Search NASA⌕ Search

SEARCH · Search NASA

Results for “paired field studies”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Results from Laboratory and Field Study of Thin Triple Pane Windows

Heat transfer through windows accounts for a significant percentage of a building’s energy use and adds substantially to the peak cooling load of a home. In recent years, improvements in glass manufacturing have enabled the use of a very thin central pane of glass similar to a cell phone screen to produce a thin triple-pane window, for finished insulated glass units (IGUs) with an overall thickness similar to standard double-pane windows. Because this highly insulating “thin triple” glass product can be incorporated into almost any existing window frame and can be fabricated at a modest added cost, the U.S. Department of Energy sponsored laboratory and field demonstration testing of thin triple-pane windows to validate thermal performance and installation requirements in real-life field settings. Thin triple pane windows were evaluated at the PNNL Lab Homes, a matched pair of manufactured houses located on PNNL’s campus in Richland, Washington and also at 16 different field study sites around the country. The experimental results include a comparison of heating, ventilation, and air-conditioning (HVAC) energy usage, condensation potential, occupant comfort, sound infiltration, and thermal performance. Field study data will be gathered through June of 2022; preliminary results are being shared in this paper. The lab houses are identical except that the reference house had standard double pane windows with assembly U-0.66 and the test house had thin triple pane windows with assembly U-0.19. Across the experimental test days, the daily HVAC savings ranged from 0.2 to 18.7 kWh (3%–18%) for the heating season and from 2.5 to 8.0 kWh (23%–41%) for the cooling season. The higher thermal performance of the thin triple-pane windows also reduced the condensation potential on the interior surface during winter months and provided more even distribution of temperatures throughout the home in comparison to the baseline. In addition to the added thermal performance, the thin triple-pane windows demonstrated significant acoustic benefits, reducing sound infiltration by 8 dB to 10 dB. For the field test portion of the project thin triple pane insulated glass units were produced by two different manufacturers, and then installed without modification into the ½” IGU pockets of the standard double pane frames of four other manufacturers. Field tests performed on existing homes in Washington, Montana, Colorado, and New York compared thin triple pane retrofits to original window conditions (before and after). Field tests at new construction sites in Minnesota, Michigan, and New York compared thin triple pane windows to commercially available solutions such as double pane or traditional triple pane (with a standard-thickness center pane). Field test work is ongoing, but preliminary results appear to follow the sound, surface temperature, and energy improvement results from the Lab Homes comparison. Additionally, reports from builders and installers indicate that thin triples require almost no added time or effort to install and look nearly identical to other windows, indicating the possibility of offering next-level performance with a product that requires very little modification to current production or installation practices, long considered a major barrier to technology uptake in the construction market.

energy efficiency, home retrofit, Windows, window ↗
DOE OSTI2020

Maximized lateral inhibition in paired magnetic domain wall racetracks for neuromorphic computing

Lateral inhibition is an important functionality in neuromorphic computing, modeled after the biological neuron behavior that a firing neuron deactivates its neighbors belonging to the same layer and prevents them from firing. In most neuromorphic hardware platforms lateral inhibition is implemented by external circuitry, thereby decreasing the energy efficiency and increasing the area overhead of such systems. Recently, the domain wall—magnetic tunnel junction (DW-MTJ) artificial neuron is demonstrated in modeling to be intrinsically inhibitory. Without peripheral circuitry, lateral inhibition in DW-MTJ neurons results from magnetostatic interaction between neighboring neuron cells. However, the lateral inhibition mechanism in DW-MTJ neurons has not been studied thoroughly, leading to weak inhibition only in very closely-spaced devices. This work approaches these problems by modeling current- and field- driven DW motion in a pair of adjacent DW-MTJ neurons. We maximize the magnitude of lateral inhibition by tuning the magnetic interaction between the neurons. The results are explained by current-driven DW velocity characteristics in response to an external magnetic field and quantified by an analytical model. Dependence of lateral inhibition strength on device parameters is also studied. Finally, lateral inhibition behavior in an array of 1000 DW-MTJ neurons is demonstrated. Our results provide a guideline for the optimization of lateral inhibition implementation in DW-MTJ neurons. Finally, with strong lateral inhibition achieved, a path towards competitive learning algorithms such as the winner-take-all are made possible on such neuromorphic devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

