Charged two-exciton emission from a single semiconductor nanocrystal
Here, we study the photoluminescence (PL) time trajectories of single CdSe/ZnS nanocrystals (NCs) as a function of the laser excitation power. At the low laser power, the PL intensity of a single NC switches between the “on” and “off” levels arising from the neutral and positively charged single excitons, respectively. With the increasing laser power, an intermediate “grey” level is formed due to the optical emission from a charged multiexciton state composed of two excitons and an extra electron. Both the inter-photon correlation and the PL decay measurements demonstrate that lifetime-indistinguishable photon pairs are emitted from this negatively charged two-exciton state.
682
- 10.1038/ncomms3661
- Oct 25, 2013
- Nature Communications
168
- 10.1103/physrevlett.94.087403
- Mar 3, 2005
- Physical Review Letters
581
- 10.1126/science.1173812
- Jun 18, 2009
- Science
96
- 10.1021/nn303396c
- Sep 26, 2012
- ACS Nano
234
- 10.1038/nnano.2012.260
- Feb 10, 2013
- Nature Nanotechnology
82
- 10.1103/physrevb.71.205317
- May 26, 2005
- Physical Review B
13
- 10.1103/physrevb.88.155440
- Oct 31, 2013
- Physical Review B
509
- 10.1021/nl0342491
- Jul 2, 2003
- Nano Letters
137
- 10.1021/nn900296q
- Aug 5, 2009
- ACS Nano
39
- 10.1021/nn4017845
- May 21, 2013
- ACS Nano
- Research Article
149
- 10.1021/acs.nanolett.6b02874
- Oct 4, 2016
- Nano Letters
Over the last two decades, intensive research efforts have been devoted to the suppressions of photoluminescence (PL) blinking and Auger recombination in metal-chalcogenide nanocrystals (NCs), with significant progresses being made only very recently in few specific NC structures. Here we show that nonblinking PL is readily available in the newly synthesized perovskite CsPbI3 NCs and that their Auger recombination of charged excitons is greatly slowed down, as signified by a PL lifetime about twice shorter than that of neutral excitons. Moreover, spectral diffusion is completely absent in single CsPbI3 NCs at the cryogenic temperature, leading to a resolution-limited PL line width of ∼200 μeV.
- Research Article
11
- 10.1021/acs.jpclett.9b03009
- Dec 3, 2019
- The Journal of Physical Chemistry Letters
Inspired by the superior optoelectronic performances of various 2D semiconductors, their new compositions and structures are being actively pursued in order to foster novel fundamental physics and device applications. As a layered semiconductor with a direct bandgap, few-layer PbI2 should have drawn much research attention due to their capability of emitting photons at short wavelengths of the visible spectrum. Here we chemically synthesize few-layer PbI2 flakes and nanoparticles, which demonstrate unique exciton properties that have rare counterparts in other 2D semiconductors. For three layers and more, the single PbI2 flakes can be utilized to show how the bandgap energy of a 2D semiconductor evolves with the changing layer thickness. The single PbI2 nanoparticles are associated with an ultranarrow photoluminescence line width of ∼1 meV, thus reflecting the influence of lateral quantum confinement on the energy-level structures of a 2D semiconductor. The above findings mark the emergence of a potent 2D platform that is more than complementary to well-studied transition-metal dichalcogenide monolayers.
- Research Article
3
- 10.1039/d2nr00761d
- Jan 1, 2022
- Nanoscale
Semiconductor quantum dots have extremely significant advantages in terms of optoelectronic devices. However, it is unfeasible to avoid the generation of charged exciton states during operation. Such states can change the radiation recombination rate and bring additional non-radiative Auger recombination channels. Herein, we synthesize high photoluminescence quantum yield medium-size CdSe/CdZnS/ZnS core/alloy shell/shell QDs. Their multiexciton spectra and dynamics were systematically studied by pump-power-dependent fluorescence blinking and time-correlated spectroscopy. The lifetimes of positively/negatively charged trions and biexcitons are estimated to be 0.74/6.1 and 0.16 ns, respectively. It demonstrated that the band-edge biexciton is influenced by the Coulomb interaction and Stark effect. The amplified spontaneous emission threshold is only 81 μJ cm-2 and can retain a long operation lifetime under continuous pumping. A vertical microcavity surface-emitting laser device is fabricated using these QDs. The coupling factor between the spontaneous emission and cavity mode is 0.81, which benefits the low stimulated emission threshold. This work provides a new perspective of the charged states in the multiexciton AR process in the QDs, implying a promising application prospect of such QDs as optical gain materials in "zero-threshold" laser fabrication.
