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DOE OSTI2018

Real-Time Procurement Strategies of a Proactive Distribution Company With Aggregator-Based Demand Response

In this paper, we present a real-time trading framework for distribution networks where a rational aggregator is identified as a broker by contracting with individual demands and dealing with the distribution company. Demand response capability is characterized by the coexistence of elastic and inelastic demand components. A one-leader multi-follower bi-level model is proposed to derive the procurement strategies, i.e., the upperlevel problem intends to maximize the profit of the proactive distribution company, while the lower-level expresses the profit maximization per rational aggregator. The proposed model is then transformed into a solvable mathematical program with equilibrium constraints through a primal-dual approach. A modified 33-bus distribution network is utilized to demonstrate the effectiveness of the proposed model.

demand response (DR)↗

DOE OSTI2020

Optimal PMU Restoration for Power System Observability Recovery After Massive Attacks

Cyber-physically resilient power system operation requires rapid recovery of situational awareness after disastrous scenarios such as massive cyber attacks. In this article, the concept of optimal sequential restoration of Phasor Measurement Units is introduced, aiming at rapid recovery of power system observability in post-attack scenarios. Additionally, the observability recovery problem is formulated as a Mixed Integer Linear Programming problem to maximize the cumulative observability level gained over time during the restoration process. Three alternative objective functions-maximizing the number of observable buses, the number of observable branches, and the total amount of observable power flow-are considered. The effectiveness of the proposed optimal strategy is verified by comparing it with heuristic approaches on the IEEE 57-bus system.

24 POWER TRANSMISSION AND DISTRIBUTION↗

DOE OSTI2022

A Non-Cooperative Game-Based Distributed Beam Scheduling Framework for 5G Millimeter-Wave Cellular Networks

Here, this paper studies the problem of distributed beam scheduling for 5G millimeter-Wave (mm-Wave) cellular networks where base stations (BSs) belonging to different operators share the same spectrum without centralized coordination among them. Our goal is to design efficient distributed scheduling algorithms to maximize the network utility, which is a function of the achieved throughput by the user equipment (UEs), subject to the average and instantaneous power consumption constraints of the BSs. We propose a Media Access Control (MAC) and a power allocation/adaptation mechanism utilizing the Lyapunov stochastic optimization framework and non-cooperative games. In particular, we first decompose the original utility maximization problem into two sub-optimization problems for each time frame, which are a convex optimization problem and a non-convex optimization problem, respectively. By formulating the distributed scheduling problem as a non-cooperative game where each BS is a player attempting to optimize its own utility, we provide a distributed solution to the non-convex sub-optimization problem via finding the Nash Equilibrium (NE) of the game whose weights are determined optimally by the Lyapunov optimization framework. Finally, we conduct simulation under various network settings to show the effectiveness of the proposed game-based beam scheduling algorithm in comparison to that of several reference schemes.

42 ENGINEERING↗

DOE OSTI2021

Dynamic Interference Management for UAV-Assisted Wireless Networks

Here, we investigate a transmission mechanism aiming to improve the data rate between a base station (BS) and a user equipment (UE) through deploying multiple relaying UAVs. We consider the effect of interference incurred by another established communication network, which makes our problem challenging and different from the state of the art. We aim to design the 3D trajectories and power allocation for the UAVs to maximize the data flow of the network while keeping the interference on the existing communication network below a threshold. We utilize the mobility feature of the UAVs to evade the (un)-intended interference caused by (un)-intentional interferers. To this end, we propose an alternating-maximization approach to jointly obtain the 3D trajectories and the UAVs transmission powers. We handle the 3D trajectory design by resorting to spectral graph the power allocation through convex optimization techniques. We also approach the problem from the intentional interferer’s perspective where smart jammers chase the UAVs to effectively degrade the data flow of the network. We also extend our work to the case for multiple UEs. Finally, we demonstrate the efficacy of our proposed method through extensive simulations.

