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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Pressure-Modulated Energy Transfer Dynamics in Mn 2+ -Doped CdS/ZnS Core/Shell Quantum Dots

Transition metal doping in semiconductor quantum dots (QDs) significantly impacts their optical properties, thus expanding the range of their potential optoelectronic applications. This study investigates the pressure-dependent energy transfer dynamics in Mn 2+ -doped CdS/ZnS core/shell QDs, focusing on how external hydrostatic pressure modulates these dynamics and optical properties. By synthesizing Mn 2+ -doped QDs with varying Mn 2+ doping concentrations, we explore the effects of the pressure on photoluminescence (PL) spectra and energy transfer efficiency. Our study reveals that increasing pressure induces a blueshift in the QD host bandgap PL and a redshift in the Mn 2+ dopant PL. The pressure-induced shifts highlight a unique modulation mechanism where the energy transfer efficiency decreases with pressure due to reduced wave function overlap between host excitons and Mn 2+ dopants. Detailed analysis of the PL quantum yields and energy transfer rate constants provides insights into these dynamics, suggesting that the pressure can effectively and reversibly regulate the energy transfer efficiencies and rates. In conclusion, these results have implications for developing pressure-sensitive configurable devices and exploring pressure-induced phenomena in doped nanomaterials.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ultrafast Symmetry Control in Photoexcited Quantum Dots

Symmetry control is essential for realizing unconventional properties, such as ferroelectricity, nonlinear optical responses, and complex topological order, thus it holds promise for the design of emerging quantum and photonic systems. Nevertheless, fast and reversible control of symmetry in materials remains a challenge, especially for nanoscale systems. Here, reversible symmetry changes are unveiled in colloidal lead chalcogenide quantum dots on picosecond timescales. Using a combination of ultrafast electron diffraction and total X-ray scattering, in conjunction with atomic-scale structural modeling and first-principles calculations, it is revealed that symmetry-broken lead sulfide quantum dots restore to a centrosymmetric phase upon photoexcitation. The symmetry restoration is driven by photoexcited electronic carriers, which suppress lead off-centering for about 100 ps. Furthermore, the change in symmetry is closely correlated with the electronic properties, and the bandgap transiently red-shifts in the symmetry-restored quantum dots. Overall, this study elucidates reversible symmetry changes in colloidal quantum dots, and more broadly defines a new methodology to optically control symmetry in nanoscale systems on ultrafast timescales.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Resonance plasmonic coupling: selective enhancement of band edge emission over trap state emission of CdSe quantum dots

The photoluminescence properties of quantum dots (QDs) are often enhanced by eliminating surface trap states through chemical methods. Alternatively, a physical approach is presented here for improving photoluminescence purity in QDs by employing frequency-specific plasmon resonance coupling. Emitter-bound plasmonic hybrids are designed by electrostatically binding negatively charged QDs in water to positively charged gold nanoparticles having a thin polymer coating. Herein, two types of QDs are used: (i) bare CdSe, which exhibits both band edge and trap state emission, and (ii) CdSe overcoated with a ZnS shell (CdSe/ZnS) devoid of trap state emission. Tuning the extinction spectrum of the plasmonic system to match the band edge emission of CdSe enables the selective enhancement of band edge emission over trap state emission. Excellent match in the extinction spectrum of the gold nanoparticle with both, experimentally calculated photoluminescence enhancement factor and theoretically calculated radiative rate enhancement signifies the role of frequency-specific plasmon resonance coupling. Plasmon-coupled photoluminescence of CdSe/ZnS is further investigated by varying the number density of emitter on the surface of plasmonic nanoparticle. An enhancement in the photoluminescence is observed at a lower emitter density of CdSe/ZnS and the photoluminescence enhancement factor closely follows the plasmon resonance. However, photoluminescence quenching occurs with an increase in CdSe/ZnS due to plasmon-assisted nonradiative energy transfer between nearby QDs, as indicated by a red shift in the PL maximum. These studies establish that resonance plasmonic coupling is a convenient physical strategy for tuning the intrinsic photoluminescence properties of QDs for various optoelectronic applications.

