Efficient Auger Recombination Research Articles

Ultrafast Visible/Near‐Infrared Dual‐Band Selective Optical Switching via Polarization Control in Layered Low‐Symmetry TlSe

AbstractDual‐band optical signals, consisting of visible and infrared wavelengths, hold significant potential in various fields such as night vision, vehicle safety, bioimaging, and optical communications. Consequently, considerable attention has focused on modulation techniques for visible‐infrared dual‐band signals, including various electrochromic devices. However, these devices often suffer from low speeds and complex structures, making them unsuitable for satisfying the current demand for ultrafast on‐chip nanophotonics. Here, an ultrafast, dual‐band selective optical switching is presented in thallium selenide (TlSe), a layered nanomaterial with low‐symmetry. Transient absorption microscopy directly reveals distinct modulation bands in the visible and near‐infrared (NIR) regions. Notably, these bands exhibit orthogonal polarization dependencies, enabling the selective modulation of visible and NIR light via polarization control. Theoretical analysis reveals that the modulation bands in the visible and NIR regions arise from the perpendicularly anisotropic excited‐state absorption of electrons and holes, respectively. This is supported by distinct ultrafast cooling times observed for electrons and holes. The modulations exhibit picosecond‐scale dynamics owing to efficient Auger recombination. These exceptional characteristics highlight the promising nature of low‐symmetry TlSe as a novel material for ultrafast dual‐band nanophotonics. Furthermore, this work provides fundamental insights into anisotropic carrier dynamics, including effective mass‐dependent cooling and many‐body interactions.

Slow Auger Recombination in Ag2Se Colloidal Quantum Dots.

Efficient Auger recombination (AR) presents a significant challenge for the advancement of colloidal quantum dot (QD)-based devices involving multiexcitons. Here, the AR dynamics of near-infrared Ag2Se QDs were studied through transient absorption experiments. As the QD radius increases from 0.9 to 2.5 nm, the biexciton lifetime (τ2) of Ag2Se QDs increases from 35 to 736 ps, which is approximately 10 times longer than that of comparable-sized CdSe and PbSe QDs. A qualitative analysis based on observables indicates that the slow Auger rate is primarily attributed to the low density of the final states. The biexciton lifetime and triexciton lifetime (τ3) of Ag2Se QDs follow R3 and R2.6 dependence, respectively. Moreover, the ratio of τ2/τ3 is ∼2.3-3.2, which is markedly lower than the value expected from statistical scaling (4.5). These findings suggest that environmentally friendly Ag2Se QDs can serve as excellent candidates for low-threshold lasers and third-generation photovoltaics utilizing carrier multiplication.

Correlation between Single-Photon Emission and Size of Cesium Lead Bromide Perovskite Nanocrystals.

Emission photon statistics of semiconductor nanocrystal quantum dots (QDs), including lead halide perovskite nanocrystals (PNCs), are important fundamental and practical optical properties. Single QDs exhibit high-probability single-photon emission owing to the efficient Auger recombination between generated excitons. Because the recombination rate depends on QD size, single-photon emission probability should be size-dependent. Previous studies have researched QDs smaller than their exciton Bohr diameters (twice the Bohr radius of excitons). Here, we investigated the relationship between the single-photon emission behavior and size of CsPbBr3 PNCs to elucidate their size threshold. Simultaneous single-nanocrystal spectroscopy and atomic force microscopy observations on single PNCs with approximately 5-25 nm edge length showed that those smaller than approximately 10 nm, which had size-dependent photoluminescence (PL) spectral shifts, exhibited high-probability single-photon emissions, which decreased linearly with PNC volume. Novel single-photon emission, size, and PL peak correlations of PNCs are important for understanding the relationship between single-photon emission and quantum confinement.

Auger scattering dynamic of photo-excited hot carriers in nano-graphite film

Charge carrier scattering channels in graphite bridging its valence and conduction band offer an efficient Auger recombination dynamic to promote low energy charge carriers to higher energy states. It is of importance to answer the question whether a large number of charge carriers can be promoted to higher energy states to enhance the quantum efficiency of photodetectors. Here, we present an experimental demonstration of an effective Auger recombination process in the photo-excited nano-graphite film. The time-resolved hot carrier thermalization was analyzed based on the energy dissipation via the Auger scattering channels. We split the Auger recombination occurrence centered at 0.40 eV energy state into scattering and recombination parts, for characterizing the scattering rate in the conduction band and the recombination rate toward the valence band. The scattering time with respect to the energy state was extracted as 8 ps · eV−1, while the recombination time with respect to the energy state was extracted as 24 ps · eV−1. Our study indicates a 300 fs delay between the hot carrier recombination and generation, leading to a 105 ps−1 · cm−3 Auger scattering efficiency. The observed duration for the Auger recombination to generate hot carriers is prolonged for 1 ps, due to the hot carriers energy relaxation bottleneck with optical-phonons in the nano-graphite. The presented analytic expression gives valuable insights into the Auger recombination dynamic to estimate its most efficient energy regime for mid-infrared photodetection.

