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At least 649 records · Page 36

Hybrid VLSI/QCA Architecture for Computing FFTs

A data-processor architecture that would incorporate elements of both conventional very-large-scale integrated (VLSI) circuitry and quantum-dot cellular automata (QCA) has been proposed to enable the highly parallel and systolic computation of fast Fourier transforms (FFTs). The proposed circuit would complement the QCA-based circuits described in several prior NASA Tech Briefs articles, namely Implementing Permutation Matrices by Use of Quantum Dots (NPO-20801), Vol. 25, No. 10 (October 2001), page 42; Compact Interconnection Networks Based on Quantum Dots (NPO-20855) Vol. 27, No. 1 (January 2003), page 32; and Bit-Serial Adder Based on Quantum Dots (NPO-20869), Vol. 27, No. 1 (January 2003), page 35. The cited prior articles described the limitations of very-large-scale integrated (VLSI) circuitry and the major potential advantage afforded by QCA. To recapitulate: In a VLSI circuit, signal paths that are required not to interact with each other must not cross in the same plane. In contrast, for reasons too complex to describe in the limited space available for this article, suitably designed and operated QCAbased signal paths that are required not to interact with each other can nevertheless be allowed to cross each other in the same plane without adverse effect. In principle, this characteristic could be exploited to design compact, coplanar, simple (relative to VLSI) QCA-based networks to implement complex, advanced interconnection schemes.

Fijany, Amir↗

Reductive pathways in molten inorganic salts enable colloidal synthesis of III-V semiconductor nanocrystals

Colloidal quantum dots, with their size-tunable optoelectronic properties and scalable synthesis, enable applications in which inexpensive high-performance semiconductors are needed. Synthesis science breakthroughs have been key to the realization of quantum dot technologies, but important group III-group V semiconductors, including colloidal gallium arsenide (GaAs), still cannot be synthesized with existing approaches. The high-temperature molten salt colloidal synthesis introduced in this work enables the preparation of previously intractable colloidal materials. We directly nucleated and grew colloidal quantum dots in molten inorganic salts by harnessing molten salt redox chemistry and using surfactant additives for nanocrystal shape control. Synthesis temperatures above 425°C are critical for realizing photoluminescent GaAs quantum dots, which emphasizes the importance of high temperatures enabled by molten salt solvents. We generalize the methodology and demonstrate nearly a dozen III-V solid-solution nanocrystal compositions that have not been previously reported.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effects of proton irradiation on luminescence and carrier dynamics of self-assembled III-V quatum dots

The effects of proton irradiation (1.5 MeV) on photoluminescence intensities and carrier dynamics were compared between III-V quantum dots and similar quantum well structures. A significant enhancement in radiation tolerance is seen with three-dimensional quantum confinement. Measurements were carried out in different quantum dot (QD) structures, varying in material (InGaAs/GaAs and InAlAs/AlGaAs), QD surface density (4x10^8 to 3x10'^10 cm^-2), and substrate orientation [(100) and (311) B]. Similar trends were observed for all QD samples. A slight increase in PL emission after low to intermediate proton doses, are also observed in InGaAs/GaAs (100) QD structures. The latter is explained in terms of more efficient carrier transfer from the wetting layer via radiation-induced defects.

nanotechnology DLTS optical properties pn diodes q↗

Physics of Quantum Structures in Photovoltaic Devices

There has been considerable activity recently regarding the possibilities of using various nanostructures and nanomaterials to improve photovoltaic conversion of solar energy. Recent theoretical results indicate that dramatic improvements in device efficiency may be attainable through the use of three-dimensional arrays of zero-dimensional conductors (i.e., quantum dots) in an ordinary p-i-n solar cell structure. Quantum dots and other nanostructured materials may also prove to have some benefits in terms of temperature coefficients and radiation degradation associated with space solar cells. Two-dimensional semiconductor superlattices have already demonstrated some advantages in this regard. It has also recently been demonstrated that semiconducting quantum dots can also be used to improve conversion efficiencies in polymeric thin film solar cells. Improvement in thin film cells utilizing conjugated polymers has also be achieved through the use of one-dimensional quantum structures such as carbon nanotubes. It is believed that carbon nanotubes may contribute to both the disassociation as well as the carrier transport in the conjugated polymers used in certain thin film photovoltaic cells. In this paper we will review the underlying physics governing some of the new photovoltaic nanostructures being pursued, as well as the the current methods being employed to produce III-V, II-VI, and even chalcopyrite-based nanomaterials and nanostructures for solar cells.

