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At least 73 records · Page 4

Observation of negative surface and interface energies of quantum dots

Surface energy is a fundamental property of materials and is particularly important in describing nanomaterials where atoms or molecules at the surface constitute a large fraction of the material. Traditionally, surface energy is considered to be a positive quantity, where atoms or molecules at the surface are less thermodynamically stable than their counterparts in the interior of the material because they have fewer bonds or interactions at the surface. Using calorimetric methods, we show that the surface energy is negative in some prototypical colloidal semiconductor nanocrystals, or quantum dots with organic ligand coatings. This implies that the surface atoms are more thermodynamically stable than those on the interior due to the strong bonds between these atoms and surfactant molecules, or ligands, that coat their surface. In addition, we extend this work to core/shell indium phosphide/zinc sulfide nanocrystals and show that the interfacial energy between these materials is highly thermodynamically favorable in spite of their large lattice mismatch. This work challenges many of the assumptions that have guided thinking about colloidal nanomaterial thermodynamics, investigates the fundamental stability of many technologically relevant colloidal nanomaterials, and paves the way for future experimental and theoretical work on nanocrystal thermodynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dephasing and error dynamics affecting a singlet-triplet qubit during coherent spin shuttling

Quantum information transport over micron to millimeter scale distances is critical for the operation of practical quantum processors based on spin qubits. One method of achieving a long-range interaction is by coherent electron spin shuttling through an array of silicon quantum dots. In order to execute many shuttling operations with high fidelity, it is essential to understand the dynamics of qubit dephasing and relaxation during the shuttling process in order to mitigate them. However, errors arising after many repeated shuttles are not yet well documented. Here, we probe decay dynamics contributing to dephasing and relaxation of a singlet-triplet qubit during coherent spin shuttling over many N repeated shuttle operations, in a small external magnetic field B 0 ≈ 0−10 mT, and in the absence of a micromagnet. We find that losses are dominated by magnetic dephasing, most visible for small N < 10 3 . However, incoherent spin-flip type shuttle errors become evident for large N > 10 3 . Additionally, we estimate shuttle error rates below 10 −4 out to at least N = 10 3 , representing an encouraging figure for future implementations of spin shuttling to entangle distant qubits.

quantum dots↗

Nonequilibrium dynamics of two-level systems directly after cryogenic alternating bias

Two-level systems (TLSs) are a dominant decoherence mechanism in superconducting qubits, microwave kinetic inductance detectors, and quantum dots. TLSs are tunneling states commonly found in amorphous materials and interfaces, which interact electromechanically, leading to energy loss. Fluctuations in the frequency of the TLSs are a significant problem for qubit operation and force recalibration every few hours. In this study, we probe the effect of alternating bias at cryogenic temperatures on TLSs in a purpose-built LC oscillator. When an in situ alternating bias is applied, the steady-state spectra of the TLSs disappear. Spectroscopy reveals transient behavior, in which the TLS frequency fluctuates on the order of minutes. Thermal cycling above 10 K reverses these effects, restoring the TLS spectrum to its original state. Importantly, the intrinsic loss tangent of the LC oscillator remains unchanged before and after the application of the alternating bias. We propose that the disappearance of the steady-state spectrum is caused by nonequilibrium energy buildup from strain in the oxide film introduced by the pulsed voltage-bias sequence. Understanding this nonequilibrium energy could shed light on TLS fluctuations and reduce the calibration requirements for qubits.

general physics↗

Induced Chirality in QDs Using Thermoresponsive Elastin-like Polypeptides

Circular dichroism (CD) spectroscopy has emerged as a potent tool for probing chiral small-molecule ligand exchange on natively achiral quantum dots (QDs). In this study, we report a novel approach to identifying QD–biomolecule interactions by inducing chirality in CdS QDs using thermoresponsive elastin-like polypeptides (ELPs) engineered with C-terminal cysteine residues. Our method is based on a versatile two-step ligand exchange process starting from monodisperse oleate-capped QDs in nonpolar media and proceeding through an easily accessed achiral glycine-capped QD intermediate. Successful conjugation of the ELPs onto the QDs is confirmed by the diagnostic CD response corresponding to the QD electronic transitions in the visible range. The resulting ELP:CdS conjugates demonstrate thermally reversible coacervation, as observed through dynamic light scattering, small-angle X-ray scattering, and electron microscopy. Furthermore, this research provides a foundation for using induced chirality in QD electronic transitions to probe QD conjugation to complex peptides and proteins, opening pathways for designing dynamic, stimuli-responsive hybrid nanomaterials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultrafast Dynamics of Plasmon-Coupled Excitons in Semiconducting Nanoplatelets

