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At least 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Charge transfer as a mechanism for chlorophyll fluorescence concentration quenching

Highly concentrated solutions of chlorophyll display rapid fluorescence quenching. The same devastating energy loss is not seen in photosynthetic light-harvesting antenna complexes, despite the need for chromophores to be in close proximity to facilitate energy transfer. A promising, though unconfirmed mechanism for the observed quenching is energy transfer from an excited chlorophyll monomer to a closely associated chlorophyll pair that subsequently undergoes rapid nonradiative decay to the ground state via a short-lived intermediate charge-transfer state. In this work, we make use of newly emerging fast methods in quantum chemistry to assess the feasibility of this proposed mechanism. We calculate rate constants for the initial charge separation, based on Marcus free-energy surfaces extracted from molecular dynamics simulations of solvated chlorophyll pairs, demonstrating that this pathway will compete with fluorescence (i.e., drive quenching) at experimentally measured quenching concentrations. We show that the rate of charge separation is highly sensitive to interchlorophyll distance and the relative orientations of chromophores within a quenching pair. We discuss possible solvent effects on the rate of charge separation (and consequently the degree of quenching), using the light-harvesting complex II (LH2) protein from rps. acidophila as a specific example of how this process might be controlled in a protein environment. Crucially, we reveal that the LH2 antenna protein prevents quenching, even at the high chlorophyll concentrations required for efficient energy transfer, by restricting the range of orientations that neighboring chlorophyll pairs can adopt.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Comprehensive Study of the Potential of Extracting and Processing Critical Minerals from Coal-Based Resources - Phase I

The Phase I report prepared for the Department of Energy addresses U.S. Executive Order 13817 titled A Federal Strategy to Ensure Secure and Reliable Supplies of Critical Minerals, issued on December 20, 2017, that lists 35 critical minerals that are vulnerable to supply disruption. A comprehensive review of each of the minerals was conducted to determine the criticality based primarily on extractability from coal-based resources. Several other factors were also considered such as gaps in supply and demand, use in current technology, and the existence of viable substitutes. It was determined that the critical minerals that show highest potential for extraction from coal-based resources are lithium, rare earth elements (REEs), cobalt, and manganese. All four of the critical minerals listed serve an important role in the technology industry, have few substitutes, and have a heavy import reliance. Most notably are lithium, which is widely used in the electric vehicle industry, and the REEs which can be found in virtually all electronic devices. The research of critical mineral extraction from coal-based resources was completed using a combination of literature review from public sources as well as cooperation from coal mines and power plants across the United States. Samples collected from six different geographical locations across the U.S. were subjected to sample preparation (i.e., pH measurement, moisture content, particle size analysis) and characterization studies using Inductively Coupled Plasma-Mass Spectroscopy (ICP-MS) and Scanning Electron Microscopy, Energy Dispersive X-Ray Spectroscopy (SEM-EDX) instruments. 27 samples of coal waste materials such as refuse, sludge, and fly ash were tested to characterize the rare earth element concentration by total rare earth elements (TREEs), heavy rare earth elements (HREEs), and light rare earth elements (LREEs). Of the 27 samples tested, 22 contained a TREE concentration higher than the threshold of 300 ppm, which is considered a viable feedstock material. 3 samples contained less than 300 ppm of TREEs; however, they were within 20 ppm of the threshold, and could potentially be considered viable sources in the future pending the advancement of more efficient extraction technologies. 2 of the 27 samples had significantly low TREE concentrations, which does not imply any potential for being a source for REEs. For the minerals identified as most critical in the literature review, a conceptual process flow diagram (PFD) was developed for their extraction from different coal-based feedstocks. The process targets selective recovery of one commodity (i.e., rare earths, lithium, cobalt, and manganese) via several hydrometallurgical separation methods. By identifying potentially extractable coal-based critical mineral resources, a study of the current and future market environments for each critical mineral, and a review of current processing methodologies for critical mineral extraction from coal-based resources, the foundation has been laid to further characterize and explore new resources and extraction techniques. As reliance on technologies in industries such as the production of electronic devices, batteries, and alloys containing critical minerals utilizing critical minerals continues to increase, a sound understanding of our nation’s dependence on and even the global criticality of certain critical minerals, will serve as a catalyst for innovation in virtually all fields of science.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2025