Raffaelle, Ryne P.↗

Nanorod length-dependent photodriven H2 production in 1D CdS–Pt heterostructures

Colloidal quantum confined semiconductor-metal heterostructures are promising candidates for solar energy conversion because their light absorbing semiconductor and catalytic components can be independently tuned and optimized. Although the light-to-hydrogen efficiencies of such systems have shown interesting dependences on the morphologies of the semiconductor and metal domains, the mechanisms of such dependences are poorly understood. Here, we use Pt tipped 0D CdS quantum dots (with ∼4.6 nm diameter) and 1D CdS nanorods (of ∼13.8, 27.8, 66.6, and 88.9 nm average rod lengths) as a model system to study the distance-dependence of charge separation and charge recombination times and their impacts on photo-driven H2 production. The H2 generation quantum efficiency increases from 0.2% ± 0.0% in quantum dots to 28.9% ± 0.4% at a rod length of 28 nm and shows negligible changes at longer rod lengths. The half-life time of electron transfer from CdS to Pt increases monotonically with rod length, from 0.7 ± 0.1 in quantum dots to 170.2 ± 29.5 ps in the longest rods, corresponding to a slight decrease in electron transfer quantum efficiency from 92% to 81%. The amplitude-weighted average lifetime of charge recombination of the electron in Pt with the hole in CdS increases from 4.7 ± 0.4 µs in quantum dots to 149 ± 34 µs in 28 nm nanorods, and the lifetime does not increase further in longer rods, resembling the trend in the observed H2 generation quantum efficiency. Our result suggests that the competition of the charge recombination process with the hole removal by the sacrificial electron donor plays a dominant role in the observed nanorod length dependent overall light driven H2 generation quantum efficiency.

Chemistry↗

Autonomous quantum absorption refrigerators

Here, we propose a quantum absorption refrigerator using the quantum physics of resonant tunneling through quantum dots. The cold and hot reservoirs are fermionic leads, tunnel coupled via quantum dots to a central fermionic cavity, and we propose configurations in which the heat absorbed from the (very hot) central cavity is used as a resource to selectively transfer heat from the cold reservoir on the left to the hot reservoir on the right. Heat transport in the device is particle-hole symmetric; we find two regimes of cooling as a function of the dot energies—symmetric with respect to the Fermi energy of the reservoirs—and we associate them with heat transfer by electrons above the Fermi level and holes below the Fermi level. We also discuss optimizing the cooling effect by fine-tuning the energy of the dots as well as their linewidth and characterize regimes where the transport is thermodynamically reversible such that the Carnot coefficient of performance is achieved with zero cooling power delivered.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Adversarial autoencoder ensemble for fast and probabilistic reconstructions of few-shot photon correlation functions for solid-state quantum emitters

Second-order photon correlation measurements [g (2) (τ) functions] are widely used to classify single-photon emission purity in quantum emitters or to measure the multiexciton quantum yield of emitters that can simultaneously host multiple excitations – such as quantum dots – by evaluating the value of g (2) (τ = 0). Accumulating enough photons to accurately calculate this value is time consuming and could be accelerated by fitting of few-shot photon correlations. Here, we develop an uncertainty-aware, deep adversarial autoencoder ensemble (AAE) that reconstructs noise-free g (2) (τ) functions from noise-dominated, few-shot inputs. The model is trained with simulated g (2) (τ) functions that are facilely generated by Poisson sampling time bins. The AAE reconstructions are performed orders-of-magnitude faster, with reconstruction errors and estimates of g (2) (τ = 0) that are lower in variance and similar in accuracy compared to Maximum likelihood estimation and Levenberg-Marquardt least-squares fitting approaches, for simulated and experimentally measured few-shot g (2) (τ) functions (~100 two-photon events) of InP/ZnS/ZnSe and CdS/CdSe/CdS quantum dots. The deep-ensemble model comprises eight individual autoencoders, allowing for probabilistic reconstructions of noise-free g (2) (τ) functions, and we show that the predicted variance scales inversely with number of shots, with comparable uncertainties to computationally intensive Markov chain Monte Carlo sampling. Furthermore, this work demonstrates the advantage of machine learning models to perform uncertainty-aware, fast, and accurate reconstructions of simple Poisson-distributed photon correlation functions, allowing for on-the-fly reconstructions and accelerated materials characterization of solid-state quantum emitters.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Materials for Ultra‐Coherent, Mobile, Electron‐Spin Qubits