Paul, Livin↗
DOE OSTI2025

Unraveling Exciton Trap Dynamics and Nonradiative Loss Pathways in Quantum Dots via Atomistic Simulations

Surface defects in colloidal quantum dots are a major source of nonradiative losses, yet the microscopic mechanisms underlying exciton trapping and recombination remain elusive. Here, we develop a model Hamiltonian based on atomistic electronic calculations to investigate exciton dynamics in CdSe/CdS core/shell QDs containing a single hole trap introduced by an unpassivated sulfur atom. By systematically varying the defect depth and reorganization energy, we uncover how defect-induced excitonic states mediate energy relaxation pathways. Our simulations reveal that a single localized defect can induce a rich spectrum of excitonic states, leading to multiple dynamical regimes, from slow, energetically off-resonant trapping to fast, cascaded relaxation through in-gap defect states. Crucially, we quantify how defect-induced polaron shifts and exciton-phonon couplings govern the balance between efficient radiative emission and rapid nonradiative decay. These insights clarify the microscopic origin of defect-assisted loss channels and suggest pathways for tailoring QD optoelectronic properties via surface and defect engineering.

Defects↗
DOE OSTI2025

Interplay between Chiro-Optical and Spin Transport Properties in Chiral CdSe Quantum Dots

The chiral-induced spin selectivity (CISS) effect offers compelling approaches for manipulating spin-dependent processes in both chemistry and physics, yet the physical mechanism(s) underpinning CISS are still debated. Here we present a study of structure-property relationships in chiral quantum dot assemblies to identify attributes of CISS-based phenomena. Our results show that the circular dichroism (CD) strength of chiral CdSe quantum dots’ primary exciton transition correlates with two CISS properties, the propensity to transmit pure spin currents and to produce spin-polarized charge currents. While the spin-polarized charge current reverses its sign with a change in the polarity of the CD signal, the pure spin current transport does not. The trends in both transport types can be rationalized in terms of chirality-induced splitting of spin sub-bands, which are modulated by chiral symmetry breaking under charge transport through the CdSe quantum dots.

cadmium selenide↗
DOE OSTI2025

Expanding Parameter Space to Enable Low-Temperature Synthesis of Crystalline Indium Phosphide Quantum Dots

Established methods to synthesize indium phosphide quantum dots (QDs) require high temperatures (>180 °C) to make high-quality material for optoelectronic applications. Nonpolar solvent environments are overwhelmingly used in InP QD synthesis to reach the necessary high temperatures and for compatibility with the reactive precursors. In this study, we explored InP QD synthesis in polar aprotic solvent environments to dramatically decrease the temperature required for InP crystallization by imparting ionicity to the precursors and stabilizing charged reaction intermediates. A custom air-free 96- well plate setup was employed to identify key factors impacting low-temperature QD formation, including an increased percentage of polar solvent, carboxylic acid choice, and inclusion of polar additives. Guided by these insights, we developed a synthesis of crystalline, green-emitting InP QDs at 60 °C in a toluene-dimethylformamide mixture. Here's, the QDs withstood established Zn 2+ and HF surface treatments, which increased the photoluminescence quantum yield to 25%. Additionally, we demonstrated the rapid synthesis of quasi-wurtzite InP QDs at room temperature in a polar solvent environment using an acid-free indium myristate precursor.

absorption↗
DOE OSTI2025

Role of Superlattice Phonons in Charge Localization Across Quantum Dot Arrays

Understanding charge transport in semiconductor quantum dot (QD) assemblies is important for developing the next generation of solar cells and light-harvesting devices based on QD technology. One of the key factors that governs the transport in such systems is related to the hybridization between the QDs. Recent experiments have successfully synthesized QD molecules, arrays, and assemblies by directly fusing the QDs, with enhanced hybridization leading to high carrier mobilities and coherent band-like electronic transport. Here, in this work, we theoretically investigate the electron transfer dynamics across a finite CdSe-CdS core-shell QD array, considering up to seven interconnected QDs in one dimension. We find that, even in the absence of structural and size disorder, electron transfer can become localized by the emergent low-frequency superlattice vibrational modes when the connecting neck between QDs is narrow. On the other hand, we also identify a regime where the same vibrational modes facilitate coherent electron transport when the connecting necks are wide. Overall, we elucidate the crucial effects of electronic and superlattice symmetries and their couplings when designing high-mobility devices based on QD superlattices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Efficient Mn 2+ Doping in Non-Stoichiometric Cesium Lead Bromide Perovskite Quantum Dots