The nuclear charge radius of 13 C

The size is a key property of a nucleus. Accurate nuclear radii are extracted from elastic electron scattering, laser spectroscopy, and muonic atom spectroscopy. The results are not always compatible, as the proton-radius puzzle has shown most dramatically. Beyond helium, precision data from muonic and electronic sources are scarce in the light-mass region. The stable isotopes of carbon are an exception. We present a laser spectroscopic measurement of the root-mean-square (rms) charge radius of 13 C and compare this with ab initio nuclear structure calculations. Measuring all hyperfine components of the 2 3 S → 2 3 P fine-structure triplet in 13 C 4+ ions referenced to a frequency comb allows us to determine its center-of-gravity with accuracy better than 2 MHz although second-order hyperfine-structure effects shift individual lines by several GHz. We improved the uncertainty of R c ( 13 C) determined with electrons by a factor of 6 and found a 3σ discrepancy with the muonic atom result of similar accuracy.

Müller, Patrick [Technical Univ. of Darmstadt (Ger↗
DOE OSTI2022

Multilevel Analysis, Design, and Modeling of Coupling Advanced Nuclear Reactors and Thermal Energy Storage in an Integrated Energy System

This report discusses the different options for coupling thermal energy storage (TES) systems to advanced nuclear power plants (A-NPPs) in order to enable flexible and hybrid plant operation. An advanced light-water reactor (A LWR), a high-temperature gas-cooled reactor (HTGR) and a liquid-metal fast reactor (LMFR) were selected as the initial use cases for demonstrating a thermally balanced energy storage coupling design for thermal power extraction. The models presented herein showcase several design considerations, focusing on optimal deployment methodologies for achieving steady-state and transient-state operation with minimum disruption to the nuclear power cycle. This first part of the study presents steady-state models developed using Aspen HYSYS®, with the thermal energy bypass for NPP-TES coupling being varied at up to 50%. The various components were sized using the Aspen Process Economic Analyzer (APEA) and Aspen Exchanger Design and Rating (EDR), when applicable. Cost functions from these models were developed using the latest publicly available data obtained from APEA V11. The TES-coupled A-NPP steady-state models and cost functions then provided a baseline for dynamic operation and process optimization by using Idaho National Laboratory (INL)’s Framework for Optimization of Resources and Economics (FORCE) tools. A stochastic optimization of the various energy storage systems coupled to the A-NPPs was then performed using the Risk Analysis Virtual Environment (RAVEN) and its dispatch optimization plugin, the Holistic Energy Resource Optimization Network (HERON). The signal processing and synthetic history capabilities of RAVEN were used to account for the unpredictable behavior of electricity markets. An autoregressive moving average (ARMA) model was used to analyze price signals from the Pennsylvania-New Jersey-Maryland (PJM) market and were applied to the HERON analysis in order to optimize a system with the best economics. Transient modeling evaluation was then performed using Modelica models within the HYBRID repository, which was developed at INL for the Department of Energy Integrated Energy Systems program for the characterization of dynamic integrated system behavior and feedback. This includes evaluation of the TES-coupled A-LWR systems’ impact on physical and thermal system response during imposed system demands. Additional TES-coupled reactor types, coupling approaches, markets, and TES technologies will be evaluated in future work.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Systematic Study of Projection Biases in Weak Lensing Analysis

The nature of Dark Energy is possibly one of the most fundamental questions in Physics today. Comprising 70% of the energy density of the Universe, and being responsible for the accelerated expansion of the Universe, this mysterious form of energy with negative pressure is challenging our current understanding of the fundamental laws of nature. Cosmological parameters like total relative matter Density Ωm, the normalization of power spectrum σ8 and their combination S8 = σ8 p Ωm/0.3 are used to quantify our understanding of the evolution of the large-scale structure in the Universe and shed light on the accelerated expansion, caused by the Dark Energy, that started about halfway through the life of the Universe. Sky surveys, like Dark Energy Survey (DES), utilize weak lensing analysis to use the observations of galaxies and their shapes and extract these cosmological parameters. By doing an exhaustive study and quantifying the projection biases in the weak lensing statistics, the research work presented in this dissertation aims to contribute to the precise measurements of the cosmological parameters Ωm, σ8, and S8. For the analysis, we used the standard cosmological model that includes dark energy as the cosmological constant. And, we used the data taken by the DES experiment, which is one of the most complete, deep, and wide field surveys of the sky today.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Sub-micrometer random-pyramid texturing of silicon solar wafers with excellent surface passivation and low reflectance

