Ultrasensitive PbS‐Quantum‐Dot Photodetectors for Visible–Near‐Infrared Light Through Surface Atomic‐Ligand Exchange

A surface atomic‐ligand exchange method is applied the first time in the construction of photodetectors (PDs) based on PbS quantum dots (QDs) for ultrasensitivity. The device thus produces a high photosensitivity to visible and near‐infrared light with a photoresponsivity up to 7.5 × 10³ A W^?1 and a high stability in air. In particular, these PbS‐QD‐based PDs show the capability of following a pulse light with a frequency up to 100 kHz well at a relatively fast response time/recovery time of ≈4/40 μs, much faster than most previous QD‐based PDs. The short response time is attributed to modification for the surface of the PbS‐QDs by cetyltrimethylammonium bromide treatment, which effectively improves the contact between the QDs and the Au electrodes, leading to extracting a high carrier mobility (≈0.142 cm² V^?1 s^?1). These findings show the great potential of PbS‐QDs as high‐speed nano‐photodetectors, and, more importantly, demonstrate the importance of the surface atomic‐ligand exchange method in the construction of QD‐based devices.     

Diode-pumped Tm:KY(WO4)2 laser passively Q-switched with PbS-doped glass

Glass doped with PbS quantum dots is presented as a saturable absorber (SA) for a passive Q-switching of a diode-pumped 1.9 μm Tm:KYW laser. Output pulses with energy of 44 μJ at a repetition rate of 2.5 kHz with an average output power of 110 mW were obtained. The Q-switching conversion efficiency was 33%. The absorption saturation intensity of the glass doped with PbS quantum dots with a mean radius of 5.2 nm at a wavelength of 2 μm was measured to be 1.5 MW/cm².     

Frequency and density dependent radiative recombination processes in III–V semiconductor quantum wells and superlattices

In this paper we review the radiative recombination processes occurring in semiconductor quantum wells and superlattices under different excitation conditions. We consider processes whose radiative efficiency depends on the photogenerated density of elementary excitations and on the frequency of the exciting field, including luminescence induced by multiphoton absorption, exciton and biexciton radiative decay, luminescence arising from inelastic excitonic scattering, and electron-hole plasma recombination.

Semiconductor quantum wells are ideal systems for the investigation of radiative recombination processes at different carrier densities owing to the peculiar wavefunction confinement which enhances the optical non-linearities and the bistable behaviour of the crystal. Radiative recombination processes induced by multi-photon absorption processes can be studied by exciting the crystal in the transparency region under an intense photon flux. The application of this non-linear spectroscopy gives direct access to the excited excitonic states in the quantum wells owing to the symmetry properties and the selection rules for artificially layered semiconductor heterostructures.

Different radiative recombination processes can be selectively tuned at exciting photon energies resonant with real states or in the continuum of the conduction band depending on the actual density of photogenerated carriers. We define three density regimes in which different quasi-particles are responsible for the dominant radiative recombination mechanisms of the crystal: (i) The dilute boson gas regime, in which exciton density is lower than 10¹⁰ cm^-2. Under this condition the decay of free and bound excitons is the main radiative recombination channel in the crystal. (ii) The intermediate density range (n < 10¹¹ cm^-2) at which excitonic molecules (biexcitons) and inelastic excitonic scattering processes contribute with additional decay mechanisms to the characteristic luminescence spectra. (iii) The high density range (n ?10¹² cm^-2) where screening of the Coulomb interaction leads to exciton ionization. The optical transitions hence originate from the radiative decay of free-carriers in a dense electron-hole plasma.

The fundamental theoretical and experimental aspects of the radiative recombination processes are discussed with special attention to the GaAs/Al _x Ga_1-x As and Ga _x In_1-x As/Al _y In_1-y As materials systems. The experimental investigations of these effects are performed in the limit of intense exciting fields by tuning the density of photogenerated quasi-particles and the frequency of the exciting photons. Under these conditions the optical response of the quantum well strongly deviates from the well-known linear excitonic behaviour. The optical properties of the crystal are then no longer controlled by the transverse dielectric constant or by the first-order dielectric susceptibility. They are strongly affected by many-body interactions between the different species of photogenerated quasi-particles, resulting in dramatic changes of the emission properties of the semiconductor.

The systematic investigation of these radiative recombination processes allows us to selectively monitor the many-body induced changes in the linear and non-linear optical transitions involving quantized states of the quantum wells. The importance of these effects, belonging to the physics of highly excited semiconductors, lies in the possibility of achieving population inversion of states associated with different radiative recombination channels and strong optical non-linearities causing laser action and bistable behaviour of two-dimensional heterostructures, respectively.     