Doping magnetic transition metal ions (e.g., Mn 2+ ) into colloidal quantum dots endows novel optical and magnetic properties to the host materials. CsPbBr 3 quantum dots (QDs) are emerging light-emitting materials with high structural and chemical flexibility in the visible spectral regime. However, efficiently doping Mn 2+ ions in CsPbBr 3 QDs remains challenging, especially when size confinement and ensemble uniformity are needed for understanding the underexplored exciton-dopant exchange interaction. Here, we introduce a doping mechanism based on electrostatic surface Mn 2+ adsorption that enables efficient Mn 2+ incorporation in strongly confined CsPbBr 3 QDs. The resultant QDs are found to have a Cs-deficient stoichiometry compared to their undoped counterparts. A redox reaction-based purification method was developed to remove Mn 2+ cations that are tightly adsorbed on the surface to determine the concentration of lattice-incorporated Mn 2+ . Our synthesis enables a Mn 2+ doping/alloying concentration of up to ∼44% with a Mn 2+ photoluminescence efficiency exceeding 90%. This allows for the determination of the intrinsic exciton-to-dopant energy transfer rate.

Hidayatova, Lamia [Univ. of Oklahoma, Norman, OK (↗
DOE OSTI2026

Double Quantum Dots with Quenched Charging Energy in PbTe Nanowires

Here, we investigate double quantum dots defined by electrostatic gating in semiconductor PbTe nanowire devices. We perform transport measurements to obtain charge stability diagrams distinguished by negligible separation between paired triple points and by the spin degeneracy of all transport resonances at zero magnetic field. We show a 4-fold splitting of high-bias stability diagram triangles in an applied magnetic field to illustrate the lifting of this spin degeneracy. We also identify patterns of narrow transport resonances in these high-bias triangles and discuss their possible physical origins. Our results represent a step toward the realization of PbTe-based spin qubits.

PbTe nanowire↗
DOE OSTI2025

Geometry-driven modeling of electron localization in InAs/GaAs double quantum dots

The coupled electronic states in two-dimensional (2D) and three-dimensional (3D) double quantum dot (DQD) systems are investigated using a phenomenological model applied to InAs/GaAs heterostructures. The single-band k • p effective potential approach previously proposed by our group is employed to numerically calculate the energy spectrum and spatial localization of a single electron, serving as an indicator of the coupling strength within the binary system. For identical quantum dots (QDs) in a DQD, the electronic states exhibit ideal coherence. We systematically vary the DQD geometry and the strength of the confinement potential (via an applied electric field) to examine the effects of symmetry breaking and the sensitivity of electron localization in both identical and nearly identical DQDs. Our results show that coherence in DQDs is highly sensitive to these subtle variations. This sensitivity can be harnessed to detect changes in the surrounding environment, such as fluctuations in chemical or electrical properties that affect the DQD system.

electron localization↗
DOE OSTI2026

Photoinduced Charge Transfer and Vibronic Coherence in CdSe Quantum Dots with Methyl Viologen Acceptors

We show herein that photoinduced charge transfer from CdSe quantum dots (QDs) to surface-bound methyl viologen (MV 2+ ) acceptors is mediated by a vibronically coherent, nonadiabatic mechanism. Broadband multidimensional electronic spectra and an analysis of coherences show that a mixed QD–MV charge-transfer (CT) state is populated on the <50 fs time scale after optical preparation of the X3 (1P 3/2 –1P e ) state, well prior to the appearance of the one-electron photoreduced ground state (MV +• ). A partial redistribution of charge from the core of the QD to the acceptor is revealed by excited-state coherences of an out-of-plane vibrational mode local to MV 2+ and of a low-frequency mode mixing a MV 2+ mode with the longitudinal optical (LO) phonon of the QD core. The ultrafast damping of these coherences indicates that excited-state wavepackets travel from the optically prepared, Franck–Condon structure through a conical intersection to reach the CT state. These results suggest that vibronically coherent processes generating CT intermediates can be exploited to improve the efficiency of QD-based solar cells and photocatalysts.