This research project has had the goal of gaining a better understanding of the physics of electrons bound to the surface of superfluid helium from both experimental and theoretical perspectives. It has particularly been aimed at two areas which had not been well studied: the relaxation and decoherence of the spin of the electrons on the helium surface and how the properties of underlying metallic layers affect the behavior of the electrons when the helium covering the metal is thin. This work is motivated in part by interest in using the spin of these electrons as a quantum bit, or qubit. Low levels of decoherence are advantageous for qubits, and moving the electrons, as one might do in a quantum processor, will be easiest if thin helium films can be employed. It had been suggested that spin decoherence should be very weak for electrons bound to superfluid He, but before this work there have been no quantitative studies of spin relaxation and decoherence. It is especially important to know how moving the electrons across the helium surface would affect their spin coherence. Calculations performed as part of this project show that the Rashba effective magnetic field, the mechanism which limits the spin coherence of mobile electrons in silicon-based devices (an actively pursued qubit technology), is exceptionally weak for electrons bound to helium. This project has identified other decoherence mechanisms which are stronger, but still weak compared to analogous silicon-based structures. Calculated spin coherence times for mobile electrons approach one day, as compared to microseconds in silicon. With coherence times of this magnitude, the spin qubit errors on helium will be completely dominated by errors in the quantum gates. In related work, the possibility of using an artificial spin-orbit interaction (a gradient magnetic field) for quantum operations on the electrons spins was considered. The calculations show that a moderate gradient field, small enough to be generated by a narrow superconducting wire, will enable high-fidelity quantum operations on electrons held in lithographically-defined quantum dots by driving them with a microwave electric field. The spin and motional coherence of the electrons is sufficient to allow high-fidelity 2-qubit quantum operations between electrons in neighboring quantum dots. As an outgrowth of experiments aiming to measure electron spin coherence it was discovered that very high densities of electrons can be stably supported on thin helium films coating ultra-smooth amorphous metallic layers. The measured densities are high enough that the electron system has almost certainly transitioned from an ordered array of electrons, known as a Wigner crystal (ordered by the electrons’ mutual repulsion), to a quantum fluid known as a Fermi liquid. This transition has been a subject of intense interest for over 40 years, since the electron Wigner crystal was first observed with electrons bound to superfluid helium, but it has never been unambiguously observed. Experiments are still underway in these new structures to definitively determine whether true quantum melting of the Wigner crystal has been demonstrated. This work has also catalyzed the development of a new approach for measuring the transport of electrons across very thin helium films, as will be needed for some of the quantum computing applications. The high electron density experiments as well as experiments with electrons bound in quantum dots have led to new techniques which may enable spin coherence measurements.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Characterization of quantum dot-like emitters in programmable arrays of nanowrinkles of 1L-WSe2

When combined with nanostructured substrates, two-dimensional semiconductors can be engineered with strain to tailor light–matter interactions on the nanoscale. Recently, room-temperature nanoscale exciton localization with controllable wrinkling in 1L-WSe2 was achieved using arrays of gold nanocones. Here, the characterization of quantum dot-like states and single-photon emitters in the 1L-WSe2/nanocone system is reported. The nanocones induce a wide range of strains, and as a result, a diverse ensemble of narrowband, potential single-photon emitters is observed. The distribution of emitter energies reveals that most reside in two spectrally isolated bands, leaving a less populated intermediate band that is spectrally isolated from the ensembles. The spectral isolation is advantageous for high-purity quantum light emitters, and anti-bunched emission from one of these states is confirmed up to 25 K. Although the spatial distribution of strain is expected to influence the orientation of the transition dipoles of the emitters, multimodal emission polarization anisotropy and atomic force microscopy reveal that the macroscopic orientation of the wrinkles is not a good predictor of dipole orientation. Finally, the emission is found to change with thermal cycling from 4 to 290 K and back to 4 K, highlighting the need to control factors such as temperature-induced strain to enhance the robustness of this quantum emitter platform. The initial characterization here shows that controlled nanowrinkles of 1L-WSe2 generate quantum light in addition to uncovering potential challenges that need to be addressed for their adoption into quantum photonic technologies.