Electron-hole plasma in pulse photoexcited single quantum wells

We report photoluminescence studies of MOCVD grown, GaAsAl_xGa_1?xAs single quantum wells which were intensly excited with a pulse dye laser at T=2K. For a well width of d～40Å, the spectra are interpreted as due to the radiative recombination of a hot electron-hole plasma confined to the well. The density of charge carriers and their temperature depend upon the excitation intensity, and vary in the range of 10¹¹–10¹³ cm^?2 and 100–500K for an absorbed photon flux of 10¹³–10¹⁶ photons-cm^?2 per pulse, respectively. The observed spectral features are identified as the e1-hh1 and e1-lh1 transitions and two additional bands which are tentatively assigned to transitions involving virtual bound states of either the electron or the hole. The electron-hole plasma spectra of the d～40Å sample are strongly polarized perpendicular to the well quantization axis. For wider wells (d～80 and 150Å) smaller photoexcited carrier densities were observed for the same absorbed photon flux. It is thus concluded that the capture efficiency of the well is small.     

Cover Picture: Contrib. Plasma Phys. 7/2013

A 250 µm thick high purity beryllium foil is symmetrically irradiated by a total of 20 laser beams at 351 nm wavelength. Each laser carries 480 J in a 1 ns long pulse, the pulses are staggered in time and focussed on a 800 µm diameter focal spot, yielding a flat top intensity profile of 2.4 × 10¹⁴ W/cm² for 3 ns on the target surface. The evolution of the mass density is modelled with the radiation‐hydrodynamics code HELIOS as function of the target depth. (© 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Spectroscopic analysis of Er transition in Mg/Er-codoped LiNbO3 crystal

We present a Judd-Ofelt spectroscopic analysis on the Mg/Er-codoped congruent lithium niobate (LiNbO₃) crystals. The Judd-Ofelt model is applied to the room temperature unpolarized absorption intensities of Er³⁺ ions on eleven transition bands to determine their intensity parameters: Ω₂=2.36×10⁻²⁰ cm², Ω₄=0.76×10⁻²⁰ cm², Ω₆=0.30×10⁻²⁰ cm² in Er:LiNbO₃ crystal heavily codoped with MgO. The radiative lifetime of ²H_9/2 becomes longer when MgO is added into Er:LiNbO₃ crystal. The experimental lifetimes are obtained using microsecond time-resolved spectra at 400 nm femtosecond pulse excitation to predict radiative quantum efficiency. Combining higher radiative quantum efficiency with longer radiative lifetime, we conclude that Mg/Er-codoped LiNbO₃ crystals are more suitable than Er: LiNbO₃ ones in laser materials.     

Multiphoton excitation and dissociation of CH3OH molecules by intense broadband YSGG:Cr:Er laser radiation in the range 2.7 µm

We have observed efficient multiphoton excitation of CH₃OH molecules by broadband pulsed YSGG:Cr:Er-laser radiation (λ=2.7 µm,τ _p =60 ns, and Δν_las～1.5 cm^?1) at fluences of 0.3-600 J/cm² under collisional and collisionless conditions. Multiphoton dissociation of CH₃OH has been realized. We discuss the role of intermode interaction, the intensity of the laser radiation, and the laser bandwidth in the excitation process.     

Optical excitation study on the efficiency droop behaviors of InGaN/GaN multiple-quantum-well structures

Efficiency droop is generally observed in electroluminescence under high current injection. Optical characterization on efficiency droop in InGaN/GaN multiple-quantum-well structures has been conducted at 12 K. Clear droop behaviors were observed for the sample excited by above-bandgap excitation of GaN with pulse laser. The results show that dislocation is not the crucial factor to droop under high carrier density injection, and Auger recombination just slightly affects the efficiency. The radiative recombination may be mainly affected by a multi-carrier-related process (diffusion and drift with a factor of n ^3.5 and n ^5.5) at the interface between GaN barrier and InGaN well.     

Photodissociation effects on pulsed laser deposited silver oxide thin films: surface‐enhanced resonance Raman scattering

Temporal Raman scattering measurements with 488, 532 and 632 nm excitation wavelengths and normal Raman studies by varying the power (from 30 W/cm² to 2 MW/cm²) at 488 nm were performed on silver oxide thin films prepared by pulsed‐laser deposition. Initially, silver oxide Raman spectra were observed with all three excitation wavelengths. With further increase in time and power, silver oxide photodissociated into silver nanostructures. High‐intensity spectral lines were observed at 1336 ± 25 and 1596 ± 10 cm⁻¹ with 488 nm excitation. No spectral features were observed with 633 nm excitation. Surface‐enhanced resonance Raman scattering theory is used to explain the complex behavior in the intensity of the 1336/1596 cm⁻¹ lines with varying power of 488 nm excitation. Copyright © 2011 John Wiley & Sons, Ltd.     