- Research Article
20
- 10.1021/acsnano.6b08040
- Feb 27, 2017
- ACS Nano
The majority of quantum dot (QD) blinking studies have used a model of switching between two distinct fluorescence intensity levels, "on" and "off". However, a distinct intermediate intensity level has been identified in some recent reports, a so-called "grey" or "dim" state, which has brought this binary model into question. While this grey state has been proposed to result from the formation of a trion, it is still unclear under which conditions it is present in a QD. By performing shell-dependent blinking studies on CdSe QDs, we report that the populations of the grey state and the on state are strongly dependent on both the shell material and its thickness. We found that adding a ZnS shell did not result in a significant population of the grey state. Using ZnSe as the shell material resulted in a slightly higher population of the grey state, although it was still poorly resolved. However, adding a CdS shell resulted in the population of a grey state, which depended strongly on its thickness up to 5 ML. Interestingly, while the frequency of transitions to and from the grey state showed a very strong dependence on CdS shell thickness, the brightness of and the dwell time in the grey state did not. Moreover, we found that the grey state acts as an on-pathway intermediate state between on and off states, with the thickness of the shell determining the transition probability between them. We also identified two types of blinking behavior in QDs, one that showed long-lived but lower intensity on states and another that showed short-lived but brighter on states that also depended on the shell thickness. Intensity-resolved single QD fluorescence lifetime analysis was used to identify the relationship between the various exciton decay pathways and the resulting intensity levels. We used this data to propose a model in which multiple on, grey, and off states exist whose equilibrium populations vary with time that give rise to the various intensity levels of single QDs and which depends on shell composition and thickness.
- Research Article
1
- 10.1016/j.jlumin.2019.02.006
- Feb 5, 2019
- Journal of Luminescence
Effect of incident laser power and incorporating polariton effects in GaN microrods
- Conference Article
- 10.1117/12.2236263
- Nov 2, 2016
When a UV photon is absorbed by a single semiconductor nanocrystal (NC), two or more excitons can be simultaneously generated through the carrier multiplication (CM) process. It is still highly debated whether the CM efficiency is truly enhanced in semiconductor NCs because all the routine CM measurements performed exclusively at the ensemble level are incapable of completely excluding the false CM signals contributed by the charged excitons. Here we place single CdSe NCs above an aluminum film and successfully resolve their UV-excited photoluminescence time trajectories where the true and false CM signals are contained in the blinking “on” and “off” levels, respectively. When the UV photon energy is ~2.46 times of the NC energy gap, an average CM efficiency of ~20.2% can be reliably estimated. The ability to detect UV-excited photoluminescence from a single NC will surely provide a great guidance for the CM applications in various light-to-electric conversion devices.