AmeriFlux FLUXNET-1F US-CF2 CAF-LTAR Cook West

This is the AmeriFlux Management Project (AMP) created FLUXNET-1F version of the carbon flux data for the site US-CF2 CAF-LTAR Cook West. This is the FLUXNET version of the carbon flux data for the site US-CF2 CAF-LTAR Cook West produced by applying the standard ONEFlux (1F) software. Site Description - CF2 has operated since May 2017 at the R.J. Cook Agronomy Farm outside of Pullman, Washington, and monitors the conventionally tilled side of a paired-catchment study that is part of the Longterm Agroecosystem Research (LTAR) site common experiment. CF2 is located in “Cook West,” a field that has been in conventional tillage since prior to 1998 and constitutes the Prevalent treatment of the common experiment. In this case, conventional tillage involves chisel plowing after the winter wheat phase of rotations (approximately every 3-4 years) and occasional harrowing. CF2 is paired with the CF1 tower location in “Cook East,” which has been in no-till since 1998 and represents the Alternative treatment of the common experiment. Both fields are planted in the same crops every year. Cook Agronomy Farm is in the high precipitation agroecological zone of the Columbia Plateau’s dryland cropping region. Crop rotations are wheat-based and include winter wheat, spring wheat, chickpea, spring canola, and winter peas. Wheat is the principal cash crop, with other crops grown in rotation for diversity, nutrient, and pest management. Soils are predominantly silt loam texture Mollisols in the Palouse, Thatuna, Naff soil series. The CF2 tower replaced US-RC2, which operated 2012-2016 in a neighboring field that was also conventionally tilled. CF2 and RC2 have distinct footprints, aspects, and soil series compositions.

Huggins, Dave↗
DOE OSTI2024

Disentangling the physics of the attractive Hubbard model as a fully interacting model of fermions via the accessible and symmetry-resolved entanglement entropies

The complicated ways in which electrons interact in many-body systems such as molecules and materials have long been viewed through the lens of local electron correlation and associated correlation functions. However, quantum information science has demonstrated that more global diagnostics of quantum states like the entanglement entropy can provide a complementary and clarifying lens on electronic behavior. One particularly useful measure that can be used to distinguish between quantum and classical sources of entanglement is the accessible entanglement, the entanglement available as a quantum resource for systems subject to conservation laws, such as fixed particle number, due to superselection rules. In this work, we introduce an algorithm and demonstrate how to compute accessible and symmetry-resolved entanglements for interacting fermion systems. This is accomplished by combining an incremental version of the swap algorithm with a recursive auxiliary field quantum Monte Carlo algorithm recently developed by the authors. We apply these tools to study the pairing and charge density waves exhibited in the paradigmatic attractive Hubbard model via entanglement. We find that the particle and spin symmetry-resolved entanglements and their related full probability distribution functions show very clear—and unique—signatures of the underlying electronic behavior even when those features are less pronounced in conventional correlation functions. Altogether, this work provides a systematic means of characterizing the entanglement within quantum systems that can grant a deeper understanding of the complicated electronic behavior that underlies quantum phase transitions and crossovers in many-body systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Strange Mesons and Gluonic Excitations

In the standard model of particle physics, the interactions between the fundamental constituents of nuclear matter, quarks and gluons, are governed by the theory of Quantum Chromodynamics (QCD). A central goal of nuclear physics is to understand how hadrons, such as protons and neutrons, are formed from these underlying quark and gluon degrees of freedom. A hadron is primarily constructed from three quarks or a quark-antiquark pair; however, the theory of QCD allows for much more exotic configurations. One of the predicted exotic configurations is known as a hybrid meson, which contains an excited gluonic field in addition to the usual quark-antiquark pair. This project aims to search for and study these gluonic excitations using the Gluonic Excitation (GlueX) experiment at Jefferson Lab in Newport News, VA. The discovery potential of the experiment will be significantly extended by studying the quark flavor composition of the meson spectrum through the completion and use of an enhanced detector to identify mesons containing strange quarks. The unprecedented statistical precision of the data collected at GlueX will allow us to search for a pattern of light-quark hybrid mesons, providing new insight into the interactions that bind the fundamental quarks and gluons into the hadrons we observe in nature.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Comparison of Spectroscopic Techniques for Determining the Peroxide Value of 19 Classes of Naturally Aged, Plant-Based Edible Oils

The peroxide value of edible oils is a measure of the degree of oxidation, which directly relates to the freshness of the oil sample. Several studies previously reported in the literature have paired various spectroscopic techniques with multivariate analyses to rapidly determine peroxide values using field portable and process instrumentation; those efforts presented “best-case scenarios” with oils from narrowly defined training and test sets. The purpose of this paper is to evaluate the use of near- and mid-infrared absorption and Raman scattering spectroscopies on oil samples from different oil classes, including seasonal and vendor variations, to determine which measurement technique or combination thereof is best for predicting peroxide values. Following peroxide value assays of each oil class using an established titration-based method, global and global-subset calibration models were constructed from spectroscopic data collected on the 19 oil classes used in this study. Spectra from each optical technique were used to create partial least squares regression calibration models to predict the peroxide value of unknown oil samples. A global peroxide value model based on near-infrared (8 mm optical path length) oil measurements produced the lowest RMSEP (4.9), followed by 24 mm optical path length near infrared (5.1), Raman (6.9) and 50 µm optical path length mid-infrared (7.3). However, it was determined that the Raman RMSEP resulted from chance correlations. Global peroxide value models based on low-level fusion of the NIR (8 and 24 mm optical path length) data and all infrared data produced the same RMSEP of 5.1. Global subset models, based on any of the spectroscopies and olive oil training sets from any class (pure, extra light, extra virgin), all failed to extrapolate to the non-olive oils. However, the near-infrared global subset model built on extra virgin olive oil could extrapolate to test samples from other olive oil classes. This work demonstrates the difficulty of developing a truly global method for determining peroxide value of oils.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Hydraulic redistribution by deeply rooted grasses and its ecohydrologic implications in the southern Great Plains of North America

