An overview is given of two distinct classes of semiconductor quantum dots, epitaxial and colloidal structures that have been studied intensely for more than 30 years by now, however, without large ...interconnection between the two involved research communities. The largely parallel and independent evolution of the two structure classes may be partly related to the origin of colloidal systems from chemistry, while epitaxial quantum dots have been addressed mostly by the physics community. These independent evolutions are somewhat surprising because the interest in optics‐related applications is shared by both communities. Here, a short summary of the development of the two structure classes, the present status of activities, and some perspectives for future developments are presented.
A short comparison of the development of the research areas of colloidal and epitaxial quantum dots during the last more than 30 years is drawn. The focus of this comparison is on optical studies and optoelectronic applications, highlighting particular strengths of the two classes of quantum dots.
Advances in colloidal quantum dots
The confinement found in colloidal semiconductor quantum dots enables the design of materials with tunable properties. García de Arquer
et al
. review the recent ...advances in methods for synthesis and surface functionalization of quantum dots that enable fine tuning of their optical, chemical, and electrical properties. These important developments have driven the commercialization of display and lighting applications and provide promising developments in the related fields of lasing and sensing. —MSL
A review highlights advances in the synthesis of colloidal quantum dots that have enabled numerous applications.
BACKGROUND
Semiconductor materials feature optical and electronic properties that can be engineered through their composition and crystal structure. The use of semiconductors such as silicon gallium arsenide sparked technologies from computers and mobile phones to lasers and satellites. Semiconductor quantum dots (QDs) offer an additional lever: Because their size is reduced to the nanometer scale in all three dimensions, the restricted electron motion leads to a discrete atom-like electronic structure and size-dependent energy levels. This enables the design of nanomaterials with widely tunable light absorption, bright emission of pure colors, control over electronic transport, and a wide tuning of chemical and physical functions because of their large surface-to-volume ratio.
ADVANCES
The bright and narrowband light emission of semiconductor QDs, tunable across the visible and near-infrared spectrum, is attractive to realize more efficient displays with purer colors. QDs are engineered compositionally and structurally to manipulate energy states and charge interactions, leading to optical gain and lasing, relevant to light emission across visible and infrared wavelengths and fiberoptic communication. Their tunable surface chemistry allows application as optical labels in bio-imaging, made possible by tethering QDs with proteins and antibodies. The manipulation of QD surfaces with capping molecules that have different chemical and physical functions can be tailored to program their assembly into semiconducting solids, increasing conductivity and enabling the transduction of photonic and chemical stimuli into electrical signals. Optoelectronic devices such as transistors and photodetectors lead to cameras sensitive to visible and infrared light. Highly crystalline QDs can be grown epitaxially on judiciously chosen substrates by using high-temperature and vacuum conditions, and their use has led to commercially viable high-performance lasers. The advent of colloidal QDs, which can be fabricated and processed in solution at mild conditions, enabled large-area manufacturing and widened the scope of QD application to markets such as consumer electronics and photovoltaics.
OUTLOOK
From a chemistry perspective, further advances in QD fabrication are needed to sustain and improve desired chemical and optoelectronic properties and to do so with high reproducibility. This entails the use of inexpensive synthesis methods and precursors that are able to retain laboratory-scale QD properties to market-relevant volumes. A better understanding of the yet-incomplete picture of QD surfaces, atomic arrangement, and metastable character is needed to drive further progress. From a regulatory perspective, added attention is needed to achieve high-quality materials that do not rely on heavy metals such as Cd, Pb, and Hg. The role of nanostructuring in toxicity and life cycle analysis for each application is increasingly important. From a materials and photophysics perspective, exciting opportunities remain in the understanding and harnessing of electrons in highly confined materials, bridging the gap between mature epitaxial QDs and still-up-and-coming colloidal QDs. The yet-imperfect quality of the latter—a price paid today in exchange for their ease of manufacture—remains a central challenge and must be addressed to achieve further-increased performance in devices. From a device perspective, colloidal QD manufacturing must advance to translate from laboratory-scale to large-area applications such as roll-to-roll and inkjet printing. Photocatalysis, in which light is used to drive chemical transformations, is an emerging field in which QDs are of interest. Quantum information technologies, which rely on the transduction of coherent light and electrons, bring new challenges and opportunities to exploit quantum confinement effects. Moving forward, opportunities remain in the design of QD-enabled new device architectures.