- Dissertation
- 10.5451/unibas-003935357
- Jan 1, 2006
Approaching a metallic tip to a single quantum emitter quenches the photolumi- nescence by opening non-radiative decay channels for the excited-state. This is one of the main problems in nano-optics research which prohibits optical studies on single emitters in contact with the tip with high resolution and high sensitivity. In this thesis I have shown that a bowtie nanoantenna can be used to overcome the quenching problem at the single chromophore level. Bowtie antenna tip in- teracts with the dipole of the single emitter. This is most probably the ¯rst study on this type of measurements which opens new pathways for many disciplines. Semiconductor nanocrystals were selected as a single emitter system due to their relatively high photo-stability. Based on °uorescence confocal studies, satura- tion behavior of single CdSefZnSg nanocrystal (NC) is studied under one- and two-photon excitation. In one-photon excitation (1PE) laser wavelength of 532 nm and in two-photon excitation (2PE) laser wavelength of 830 nm were used to excite the °uorophore. Due to the broad distribution in photoluminescence (PL) intensity of nanocrystals, power dependence studies were done based on an average over » 90 nanocrystals. Using focused ion beam, bowtie antennas are sculptured at the apices of silicon nitride AFM tips, which were fully-coated with a homogeneous layer of 40 nm of aluminum ¯lm. Details of structuring procedures used to fabricate well-de¯ned bowtie antennas with smallest possible feedgaps are described. Interaction of bowtie nanoantennas with single semicon- ductor nanocrystals, is investigated using PL intensity and excited-state lifetime of the nanocrystal as two intrinsic signatures of the single emitter. Proximity of the feedgap of a bowtie nanoantenna to a single nanocrystal under one-photon excitation leads to enhanced emission in addition to enhanced excitation. This e®ect is shown, by increasing the PL intensity of the nanocrystal and shortened lifetime, in contact with the bowtie antenna feedgap. These results were com- pared with a fully-coated tip which lead to complete quenching of the nanocrystal PL. Thus, the observed e®ects in PL intensity and lifetime of the nanocrystal in contact with the antenna are originated from the metallic nanostructure. Under two-photon excitation, PL intensity is enhanced but there is no change in the lifetime of the nanocrystal in contact with the bowtie antenna. This is caused by enhanced excitation through the antenna, induced by enlarging the absorption cross section of the nanocrystal in contact with the antenna. Since, °uorescence of single nanocrystal in contact with the bowtie antenna is not quenched, more detailed studies on their interaction were performed. Under two-photon excita- tion absorption cross section of one nanocrystal was measured with and without the presence of antenna. Free nanocrystal showed a two-photon absorption cross section in the order of 6:3£10i37cm4s which in contact with the bowtie antenna increased to 20:2£10i37cm4s. This proves that enhanced excitation observed in 2PE is caused by a larger absorption cross section of the system induced by the antenna structure. Emission polarization of nanocrystals was studied under 1PE using polarization microscopy. From these studies, in- and out-of-plane angles as well as the absolute value of the projection of the transition dipole moment on the sample plane were determined. Results showed in contact with the bowtie antenna, the in-plane angle turns towards the orientation of the antenna. This is induced by the strong dipole of the antenna in contact with the nanocrystal. Moreover, modulation depth and the absolute value of the transition dipole were increased dramatically in contact with the bowtie nanostructure. The results show that antenna/NC system has a highly polarized emission, whose polar- ization direction is determined by the antenna dipole. Photon antibunching of nanocrystals under 1PE was done with and without the presence of the antenna tip. Shorter lifetime of the excited-state in contact with the bowtie antenna immediately appears in antibunching results. This shows that the dead time for single photon generation, caused by excitation-recombination cycles, is much shorter in contact with the antenna. Therefore, a nanocrystal in contact with the bowtie antenna is a more e±cient single photon source. Moreover, taking into account the emission polarization of the antenna/NC system, polarization of single photons generated from the nanocrystal in contact with the antenna can be tuned by antenna orientation. Thus, single photons provided by antenna/NC system can have strong potentials in quantum cryptography. As a result, coupling single quantum emitters (here nanocrystal) to bowtie nanoantennas will produce a new type of emitter with widely adjustable photophysical properties, which can be called a tunable superemitter. Emission characteristics of the antenna/NC system is highly determined by the coupling intra-superemitter.