Physics↗

Imaging Electrons in Two Dimensional Materials (Final report)

Two-dimensional (2D) materials have extraordinary characteristics that offer promising new approaches for science and technology. Electrons in graphene can move ballistically through a sheet, even though it is only a single atom thick. And transition metal dichalcogenide materials can be cleaved into 2D flakes of all types – metals, semiconductors, insulators, magnetic materials, and superconductors. To benefit from these discoveries, the science needs to be understood to transform 2D materials into useful new devices and systems. The evolution in time of atomic scale graphene structures has been studied in time with a transmission electron microscope (TEM), and ballistic transport of electrons in graphene was been imaged using a cooled scanning probe microscope (SPM), as well as electron motion in MoS 2 . Graphene is only one atom thick but is extremely strong, creating the opportunity to fabricate atomic scale structures in the lateral direction. Using an atomic resolution TEM, a suspended sheet of graphene can be shaped by a Si impurity atom on its surface that acts like a chisel to open up apertures, one atom at a time. The electrons in the TEM provide both the chiseling energy and the ability to image the results. Electrons and holes in graphene form a new type of electronic system with conical conduction and valence bands that meet at the Dirac point, with no energy gap. For moderate densities, the carriers form a Fermi liquid with ballistic transport over micron-scale distances. Using a cooled SPM the cyclotron orbit of electrons in graphene has been imaged. In the magnetic focusing regime, electrons leaving a point contact circle around and leave from a second point contact when the cyclotron diameter is equal to the contact spacing. The paths of electrons are focused - they enter at different angles but converge again at the exiting contact. When the SPM tip knocks an electron out of its orbit, an imaging signal is created. The ballistic motion of carriers in graphene opens the way for ballistic devices that manipulate beams of electrons and holes. Our collaborator Gil-Ho Lee, in Philip Kim's group, created a collimating contact by placing zig-zag absorbers on either side of entering electrons. Our cooled SPM was used to image the electron beam and determine its 9-degree halfwidth. By changing the gate voltage, a collimated beam of holes was also created, opening the way for colliding beam experiments. Coherent beams of carriers are desirable for quantum information processing. Via Andreev reflection, superconducting contacts can covert Cooper pairs in a superconductor to an ingoing and outgoing electrons and holes. Using our cooled SPM, Andreev reflection was imaged from a superconducting contact on a graphene device. Magnetic focusing was used to create an incoming beam of electrons and an outgoing beam of holes, detected by a third point contact. The images show a clear transition from normal reflection above the superconducting transition temperature to Andreev reflection as the device is cooled. Transition metal dichalcogenides offer a wide array of materials that can be exfoliated into ultrathin 2D sheets. A cooled SPM can be used to detect quantum dots as well as to image electron flow. The tip charge capacitively couples to electrons on the dot, acting as a gate to tune the dot conductance. Coulomb blockade peaks appear as a bullseye pattern in an SPM image as the tip is raster scanned above the dot. This approach was used to detect quantum dots in a MoS 2 channel as the carrier density was reduced and electrons pooled in low energy points. Through our DOE supported research, cooled SPM imaging has proven to be a very useful tool to uncover the motion of electrons and holes in the new quantum materials graphene and MoS 2 .