Semiconductor quantum dot technologies.
Quantum dots feature widely tunable and distinctive optical, electrical, chemical, and physical properties. They span energy harvesting, illumination, displays, cameras, sensors, communication and information technology, biology, and medicine, among others. These have been exploited to realize efficient lasers, displays, biotags, and solar harvesting devices available in the market and are emerging in photovoltaics, sensing, and quantum information.
In quantum-confined semiconductor nanostructures, electrons exhibit distinctive behavior compared with that in bulk solids. This enables the design of materials with tunable chemical, physical, electrical, and optical properties. Zero-dimensional semiconductor quantum dots (QDs) offer strong light absorption and bright narrowband emission across the visible and infrared wavelengths and have been engineered to exhibit optical gain and lasing. These properties are of interest for imaging, solar energy harvesting, displays, and communications. Here, we offer an overview of advances in the synthesis and understanding of QD nanomaterials, with a focus on colloidal QDs, and discuss their prospects in technologies such as displays and lighting, lasers, sensing, electronics, solar energy conversion, photocatalysis, and quantum information.
Symmetries are the underlying principles of fundamental interactions in nature. Chaos in a quantum system may emerge from breaking these symmetries. Compared to vacuum, crystals are attractive for ...studying quantum chaos, as they not only break spatial isotropy, but also lead to novel quasiparticles with modified interactions. Here we study yellow Rydberg excitons in cuprous oxide which couple strongly to the vacuum light field and interact significantly with crystal phonons, leading to inversion symmetry breaking. In a magnetic field, time-reversal symmetry is also broken and the exciton states show a complex splitting pattern, resulting in quadratic level repulsion for small splittings. In contrast to atomic chaotic systems in a magnetic field, which show only a linear level repulsion, this is a signature of a system where all anti-unitary symmetries are broken simultaneously. This behaviour can otherwise be found only for the electro-weak interaction or engineered billiards.
Light is often characterized only by its classical properties, like intensity or coherence. When looking at its quantum properties, described by photon correlations, new information about the state ...of the matter generating the radiation can be revealed. In particular the difference between independent and entangled emitters, which is at the heart of quantum mechanics, can be made visible in the photon statistics of the emitted light. The well-studied phenomenon of superradiance occurs when quantum-mechanical correlations between the emitters are present. Notwithstanding, superradiance was previously demonstrated only in terms of classical light properties. Here, we provide the missing link between quantum correlations of the active material and photon correlations in the emitted radiation. We use the superradiance of quantum dots in a cavity-quantum electrodynamics laser to show a direct connection between superradiant pulse emission and distinctive changes in the photon correlation function. This directly demonstrates the importance of quantum-mechanical correlations and their transfer between carriers and photons in novel optoelectronic devices.
Abstract
The lead halide perovskites demonstrate huge potential for optoelectronic applications, high energy radiation detectors, light emitting devices and solar energy harvesting. Those materials ...exhibit strong spin-orbit coupling enabling efficient optical orientation of carrier spins in perovskite-based devices with performance controlled by a magnetic field. Here we show that elaborated time-resolved spectroscopy involving strong magnetic fields can be successfully used for perovskites. We perform a comprehensive study of high-quality lead halide perovskite CsPbBr
3
crystals by measuring the exciton and charge carrier
g
-factors, spin relaxation times and hyperfine interaction of carrier and nuclear spins by means of coherent spin dynamics. Owing to their ‘inverted’ band structure, perovskites represent appealing model systems for semiconductor spintronics exploiting the valence band hole spins, while in conventional semiconductors the conduction band electrons are considered for spin functionality.
•We examine performance of borehole heat exchanger with a layered subsurface.•Both thermal and hydraulic properties of the borehole field are investigated.•Both homogenous and stratified ground ...models give similar thermal output of BHE.•Stratified model indicates less heat is transferred in aquiclude than aquifers.•Length of the BHEs can be reduced due to the lower heat performance of basal layer.