- Research Article
7
- 10.1016/j.jma.2023.11.005
- Dec 10, 2023
- Journal of Magnesium and Alloys
Interplay of laser power and pore characteristics in selective laser melting of ZK60 magnesium alloys: A study based on in-situ monitoring and image analysis
- Research Article
99
- 10.1016/j.jallcom.2018.06.039
- Jun 5, 2018
- Journal of Alloys and Compounds
Influence of Ni coating on interfacial reactions and mechanical properties in laser welding-brazing of Mg/Ti butt joint
- Research Article
- 10.1080/09507119909447411
- Jan 1, 1999
- Welding International
Summary This paper describes an investigation into the behaviour of helium bubbles in helium-doped austenitic stainless steel weldments by scanning electron microscopy (SEM), transmission electron microscopy (TEM) and numerical calculations. The stainless steel was helium ion implanted and welded with a YAG laser apparatus. Helium ion implantation in the sample was performed with an 8 MeV implantation apparatus. The samples were doped with 1.0 × 1019 atoms/m2 at 5 MeV and then doped with 2.45 × 1019 atoms/m2 at 6 MeV. The results obtained may be summarised as follows. 1. At a low laser power, large helium bubbles of 3–4 μm size are formed at the weld bead/base metal interface, i.e. on the weld metal side of the weld bond region. The amount of weld metal increases, and the helium concentration decreases, with an increasing laser power. The helium bubbles therefore tend to have a diameter as small as under 1 μm. The results of the numerical calculations suggest that the helium concentration in the weld metal is more than 10 appm. Helium-free samples contain no helium bubbles. 2. Helium bubbles with a diameter of less than 0.2 μm are also formed at the grain boundaries in the heat-affected zone (HAZ). The helium bubble region increases with an increasing laser power. 3. The results of the TEM observations suggest that fine helium bubbles of under 0.2 μm size are formed at the dendrite cell boundaries in the weld metal. Their size tends to increase with an increasing laser power. 4. When helium ion implanted samples are laser-welded, helium bubbles are formed in the weld metal and HAZ. Any increases in the laser power and welding speed decrease the helium concentration. Even at helium concentrations of 2.9 and 3.8 appm, helium bubble-induced microcracking occurs at the dendrite cell boundaries in the weld metal.
- Research Article
5
- 10.1016/j.addlet.2022.100097
- Dec 1, 2022
- Additive Manufacturing Letters
• Increasing the laser power in LP-DED enlarged the melt pools in NASA HR-1 alloy. • Heat treatment reduced Ti segregation, occurring after NASA HR-1 deposition. • Material hardness increased with stress relief due to formed precipitate nuclei. • NASA HR-1 hardness and ductility improved with conducting heat treatment. This study investigated the microstructure and tensile properties of the NASA HR-1 (Fe-Ni-Cr) alloy using the laser powder directed energy deposition (LP-DED) process. Laser power and spot size were varied for deposition, and it was noted that low laser power could result in higher cooling rates and finer microstructure. The melt pool depth and width and the defect content increased with the increase in laser power. Out of several laser power (i.e., 350, 750, 1070, 2000, and 2620 W), the samples deposited using 750 W demonstrated the highest material density. In addition, the effects of heat treatment on the microstructure and tensile properties were investigated. It was found that a heat treatment schedule consisting of stress relief, homogenization, solution treatment, and aging could thoroughly homogenize the microstructure (i.e., remove the as-solidified dendritic microstructure), result in relatively uniform, equiaxed grains, and increase the material hardness. Importantly, this heat treatment schedule efficiently reduced titanium segregation, preventing the formation of deleterious needle-shaped η (Ni 3 Ti) precipitates in NASA HR-1, known to be detrimental to mechanical properties and resulted in almost comparable tensile properties with varying laser power.
- Research Article
- 10.1016/j.promfg.2016.12.034
- Dec 26, 2016
- Procedia Manufacturing
Microstructural Evolution and Mechanical Properties of Laser Processed Ti6Al4V Sheets
- Research Article
60
- 10.1103/physrevb.81.115429
- Mar 17, 2010
- Physical Review B
Field-emission patterns from a clean tungsten tip apex induced by femtosecond laser pulses have been investigated. Strongly asymmetric field-emission intensity distributions are observed depending on three parameters: (1) the polarization of the light, (2) the azimuthal and (3) the polar orientation of the tip apex relative to the laser incidence direction. In effect, we have realized an ultrafast pulsed field-emission source with site selectivity of a few tens of nanometers. Simulations of local fields on the tip apex and of electron emission patterns based on photo-excited nonequilibrium electron distributions explain our observations quantitatively. Electron emission processes are found to depend on laser power and tip voltage. At relatively low laser power and high tip voltage, field-emission after two-photon photo-excitation is the dominant process. At relatively low laser power and low tip voltage, photoemission processes are dominant. As the laser power increases, photoemission from the tip shank becomes noticeable.
