Quantum Confinement Research Articles

Wavelength-tunable high-fidelity entangled photon sources enabled by dual Stark effects

The construction of a large-scale quantum internet requires quantum repeaters containing multiple entangled photon sources with identical wavelengths. Semiconductor quantum dots can generate entangled photon pairs deterministically with high fidelity. However, realizing wavelength-matched quantum-dot entangled photon sources faces two difficulties: the non-uniformity of emission wavelength and exciton fine-structure splitting induced fidelity reduction. Typically, these two factors are not independently tunable, making it challenging to achieve simultaneous improvement. In this work, we demonstrate wavelength-tunable entangled photon sources based on droplet-etched GaAs quantum dots through the combined use of AC and quantum-confined Stark effects. The emission wavelength can be tuned by ~1 meV while preserving an entanglement fidelity f exceeding 0.955(1) in the entire tuning range. Based on this hybrid tuning scheme, we finally demonstrate multiple wavelength-matched entangled photon sources with f > 0.919(3), paving the way towards robust and scalable on-demand entangled photon sources for quantum internet and integrated quantum optical circuits.

Fluorescent carbon dots for sensing applications: a review.

Luminescent carbon dots (CDs) are important class of nanomaterials with fantastic photoluminescence (PL) properties, great biocompatibility, extraordinary solubility in water, minimal expense, and so on. There are many methods for their preparation and they are mainly classed into two groups, top-down and bottom-up approaches. In order to understand the origin of fluorescence in quantum CDs, three mechanisms have been proposed namely molecular state, surface state, and quantum confinement phenomenon. Fluorescent CDs have significant application in the fields of biochemical sensing, photocatalysis, bioimaging, delivery of drugs, and other related fields. In this review article the application of quantum dots as detecting component, for the sensing of different targets, has been summed up. In fact, the detection of several analytes including, anions, cations, small molecules, polymers, cells, and microscopic organisms has been discoursed. Moreover, the future aspects of CDs as detecting resources have been explored.

Investigation of the Driving Force of Replacing Adsorbed Hydrocarbons by CO2 in Organic Matter from an Energy Perspective.

Carbon dioxide (CO2) has been widely used to enhance the recovery of adsorbed hydrocarbons from the organic matter (OM) in shale formations. To reveal the driving force of replacing adsorbed hydrocarbons from OM by CO2, we performed molecular dynamics (MD) simulations of the replacement process and calculated the interaction forces between CO2 and hydrocarbons. In addition, based on the umbrella sampling method, steered MD simulations were performed, and the free energy profiles of hydrocarbons were obtained using the weighted histogram analysis method. Results show that the condition of the hydrocarbon replacement by CO2 requires the hydrocarbon to have sufficient kinetic energy or to have a sufficiently large attractive force exerted to ensure that the hydrocarbon escapes the potential well of the OM. The attractive forces exerted on hydrocarbon molecules by CO2 can significantly decrease the energy barrier associated with hydrocarbon movement away from the OM surface. Furthermore, both CO2 and supercritical CO2 can effectively displace adsorbed hydrocarbon gas (methane) on the OM, while supercritical CO2 is required to enhance the recovery of adsorbed hydrocarbon oil (n-dodecane). The results obtained in this study provide guidance for enhancing the recovery of adsorbed hydrocarbons by CO2 in shale formations.

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Research on the Quantum Confinement of Carriers in the type-I Quantum Wells Structure

Abstract Quantum confinement is recognized to be an inherent property in low-dimensional structures. Traditionally it is believed that the carriers trapped within the well cannot escape due to the discrete energy levels. However, our previous research has revealed efficient carrier escape in low-dimensional structures, contradicting this conventional understanding. In this study, we review the energy band structure of quantum wells along the growth direction considering it as a superposition of the bulk material dispersion and quantization energy dispersion resulting from the quantum confinement across the whole Brillouin zone. By accounting for all wave vectors, we obtain a certain distribution of carrier energy at each quantized energy level, giving rise to the energy subbands. These results enable carriers to escape from the well under the influence of an electric field. Additionally, we have compiled a comprehensive summary of various energy band scenarios in quantum well structures, relevant to carrier transport. Such a new interpretation holds significant value in deepening our comprehension of low-dimensional energy bands, discovering new physical phenomena, and designing novel devices with superior performance.