Exciton-plasmon coupling in nanomaterials produces many relevant phenomena for photonics applications including increased light-matter interactions, enhanced radiative rates of quantum emitters, and coherent energy exchange. In the case of exciton coupling to surface plasmon polaritons (SPPs), dispersive interactions controlled by the wavevector of optical excitation create the opportunity for tunable optical emission. Strong temporal impacts on exciton lifetimes can also occur in coupled systems, creating the opportunity for ultrafast control of exciton lifetime via changes in electronic coupling magnitude to a dispersive SPP. The coupling strength can be impacted by the morphology of the nanomaterials. Here, in this study, we utilize colloidal semiconductor nanoplatelets deposited onto thin silver plasmonic films, and compare the results to semiconductor quantum dots deposited on the silver films. We map the dispersion of the coupled systems and measure the ultrafast transient absorption response of the coupled systems. Due to the larger interaction areas of the nanoplatelets that lie flat on the silver films, a greater degree of coupling is found for the nanoplatelets, and much faster temporal responses are found as compared to quantum dots. Fresnel theory calculations that incorporate heavy and light hole features can reproduce the dispersion of the nanoplatelet-silver film, and a simple three-state model is developed to provide insights into the nature of the coupling at different photon energies along the dispersion curve.

colloidal semiconductor nanoplatelets↗

Introduction to special issue: Colloidal quantum dots

The quantum confinement effect has driven the development and exploration of colloidal semiconductor nanocrystals over approximately the past three decades. These semiconductor nanostructures are typically synthesized as stable colloidal dispersions in solution-phase chemical batch reactions at relatively low temperatures. Researchers have developed a wide range of reaction conditions to produce a variety of shapes, compositions, and structures with well-controlled sizes and low polydispersities. The shape can be controlled to produce confinement in one, two, or all three spatial dimensions, the latter defining a “quantum dot.” Combining two or more semiconductors within the various nanostructures produces additional optical and electronic degrees of freedom. These mixed compositional nanostructures have properties not accessible in bulk semiconductor systems. Further, researchers have fabricated novel nanoheterostructures, such as “dot-in-rods,” quantum wells, core/shell structures, giant-core/shell tetrapods where the core is one material and the arm is another, Janus structures that consist of spherical structures with well-defined internal heterostructures, nano-dumbbells, hollow-core structures, and many other novel and interesting structures. The structural variations are seemingly only limited by the creativity of the various researchers engaged in these endeavors.

36 MATERIALS SCIENCE↗

Si/SiGe QuBus for single electron information-processing devices with memory and micron-scale connectivity function

The connectivity within single carrier information-processing devices requires transport and storage of single charge quanta. Single electrons have been adiabatically transported while confined to a moving quantum dot in short, all-electrical Si/SiGe shuttle device, called quantum bus (QuBus). Here we show a QuBus spanning a length of 10 μm and operated by only six simply-tunable voltage pulses. We introduce a characterization method, called shuttle-tomography, to benchmark the potential imperfections and local shuttle-fidelity of the QuBus. The fidelity of the single-electron shuttle across the full device and back (a total distance of 19 μm) is (99.7 ± 0.3) %. Using the QuBus, we position and detect up to 34 electrons and initialize a register of 34 quantum dots with arbitrarily chosen patterns of zero and single-electrons. The simple operation signals, compatibility with industry fabrication and low spin-environment-interaction in 28 Si/SiGe, promises long-range spin-conserving transport of spin qubits for quantum connectivity in quantum computing architectures.