42 ENGINEERING↗

DOE OSTI2018

Downregulation of HOXA13 sensitizes human esophageal squamous cell carcinoma to chemotherapy

Background Chemoresistance often develops in esophageal squamous cell carcinoma (ESCC), leading to poor prognosis. HOX genes play a crucial role in embryonic development and cell differentiation. Studies have recently linked HOX with chemoresistance, thus we explored whether HOXA13 is involved in ESCC chemoresistance. Methods One hundred thirty‐one ESCC patients who received neoadjuvant chemotherapy were enrolled. HOXA13 expression was examined by immunohistochemistry. RNA interference was used to knock down the HOXA13 expression in KYSE70 and transfected HOXA13 plasmid to overexpress HOXA13 in KYSE510 cells. We examined half‐maximal inhibitory concentration of cisplatin, apoptosis, and epithelial‐to‐mesenchymal transition (EMT) in ESCC cell lines with different HOXA13 expression levels by cell counting kit‐8, flow cytometry, and transwell analysis. Results The median survival of patients with high HOXA13 expression was significantly shorter than those with low expression ( P = 0.027). HOXA13 was associated with worse tumor regression grade ( P = 0.009). Low HOXA13 expressed cells decreased the half‐maximal inhibitory concentration of cisplatin ( P < 0.05), increased cisplatin‐induced apoptosis ( P < 0.05), and decreased EMT ( P < 0.05) compared with high HOXA13 expressed cells. In low HOXA13 expressed cells, cleaved caspase‐3 and cleaved PARP expression induced by cisplatin increased, while expression of E‐cadherin and Snail protein, markers of EMT, was upregulated and downregulated, respectively. EMT decreased in low HOXA13 expressed cells. Conclusion High HOXA13 expression was associated with inferior tumor regression grade and poor overall survival in ESCC patients treated with neoadjuvant chemotherapy. HOXA13 increased cisplatin‐resistance and promoted EMT in ESCC cells.

Shi, Qi↗

DOE OSTI2018

Guidelines and considerations for designing field experiments simulating precipitation extremes in forest ecosystems

1. Precipitation regimes are changing in response to climate change, yet understanding of how forest ecosystems respond to extreme droughts and pluvials remains incomplete. As future precipitation extremes will likely fall outside the range of historical variability, precipitation manipulation experiments (PMEs) are critical to advancing knowledge about potential ecosystem responses. However, few PMEs have been conducted in forests compared to short-statured ecosystems, and forest PMEs have unique design requirements and constraints. Moreover, past forest PMEs have lacked coordination, limiting cross-site comparisons. Here, we review and synthesize approaches, challenges, and opportunities for conducting PMEs in forests, with the goal of guiding design decisions, while maximizing the potential for coordination. 2. We reviewed 63 forest PMEs at 70 sites world-wide. Workshops, meetings, and communications with experimentalists were used to generate and build consensus around approaches for addressing the key challenges and enhancing coordination. 3. Past forest PMEs employed a variety of study designs related to treatment level, replication, plot and infrastructure characteristics, and measurement approaches.Important considerations for establishing new forest PMEs include: selecting appropriate treatment levels to reach ecological thresholds; balancing cost, logistical complexity, and effectiveness in infrastructure design; and preventing unintended water subsidies. Response variables in forest PMEs were organized into three broad tiers reflecting increasing complexity and resource intensiveness, with the first tier representing a recommended core set of common measurements. 4. Differences in site conditions combined with unique research questions of experimentalists necessitate careful adaptation of guidelines for forest PMEs to balance local objectives with coordination among experiments. We advocate adoption of a common framework for coordinating forest PME design to enhance cross-site comparability and advance fundamental knowledge about the response and sensitivity of diverse forest ecosystems to precipitation extremes.

Climate Extremes, drought, ecological thresholds, ↗

DOE OSTI2026

Comprehensive framework for assessing and optimizing existing research networks

Conservation, monitoring, and research networks, or collections of ecological research sites unified under a common mission of data collection or a research mission, are essential infrastructure for understanding large landscapes. However, most networks developed opportunistically over decades rather than through systematic design, creating potential limitations in the ability to address conservation challenges across entire regions. We developed a framework to evaluate how well an existing research network represents the environmental conditions its members study and devised an approach to rank sites of priority for strategic expansion. Our approach measures performance through environmental representativeness, geographic coverage, and adequacy for scientific inference and thus optimizes limited monitoring resources to maximize scientific impact. We demonstrated this approach with the U.S. Department of Agriculture (USDA) Forest Service Experimental Forests and Ranges Network (EFRN), a 79‐site network across the United States that grew opportunistically over a century. At the national scale, the network effectively captured high‐biomass forests important for carbon cycle research; 82% of forest biomass was in well‐represented areas. Some areas in Texas, Florida, the Rocky Mountains, and the West Coast had no relevant EFRN sites, which limits the ability to make regional inferences. A fundamental challenge for the EFRN was that sites improving regional extent coverage sometimes provided minimal national benefits, which can create conflicts between local and global priorities. Adding the highest‐ranked candidate site provided a relevant site for 17% of currently poorly represented 1‐km pixel cells nationally, but regional and national site rankings varied considerably due to nested spatial inference. This framework provides quantitative tools for strategic infrastructure decision‐making, ensures that limited monitoring resources maximize conservation impact, and can be applied broadly to address the widespread challenge of optimizing conservation and monitoring networks worldwide.

