode lasing. Third, we discuss possible gain mechanisms, i.e., excitonic gain and electron–hole plasma (EHP) gain, in ZnO. A special interest is also devoted to the Mott carrier density, which is a crucial parameter to distinguish between excitonic and EHP contributions to lasing. Lastly, recent developments on exciton–polariton lasers based on ZnO microcavities are introduced.

(Invited) Quantum Well Architecture to Realize High Optical Gain Lasing Media

Photonic applications of semiconductor quantum dots (QDs) had significant drawbacks due to their ultrafast Auger decay of multiple excitons. These nonradiative processes have hindered the performance of electroluminescent and lasing devices. The emergence of the colloidal quantum well (QW) architecture where semiconductor quantum shell with an inverted QD geometry has led to suppressed Auger recombination. Ultra long biexciton lifetime (>10 ns) and large biexciton quantum yields has been achieved through spatial separation promoted by the QW geometry. Moreover, architecture induced exciton-exciton repulsions have led to the splitting of exciton and biexciton optical transitions which resulted in the single exciton gain mode along with the biexciton gain mode. High biexciton lifetime and the longest reported single exciton gain lifetime (>6 ns) has rendered this geometry a worthy candidate for the development of optically and electrically pumped gain media

Gain roll-off in cadmium selenide colloidal quantum wells under intense optical excitation

Colloidal quantum wells, or nanoplatelets, show among the lowest thresholds for amplified spontaneous emission and lasing among solution-cast materials and among the highest modal gains of any known materials. Using solution measurements of colloidal quantum wells, this work shows that under photoexcitation, optical gain increases with pump fluence before rolling off due to broad photoinduced absorption at energies lower than the band gap. Despite the common occurrence of gain induced by an electron–hole plasma found in bulk materials and epitaxial quantum wells, under no measurement conditions was the excitonic absorption of the colloidal quantum wells extinguished and gain arising from a plasma observed. Instead, like gain, excitonic absorption reaches a minimum intensity near a photoinduced carrier sheet density of 2 × 1013 cm−2 above which the absorption peak begins to recover. To understand the origins of these saturation and reversal effects, measurements were performed with different excitation energies, which deposit differing amounts of excess energy above the band gap. Across many samples, it was consistently observed that less energetic excitation results in stronger excitonic bleaching and gain for a given carrier density. Transient and static optical measurements at elevated temperatures, as well as transient X-ray diffraction of the samples, suggest that the origin of gain saturation and reversal is a heating and disordering of the colloidal quantum wells which produces sub-gap photoinduced absorption.

Research and Progress of Transparent, Flexible Tin Oxide Ultraviolet Photodetector

Optical detection is of great significance in various fields such as industry, military, and medical treatment, especially ultraviolet (UV) photodetectors. Moreover, as the demand for wearable devices continues to increase, the UV photodetector, which is one of the most important sensors, has put forward higher requirements for bending resistance, durability, and transparency. Tin oxide (SnO2) has a wide band gap, high ultraviolet exciton gain, etc., and is considered to be an ideal material for preparing UV photodetectors. At present, SnO2-based UV photodetectors have a transparency of more than 70% in the visible light region and also have excellent flexibility of 160% tensile strain. Focusing on SnO2 nanostructures, the article mainly summarizes the progress of SnO2 UV photodetectors in flexibility and transparency in recent years and proposes feasible optimization directions and difficulties.

Electrical Switching of Optical Gain in Perovskite Semiconductor Nanocrystals.

Perovskite semiconductor nanocrystals are promising for optical amplification and laser applications benefiting from efficient optical gain generation. Nevertheless, the pump threshold is limited by more than one exciton per nanocrystal required to generate population inversion in neutral nanocrystals due to the level degeneracy. Here, we show that by charging nanocrystals with current injection, the level degeneracy can be lifted to generate charged exciton gain with markedly low excitation density. On the basis of the scenario, we have demonstrated electrical switching of amplified spontaneous emission in films of CsPbBr3 nanocrystals sandwiched by two electrodes with over 50% threshold reduction owing to charged excitons. Our work provides an effective approach to electrically modulated optical gain in colloidal perovskite nanocrystals for potential applications in advanced laser and information technology.