Investigating the optical properties and electronic structure of gallium phosphide nanotubes doped with arsenic via implementing first-principles calculations.

This study investigates the impact of arsenic doping on the optical characteristics and electronic structure of zigzag (8, 0) and armchair (4, 4) gallium phosphide nanotubes using first-principles calculations based on the GaP1-xAsx system, where x = 0, 0.25, 0.5, 0.75, and 1. The electronic calculations showed that doping more arsenic atoms reduces the energy band gap for zigzag and armchair GaPAs nanotubes. PDOS analysis indicates that Ga-4p and P-3p orbitals play a significant role in determining the electronic properties of the GaP nanotube. The dominance of Ga-4p and P-3p orbitals in both the valence and conduction bands indicates their importance across the energy spectrum of the material. The complex dielectric function and absorption coefficient of zigzag and armchair GaP1-xAsx nanotubes are calculated for incident radiation with energies ranging from 1 to 6.2eV. Optical results revealed that both zigzag and armchair GaPNTs exhibit strong absorption in the UV-visible regions due to electronic transitions between different Van Hove singularities. Also, due to quantum confinement effects, pure zigzag gallium phosphide nanotube exhibited two absorption edges at wavelengths (273 and 375nm). These edges stand from the energy level's quantization in the nanotube construction, affecting the absorption characteristics. Substitutional doping by arsenic atoms changes the absorption edge to the long wavelengths due to decreased bandgap energy. Investigating electronic structures and optical properties of nanotubes proposes several advantages, such as understanding the doping effects on the nanotube structure and contributing to the direction of the experimental studies. These computational studies play a key role in developing the applications of nanomaterials. Calculations of density functional theory (DFT) are achieved via the SIESTA package. SIESTA is a powerful and effective tool for executing DFT calculations on a large system of atoms. It generates numerous output files covering detailed information about the electronic structure, optical properties, total energy, optimized geometry, and other computed properties. The generalized gradient approximation GGA with Perdew-Burke-Ernzerhof PBE functional was used. A vacuum region of 10 A0 was applied to avoid the interactions of adjacent nanotubes.

Strain-graded quantum dots with spectrally pure, stable and polarized emission

Structural deformation modifies the bandgap, exciton fine structure and phonon energy of semiconductors, providing an additional knob to control their optical properties. The impact can be exploited in colloidal semiconductor quantum dots (QDs), wherein structural stresses can be imposed in three dimensions while defect formation is suppressed by controlling surface growth kinetics. Yet, the control over the structural deformation of QDs free from optically active defects has not been reached. Here, we demonstrate strain-graded CdSe-ZnSe core-shell QDs with compositionally abrupt interface by the coherent pseudomorphic heteroepitaxy. Resulting QDs tolerate mutual elastic deformation of varying magnitudes at the interface with high structural fidelity, allowing for spectrally stable and pure emission of photons at accelerated rates with near unity luminescence efficiency. We capitalize on the asymmetric strain effect together with the quantum confinement effect to expand emission envelope of QDs spanning the entire visible region and exemplify their use in photonic applications.

From Seeds to Supermassive Black Holes: Capture, Growth, Migration, and Pairing in Dense Protobulge Environments