additional site↗

DOE OSTI2022

Temperature optimum for marsh resilience and carbon accumulation revealed in a whole ecosystem warming experiment

Coastal marshes are globally important, carbon dense ecosystems simultaneously maintained and threatened by sea-level rise. Warming temperatures may increase wetland plant productivity and organic matter accumulation, but temperature-modulated feedbacks between productivity and decomposition make it difficult to assess how wetlands and their thick, organic rich soils will respond to climate warming. Here, we actively increased aboveground plant-surface and below-ground soil temperatures in two marsh plant communities, and found that a moderate amount of warming (1.7°C above ambient temperatures) consistently maximized root growth, marsh elevation gain, and below-ground carbon accumulation. Marsh elevation loss observed at higher temperatures was associated with increased carbon mineralization and increased microtopographic heterogeneity, a potential early warning signal of marsh drowning. Here, maximized elevation and below-ground carbon accumulation for moderate warming scenarios uniquely suggest linkages between metabolic theory of individuals and landscape-scale ecosystem resilience and function, but our work indicates nonpermanent benefits as global temperatures continue to rise.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

PlanHab * : hypoxia does not worsen the impairment of skeletal muscle oxidative function induced by bed rest alone

Key points Superposition of hypoxia on 21 day bed rest did not worsen the impairment of skeletal muscle oxidative function induced by bed rest alone. A significant impairment of maximal oxidative performance was identified downstream of cardiovascular O 2 delivery, involving both the intramuscular matching between O 2 supply and utilization and mitochondrial respiration. These chronic adaptations appear to be relevant in terms of exposure to spaceflights and reduced gravity habitats (Moon or Mars), as characterized by low gravity and hypoxia, in patients with chronic diseases characterized by hypomobility/immobility and hypoxia, as well as in ageing. Abstract Skeletal muscle oxidative function was evaluated in 11 healthy males (mean ± SD age 27 ± 5 years) prior to (baseline data collection, BDC) and following a 21 day horizontal bed rest (BR), carried out in normoxia ( = 133 mmHg; N‐BR) and hypoxia ( = 90 mmHg; H‐BR). H‐BR was aimed at simulating reduced gravity habitats. The effects of a 21 day hypoxic ambulatory confinement ( = 90 mmHg; H‐AMB) were also assessed. Pulmonary O 2 uptake ( ), vastus lateralis fractional O 2 extraction (changes in deoxygenated haemoglobin + myoglobin concentration, Δ[deoxy(Hb + Mb)]; near‐infrared spectroscopy) and femoral artery blood flow (ultrasound Doppler) were evaluated during incremental one‐leg knee‐extension exercise (reduced constraints to cardiovascular O 2 delivery) carried out to voluntary exhaustion in a normoxic environment. Mitochondrial respiration was evaluated ex vivo by high‐resolution respirometry in permeabilized vastus lateralis fibres. decreased ( P < 0.05) after N‐BR (0.98 ± 0.13 L min −1 ) and H‐BR (0.96 ± 0.17 L min −1 ) vs . BDC (1.05 ± 0.14 L min −1 ). In the presence of a decreased (by ∼6–8%) thigh muscle volume, normalized per unit of muscle mass was not affected by both interventions. Δ[deoxy(Hb + Mb)] peak decreased ( P < 0.05) after N‐BR (65 ± 13% of limb ischaemia) and H‐BR (62 ± 12%) vs . BDC (73 ± 13%). H‐AMB did not alter or Δ[deoxy(Hb + Mb)] peak . An overshoot of Δ[deoxy(Hb + Mb)] was evident during the first minute of unloaded exercise after N‐BR and H‐BR. Arterial blood flow to the lower limb during both unloaded and peak knee extension was not affected by any intervention. Maximal ADP‐stimulated mitochondrial respiration decreased ( P < 0.05) after all interventions vs . control. In 21 day N‐BR, a significant impairment of oxidative metabolism occurred downstream of cardiovascular O 2 delivery, affecting both mitochondrial respiration and presumably the intramuscular matching between O 2 supply and utilization. Superposition of H on BR did not worsen the impairment induced by BR alone.