Subwavelength-Polarized Quasi-Two-Dimensional Perovskite Single-Mode Nanolaser.

When approaching the subwavelength or deep subwavelength scale, there is a fundamental trade-off between the ultimate shrinking size and the performance for miniaturized lasers. Herein, to overcome this trade-off, we investigated the excitonic gain nature of quasi-two-dimensional (quasi-2D) perovskites and revealed that both singlet excitons and polarons would make nearly the entire contribution within ∼50 ps to a high net gain of 558 cm-1. Inspired by the gain characteristic, we successfully shrank the quasi-2D perovskites laser to the subwavelength scale using only a layer of ultraviolet glue and a glass substrate in the vertical dimension. In spite of the compact and simple cavity structure, single-mode lasing with a highly linear polarization degree of 81% and a quality factor of 1635 was achieved. The extremely short cavity, excellent lasing performance, and simple structure of the quasi-2D perovskite laser are expected to provide insights into next-generation integrated laser sources.

Excitonic complexes and optical gain in two-dimensional molybdenum ditelluride well below the Mott transition

Semiconductors that can provide optical gain at extremely low carrier density levels are critically important for applications such as energy efficient nanolasers. However, all current semiconductor lasers are based on traditional semiconductor materials that require extremely high density levels above the so-called Mott transition to realize optical gain. The new emerging 2D materials provide unprecedented opportunities for studying new excitonic physics and exploring new optical gain mechanisms at much lower density levels due to the strong Coulomb interaction and co-existence and mutual conversion of excitonic complexes. Here, we report a new gain mechanism involving charged excitons or trions in electrically gated 2D molybdenum ditelluride well below the Mott density. Our combined experimental and modelling study not only reveals the complex interplay of excitonic complexes well below the Mott transition but also establishes 2D materials as a new class of gain materials at densities 4–5 orders of magnitude lower than those of conventional semiconductors and provides a foundation for lasing at ultralow injection levels for future energy efficient photonic devices. Additionally, our study could help reconcile recent conflicting results on 2D materials: While 2D material-based lasers have been demonstrated at extremely low densities with spectral features dominated by various excitonic complexes, optical gain was only observed in experiments at densities several orders of magnitude higher, beyond the Mott density. We believe that our results could lead to more systematic studies on the relationship between the mutual conversion of excitonic species and the existence of optical gain well below the Mott transition.

Excitonic gain and laser emission from mixed-cation halide perovskite thin films

Organic–inorganic halide perovskites have recently developed into a potential semiconductor coherent light emitter candidate beyond their promise in solar cell applications. However, despite the ample demonstrations of perovskite lasers, experimental results on the origin of optical gain in perovskites are still elusive. Here, we analyze the excitonic gain in the green from mixed-cation halide perovskites Cs0.17[CH(NH2)2]0.83PbBr3 (Cs0.17FA0.83PbBr3) by both low temperature absorption/emission spectroscopies and ultrafast pump–probe transient absorption experiments. The perovskite thin films show a robust excitonic feature up to room temperature, with estimated exciton binding energy E b =43.8 meV, which can be maintained under high electronic excitations that are required for lasers. By using a high-quality (Q=1350) vertical cavity consisting of sputtered dielectric HfO2/SiO2 distributed Bragg reflectors with perovskite optical gain medium embedded inside, we have demonstrated excitonic-gain-enabled optically pumped lasing, with improved threshold of 13.5±1.4 μJ/cm2 and device longevity lifetime >35 h (108 laser shots) at ambient environment under sustained pulsed optical excitations (3.493 eV, τpulse=0.34 ns, 1 kHz). Understanding and exploiting excitonic gain from perovskite thin film materials may help to further boost the performance of perovskite-based lasers.