Cadmium selenide↗
DOE OSTI2024

Photoluminescence Switching in Quantum Dots Connected with Carboxylic Acid and Thiocarboxylic Acid End-Group Diarylethene Molecules

We contrast the switching of photoluminescence (PL) of PbS quantum dots (QDs) cross-linked with photochromic diarylethene molecules with different end groups, 4,4′-(1-cyclopentene-1,2-diyl)bis[5-methyl-2-thiophenecarboxylic acid] ( 1C ) and 4,4′-(1-cyclopentene-1,2-diyl)bis[5-methyl-2-thiophenethiocarboxylic acid] ( 2T ). Our results show that the QDs cross-linked with the carboxylic acid end group molecules ( 1C ) exhibit a greater amount of switching in photoluminescence intensity compared to QDs cross-linked with the thiocarboxylic acid end group ( 2T ). We also demonstrate that regardless of the molecule used, greater switching amounts are observed for smaller quantum dots. Varying these parameters allows for the fabrication of photoswitches with tunable PL change. We relate these observations to the differences in the HOMO energy levels between the QDs and the photochromic molecules. Our findings demonstrate how the size of the QDs and the energy levels of the linker ligands influences the charge tunneling rate and thus the PL switching performance in tunneling-based photoswitches.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Ultrafast nonlinear absorption of Haldane model quantum dots

We study theoretically the nonlinear absorbance of Haldane model quantum dots (QDs) placed in the field of an ultrashort and strong optical pulse. The absorbance strongly depends on the frequency of the pulse. When the frequency of the pulse is much less than the QD bandgap, the absorbance shows strong dependence on the pulse amplitude and, as a function of an internal phase of the Haldane model, the absorbance has maxima at intermediate values of the phase. When the frequency of the pulse becomes closer to, but still less than, the bandgap, the absorbance has a weak dependence on the pulse amplitude and, as a function of the internal phase, it has a maximum at the phase of 900 when the QD bandgap also has the smallest value. Furthermore, nonlinear electron dynamics in such QD systems changes from almost reversible one at small pulse frequencies to highly irreversible dynamics at large frequencies of the pulse.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Dynamic Nanocrystal-Ligand Boundaries: Reversible Photoinduced Ligand Detachment from Quantum Dots in Solution

The porosity of ligand shells of colloidal quantum dots (QDs) can influence the overall rate and yield of charge transfer processes occurring at their surfaces. However, the density of ligand shells on QDs can also influence their colloidal and photochemical stability. We used time-resolved infrared spectroscopy to show that photoinduced ligand detachment, the tendency for certain ligands to detach from QD surfaces when the nanocrystals are promoted to their excitonic excited states, can be used to transiently enhance the porosity of oleic acidpassivated CdSe QDs in solution. Furthermore, we synthesized CdSe QDs with varying ligand shell densities to examine the corresponding influence that van der Waals interactions among ligands have on the yield of photoinduced ligand detachment and the time scale on which ligands return to QD surfaces. We observed that oleic acid ligands on CdSe QDs with lower shell densities have a higher probability of escape for longer periods of time. Despite this, oleic acid ligands on fully passivated CdSe QDs are still able to photodetach, resulting in a transient increase of their ligand shell porosity. In contrast, QDs with multilayer ligand coronas exhibit negligible photoinduced ligand detachment because the outer molecular layers introduce a type of cage effect, preventing the escape of the interior ligands. Our findings suggest the intriguing possibility that photoinduced ligand detachment can be used to transiently decrease the density of ligand shells of QDs to facilitate charge transfer processes while still allowing them to be fully passivated between excitation events for photochemical and colloidal stability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Interligand Coupling Drives Fast Triplet Energy Transfer Routes in PbS/Tetracene Quantum Dot Hybrids