The origins and mergers of supermassive black holes (SMBHs) remain a mystery. We describe a scenario from a novel multiphysics simulation featuring rapid (≲1 Myr) hyper-Eddington gas capture by a ∼1000 M ⊙ “seed” black hole (BH) up to supermassive (≳106 M ⊙) masses in a massive, dense molecular cloud complex typical of high-redshift starbursts. Due to the high cloud density, stellar feedback is inefficient, and most of the gas turns into stars in star clusters that rapidly merge hierarchically, creating deep potential wells. Relatively low-mass BH seeds at random positions can be “captured” by merging subclusters and migrate to the center in ∼1 freefall time (vastly faster than dynamical friction). This also efficiently produces a paired BH binary with ∼0.1 pc separation. The centrally concentrated stellar density profile (akin to a “protobulge”) allows the cluster as a whole to capture and retain gas and build up a large (parsec-scale) circumbinary accretion disk with gas coherently funneled to the central BH (even when the BH radius of influence is small). The disk is “hypermagnetized” and “flux-frozen”: dominated by a toroidal magnetic field with plasma β ∼ 10−3, with the fields amplified by flux-freezing. This drives hyper-Eddington inflow rates ≳1 M ⊙ yr−1, which also drive the two BHs to nearly equal masses. The late-stage system appears remarkably similar to recently observed high-redshift “little red dots.” This scenario can provide an explanation for rapid SMBH formation, growth, and mergers in high-redshift galaxies.

In Ukrainian

Brownian motors belong to the class of nanoscale devices that use the thermal noise of the environment as one of the necessary components in the mechanism of their operation. Today, there are a lot of practical implementations of such nanomachines, both inorganic, fairly simple mechanisms produced artificially, and more complex ones created from separate biological components available at the cellular level. One of the options for implementing the mechanism of straightening the chaotic thermal noise of the environment into unidirectional motion is the presence of a motor particle in the field of action of an asymmetric periodic stationary potential, which undergoes certain small disturbances (fluctuations) periodically over time. To describe such asymmetric one-dimensional structures (for example, dipole chains or fibers of the cytoskeleton) in the theory of Brownian motors, two model potentials are most often used: piecewise linear sawtooth and double sinusoidal. In this work, within the framework of the approximation of small fluctuations, a model of a pulsating Brownian motor with a stationary double sinusoidal potential and a disturbing small harmonic signal is considered. A new method of parametrization of such a problem is proposed, which allows to separate the contributions from various factors affecting the operation of the ratchet, and the numerical procedure for calculating the average speed of the directional movement of nanoparticles for the selected type of model potentials is specified. A number of numerical dependences of the average speed on the main parameters of the system were obtained. Peculiarities of the behavior of the motor as dependent on the parameter responsible for asymmetry and the number of potential wells on the spatial period of the stationary potential have been investigated. It is shown that the direction of the generated flux of nanoparticles depends not only on the phase shift between the stationary and fluctuating components of the potential, but also on the temperature of the system and the frequency of fluctuations, i.e., a possibility of temperature-frequency control of the direction of movement in the considered model has been found. Diagrams have been constructed that allow you to choose the ratio between the parameters of the nanomotor to create a flux of particles in the desired direction.

Nonvolatile Control of Valley Polarized Emission in 2D WSe2-AlScN Heterostructures.

Achieving robust and electrically controlled valley polarization in monolayer transition metal dichalcogenides (ML-TMDs) is a frontier challenge for realistic valleytronic applications. Theoretical investigations show that the integration of 2D materials with ferroelectrics is a promising strategy; however, an experimental demonstration has remained elusive. Here, we fabricate ferroelectric field-effect transistors using a ML-WSe2 channel and an Al0.68Sc0.32N (AlScN) ferroelectric dielectric and experimentally demonstrate efficient tuning as well as non-volatile control of valley polarization. We measure a large array of transistors and obtain a maximum valley polarization of ∼27% at 80 K with stable retention up to 5400 s. The enhancement in the valley polarization is ascribed to the efficient exciton-to-trion (X-T) conversion and its coupling with an out-of-plane electric field, viz., the quantum-confined Stark effect. This changes the valley depolarization pathway from strong exchange interactions to slow spin-flip intervalley scattering. Our research demonstrates a promising approach for achieving non-volatile control over valley polarization for practical valleytronic device applications.

Photoluminescence Quenching Upon Growth of Metal Nanoparticles: Quantum-Mechanical Views.