97 MATHEMATICS AND COMPUTING↗

Experimental realization of an extended Fermi-Hubbard model using a 2D lattice of dopant-based quantum dots

The Hubbard model is an essential tool for understanding many-body physics in condensed matter systems. Artificial lattices of dopants in silicon are a promising method for the analog quantum simulation of extended Fermi-Hubbard Hamiltonians in the strong interaction regime. However, complex atom-based device fabrication requirements have meant emulating a tunable two-dimensional Fermi-Hubbard Hamiltonian in silicon has not been achieved. Here, we fabricate 3 × 3 arrays of single/few-dopant quantum dots with finite disorder and demonstrate tuning of the electron ensemble using gates and probe the many-body states using quantum transport measurements. By controlling the lattice constants, we tune the hopping amplitude and long-range interactions and observe the finite-size analogue of a transition from metallic to Mott insulating behavior. We simulate thermally activated hopping and Hubbard band formation using increased temperatures. As atomically precise fabrication continues to improve, these results enable a new class of engineered artificial lattices to simulate interactive fermionic models.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Quantum Computation Using Optically Coupled Quantum Dot Arrays

A solid state model for quantum computation has potential advantages in terms of the ease of fabrication, characterization, and integration. The fundamental requirements for a quantum computer involve the realization of basic processing units (qubits), and a scheme for controlled switching and coupling among the qubits, which enables one to perform controlled operations on qubits. We propose a model for quantum computation based on optically coupled quantum dot arrays, which is computationally similar to the atomic model proposed by Cirac and Zoller. In this model, individual qubits are comprised of two coupled quantum dots, and an array of these basic units is placed in an optical cavity. Switching among the states of the individual units is done by controlled laser pulses via near field interaction using the NSOM technology. Controlled rotations involving two or more qubits are performed via common cavity mode photon. We have calculated critical times, including the spontaneous emission and switching times, and show that they are comparable to the best times projected for other proposed models of quantum computation. We have also shown the feasibility of accessing individual quantum dots using the NSOM technology by calculating the photon density at the tip, and estimating the power necessary to perform the basic controlled operations. We are currently in the process of estimating the decoherence times for this system; however, we have formulated initial arguments which seem to indicate that the decoherence times will be comparable, if not longer, than many other proposed models.

Pradhan, Prabhakar↗

Bit-Serial Adder Based on Quantum Dots

A proposed integrated circuit based on quantum-dot cellular automata (QCA) would function as a bit-serial adder. This circuit would serve as a prototype building block for demonstrating the feasibility of quantum-dots computing and for the further development of increasingly complex and increasingly capable quantum-dots computing circuits. QCA-based bit-serial adders would be especially useful in that they would enable the development of highly parallel and systolic processors for implementing fast Fourier, cosine, Hartley, and wavelet transforms. The proposed circuit would complement the QCA-based circuits described in "Implementing Permutation Matrices by Use of Quantum Dots" (NPO-20801), NASA Tech Briefs, Vol. 25, No. 10 (October 2001), page 42 and "Compact Interconnection Networks Based on Quantum Dots" (NPO-20855), which appears elsewhere in this issue. Those 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 QCA-based 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. To enable a meaningful description of the proposed bit-serial adder, it is necessary to further recapitulate the description of a quantum-dot cellular automation from the first-mentioned prior article: A quantum-dot cellular automaton contains four quantum dots positioned at the corners of a square cell. The cell contains two extra mobile electrons that can tunnel (in the quantum-mechanical sense) between neighboring dots within the cell. The Coulomb repulsion between the two electrons tends to make them occupy antipodal dots in the cell. For an isolated cell, there are two energetically equivalent arrangements (denoted polarization states) of the extra electrons. The cell polarization is used to encode binary information. Because the polarization of a nonisolated cell depends on Coulomb-repulsion interactions with neighboring cells, universal logic gates and binary wires could be constructed, in principle, by arraying QCA of suitable design in suitable patterns. Again, for reasons too complex to describe here, in order to ensure accuracy and timeliness of the output of a QCA array, it is necessary to resort to an adiabatic switching scheme in which the QCA array is divided into subarrays, each controlled by a different phase of a multiphase clock signal. In this scheme, each subarray is given time to perform its computation, then its state is frozen by raising its inter-dot potential barriers and its output is fed as the input to the successor subarray. The successor subarray is kept in an unpolarized state so it does not influence the calculation of preceding subarray. Such a clocking scheme is consistent with pipeline computation in the sense that each different subarray can perform a different part of an overall computation. In other words, QCA arrays are inherently suitable for pipeline and, moreover, systolic computations. This sequential or pipeline aspect of QCA would be utilized in the proposed bit-serial adders.