In the current design of borehole heat exchangers (BHEs), the ground is commonly considered to be homogenous. However, in a layered subsurface, thermal performance of BHE can deviate drastically with different strata. Thereby, analysis of the heat transfer of a BHE with different geological layers is important for optimal sizing of BHE.
In this paper, we examine thermal performance of BHEs settled in a ground with five bedded sedimentary layers. Thermal and hydraulic properties of the borehole field are firstly investigated. Based on the experimental data, a numerical model is developed to examine thermal exchange of the BHEs in this layered subsurface. Two modeling approaches, where the ground properties considered to be homogenous or stratified, are implemented. Numerical results from both approaches are validated and they give similar thermal output of the BHEs. The model with a stratified subsurface further indicates that there is only 74.1% amount of heat transferred in the basal layer with negligible groundwater flow as compared to that of aquifer layers.
Abstract
The ability to generate and control strong long-range interactions via highly excited electronic states has been the foundation for recent breakthroughs in a host of areas, from atomic and ...molecular physics to quantum optics and technology. Rydberg excitons provide a promising solid-state realization of such highly excited states, for which record-breaking orbital sizes of up to a micrometer have indeed been observed in cuprous oxide semiconductors. Here, we demonstrate the generation and control of strong exciton interactions in this material by optically producing two distinct quantum states of Rydberg excitons. This is made possible by two-color pump-probe experiments that allow for a detailed probing of the interactions. Our experiments reveal the emergence of strong spatial correlations and an inter-state Rydberg blockade that extends over remarkably large distances of several micrometers. The generated many-body states of semiconductor excitons exhibit universal properties that only depend on the shape of the interaction potential and yield clear evidence for its vastly extended-range and power-law character.
•We examine heating and cooling performance of a GSHP system.•Similar thermal performance of the BHEs with three different borehole diameters.•COP of the GSHP system is estimated to be 3.9 for a ...typical winter day.•EER of the GSHP system is assessed to be 8.0 for a typical summer day.•SEER increases along the years, whereas seasonal COP decreases at the same period.
This paper examines thermal performance of a ground source heat pump (GSHP) system. The GSHP system was installed in an office building in Nuremberg city of Germany. In order to evaluate system performance the GSHP system has been continuously monitored for 4 years. Heating and cooling performance of the GSHP system is analyzed based on the accumulated data.
Major findings of this work include: (1) coefficient of performance (COP) is estimated to be 3.9 for a typical winter day and energy efficiency ratio (EER) is assessed to be 8.0 for a typical summer day. These results indicate that the GSHP system has a higher efficiency for building cooling than building heating. (2) For a long-term period, the seasonal energy efficiency ratio (SEER) of the GSHP system is observed to increase by 8.7% annually, whereas the seasonal COP is decreased by 4.0% over a 4-year period. The heating and cooling performance of the GSHP system migrates in opposite trend is caused by the unevenly distributed heating and cooling load of the building. This phenomenon deserves serious attention in the design of future GSHP systems in order to avoid the reducing of energy efficiency over long-term operation.
We report a time-resolved study of the photoluminescence of CdSe colloidal nanoplatelets with two different thicknesses. By studying the exciton recombination dynamics we assess the exciton fine ...structure in these systems. The splitting between bright and dark excitons is enhanced compared to epitaxial quantum well structures as result of dielectric confinement. Despite of strong variations in the absolute magnitude, by comparison with literature data we find a relatively slightly varying bright–dark exciton lifetime ratio in very different CdSe-based colloidal nanostructures, regardless of growth technique and of core and shell properties such as materials, dimensions, etc. This finding points to a universal mechanism in the dark exciton recombination.
Coherent control of a strongly inhomogeneously broadened system, namely, InAs self-assembled quantum dots, is demonstrated. To circumvent the deleterious effects of the inhomogeneous broadening, ...which usually masks the results of coherent manipulation, we use prepulse two-dimensional coherent spectroscopy to provide a size-selective readout of the ground, exciton, and biexciton states. The dependence on the timing of the prepulse is due to the dynamics of the coherently generated populations. To further validate the results, we performed prepulse polarization dependent measurements and confirmed the behavior expected from selection rules. All measured spectra can be excellently reproduced by solving the optical Bloch equations for a 4-level system.
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