Select emerging solar cell technologies, ranging from very narrow screen-printed fingers to perovskite/silicon tandems, would benefit from a reduction of the height of the standard pyramidal texture of monocrystalline silicon wafers to below 1 μm. However, fabricating such small surface features usually compromises the requisite low reflectance and high passivation quality. Through systematic design of experiments, we demonstrate that conventional alkaline-based wet-chemical etching processes can be tuned to produce dense, spatially homogeneous, and uniformly sized sub-micrometer pyramids. Precise texture size can be further controlled by adding potassium silicate to the texturing solution to effectively slow the pyramid growth rate and promote nucleation. With pyramid size distribution data—extracted from multiple atomic force microscopy images across each wafer—we demonstrate 16 nanotextures with average pyramid sizes ranging from 62 to 512 nm, with the largest having only 0.3% of its pyramids taller than 1 μm. Six of the nanotextures exhibit light trapping and surface defect densities comparable to state-of-the-art microtextured wafers. In conclusion, the best nanotexture achieved an AM1.5G-weighted reflectance of 11.8% and a minority-carrier lifetime of 3.4 ms after passivation with amorphous silicon, demonstrating that smaller textures need not deteriorate solar cell performance.

14 SOLAR ENERGY↗
DOE OSTI2023

Synthetic Electricity Market Data Generation and HERON Use Case Setup of Advanced Nuclear Reactors Coupled with Thermal Energy Storage Systems

This study evaluates and optimizes advanced nuclear reactors coupled with thermal energy storage (TES) systems in an Integrated Energy System (IES) architecture to enable advanced nuclear power plants (A NPP) to participate in multi-commodity markets, thus enhancing their economic competitiveness. Nuclear-TES coupling scenarios studied herein are designed attenuate the nuclear heat dynamics and defer energy delivery to a later time, enabling the nuclear reactor to continue operating at or near steady-state design conditions as usual while also enabling flexible generation. Three A-NPPs, namely, an advanced light-water reactor (A LWR), a high temperature gas-cooled reactor (HTGR) and a liquid-metal fast reactor (LMFR) were selected as the initial use cases for demonstrating the technoeconomic of thermally balanced energy storage coupling design for thermal power extraction. Each of the reactor technologies were evaluated in two different electricity markets. Stochastic optimization approach was adopted which included the evaluation of price signals from the Pennsylvania-New Jersey-Maryland (PJM) market, and Electric Reliability Council of Texas (ERCOT), using an autoregressive moving average (ARMA) model. Risk Analysis Virtual Environment (RAVEN) tool and its dispatch optimization plugin, the Holistic Energy Resource Optimization Network (HERON), were used to perform dispatch and capacity optimization, using the price data provided by the ARMA models. The results from the Nuclear-TES use cases will be used to design and characterize dynamic integrated system behavior and feedback.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2026

Design of a Cryogenic Assembly for Comparing Qubit Infrared Packaging Inefficiencies

It is well known that everything emits infrared (IR) light in the form of thermal radiation. IR radiation on superconducting qubits carries enough energy to cause decoherence and so-called “quasiparticle poisoning.” Therefore, proper IR shielding is needed to keep the qubit in a high coherence state. However, trying to extract IR-specific information from a qubit is difficult, so a microwave kinetic inductance detector (MKID) can be used instead. We show that the IR shielding inefficiencies of MKID packages can only be compared with other packaging inefficiencies. We create a cryogenic assembly CAD design, consisting of magnetic shield cans, a copper mounting plate and mounts, and an MKID enclosure, which thermalizes the assembly to dilution refrigerator temperatures. Phase 1 of this design involves using a narrowband IR laser source to test the IR shielding of packaging at the laser’s wavelength. When the best IR shielding packaging is determined, the superconducting qubit can replace the MKID, allowing the qubit to avoid decoherence due to IR radiation and boost its performance and coherence lifetime.