Salvadego, Desy↗

DOE OSTI2023

Evaluation of Spray and Combustion Models for Simulating Dilute Combustion in a Direct-Injection Spark-Ignition Engine

Dilute combustion in spark-ignition engines has the potential to improve thermal efficiency by mitigating knock and by reducing throttling and wall heat losses. However, ignition and combustion processes can become unstable for dilute operation due to a lowered laminar flame speed, resulting in excessive cycle-to-cycle variability (CCV) of the combustion process. To compensate for the slower combustion in less reactive mixtures, a modified intake port geometry can be employed to generate a strong tumble flow in the cylinder and elevate turbulence levels around the spark plug, thereby promoting a faster transition to turbulent deflagration. Consequently, optimizing combustion chamber geometry and operating strategy is crucial to maximizing the benefits of using dilute combustion with enhanced in-cylinder turbulence across a wide range of operating conditions. Computational fluid dynamics (CFD) simulations can be utilized for virtual engine optimization tasks, but this would require the models to be truly predictive regarding the impact of changes to the engine design and operational parameters.In this study, multicycle large-eddy simulations (LES) are performed for a direct-injection spark-ignition engine to investigate the model performance in predicting engine combustion characteristics with respect to changes in the intake configuration. A tumble plate that blocks the lower part of the intake port inlet is used to vary the tumble. A set of CFD models that have been recently developed are employed, which takes into account the drag of nonspherical droplets, flash-boiling behavior of liquid sprays, spray-wall interaction, surrogate formulation of a research-grade E10 gasoline, and fast chemical kinetic solvers. Simulation results are compared to experimental engine data in terms of cylinder pressure, apparent heat release rate, mass fraction burned timing, and flame images. It is found that LES employing the state-of-the-art CFD models are capable of properly predicting the spray processes and reproducing the measured mean cylinder pressure for the case with the tumble plate. On the other hand, the LES over-predicts the combustion rate during the early combustion stage and under-estimates the CCV, and these discrepancies become larger when the tumble plate is removed.

computational fluid dynamics simulation↗

DOE OSTI2023

Reman Co-Design: A Combined Design and Remanufacturing Optimization Framework for the Sustainable Design of High-Value Components

Remanufacturing is a process that returns end-of-life equipment to as-new conditions and offers numerous environmental and economic benefits. To fully capitalize on remanufacturing, its synergistic interactions with design must be fully realized and addressed during the design stage. Although this fact is widely recognized in the literature, most of the current studies focus primarily either on the design or remanufacturing aspects of design for remanufacturing (DfRem). In an effort to offer a more integrated DfRem approach than those reported in the literature, we propose a new combined design and remanufacturing optimization (reman co-design) framework that takes a holistic approach by leveraging the intricate interplay between design and remanufacturing. Here, the aim of this formulation is to identify the optimal decisions that maximize the benefits of remanufacturing throughout the entire lifespan of a product. To showcase the utility of the new formulation, we are using a case study of a hydraulic manifold, (re)manufactured by John Deere. Using this industry example, we compare the results of reman co-design to the ones from a decoupled remanufacturing design approach. Results reveal that remanufacturing benefits are better realized and improved upon when using the developed reman co-design approach.

design for X↗

DOE OSTI2018

SEMI-ACTIVE CONTROL FOR TWO-BODY OCEAN WAVE ENERGY CONVERTER BY USING HYBRID MODEL PREDICTIVE CONTROL

Model predictive control (MPC) has been considered as one important feed-forward optimal control strategy for ocean wave energy converter (WEC) targeted on power maximization. The capability of MPC to handle system constraints (ex. stroke, velocity, actuator limitations), and the availability to provide optimal solution for linear system provide potential for the implementation of such algorithm in the WEC control. However, currently, only active MPC control has been introduced for single and two-body WECs. Such control strategy may introduce negative power during the optimization process, since the power take-off (PTO) damping has no constraint. In this paper, we proposed a hybrid MPC strategy in limiting both the PTO damping force and PTO damping to avoid negative power generation during cost function minimization (negative power minimization) for the two-body WEC. The problem is formulated into a quadratic programming (QP) problem targeted at power maximization. However, the standard QP problem formulation cannot be directly applied to the semi-active control problem due to the PTO damping constraints. Therefore, the problem is reformulated as a Mixed-integer Quadratic Programming (MIQP) problem, which contains logical switch to select constraint matrices based on the sign of the relative velocity between the buoy and submerged body. The optimal solution is compared with those of the active MPC control strategy and the passive model with the same irregular wave input.