In dictating the optical processes in metal nanoparticles, for instance, quantum nature of free electrons is significantly dominant and plays very crucial roles at the level of nanoscale dimensions of materials. As consequences of the quantum-confinement effects on the conduction electrons, surface-plasmon resonance induced optical absorption and light emission properties of metal nanoparticles are found to be strongly dependent on physical dimensions of the nanomaterials. In addition, surface-confined acoustic vibration (phonon) modes have been experimentally observed to depend on the sizes of the metal nanoparticles. Also, interestingly, tuning of the surface-plasmon resonance condition is found to enhance the intensity of the acoustic Raman modes in metal nanoparticles. The study highlights the role of plasmon-phonon coupling in Co metal nanoparticles embedded in a silica-glass. In the research field of nanosciences and nanotechnologies, extraordinary behaviour and properties of nanoscale matters are investigated. In this context, interesting studies have been discussed in this review article to elaborate optical, chemical and photoluminescence properties of nanoscale Ag metal particles. Subtle detection of optical phenomena associated with the excited many-body electronic processes in the metal nanoparticles, for example, are very interesting but definitely challenging. Here we make an attempt to find out how the thermal growth of Ag metal nanoparticles in a glass matrix snuffs out the light emission from the samples? Quantum mechanical interpretations of the underlying processes about the quenching of photoluminescence phenomena with the growth of the metal nanoparticles will help to fine tune the optical properties of plasmonic systems as well as to harness potential applications of the nanomaterials.

Microstructural, Electrical, and Tribomechanical Properties of Mo-W-C Nanocomposite Films.

This study investigates the phase composition, microstructure, and their influence on the properties of Mo-W-C nanocomposite films deposited by dual-source magnetron sputtering. The synthesised films consist of metal carbide nanograins embedded in an amorphous carbon matrix. It has been found that nanograins are composed of the hexagonal β-(Mo2 + W2)C phase at a low carbon source power. An increase in the power results in the change in the structure of the carbide nanoparticles from a single-phase to a mixture of the β-(Mo2 + W2)C and NaCl-type α-(Mo + W)C(0.65≤k≤1) solid-solution phases. The analysis of electrical properties demonstrates that the nanograin structure of the films favours the occurrence of hopping conductivity. The double-phase structure leads to a twofold increase in the relaxation time compared to the single-phase one. Films with both types of nanograin structures exhibit tunnelling conductance without the need for thermal activation. The average distance between the potential wells produced by the carbide nanograins in nanocomposite films is approximately 3.4 ± 0.2 nm. A study of tribomechanical properties showed that Mo-W-C films composed of a mixture of the β-(Mo2 + W2)C and α-(Mo + W)C(0.65≤k≤1) phases have the highest hardness (19-22 GPa) and the lowest friction coefficient (0.15-0.24) and wear volume (0.00302-0.00381 mm2). Such a combination of electrical and tribomechanical properties demonstrates the suitability of Mo-W-C nanocomposite films for various micromechanical devices and power electronics.

Energy-Conserving Surface Hopping for Auger Processes.

Auger-type processes are ubiquitous in nanoscale materials because quantum confinement enhances Coulomb interactions, and there exist large densities of states. Modeling Auger processes requires the modification of nonadiabatic (NA) molecular dynamics algorithms to include transitions caused by both NA and Coulomb couplings. The system is split into quantum and classical subsystems, e.g., electrons and vibrations, and as a result, energy conservation becomes nontrivial. In surface hopping, an electronic transition induced by NA coupling is accompanied by a classical velocity readjustment to ensure conservation of the total quantum-classical energy. A different treatment is needed for Auger transitions driven by Coulomb interactions. We develop a nonadiabatic molecular dynamics methodology that meticulously differentiates the energy redistribution accompanying hops induced by the NA coupling and the Coulomb interaction and correctly conserves the total energy at each transition. If the transition is driven by a Coulomb interaction, the hop energy is redistributed within the quantum electronic subsystem only. If the transition is NA, the energy is redistributed between the quantum and classical subsystems. Properly maintaining energy conservation for both types of transitions is crucial to generate a correct order of events, obtain accurate transition times, maintain a proper statistical distribution of state populations, and reach thermodynamic equilibrium. We test the method with biexciton annihilation and Auger-assisted hot electron relaxation in a CdSe quantum dot. The sequence of Auger and phonon-driven processes and the calculated time scales are in excellent agreement with the experimental results. The developed approach can be coupled with any surface-hopping method and provides a crucial practical advance to study charge-carrier dynamics in the nanoscale and condensed matter systems.