Mailliard, Robert J. [Fermilab] (ORCID:00090000277↗
DOE OSTI2024

Time-of-flight detection of terahertz phonon-polariton

A polariton is a fundamental quasiparticle that arises from strong light-matter interaction and as such has attracted wide scientific and practical interest. When light is strongly coupled to the crystal lattice, it gives rise to phonon-polaritons (PPs), which have been proven useful in the dynamical manipulation of quantum materials and the advancement of terahertz technologies. Yet, current detection and characterization methods of polaritons are still limited. Traditional techniques such as Raman or transient grating either rely on fine-tuning of external parameters or complex phase extraction techniques. To overcome these inherent limitations, we propose and demonstrate a technique based on a time-of-flight measurement of PPs. We resonantly launch broadband PPs with intense terahertz fields and measure the time-of-flight of each spectral component with time-resolved second harmonic generation. The time-of-flight information, combined with the PP attenuation, enables us to resolve the real and imaginary parts of the PP dispersion relation. We demonstrate this technique in the van der Waals magnets NiI 2 and MnPS 3 and reveal a hidden magnon-phonon interaction. We believe that this approach will unlock new opportunities for studying polaritons across diverse material systems and enhance our understanding of strong light-matter interaction.

condensed-matter physics↗
DOE OSTI2025

Unexpected origin of the quantum efficiency reduction in long-wavelength (In,Ga)⁢N light-emitting diodes

Differential carrier lifetime (DCL) measurements were performed on c-plane In 𝑥 ⁢Ga 1−𝑥⁢ N/Ga⁢N single-quantum-well (QW) light-emitting diodes (LEDs) with varying indium-content QWs (x = 13.5%, 16%, 22%), emitting with violet, blue, and green wavelengths. The recombination lifetimes of LEDs were found to increase with increasing indium composition, resulting in increased carrier densities n measured by DCL. Extraction of the A coefficients, which are assumed to not vary with n, and of the effective B(n) and C(n) coefficients of the ABC model of the internal quantum efficiency (IQE) of QWs showed no significant changes in the A coefficient with increasing indium content [In] in the In 𝑥 ⁢Ga 1−𝑥 ⁢N QW, and a reduction in the B(n) and C(n) coefficients with increasing [In]. When looking at the Shockley-Read-Hall (SRH) recombination rate An, the radiative recombination rate B(n)𝑛 2 , and the Auger-Meitner (AM) recombination rate C(n)𝑛 3 , we observed that at any given n, the SRH rate is the same for the three [In] measured, while the radiative rate decreases (by up to approximately 9 times) and the AM rate decreases (by up to approximately 7 times) with increasing indium content. This shows that the larger reduction in radiative recombination rates relative to nonradiative recombination rates with increasing [In] is the largest contributor to the decreased quantum efficiencies of LEDs (the “green gap”) at any given n. While some of the reduction in the effective recombination coefficients B(n) and C(n) can be explained by the reduced wave-function overlaps of the QW with increasing indium content, the larger reduction of B(n) relative to C(n) motivates further study of the intrinsic recombination coefficients 𝐵 0 and 𝐶 0 of bulk In 𝑥 ⁢Ga 1−𝑥 ⁢N alloys and how they are related to the effective recombination coefficients B(n) and C(n) in QWs. The relative contributions of nonradiative recombination are enhanced at any given current density due to the sublinear relationship between the carrier density n and the current density. Thus, the solution to the green gap, up to any intrinsic limitations set by the indium content of the QW, from an IQE perspective, requires the design of long-wavelength (In,Ga)⁢N LEDs with improved wave-function overlaps that can operate with a lower carrier density at any given current density.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Design of a Cryogenic Assembly for Comparing Qubit Infrared Packaging Inefficiencies

It is well known that everything emits infrared (IR) light in the form of thermal radiation. IR radiation on superconducting qubits carries enough energy to cause decoherence and so-called “quasiparticle poisoning.” Therefore, proper IR shielding is needed to keep the qubit in a high-coherence state. However, trying to extract IR-specific information from a qubit is difficult, so a microwave kinetic inductance detector (MKID) can be used instead. We show that the IR shielding inefficiencies of MKID packages can only be compared with other packaging inefficiencies. We create a cryogenic assembly CAD design, consisting of magnetic shield cans, a copper mounting plate and mounts, and an MKID enclosure, which thermalizes the assembly to dilution refrigerator temperatures. Phase 1 of this design involves using a narrowband IR laser source to test the IR shielding of packaging at the laser’s wavelength. When the best IR shielding packaging is determined, the superconducting qubit can replace the MKID, allowing the qubit to avoid decoherence due to IR radiation and boost its performance and coherence lifetime.