Fijany, Amir↗

Fabricating Single Crystal Quantum Dot Solids

The central goal of this research program was to establish fundamental synthesis and processing principles to enable the fabrication of single crystal quantum dot solids (QDS) with programmable structure (i.e., hexagonal and square) and composition. Our approach towards that goal leveraged access to and experience with unique in-situ, multi-probe characterization techniques to understand and ultimately control the fundamental relationship between processing conditions and nucleation and growth of QDS. The program integrated synthesis and fabrication (Hanrath) with in-situ TEM analysis (Kourkoutis) and computational modeling (Clancy) to gain atomic-level insights into the underlying physical phenomena governing assembly and attachment and to guide the development of optimized processing methods. We have established a foundational understanding of physicochemical interactions of self-assembly at a fluid interface, superlattice structure transformation pathways, the critical role of disorder during the initial dimerization of colloidal quantum dot monomers, and the residual strain distribution within the inter-dot epitaxial bridge which hampers the formation of novel electronics states of the quantum dot solids. Collectively, these insights have contributed towards advancing the mechanistic understanding of the complex choreography of assembly and attachment as well as understanding what currently limits further advances in high-fidelity quantum dot solids and tiles.

36 MATERIALS SCIENCE↗

Spin-related phenomena in spin 3/2 charge carrier holes systems

Charge carrier holes provide a remarkable system for spintronics and quantum information technology. In this review paper, I discuss spin-related phenomena in three-dimensional and low-dimensional hole systems. Special attention is paid to the mutual transformation of heavy and light holes at the boundary of quantum wells and wires that governs values of parameters defining hole spectra in quantum wells, wires and dots, such as effective masses, g-factors and Rashba and Dresselhaus spin–orbit constants. Recently, topological phenomena in condensed matter systems, such as emergence of Majorana zero modes and non-Abelian phases in the fractional quantum Hall effect, sparked considerable interest of researchers. Charge carrier holes turn out to be a remarkable setting for possible observation of these phenomena and advancing topological quantum computing. I discuss the spectra and wavefunctions of two-dimensional holes in magnetic field. While there is a semiclassical range of parameters when heavy and light holes can be described by equidistant Landau levels, ground-level holes and holes in a few low-lying excited states behave as species completely different from electrons. Especially interesting are crossings in hole spectra in magnetic field. Hole–hole interactions can substantially differ from electron–electron interactions. Apart from the difference in exchange splitting, this shows in possible emergence of even denominator fractional quantum Hall state in the ground hole level in magnetic field. I also briefly discuss spintronic phenomena, such as mutual transformation of angular momentum (spin) of holes and electric current, as well as spin-related interference effects in hole transport. Recent developments in a system of Ge hole quantum dots offer new perspectives for hole-based systems.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Colloidal Dispersions of Sterically and Electrostatically Stabilized PbS Quantum Dots: Structure Factors, Second Virial Coefficients, and Film-Forming Properties

Electrostatically stabilized nanocrystals (NCs) and, in particular, quantum dots (QDs) hold promise for forming strongly coupled superlattices due to their compact and electronically conductive surface ligands. However, studies of the colloidal dispersion and interparticle interactions of electrostatically stabilized sub-10 nm NCs have been limited, hindering the optimization of their colloidal stability and self-assembly. In this study, we employed small-angle X-ray scattering (SAXS) experiments to investigate the interparticle interactions and arrangement of PbS QDs with thiostannate ligands (PbS-Sn2S64-) in polar solvents. The study reveals significant deviations from the ideal solution behavior in electrostatically stabilized QD dispersions. Our results demonstrate that PbS-Sn2S64- QDs exhibit long-range interactions within the solvent, in contrast to the short-range steric repulsion characteristic of PbS QDs with oleate ligands (PbS-OA). Introducing highly charged multivalent electrolytes screens electrostatic interactions between charged QDs, reducing the length scale of the repulsive interactions. Furthermore, we calculated the second virial (B2) coefficients from SAXS data, providing insights into how surface chemistry, solvent, and size influence pair potentials. Finally, we explore the influence of long-range interparticle interactions of PbS-Sn2S64- QDs on the morphology of films produced by drying or spin-coating colloidal solutions. The long-range repulsive term of PbS-Sn2S64- QDs promotes the formation of amorphous films, and screening the electrostatic repulsion by the addition of an electrolyte enables the formation of crystalline domains. These findings highlight the critical role of NC-NC interactions in tailoring the properties of functional materials made of colloidal NCs.