Direct bandgap quantum wells in hexagonal Silicon Germanium

Silicon is indisputably the most advanced material for scalable electronics, but it is a poor choice as a light source for photonic applications, due to its indirect band gap. The recently developed hexagonal Si1−xGex semiconductor features a direct bandgap at least for x > 0.65, and the realization of quantum heterostructures would unlock new opportunities for advanced optoelectronic devices based on the SiGe system. Here, we demonstrate the synthesis and characterization of direct bandgap quantum wells realized in the hexagonal Si1−xGex system. Photoluminescence experiments on hex-Ge/Si0.2Ge0.8 quantum wells demonstrate quantum confinement in the hex-Ge segment with type-I band alignment, showing light emission up to room temperature. Moreover, the tuning range of the quantum well emission energy can be extended using hexagonal Si1−xGex/Si1−yGey quantum wells with additional Si in the well. These experimental findings are supported with ab initio bandstructure calculations. A direct bandgap with type-I band alignment is pivotal for the development of novel low-dimensional light emitting devices based on hexagonal Si1−xGex alloys, which have been out of reach for this material system until now.

Lateral Confinement in 2D Nanoplatelets: A Strategy to Expand the Colloidal Quantum Engineering Toolbox

AbstractAmong colloidal nanocrystals, 2D nanoplatelets offer a unique set of properties with exceptionally narrow luminescence and low lasing thresholds. Furthermore, their anisotropic shape expands the playground for the complex design of heterostructures where spectra but also scattering rates can be engineered. A challenge that still remains is to combine shell growth which makes NPLs stable, with spectral tunability. Indeed, most reported shelled nanoplatelets end up being red emitters due to a loss of quantum confinement. Here, the combination of both lateral and in‐plane confinements within a single heterostructure is explored. A CdS/CdSe/CdS/CdZnS core–crown–crown shell structure that enables yellow emission is grown and that is responsive to a large range of excitation including visible photons, X‐ray photons, electron beams, and electrical excitations. k.p simulations predict that emission tunability of up to several 100 s of meV can be obtained in ideal structures. This material also displays stimulated emission resulting from bi‐exciton emission with a low threshold. Once integrated into an LED stack, this material is compatible with sub‐bandgap excitation and exhibits high luminance. Scaling of the electroluminescence properties by downsizing the pixel size is also investigated.

Impact of quantum size effects to the band gap of catalytic materials: a computational perspective*

The evolution of nanotechnology has facilitated the development of catalytic materials with controllable composition and size, reaching the sub-nanometer limit. Nowadays, a viable strategy for tailoring and optimizing the catalytic activity involves controlling the size of the catalyst. This strategy is underpinned by the fact that the properties and reactivity of objects with dimensions on the order of nanometers can differ from those of the corresponding bulk material, due to the emergence of quantum size effects. Quantum size effects have a deep influence on the band gap of semiconducting catalytic materials. Computational studies are valuable for predicting and estimating the impact of quantum size effects. This perspective emphasizes the crucial role of modeling quantum size effects when simulating nanostructured catalytic materials. It provides a comprehensive overview of the fundamental principles governing the physics of quantum confinement in various experimentally observable nanostructures. Furthermore, this work may serve as a tutorial for modeling the electronic gap of simple nanostructures, highlighting that when working at the nanoscale, the finite dimensions of the material lead to an increase of the band gap because of the emergence of quantum confinement. This aspect is sometimes overlooked in computational chemistry studies focused on surfaces and nanostructures.

Intraband Cooling and Auger Recombination in Weakly to Strongly Quantum-Confined CsPbBr3 Perovskite Nanocrystals.