Mailliard, Robert J. [Fermilab] (ORCID:00090000277↗
DOE OSTI2026

Design of a Cryogenic Assembly for Comparing Qubit Infrared Packaging Inefficiencies

It is well known that everything emits infrared (IR) light in the form of thermal radiation. IR radiation on superconducting qubits carries enough energy to cause decoherence and so-called “quasiparticle poisoning.” Therefore, proper IR shielding is needed to keep the qubit in a high-coherence state. However, trying to extract IR-specific information from a qubit is difficult, so a microwave kinetic inductance detector (MKID) can be used instead. We show that the IR shielding inefficiencies of MKID packages can only be compared with other packaging inefficiencies. We create a cryogenic assembly CAD design, consisting of magnetic shield cans, a copper mounting plate and mounts, and an MKID enclosure, which thermalizes the assembly to dilution refrigerator temperatures. Phase 1 of this design involves using a narrowband IR laser source to test the IR shielding of packaging at the laser’s wavelength. When the best IR shielding packaging is determined, the superconducting qubit can replace the MKID, allowing the qubit to avoid decoherence due to IR radiation and boost its performance and coherence lifetime.

Mailliard, Robert J. [Fermilab] (ORCID:00090000277↗
DOE OSTI2026

Design of a Cryogenic Assembly for Comparing Qubit Infrared Packaging Inefficiencies

It is well known that everything emits infrared (IR) light in the form of thermal radiation. IR radiation on superconducting qubits carries enough energy to cause decoherence and so-called “quasiparticle poisoning.” Therefore, proper IR shielding is needed to keep the qubit in a high-coherence state. However, trying to extract IR-specific information from a qubit is difficult, so a microwave kinetic inductance detector (MKID) can be used instead. We show that the IR shielding inefficiencies of MKID packages can only be compared with other packaging inefficiencies. We create a cryogenic assembly CAD design, consisting of magnetic shield cans, a copper mounting plate and mounts, and an MKID enclosure, which thermalizes the assembly to dilution refrigerator temperatures. Phase 1 of this design involves using a narrowband IR laser source to test the IR shielding of packaging at the laser’s wavelength. When the best IR shielding packaging is determined, the superconducting qubit can replace the MKID, allowing the qubit to avoid decoherence due to IR radiation and boost its performance and coherence lifetime.

Mailliard, Robert J. [Fermilab] (ORCID:00090000277↗
DOE OSTI2026

CMS Outer Tracker Module QA

It is well known that everything emits infrared (IR) light in the form of thermal radiation. IR radiation on superconducting qubits carries enough energy to cause decoherence and so-called “quasiparticle poisoning.” Therefore, proper IR shielding is needed to keep the qubit in a high-coherence state. However, trying to extract IR-specific information from a qubit is difficult, so a microwave kinetic inductance detector (MKID) can be used instead. We show that the IR shielding inefficiencies of MKID packages can only be compared with other packaging inefficiencies. We create a cryogenic assembly CAD design, consisting of magnetic shield cans, a copper mounting plate and mounts, and an MKID enclosure, which thermalizes the assembly to dilution refrigerator temperatures. Phase 1 of this design involves using a narrowband IR laser source to test the IR shielding of packaging at the laser’s wavelength. When the best IR shielding packaging is determined, the superconducting qubit can replace the MKID, allowing the qubit to avoid decoherence due to IR radiation and boost its performance and coherence lifetime.

Hobbeheydar, Samuel [Carnegie Mellon U. (main); Fe↗
DOE OSTI2024

Lattice QCD estimates of thermal photon production from the QGP

Thermal photons produced in heavy-ion collision experiments are an important observable for understanding quark-gluon plasma (QGP). The thermal photon rate from the QGP at a given temperature can be calculated from the spectral function of the vector current correlator. Extraction of the spectral function from the lattice correlator is known to be an ill-conditioned problem, as there is no unique solution for a spectral function for a given lattice correlator with statistical errors. The vector current correlator, on the other hand, receives a large ultraviolet contribution from the vacuum, which makes the extraction of the thermal photon rate difficult from this channel. We therefore consider the difference between the transverse and longitudinal part of the spectral function, only capturing the thermal contribution to the current correlator, simplifying the reconstruction significantly. The lattice correlator is calculated for light quarks in quenched QCD at T = 470 MeV ( ∼ 1.5 T c ), as well as in 2 + 1 flavor QCD at T = 220 MeV ( ∼ 1.2 T p c ) with m π = 320 MeV . In order to quantify the nonperturbative effects, the lattice correlator is compared with the corresponding NLO + LPM LO estimate of correlator. The reconstruction of the spectral function is performed in several different frameworks, ranging from physics-informed models of the spectral function to more general models in the Backus-Gilbert method and Gaussian process regression. We find that the resulting photon rates agree within errors. Published by the American Physical Society 2024