Characterization and Analysis of 1.3-μm InAs/InGaAs Self-Assembled Quantum Dot Lasers

High performance 1.3-μm GaAs-based InAs/InGaAs quantum dot (QD) lasers have been fabricated. The QD lasers have demonstrated low threshold current, high output power as well as high temperature operation. Temperature-dependent (20–100 °C) and excitation power-dependent (12–700 mW) photoluminescence (PL) measurements have been carried out on the QD laser structures. Both ground state (GS) and excited state (ES) luminescence has been observed in the PL spectra as well as in the lasing spectra. Rate equations were used to interpret the PL behavior of the QD structures. High radiative recombination efficiency in the QD structure has been verified even at 100 °C. The excitonic modal gain has been calculated and compared with the experimentally obtained modal gain value by the Hakki–Paoli method from the QD laser with good agreement.

Ultraviolet Lasing Characteristics of ZnS Microbelt Lasers

Investigation on the room-temperature ultraviolet lasing characteristics of a single ZnS microbelt laser is presented. Lasing emission with peak wavelength at round 335 nm is observed from the hexagonal-wurtzite phase of ZnS microbelt under optical excitation. This is due to the Fabry-Perot resonance along the length of the microbelt. By studying the low-temperature and time-resolved photoluminescence, it is verified that the corresponding lasing characteristics are attributed to the excitonic optical gain process. Furthermore, the rectangular cross-sectional nanostructure of ZnS microbelt suppresses TM polarization for excitation power lower than ~1.4 times the threshold. Hence, ZnS microbelts can be a promising building block to realize ultraviolet semiconductor lasers with control of laser polarization.

Nonlinear emission characteristics of quantum dot–micropillar lasers in the presence of polarized optical feedback

We report on electrically pumped quantum dot–microlasers in the presence of polarized self-feedback. The high-β microlasers show two orthogonal, linearly polarized emission modes which are coupled via the common gain medium. This coupling is explained in terms of gain competition between the two lasing modes and leads to distinct differences in their input–output characteristics. By applying polarized self-feedback via an external mirror, we are able to control the laser characteristics of the emission modes in terms of the output power, the coherence time and the photon statistics. We find that linearly polarized self-feedback stabilizes the lasing of a given mode, while cross-polarized feedback between the two modes reduces strongly the intensity of the other emission mode showing particular high-intensity fluctuations and even super-thermal values of the photon autocorrelation function g(2)(τ) at zero delay. Measurements of g(2)(τ) under external feedback also allow us to detect revival peaks associated with the round trip time of the external cavity. Analyzing the damping and shape of the g(2)(τ) revival peaks by a phenomenological model provides us insight into the underlying physics such as the effective exciton lifetime and gain characteristics of the quantum dots in the active region of these microlasers.

Nearly Temperature‐Independent Threshold for Amplified Spontaneous Emission in Colloidal CdSe/CdS Quantum Dot‐in‐Rods

Nearly Temperature‐Independent Threshold for Amplified Spontaneous Emission in Colloidal CdSe/CdS Quantum Dot‐in‐Rods

Wave-function Monte Carlo method for polariton condensates

We present a quantum jump approach to describe coupled quantum and classical systems in the context of Bose-Einstein condensation in the solid state. In our formalism, the excitonic gain medium is described by classical rate equations, while the polariton modes are described fully quantum mechanically. We show the equivalence of our method with a master equation approach. As an application, we compute the linewidth of a single mode polariton condensate. Both the line broadening due to the interactions between polaritons and the interactions with the reservoir excitons is taken into account.

Laser emission with excitonic gain in a ZnO planar microcavity

The lasing operation of a ZnO planar microcavity under optical pumping is demonstrated from T=80 to 300 K. At the laser threshold, the cavity switches from the strong coupling to the weak coupling regime. A gain-related transition, which appears while still observing polariton branches and, thus, with stable excitons, is observed below 240 K. This shows that exciton scattering processes, typical of II-VI semiconductors, are involved in the gain process.