Semiconductor nanocrystals (NCs) with size-tuned energy gaps present unique and desirable properties for optoelectronic applications. Recent synthetic advancements offer routes to spheroidal CsPbBr3 perovskite NCs in the strong quantum confinement regime with narrow size dispersion. Using tunable femtosecond laser pulses, we examine intraband carrier relaxation using transient absorption spectroscopy and show that, across the transition from weak to strong confinement, hot carrier lifetime increases compared to larger bulk-like particles. However, further increases of confinement subsequently lead to a reduction of the hot carrier lifetime and increase of the non-radiative Auger recombination rate. Finally, we show that hot carrier lifetimes increase as a function of excess energy above the band gap less sensitively under high confinement in comparison to the bulk. Understanding such unique trends is important for maximizing hot carrier lifetimes for use in next-generation hot carrier devices as well as evaluating the transition from weak to strong confinement.

Lateral Quantum Confinement Effect on High-TC Superconducting FeSe Monolayer.

Despite decades of research in spatially confined superconducting systems to understand the modification of superconductivity from reduced length scales, the investigation of the quantum confinement effect on high-temperature superconductors remains an outstanding challenge. Here, we report scanning tunneling spectroscopy measurements on laterally confined FeSe monolayers on SrTiO3 substrates, which are formed by epitaxially growing FeSe films with a coverage less than one unit cell. Comparing to the uniform regions of FeSe monolayers, the peninsula regions at the monolayer boundary exhibit reduced Fermi energy and undiminished superconductivity, leading to a putative crossover from a Bardeen-Cooper-Schrieffer state to a Bose-Einstein condensate state. In isolated FeSe monolayer islands, superconductivity is shown to exist in samples of smaller volume in contrast to conventional superconductors, while the validity of Anderson's criterion remains fulfilled. Our work reveals lateral quantum confinement effects in unconventional superconductors to enrich the understanding of high-temperature superconductivity in low-dimensional systems.

Counterion docking: a general approach to reducing energetic disorder in doped polymeric semiconductors

Molecular doping plays an important role in controlling the carrier concentration of organic semiconductors. However, the introduction of dopant counterions often results in increased energetic disorder and traps due to the molecular packing disruption and Coulomb potential wells. To date, no general strategy has been proposed to reduce the counterion-induced structural and energetic disorder. Here, we demonstrate the critical role of non-covalent interactions (NCIs) between counterions and polymers. Employing a computer-aided approach, we identified the optimal counterions and discovered that NCIs determine their docking positions, which significantly affect the counterion-induced energetic disorder. With the optimal counterions, we successfully reduced the energetic disorder to levels even lower than that of the undoped polymer. As a result, we achieved a high n-doped electrical conductivity of over 200 S cm−1 and an eight-fold increase in the thermoelectric power factor. We found that the NCIs have substantial effects on doping efficiency, polymer backbone planarity, and Coulomb potential landscape. Our work not only provides a general strategy for identifying the most suitable counterions but also deepens our understanding of the counterion effects on doped polymeric semiconductors.

Unraveling the effects of non-parabolicity on electron energy levels in InP/InAs/InP heterostructures

In this research, electron energy levels were calculated analytically using Nelson’s formula, the shooting method, and Garrett’s formula for effective mass. These calculations were performed for a rectangular finite deep potential well, focusing on the InP/InAs/InP heterostructure, which is a narrow-bandgap semiconductor system. Our results demonstrate that the nonparabolicity of the dispersion has a more significant effect on higher energy levels compared to lower ones, with deviations of up to 15% for the third energy level. An equation estimating the number of observable energy levels in the potential well is suggested, revealing that considering nonparabolicity leads to a 20% increase in the number of levels compared to the parabolic dispersion case. The relationship between the widths of infinite and finite potential wells for equivalent energy levels follows a linear behaviour, with bonding coefficients ranging from 95,93% to 97,49% and a maximum difference of 1.5% between parabolic and non-parabolic cases. The transcendental equation for the energy levels is linearized, yielding a fourth-order equation that provides results within 98% accuracy compared to the original equation. These findings contribute to the understanding of the energy distribution in InP/InAs/InP heterostructures with a view to their application in optoelectronic devices such as lasers, light-emitting diodes