PbS colloidal quantum dot/ZnO‐based bulk‐heterojunction solar cells with high stability under continuous light soaking

PbS colloidal quantum dot (CQD)‐based depleted bulk‐heterojunction solar cells were constructed, using the 1.2 μm thick nanowire array infiltrated with PbS QDs bearing Br ligands. The long‐term stability tests were performed on the solar cells without encapsulation in air under continuous light soaking using a Xe lamp with an AM1.5G filter (100 mW cm^?2). Time course of solar cell performances during the tests showed two time periods with distinct behavior, that is, the initial transient time period and the relatively stable region following it. The power conversion efficiency was found to keep approximately 90% of the initial value at the end of the 3000 h light soaking test. The stability tests suggest that the PbS surface modification or passivation reactions play an important role in achieving such a high stability, and demonstrate that PbS CQD/ZnO nanowire array‐based depleted bulk‐heterojunction solar cells are highly stable. (© 2014 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

Enhancing the performance of thin film CdS/PbS photovoltaic solar cells

This work investigates dependence of the short-circuit current density, open-circuit voltage, fill factor and efficiency of a thin film CdS/PbS solar cell on thickness of transparent conductive oxide (TCO) layer, thickness of window layer (CdS), concentration of uncompensated acceptors (width of space-charge region), carrier lifetime in PbS and the reflectivity from metallic back contact. The effect of optical losses, front and rear recombination losses as well as the recombination losses on space-charge region are also considered in this study. As a result, by thinning the front contact layer indium tin oxide from 400 to 100 nm and window layer (CdS) from 200 to 100 nm it is possible to reduce the optical losses from 32 to 20%. The effect of electron lifetime on the internal and external quantum efficiency can be neglected at high width of the space-charge region. The maximum current density of 18.4 mA/cm² is achieved at wide space-charge region (concentration of uncompensated acceptors = 10¹⁵ cm^?3) and the longest lifetime (τ_n = 10^?6 s) where the optical and recombination losses are about 55%. The maximum efficiency of 5.17%, maximum open-circuit voltage of 417 mV and approximately fixed fill factor of 74% are yielded at optimum conditions such as: electron lifetime = 10^?6 s; concentration of uncompensated acceptors = 10¹⁶ cm^?3; thickness of TCO = 100 nm; thickness of CdS = 100 nm; velocity of surface and rear recombination = 10⁷ cm/s and thickness of absorber layer = 3 μm. When the reflectance from the back contact is 100%, the cell parameters improve and the cell efficiency records a value of 6.1% under the above conditions.     

All‐optical modulation based on silicon quantum dot doped SiOx:Si‐QD waveguide

All‐optical modulation based on silicon quantum dot doped SiO_x:Si‐QD waveguide is demonstrated. By shrinking the Si‐QD size from 4.3 nm to 1.7 nm in SiO_x matrix (SiO_x:Si‐QD) waveguide, the free‐carrier absorption (FCA) cross section of the Si‐QD is decreased to 8 × 10⁻¹⁸ cm² by enlarging the electron/hole effective masses, which shortens the PL and Auger lifetime to 83 ns and 16.5 ps, respectively. The FCA loss is conversely increased from 0.03 cm⁻¹ to 1.5 cm⁻¹ with the Si‐QD size enlarged from 1.7 nm to 4.3 nm due to the enhanced FCA cross section and the increased free‐carrier density in large Si‐QDs. Both the FCA and free‐carrier relaxation processes of Si‐QDs are shortened as the radiative recombination rate is enlarged by electron–hole momentum overlapping under strong quantum confinement effect. The all‐optical return‐to‐zero on‐off keying (RZ‐OOK) modulation is performed by using the SiO_x:Si‐QD waveguides, providing the transmission bit rate of the inversed RZ‐OOK data stream conversion from 0.2 to 2 Mbit/s by shrinking the Si‐QD size from 4.3 to 1.7 nm.     

CdSe/CdMnSe多量子阱的激子光学性质的研究

用分子束外延在GaAs衬底上生长了CdSe/CdMnSe多量子阱结构.利用X射线衍射(XRD)、变密度激发的PL光谱、变温度PL光谱和变密度激发的ps时间分辨光谱研究了CdSe/CdMnSe多量子阱结构和激子复合特性.讨论了随温度升高辐射线宽展宽和辐射复合效率降低的机理.发现不同激发密度下发光衰减时间不同,认为它的机理可能是无辐射复合引起的.在该材料中观测到激子激子散射发射峰,它被变密度激发和变温度PL光谱所证实. 关键词： CdSe/CdMnSe 量子阱 光学性质     