36 MATERIALS SCIENCE↗

Solid State Quantum Refrigeration Superconducting, Absorption and Measurement Based (Final Technical Report)

During this DOE grant, DE-SC0017890, in place for the past six years, all proposed research was carried out and published in peer-reviewed papers, as well as other projects that emerged during the research. In that effort the research team accomplished all proposed research, as well as many closely related research projects discovered and conceived of during the grant. These works included “Efficient Quantum Measurement Engines”, a work published in Physical Review Letters, giving a theory of quantum measurement-based engines, which uses quantum measurement as a resource. These engines are designed to efficiently convert energy from the stochastic quantum measurement process into useful work. Further publications include “Experimental Realization of a Quantum Dot Energy Harvester”, a joint theory and experimental work in collaboration with the group of Charles Smith in Cambridge, UK, as well as long time theoretical collaborators, Rafael Sánchez and Björn Sothmann. This work, featured as an Editor’s Suggestion in Physical Review Letters, realized an earlier theoretical proposal of ours, whereby two resonant tunneling quantum dots are connected to a central electronic cavity that is heated by a hot energy source. We also published “Superconducting Quantum Refrigerator: Breaking and Rejoining Cooper Pairs with Magnetic Field Cycles” a work done in collaboration with experimentalist Francesco Giazotto from ENS Pisa, Italy, which also resulted in a patent. This paper, published in Phys. Rev. Applied, advanced the concept of a cyclic fridge based on the normal/superconducting phase transition together with layered materials separated by tunnel junctions. We also completed the proposed research on a heat transistor, publishing “Thermal transistor and thermometer based on Coulomb-coupled conductors”, carried out as a collaboration between my group and theorists Splettstoesser (Lund U., Sweden), Sothmann (U. Duisburg-Essen, Germany), and Sánchez (U. Autónoma de Madrid, Spain). We carried out an analysis of a quantum coupled to a quantum point contact as a sensitive thermometer and heat transistor. We found the optimal statistical estimator for the temperature and compared it with experiments on the same type of devices. We also investigated autonomous quantum absorption refrigerators using quantum dots to cool by using a very hot thermal reservoir to drive heat between two other reservoirs. In the article “Quantifying the quantum heat contribution from a driven superconducting circuit”, we demonstrated that for a driven superconducting circuit, we showed heat flow provided by a hot source to the qubit can be switched on and off by varying external parameters, the frequency and the intensity of the driving. In the work “Stochastic thermodynamic cycles of a mesoscopic thermoelectric engine”, we reconsidered the autonomous thermoelectric heat engine in terms of underlying cycles. Rather than periodic behavior, the cycles were stochastic in nature. Nevertheless, by undertaking a graph theoretical analysis of the elementary transport processed, great quantitative and qualitative insight could be found. We also considered the quantum measurement process and showed that a quantum version of Maxwell’s demon could be related to the work extraction of a quantum system, closely related to arrow-of-time measures for quantum measurement, as described in our article “Thermodynamics of quantum measurement and Maxwell's demon's arrow of time”. This work was selected in Phys. Rev. A as an Editor’s Suggestion. A recent preprint titled “Cyclic Superconducting Quantum Refrigerators Using Guided Fluxon Propagation” accomplished an important piece of this grant: to propose a new kind of quantum refrigerator using the dynamics of fluxons in a type II superconductor. This invention envisioned a race-track type geometry where fluxons are confined. By applying a gradient of magnetic field together with electric current in a Corbino geometry, the circulating fluxons can actively cool a cold reservoir, realizing a new type of cyclic superconducting refrigerator. We also investigated the possibility of thermal control from different points of view. The application of quantum measurement to the system gives a new kind of control on the system of interest – we have pioneered this approach and shown that measurement can boost the thermal power of quantum engines as described in “Continuous measurement boosted adiabatic quantum thermal machines”. The ability to have heat flows on demand is an outstanding challenge, and we have provided new solutions to this problem in Thermal control across a chain of electronic nanocavities” for a chain of electron cavities using gating voltage control. The control methods using qubit/qubit coupling to create absorption fridges at their most fundamental level have also been developed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Confinement of excited states in two-dimensional, in-plane, quantum heterostructures