Astronomy & Astrophysics↗
DOE OSTI2021

Prompt Gamma Analysis of ARIES Materials and Updates to the 2015 Calibration Equations

Prompt gamma (PG) analysis is a nondestructive, nuclear, elemental analysis technique that uses charged particle reactions to interrogate a sample, and elements present in the sample matrix are identified through the characteristic gamma-rays emitted from the product nuclei in alpha-p and alpha-n nuclear reactions. This technique has been applied to plutonium oxide packaged in over 4,000 individual 3013 containers, and the concentrations of certain light elements were determined from the integrated peak areas based on a calibration that was published previously. This report provides the results for a new population of 3013 containers packaged with oxide materials produced by the conversion of metal by Advanced Recovery and Integrated Extraction System (ARIES) project using the direct metal oxidation (DMO) process and muffle furnaces. New PG and analytical chemistry data collected since 2015 were added to the existing calibration data sets to refine the calibration parameters. Calibration equations were also developed for determining beryllium and fluorine at low concentrations in high-purity ARIES product oxides. The new fluorine calibration provides an order of magnitude greater sensitivity and results in an additional 1,408 containers in the original population identified as having fluorine as an impurity. Additionally, equations for calculating the lower limits of detection (LLDs) as a function of the actual counting time (live time) were obtained using WLS regression technique for samples in the calibration data set. This resulted in changes to the LLDs published previously.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Identifying Light-Duty Vehicle Travel from Large-Scale Multimodal Wearable GPS Data with Novelty Detection Algorithms

Identifying travel mode within travel survey data sets, especially light-duty vehicle (LDV) travel, is foundational, though nontrivial, to travel behavior analysis and fuel consumption estimation. Current travel mode detection approaches require well-sampled and balanced data sets with ground truth travel mode labels. They are rarely applied and validated on large-scale, real-world data sets, which may not satisfy the data requirements. This paper proposes an LDV travel mode detection model as a supplement to current travel mode detection methods, for the case when the training set is highly (and/or completely) unbalanced, to the extent that classical machine-learning approaches become difficult or impossible to deploy. The proposed model uses a novelty detection technique-one-class support vector machines (OCSVMs)-and a novel exhaustive feature extraction (EFE) technique on continuous time series data (i.e., Global Positioning System [GPS] speed profiles) for single-mode trip trajectories. Training and validation of the model are conducted on a large-scale, real-world data set. The proposed method accurately identifies LDV trips from a broad set of multimodal trips by leveraging a wealth of preexisting in-vehicle GPS travel data. Additional sensitivity analysis sheds light on the optimal training size, which will benefit applications limited by highly imbalanced data. The paper also discusses performance comparison with regular machine-learning approaches, the model's robustness, and the potential to extend the proposed model to multimodal prediction.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Fast Near-Infrared Photodetection Using III–V Colloidal Quantum Dots

Colloidal quantum dots (CQDs) are promising materials for infrared (IR) light detection due to their tunable bandgap and their solution processing; however, to date, the time response of CQD IR photodiodes is inferior to that provided by Si and InGaAs. It is reasoned that the high permittivity of II–VI CQDs leads to slow charge extraction due to screening and capacitance, whereas III–Vs—if their surface chemistry can be mastered—offer a low permittivity and thus increase potential for high-speed operation. In initial studies, it is found that the covalent character in indium arsenide (InAs) leads to imbalanced charge transport, the result of unpassivated surfaces, and uncontrolled heavy doping. Surface management using amphoteric ligand coordination is reported, and it is found that the approach addresses simultaneously the In and As surface dangling bonds. The new InAs CQD solids combine high mobility (0.04 cm 2 V -1 s -1 ) with a 4× reduction in permittivity compared to PbS CQDs. Finally, the resulting photodiodes achieve a response time faster than 2 ns—the fastest photodiode among previously reported CQD photodiodes—combined with an external quantum efficiency (EQE) of 30% at 940 nm.

36 MATERIALS SCIENCE↗