The binding of photoactive organic ligands to inorganic quantum dots (QDs) creates a versatile hybrid architecture that allows access to photophysical processes such as efficient triplet exciton generation with near-infrared radiation. Here we report the subnanosecond generation of a hybrid triplet state with mixed ligand-QD character by replacing native oleate ligands on small PbS QDs with 5,12-tetracenepropiolic acid, a bifunctional ligand with two carboxylic acids that tends to lie face-on with the QD surface at low loadings. The face-on geometry engenders a regime of strong electronic coupling that is evident in steady-state absorption and hastens triplet energy flow by several orders of magnitude compared with more typical tetracene-based ligands exhibiting weak coupling. We further determined via Fourier transform infrared (FTIR) and supported by density functional theory (DFT)-based geometry optimizations that high ligand loading causes a shift in QD-ligand mutual disposition toward an edge-on geometry that instigates the formation of intermolecular excited states characterized by triplet excimer-like features in photoluminescence and transient absorption. Our results demonstrate the ability to control strongly coupled ligand-QD systems toward ultrafast generation of photophysically relevant species such as triplets that are valuable for photon upconversion and catalysis.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Modeling a Strain and Piezo Potentials in an InAs/GaAs Quantum Dot

We investigated the single-electron spectrum of an InAs/GaAs quantum dot (QD) using an effective potential model developed in previous studies. Our objective was to explore the limits of applicability of this model. We conducted numerical simulations, introducing a piezoelectric potential as a perturbation to the effective potential. The profile of this additional potential was derived from theoretical numerical studies presented in the literature. We analyzed the impact of variations in this profile within the framework of the perturbation theory. Our findings indicate that within a variation range of 25%, the effective potential model remains applicable.

42 ENGINEERING↗
DOE OSTI2025

Crystalline-symmetry-protected Majorana modes in coupled quantum dots

We propose a minimalist architecture for achieving various crystalline-symmetry-protected Majorana modes in an array of coupled quantum dots. Our framework is motivated by the recent experimental demonstrations of two-site and three-site artificial Kitaev chains in a similar setup. We find that introducing a π-phase domain wall in the Kitaev chain leads to a pair of mirror-protected Majorana zero modes located at or near the junction. Joining two π junctions into a closed loop, we can simulate two distinct classes of two-dimensional higher-order topological superconducting phases, both carrying symmetry-protected Majorana modes around the sample corners. As an extension of the π junction, we further consider a general vertex structure where n Kitaev chains meet, i.e., a Kitaev n vertex. We prove that such an n vertex, if respecting a dihedral symmetry group D n , necessarily carries n vertex-bound Majorana modes protected by the D n symmetry. Resilience of the junction and vertex Majorana bound states against disorder and correlation effects is also discussed. Our architecture paves the way for designing, constructing, and exploring a wide variety of artificial topological crystalline phases in quantum-dot experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Nonequilibrium steady-state thermoelectrics of Kondo-correlated quantum dots

The transport across a Kondo-correlated quantum dot coupled to two leads with independent temperatures and chemical potentials is studied using a controlled nonperturbative, and in this sense numerically exact, treatment based on a hybrid numerical renormalization group combined with time-dependent density matrix renormalization group (NRG-tDMRG). In the Kondo regime, for sufficiently large fixed voltage bias V ≳ T K , with T K the Kondo temperature, we find a peak in the conductance vs the temperature gradient Δ⁢T = T R - T L across left and right lead. Focusing then on zero voltage bias but finite ΔT far beyond linear response, we reveal the dependence of the characteristic zero-bias conductance on the individual lead temperatures. Here, we find that the finite-Δ⁢T data behaves quantitatively similar to linear response with an effective equilibrium temperature derived from the different lead temperatures. The regime of sign changes in the Seebeck coefficient, signaling the presence of Kondo correlations, and its dependence on the individual lead temperatures provide a complete picture of the Kondo regime in the presence of finite-temperature gradients. The results from the zero-bias conductance and Seebeck coefficient studies unveil an approximate “Kondo circle” in the T L /T R plane as the regime within which the Kondo correlations dominate. We also study the heat current and the corresponding heat conductance vs finite Δ⁢T. We provide a polynomial fit for our numerical results for the thermocurrent as a function of the individual lead temperatures, which may be used to fit experimental data in the Kondo regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