Quantum efficiency and radiative lifetime in degenerate n-type GaAs

The hole lifetime, the radiative lifetime, the non-radiative lifetime, and the internal quantum efficiency in degenerate n-type GaAs crystals have been investigated with a simplified model of degenerate semiconductors, in which the recombination constant B is approximately proportional to the$\text{?13}\text{8}$ power of the electron density.In n-type GaAs at 77 K, the radiative lifetime reaches a minimum equal to 4 × 10^?9 sec. at 6 × 10¹⁷ cm^?3, and the internal quantum efficiency exhibits a maximum equal to 50% at 8 × 10¹⁷cm^?3, in good agreement with the theoretical prediction of Dumke and the experiments of Cusano. At high impurity concentrations, the polytropy effect is taken into account in the case of GaAs crystals doped with tellurium and selenium. Finally, it is suggested that, for a given high concentration, the internal quantum efficiency increases with increasing temperature, in accordance with the observed results.     

Electron-hole liquid in GaS

Photoluminescence spectra of “pure” GaS are recorded under high excitation levels and low temperatures between 1.9 and 10K. This work reports a new and broad band which dominates the spectrum at high excitation intensities and temperatures near 1.9K. Its dependence on the excitation level is highly superlinear. When temperature is raised from 1.9 to 10K the spectrum observed of low excitation levels is recovered. We interpret the band here observed as due to radiative recombination from electron-hole droplets. From best fitting between experimental spectrum and calculated theoretical curves the critical density and the condensation energy are estimated as, n_c = 4.5 × 10²⁰ cm^?3 and φ = 9.0 meV.     

Lattice dynamics in two-photon-excited CdS studied by picosecond time-resolved X-ray diffraction

Lattice dynamics and radiative processes in single-crystal cadmium sulfide induced by two-photon excitation with a femtosecond laser are investigated. The development of lattice expansion is directly observed by picosecond time-resolved X-ray diffraction. The obtained lattice dynamics are explained on the basis of a thermally induced impulsive-strain model. The model calculation indicates that two- and more-photon absorption processes occur and that reflectivity rapidly increases under laser irradiation. In photoluminescence spectroscopy, the spectra for TW cm⁻² excitation are shifted to lower energy and show an additional shoulder at 2.35 eV. Furthermore, emission due to Fabry-Perot laser modes with self-formed cavities was observed under 11 TW cm⁻² excitation. The discrepancy between carrier densities deduced from the lattice expansion and the PL spectra indicates that the predominant process at a higher carrier density is not radiative recombination, but Auger recombination followed by lattice heating.     

Radiative recombination of free excitons in GaAs quantum wells

We have measured the radiative lifetime of excitons in GaAs quantum wells under resonant excitation at 10 K using time resolved luminescence spectroscopy with 6 ps time resolution. The luminescence decay has two components: a fast one with a time constant τ₁ (∼ 17 - 40 ps) and a slow one with a time constant τ₂ (∼ 80 - 300 ps). τ₂ is the lifetime of thermalised excitens at 10 K. τ₁ is due to two mechanisms in parallel: the radiative recombination of excitons with k_u < K₀ and the scattering by acoustical phonens into non radiative exciton states (k_u > k₀ and J = 2). The variation with temperature of τ₁ gives the lifetime of the excitons at k = 0, τ₀, which varies between 20 and 50 ps depending on the sample.     

Exciton relaxation in PbS quantum dots

Exciton relaxation in PbS quantum dots (QDs) in glass and tetrachloroethylene have been investigated and the radiative and non‐radiative relaxation rates of the lowest 1S–1S state have been measured. An estimate of the carrier intra‐band transition rates and their transfer efficiency is calculated. The dependence of the exciton dynamics on the QD surface properties is presented and discussed. (© 2010 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

High critical oxygen concentration in microcrystalline silicon solar cells

For microcrystalline silicon based p–i–n solar cells the effect of deposition conditions on the critical oxygen concentration was investigated. All solar cells were prepared by 13.56 MHz plasma‐enhanced chemical vapour deposition. The critical oxygen concentration defines the lowest oxygen concentration in the intrinsic absorber layer causing a deterioration of the solar cell performance. For intentional contamination of ～1.2–1.3 µm thick i‐layers, the oxygen was inserted by a controllable leak at the process gases supply line, i.e. by a gas pipe leak. For µc‐Si:H deposited at a discharge power of 0.53 W/cm² we find a critical oxygen concentration of 1–2 × 10¹⁹ cm^–3 in agreement with values commonly reported in literature. However, changing the deposition conditions, we find that the critical oxygen concentration in µc‐Si:H cells is not fixed. At reduced power of 0.20 W/cm² a much higher value for the critical oxygen concentration of 1 × 10²⁰ cm^–3 is observed. (© 2010 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)