Interactions of bound excitons in doped core/shell quantum dot heterostructures

Spatial localization to a defect or a dopant of one of the charge carriers comprising an exciton, has a significant effect on the optical properties of bulk semiconductors. It is not clear, however, how these effects would change when considering semiconductor nanocrystals in the strong confinement regime. As we show here, under strong confinement, doping has a dramatic effect on the energetics of multiply excited states, which exhibit a strong size dependence. This is experimentally shown by performing multiexciton spectroscopy of CdSe/CdS and ZnSe/CdS colloidal quantum dot (QD) heterostructures, whose cores are nucleation-doped with few atoms of tellurium, leading to localization of the holes. The biexciton (BX) is shown to be strongly blueshifted relative to the bound exciton, in stark contrast with the corresponding undoped nanocrystals exhibiting a BX redshift. The energetics of the BX is shown to be determined mostly by the energy difference between the dopant state and the valence-band edge while the emission color is mostly determined by quantum confinement in the conduction band. By tailoring the nanocrystal's structure we can thus independently control the emission color, the radiative decay rate and the BX repulsion. QD heterostructures harboring bound excitons are therefore excellent candidates for colloidal-based gain devices required to operate in the single exciton gain regime.

High temperature excitonic lasing characteristics of randomly assembled SnO2 nanowires

The lasing characteristics of randomly assembled SnO2 nanowires, whose excitonic gain is attributed to the exciton states bounded to the surface defects, are studied from room temperature up to 500 K. It is found that the amount of excited carriers under the lasing conditions is well below the Mott density of SnO2 so that high pumping intensities have less influence on the radiative recombination mechanism and wavelength of the lasing peaks. Furthermore, the redshift of lasing peaks is mainly due to the reduction of bandgap energy of SnO2 with the increase of temperature.

Ultraviolet coherent random lasing in randomly assembled SnO2 nanowires

Although nanostructured SnO2 exhibited ultraviolet stimulated emission at room temperature, the low emission intensities and occurrence of gain saturation restricted them to be considered as luminescent materials for semiconductor lasers. In this letter, we find that a large ultraviolet excitonic gain can be obtained from SnO2 nanowires coated with an amorphous layer. Under effective pumping, ultraviolet coherent random lasing can be realized from randomly assembled SnO2 nanowires at room temperature.

Submonolayer quantum dots for high speed surface emitting lasers.

We report on progress in growth and applications of submonolayer (SML) quantum dots (QDs) in high-speed vertical-cavity surface-emitting lasers (VCSELs). SML deposition enables controlled formation of high density QD arrays with good size and shape uniformity. Further increase in excitonic absorption and gain is possible with vertical stacking of SML QDs using ultrathin spacer layers. Vertically correlated, tilted or anticorrelated arrangements of the SML islands are realized and allow QD strain and wavefunction engineering. Respectively, both TE and TM polarizations of the luminescence can be achieved in the edge-emission using the same constituting materials. SML QDs provide ultrahigh modal gain, reduced temperature depletion and gain saturation effects when used in active media in laser diodes. Temperature robustness up to 100 °C for 0.98 μm range vertical-cavity surface-emitting lasers (VCSELs) is realized in the continuous wave regime. An open eye 20 Gb/s operation with bit error rates better than 10−12has been achieved in a temperature range 25–85 °Cwithout current adjustment. Relaxation oscillations up to ∼30 GHz have been realized indicating feasibility of 40 Gb/s signal transmission.

Zinc oxide – analogue of GaN with new perspective possibilities

AbstractZinc oxide due to specific electrical, optical and acoustic properties is the important semiconductor material, which has many various applications. There is growing interest in ZnO due to its potential applicability for optoelectronic devices such as light‐emitting diodes, laser diodes and detectors for UV wavelength range. ZnO properties are very close to those of widely recognized semiconductor GaN. The band gap of ZnO (3.37 eV) is close to that of GaN (3.39 eV) but ZnO exciton binding energy (60 meV) is twice larger than that of GaN (28 meV). Optically pumped UV lasing have been demonstrated at room temperature using high textured ZnO films. The excitonic gain close to 300 cm–1 was achieved. ZnO thin films are expected to have higher quantum efficiency in UV semiconductor laser than GaN. The physical properties of ZnO are considered. PEMOCVD technology was used to deposit piezoelectric and highly transparent electroconductive ZnO films. Their properties are discussed. The experiments on polycrystalline ZnO films deposited by RF magnetron sputtering at different partial pressure of oxygen are presented. AFM images were studied in tapping mode for deposited films. The investigated films were dielectric ones and had optical transparency within 65‐85% at thickness in the interval 0.2‐0.6 μm. (© 2004 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)