16 TIDAL AND WAVE POWER↗

DOE OSTI2020

Investigating the Impact of Power-Take-Off System Parameters and Control Law on a Rotational Wave Energy Converter’s Peak-to-Average Power Ratio Reduction

Due to the irregular nature of real waves, the power captured in a wave energy converter (WEC) system is highly variable. This is an important barrier to the effective use of WECs. To address this challenge, this study focuses on a rotational WEC power-take-off system in which high-speed and high-efficiency generators along with a torque/power smoothing inertia element can be effectively utilized. In the first phase of this study, the U.S. Department of Energy’s reference model 3 (WEC-Sim RM3; two-body point absorber), along with a slider-crank WEC, were integrated for linear to rotational conversion. Relative motion between the float and spar in RM3 was the driving force for this slider-crank WEC, which is connected to a motor/generator set through a gearbox. RM3 geometry was scaled down by 25 times to work within the limits of the physical motor/generator set used in the experimentation. Once the integration in a hardware-in-the-loop simulation environment was successfully completed, data on the peak-to-average power ratio was collected for various wave conditions including regular and irregular waves. The control algorithm designed to keep the system in resonance with waves was able to maintain relatively high speed depending on the specific gear ratio and wave period. Initial results with hardware-in-the-loop simulations reveal that gear ratio and crank radius have a strong impact on the peak-to-average power ratio. In addition, it was found that output power from the generator was maximized at a larger gear ratio, as the crank radius was increased.

50 EE - Wind and Water Power Program - Water (EE-4↗

DOE OSTI2020

Numerical Model Development of a Variable-Geometry Attenuator Wave Energy Converter

Because the wave energy industry is still in its infancy, an optimal design for wave energy converters (WECs) has yet to be established; more work is needed to explore various cost-reduction pathways. The primary cost-reduction pathway considered for this work is the optimization of the geometric profile on an attenuator WEC to maximize power production while, at the same time, minimizing capital expenditures through the use of variable-geometry modules. In this investigation, the variable-geometry modules consist of inflatable bags placed on either side of a base central steel cylinder that would be inflated in low-moderate sea states to maximize power capture and then deflated in moderate-extreme sea states to minimize wave loading. The numerical model and simulation of the attenuator WEC were developed and completed using WEC-Sim, which is an open-source code that is appropriate for use in evaluating the dynamic response of the different WEC models in operational seas. The power production estimates were obtained from the Wave Energy Prize (WEP) sea states, which are representative of U. S. deployment sites, to calculate the average climate capture width that is used in the WEP ACE calculation. Preliminary capital expenditure costs were obtained assuming the base central steel cylinder mass was equal to the fluid displaced mass, minus the mass of the variable-geometry bags. The additional weight required to offset the additional buoyancy from the variable-geometry bags was assumed to come from the addition of seawater ballast. The variable-geometry attenuator model was found to have a similar power capture efficiency as a fixed-body model, but is expected to have a lower characteristic capital expenditure given its more streamlined profile, which demonstrates that variable-geometry modules may provide a realistic cost-reduction pathway to help design a more cost-competitive WEC.

50 EE - Wind and Water Power Program - Water (EE-4↗

DOE OSTI2018

Broadband anti-reflective coatings for cosmic microwave background experiments

The desire for higher sensitivity has driven ground-based cosmic microwave background (CMB) experiments to employ ever larger focal planes, which in turn require larger reimaging optics. Practical limits to the maximum size of these optics motivates the development of quasi-optically-coupled (lenslet-coupled), multi-chroic detectors. These detectors can be sensitive across a broader bandwidth compared to waveguide-coupled detectors. However, the increase in bandwidth comes at a cost: the lenses (up to ~700 mm diameter) and lenslets (~5 mm diameter, hemispherical lenses on the focal plane) used in these systems are made from high-refractive-index materials (such as silicon or amorphous aluminum oxide) that reflect nearly a third of the incident radiation. In order to maximize the faint CMB signal that reaches the detectors, the lenses and lenslets must be coated with an anti-reflective (AR) material. The AR coating must maximize radiation transmission in scientifically interesting bands and be cryogenically stable. Such a coating was developed for the third generation camera, SPT-3G, of the South Pole Telescope (SPT) experiment, but the materials and techniques used in the development are general to AR coatings for mm-wave optics. The three-layer polytetra uoroethylene-based AR coating is broadband, inexpensive, and can be manufactured with simple tools. The coating is field tested; AR coated focal plane elements were deployed in the 2016-2017 austral summer and AR coated reimaging optics were deployed in 2017-2018.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