SAXS↗

Controlled Organization of Inorganic Materials Using Biological Molecules for Activating Therapeutic Functionalities

Precise control over the assembly of biocompatible three-dimensional (3D) nanostructures would allow for programmed interactions within the cellular environment. Nucleic acids can be used as programmable crosslinkers to direct the assembly of quantum dots (QDs) and tuned to demonstrate different interparticle binding strategies. In this work, morphologies of self-assembled QDs are evaluated via gel electrophoresis, transmission electron microscopy, small-angle X-ray scattering, and dissipative particle dynamics simulations, with all results being in good agreement. The controlled assembly of 3D QD organizations is demonstrated in cells via the colocalized emission of multiple assembled QDs, and their immunorecognition is assessed via enzyme-linked immunosorbent assays. RNA interference inducers are also embedded into the interparticle binding strategy to be released in human cells only upon QD assembly, which is demonstrated by specific gene silencing. The programmability and intracellular activity of QD assemblies offer a strategy for nucleic acids to imbue the structure and therapeutic function into the formation of complex networks of nanostructures, while the photoluminescent properties of the material allow for optical tracking in cells in vitro.

36 MATERIALS SCIENCE↗

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 control of exciton wave functions in 2D semiconductors

Excitons—bound electron-hole pairs—play a central role in light-matter interaction phenomena and are crucial for wide-ranging applications from light harvesting and generation to quantum information processing. A long-standing challenge in solid-state optics has been to achieve precise and scalable control over excitonic motion. We present a technique using nanostructured gate electrodes to create tailored potential landscapes for excitons in 2D semiconductors, enabling in situ wave function shaping at the nanoscale. Our approach forms electrostatic traps for excitons in various geometries, such as quantum dots, rings, and arrays thereof. We show independent spectral tuning of spatially separated quantum dots, achieving degeneracy despite material disorder. Owing to the strong light-matter coupling of excitons in 2D semiconductors, we observe unambiguous signatures of confined exciton wave functions in optical reflection and photoluminescence measurements. This work unlocks possibilities for engineering exciton dynamics and interactions at the nanometer scale, with implications for optoelectronic devices, topological photonics, and quantum nonlinear optics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Quantum simulation of an exotic quantum critical point in a two-site charge Kondo circuit

Tuning a material to the cusp between two distinct ground states can produce physical properties that are unlike those in either of the neighbouring phases. Advances in the fabrication and control of quantum systems have raised the tantalizing prospect of artificial quantum simulators that can capture such behaviour. A tunable array of coupled qubits should have an appropriately rich phase diagram, but realizing such a system with either tunnel-coupled semiconductor quantum dots or metal nanostructures has proven difficult. The challenge for scaling up to clusters or lattices is to ensure that each element behaves essentially identically and that the coupling between elements is uniform, while also maintaining tunability of the interactions. Here we study a nanoelectronic circuit comprising two coupled hybrid metal–semiconductor islands, combining the strengths of both materials to form a potentially scalable platform. The semiconductor component allows for controllable inter-site couplings at quantum point contacts, while the metal component’s effective continuum of states means that different sites can be made equivalent by tuning local potentials. The couplings afforded by this architecture can realize an unusual quantum critical point resulting from frustrated Kondo interactions. In this study, the observed critical behaviour matches theoretical predictions, verifying the success of our experimental quantum simulation.

36 MATERIALS SCIENCE↗