- Research Article
1
- 10.1016/j.mfglet.2024.09.057
- Oct 1, 2024
- Manufacturing Letters
Effect of laser beam incident angle on welding of Ti6Al4V with fiber lasers
- Research Article
11
- 10.1016/j.mtcomm.2023.105615
- Feb 11, 2023
- Materials Today Communications
Influence of laser power on microstructure evolution and properties of laser cladded FeNiCoCrMo HEA coatings
- Research Article
- 10.1088/2631-8695/ad923d
- Dec 1, 2024
- Engineering Research Express
This research investigates the influence of layer thickness, laser power, and sintering orientation on the mechanical properties of aged Polyamide-12 (PA-12) FS3300PA using the Selective Laser Sintering (SLS) 3D printing method. Specimens were sintered with three different layer thicknesses, laser powers, and sintering orientations using SLS. The study also aimed to examine the resulting powder morphology, mechanical properties, and tensile fracture behaviors of the aged (more than eight continuously sintering cycles) and virgin FS3300PA powders. The specimens divided into ten groups: nine groups of aged powder and one group of virgin powder as a benchmark. The nine groups of aged powder were sintered with three different layer thicknesses (0.07 mm, 0.12 mm, and 0.15 mm), laser powers (65 W, 70 W, and 75 W), and orientations (YZY 0°, YZY 90°, and XYY 0°). The selections of these laser power and layer thickness values for the sintering setting are due to machine and material parameter limitation. The results from these parameters then compared with those of the virgin powder, which sintered using the parameters provided by the manufacturer, in terms of powder morphology, mechanical properties, and tensile fracture behaviours. Observation made using scanning electron microscope (SEM) revealed that there were not many changes in shape, size, and distribution between the virgin and aged powder, but slightly larger sizes and the presence of cracks found in the aged powder. The tensile strength, elongation at break value, and Young’s modulus all shared a similar trend, increasing with higher laser power but decreasing with increased layer thickness. Regarding the fracture morphologies, the number of pores and dimples decreased with increased laser power but increased with thicker layer thickness. There was also the occurrence of un-molten powder, especially in specimens sintered at the YZY 90° orientation with lower laser power and thicker layer thickness.
- Research Article
5
- 10.1016/j.ijrmhm.2023.106484
- Nov 14, 2023
- International Journal of Refractory Metals and Hard Materials
Numerical and experimental study of RHEAs surface morphology and defect in selective laser melting
- Research Article
122
- 10.1016/j.addma.2018.08.028
- Aug 25, 2018
- Additive Manufacturing
Microstructure evolution of 316L produced by HP-SLM (high power selective laser melting)
- Research Article
1
- 10.1002/crat.202200063
- Sep 30, 2022
- Crystal Research and Technology
A Zr‐based amorphous alloy (thickness = 2 mm) is welded by laser welding. The phase composition and microstructure of the welding joints under different laser powers are analyzed by optical microscopy, X‐ray diffraction, and scanning electron microscopy. Mechanical properties of the welded joints under different laser powers are examined using microhardness and tensile testers. The glass forming ability and thermal stability of the welded joints are investigated using differential scanning calorimetry. With an increase in laser power, the degree of crystallization of welded joints increases, their microhardness is in the range 502.3–546.9 HV0.2, and tensile strength is up to 583 MPa (75% of that of the Zr‐based amorphous alloy). Through the research of the article, it can be found that when the laser power increases, the crystallization degree of the welded joint first increases rapidly and then tends to be stable. The lower laser power should be used as far as possible in the case of penetration.
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