Collective enhancement of quantum coherence in coupled quantum dot films

Colloidal semiconductor quantum dots (QDs) are attractive materials that provide unique photophysics of multiple electron-hole pairs (multiexcitons) in strongly quantum confined systems. Multiexciton phenomena such as efficient Auger recombination have been intensively investigated with respect to individual QDs. However, the cooperative nature of QDs, especially in terms of multiexciton coherence, has not been elucidated thus far. Here, we report the observation of the collective enhancement of quantum coherence in coupled QD films. Using a photocurrent quantum interference technique, we find that the multiexciton quantum coherence in coupled QDs is significantly increased compared to the case of isolated QDs. This cooperative effect is induced by the coherent electronic coupling between QDs. Our results clarify the enhancement mechanism in coupled quantum systems and open the door to advanced optoelectronic applications such as coherent amplifiers and frequency upconverters.

Photo-induced droop in blue to red light emitting InGaN/GaN single quantum wells structures

The variation of the internal quantum efficiency (IQE) of single InGaN quantum well structures emitting from blue to red is studied as a function of the excitation power density and the temperature. By changing the well width, the indium content, and adding a strain compensation AlGaN layer, we could tune the intrinsic radiative recombination rate by changing the quantum confined Stark effect, and we could modify the carrier localization. Strong quantum confined Stark effect and carrier localization induce an increase in the carrier density and then favor Auger non-radiative recombination in the high excitation range. In such high excitation conditions with efficient Auger recombination, the variation of the IQE with the photo-excitation density P is ruled by a universal power law independent of the design: IQE = IQEMAX – a log10P with a close to 1/3. The temperature dependences of the different recombination mechanisms are determined. At low temperature, both quantum confined Stark effect and carrier localization trigger electron-electron repulsions and therefore the onset of the Auger effect. The increase in the value of coefficient C with changing temperature reveals indirect Auger recombination that relates to the interactions of the carriers with other phonons than the longitudinal optical one.

Biexciton Auger Recombination in CdSe/CdS Core/Shell Semiconductor Nanocrystals.

A theoretical study of the positive and negative trion channels in the nonradiative Auger recombination of band-edge biexcitons (BXs) in CdSe/CdS core/shell nanocrystals (NCs) is presented. The theory takes into account the BX fine-structure produced by NC asymmetry and hole-hole exchange interaction. The calculations show that growth of CdS shell upon CdSe core suppresses the rate of the Auger recombination via negative trion channel, while the more efficient Auger recombination via positive trion channel shows much weaker dependence on the shell thickness. The demonstrated oscillatory dependence of the BX Auger rate on the core and shell sizes is explained qualitatively in terms of overlap of the ground and excited carrier wave functions. The calculations show that raise of temperature accelerates the Auger recombination in CdSe/CdS NCs due to reduction of the bulk energy gaps of CdSe and CdS.

Off-State Quantum Yields in the Presence of Surface Trap States in CdSe Nanocrystals: The Inadequacy of the Charging Model To Explain Blinking

In the charging model the fluorescence intermittency observed in semiconductor nanocrystals is explained in terms of an Auger-mediated quenching of the photoluminescence in the presence of a single additional charge delocalized in the dot core. The validity of this description has however been challenged by recent experimental results. A realistic scenario that is often proposed to explain the origin of the extra charge, portrays the latter as the result of photogeneration followed by trapping of one of the particles at the surface. The effects of the presence of a surface-localized charge were however not considered in any of the models that led to the challenge. This study addresses this fundamental issue. Using ab-initio-uality wavefunctions within the semiempirical pseudopotential approach, the predictions of the charging model are here thoroughly tested for all possible configurations that could exhibit efficient Auger recombination and, therefore, be responsible for the quenching of the PL in the off state. The results, although confirming the conclusion that the presently accepted charging model is inadequate to explain blinking in NCs, suggest multiple charging as a possible origin of off states with very low quantum ield. A modification to one of the recently proposed phenomenological blinking models is suggested to account for this feature.

The femtosecond optical response of porous, amorphous and crystalline silicon

The carrier dynamics in porous silicon have been investigated using femtosecond time-resolved spectroscopy. The results are compared to those obtained under identical conditions on a-Si:H, crystalline silicon and GaAs. Porous silicon is an indirect bandgap material with a free carrier absorption cross section that is lower than that of a-Si:H and comparable to that of crystalline silicon. Our measurements indicate carrier trapping within 200 fs followed by a slower decay on a subnanosecond time scale that speeds up at elevated injected densities. This effect is interpreted as efficient Auger recombination of carriers generated in, and confined to, nanometer sized crystallites.