Optimizing Transmission of Acoustic Signals to Monitor Internal Conditions of Canisters for Dry Storage of Commercial Spent Nuclear Fuel

Safe storage of spent nuclear fuel (SNF) is critical to the nuclear fuel cycle and the future of nuclear energy. In the United States, SNF is stored primarily via two methods regulated by the U.S. Nuclear Regulatory Commission: wet storage in SNF pools and dry storage in dry cask storage systems (DCSSs). After about five years of cooling in spent fuel pools, the fuel assemblies are transferred into DCSSs, and the systems are filled with helium and sealed by welding. Deterioration of conditions inside of a DCSS is reflected in changes in the internal gas properties; this motivates the development of acoustic techniques to monitor internal gas properties, over extended storage periods, using sensors mounted on the exterior of the storage packages. However, a major challenge in collecting acoustic signals is the impedance mismatch between the steel canister shell and the gas. Only a small fraction of the ultrasonic signal can be transmitted through the gas medium. This paper documents experimental studies conducted on a full-scale canister mock-up to capture the gas-borne signals. Damping materials were pasted on the outside, and blocking and unblocking tests were conducted to identify the gas-borne signal. The results show that the excitation frequency plays an important role in maximizing the gas-borne signals. The gas-borne signal was successfully detected at around the theoretical time-of-flight. A high signal-to-noise ratio was achieved in the measurements. Next, the acoustic impedance matching layers were introduced, and the gas signal was drastically improved compared with that using no AIM layers.

Spent nuclear fuel (SNF), Canisters, Internal cond↗

DOE OSTI2025

Black-box optimization of CT acquisition and reconstruction parameters: a reinforcement learning approach

Protocol optimization is critical in Computed Tomography (CT) for achieving desired diagnostic image quality while minimizing radiation dose. Due to the inter-effect of influencing CT parameters, traditional optimization methods rely on the testing of exhaustive combinations of these parameters. This poses a notable limitation due to the impracticality of exhaustive parameter testing. This study introduces a novel methodology leveraging Virtual Imaging Trials (VITs) and reinforcement learning to more efficiently optimize CT protocols. Computational phantoms with liver lesions were imaged using a validated CT simulator and reconstructed with a novel CT reconstruction Toolkit. The optimization parameter space included tube voltage, tube current, reconstruction kernel, slice thickness, and pixel size. The optimization process was done using a Proximal Policy Optimization (PPO) agent which was trained to maximize the Detectability Index (d’) of the liver lesion for each reconstructed image. Results showed that our reinforcement learning approach found the absolute maximum d’ across the test cases while requiring 79.7% fewer steps compared to an exhaustive search, demonstrating both accuracy and computational efficiency, offering a efficient and robust framework for CT protocol optimization. The flexibility of the proposed technique allows for use of varying image quality metrics as the objective metric to maximize for. Our findings highlight the advantages of combining VIT and reinforcement learning for CT protocol management.

Fenwick, David [Duke University Medical Center]↗

DOE OSTI2025

Plasmonic pathway to hybrid nanomaterials through energy transfer

Plasmon-induced resonance energy transfer (PIRET) is a promising approach for plasmonic photocatalysis and energy conversion, but challenges include elucidating the mechanism and maximizing its efficiency, both of which are hampered by competing processes. Another challenge is demonstrating that PIRET can photoinitiate reactions that follow efficient pathways compared to bulk processes. We report a plasmon-induced route to plasmonic-polymer hybrid nanomaterials using in operando single-particle spectroelectrochemistry. An energy transfer efficiency of 40% is achievable when the spectral overlap between gold nanorod scattering and polymer absorption is maximized. We also show that PIRET-initiated polymerization proceeds through a different mechanism than bulk polymerization, supported by spectroscopic evidence and density functional theory calculations, highlighting efficient energy cascading from photon to plasmon to exciton and, lastly, to unconventional light-initiated chemistry.

Oh, Hyuncheol [University of Illinois Urbana-Champ↗