Two-dimensional (2D) semiconductors are promising candidates for optoelectronic application and quantum information processes due to their inherent out-of-plane 2D confinement. In addition, they offer the possibility of achieving low-dimensional in-plane exciton confinement, similar to zero-dimensional quantum dots, with intriguing optical and electronic properties via strain or composition engineering. However, realizing such laterally confined 2D monolayers and systematically controlling size-dependent optical properties remain significant challenges. Here, we report the observation of lateral confinement of excitons in epitaxially grown in-plane MoSe 2 quantum dots (~15-60 nm wide) inside a continuous matrix of WSe 2 monolayer film via a sequential epitaxial growth process. Various optical spectroscopy techniques reveal the size-dependent exciton confinement in the MoSe 2 monolayer quantum dots with exciton blue shift (12-40 meV) at a low temperature as compared to continuous monolayer MoSe 2 . Finally, single-photon emission (g 2 (0) ~ 0.4) was also observed from the smallest dots at 1.6 K. Our study opens the door to compositionally engineered, tunable, in-plane quantum light sources in 2D semiconductors.

42 ENGINEERING↗

Live-Cell Quantum Dot-Based Tracking of Plant & Microbial Extracellular Vesicles

All cellular organisms examined to date release various types of small vesicles called extracellular vesicles (EVs). They were originally thought to be unimportant, but research into EVs as carriers of key messages for communication within large, multicellular organisms or between interacting organisms has gained interest in many different scientific areas of study. Recently, it was discovered that both plants and their pathogenic fungi generate EVs and they are important vehicles for sending plant signals to thwart invasion by fungal pathogens, and in response, fungi use EVs to help evade plant defenses. This project aimed to develop new ways to visualize EVs and their potential nucleic acid cargo isolated from the crop plant, sorghum. We adapted a click chemistry-based method for making quantum dot-based RNA sensors, which will be a useful tool for others studying small RNAs. These sensors were not used detect RNA in sorghum EVs because unlike EVs from Arabidopsis, sorghum EVs were not enriched for specific small RNAs. This interesting difference shifted the project in an exciting direction, which focused on comparing EV proteomes. Our study discovered that greater than 60% of Arabidopsis EV proteins were also found in the sorghum EV proteome, revealing a partial conservation between a eudicot and monocot plant. These studies have raised new, fundamental questions on the conserved function of EVs in plants.

59 BASIC BIOLOGICAL SCIENCES↗

Quantum Monte Carlo Method in the Steady State

We present a numerically exact steady-state inchworm Monte Carlo method for nonequilibrium quantum impurity models. Rather than propagating an initial state to long times, the method is directly formulated in the steady state. This eliminates any need to traverse the transient dynamics and grants access to a much larger range of parameter regimes at vastly reduced computational costs. We benchmark the method on equilibrium Green’s functions of quantum dots in the noninteracting limit and in the unitary limit of the Kondo regime. We then consider correlated materials described with dynamical mean field theory and driven away from equilibrium by a bias voltage. We show that the response of a correlated material to a bias voltage differs qualitatively from the splitting of the Kondo resonance observed in bias-driven quantum dots.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ordered nanoparticle arrays formed on engineered chaperonin protein templates

Traditional methods for fabricating nanoscale arrays are usually based on lithographic techniques. Alternative new approaches rely on the use of nanoscale templates made of synthetic or biological materials. Some proteins, for example, have been used to form ordered two-dimensional arrays. Here, we fabricated nanoscale ordered arrays of metal and semiconductor quantum dots by binding preformed nanoparticles onto crystalline protein templates made from genetically engineered hollow double-ring structures called chaperonins. Using structural information as a guide, a thermostable recombinant chaperonin subunit was modified to assemble into chaperonins with either 3 nm or 9 nm apical pores surrounded by chemically reactive thiols. These engineered chaperonins were crystallized into two-dimensional templates up to 20 microm in diameter. The periodic solvent-exposed thiols within these crystalline templates were used to size-selectively bind and organize either gold (1.4, 5 or 10nm) or CdSe-ZnS semiconductor (4.5 nm) quantum dots into arrays. The order within the arrays was defined by the lattice of the underlying protein crystal. By combining the self-assembling properties of chaperonins with mutations guided by structural modelling, we demonstrate that quantum dots can be manipulated using modified chaperonins and organized into arrays for use in next-generation electronic and photonic devices.

Chaperonins/chemistry/ultrastructure↗