Perennial bioenergy crops with deep (>1 m) rooting systems, such as switchgrass (Panicum virgatum L.), are hypothesized to increase carbon storage in deep soil. Deeply rooted plants may also affect soil hydrology by accessing deep soil water for transpiration, which can affect soil water content and infiltration in deep soil layers, thereby affecting groundwater recharge. Using stable H and O isotope (δ 2 H and δ 18 O) and 3 H values, we studied the soil water conditions at 20–30 cm intervals to depths of 2.4–3.6 m in paired fields of switchgrass and shallow rooted crops at three sites in the southern Great Plains of North America. We found that soil under switchgrass had consistently higher soil water content than nearby soil under shallow-rooted annual crops by a margin of 15%–100%. Soil water content and isotopic depth profiles indicated that hydraulic redistribution of deep soil water by switchgrass roots explained these observed soil water differences. To our knowledge, these are the first observations of hydraulic redistribution in deeply rooted grasses, and complement earlier observations of dynamic soil water fluxes under shallow-rooted grasses. Hydraulic redistribution by switchgrass may be a strategy for drought avoidance, wherein the plant may actively prevent water limitation. Furthermore, this raises the possibility that deeply rooted grasses may be used to passively subsidize soil water to more shallow-rooted species in inter-cropping arrangements.

3H↗
DOE OSTI2020

Horn Mountain Offshore Oil Field Case Study

This document is one of three offshore post-primary CO 2 enhanced oil recovery project case studies that compares the modeling results from an industry standard compositional simulator (“GEM”) and a variant of the FE/NETL CO 2 Prophet Model (CO 2 Prophet Model), which determined the CO 2 Prophet Model was able to reasonably represent the performance of the CO 2 flood modeled using the more sophisticated GEM. This case study uses the Horn Mountain oil field NFB M Sand, in the field's North fault block, using three pairs of wells. Each pair of wells is a line drive pattern design (one CO 2 injector and one production well). Four 20-year injection scenarios were assessed, varying CO 2 injector well placements. A version of the CO 2 Prophet Model is available on NETL’s website under the Collection Name: FE/NETL CO 2 Prophet Model.

02 PETROLEUM↗
DOE OSTI2022

Testing the role of AGN on the star formation and metal enrichment of ‘twin galaxies’

Here, we explore the effect of AGN activity on the star formation history of galaxies by analysing the stellar population properties of 10 pairs of nearby twin galaxies – selected as being visually similar except for the presence of an AGN. The selection of such twin samples represents a method to study AGN feedback, as recently proposed by del Moral Castro et al. We use integral field unit (IFU) data from CALIFA, stacked within three fixed apertures. AGN galaxies in a twin pair suggest more evolved stellar populations than their non-AGN counterpart 90 per cent of the time, regardless of aperture size. A comparison with a large sample from SDSS confirms that most twins are representative of the general population, but in each twin the differences between twin members is significant. A set of targeted line strengths reveal the AGN member of a twin pair is older and more metal-rich than the non-AGN galaxy, suggesting AGN galaxies in our sample may either have an earlier formation time or follow a different star formation and chemical enrichment history. These results are discussed within two simple, contrasting hypotheses for the role played by AGN in galaxy evolution, which can be tested in the future at a greater detail with the use of larger data sets.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

On the Virasoro six-point identity block and chaos

We study six-point correlation functions in two dimensional conformal field theory, where the six operators are grouped in pairs with equal conformal dimension. Assuming large central charge $c$ and a sparse spectrum, the leading contribution to this correlation function is the six-point Virasoro identity block - corresponding to each distinct pair of operators fusing into the identity and its descendants. We call this the star channel. One particular term in the star channel identity block is the stress tensor $SL(2,\mathbb{R})$ (global) block, for which we derive an explicit expression. In the holographic context, this object corresponds to a direct measure of nonlinear effects in pure gravity. We calculate additional terms in the star channel identity block that contribute at the same order at large $c$ as the global block using the novel theory of reparametrizations, which extends the shadow operator formalism in a natural way. We investigate these blocks' relevance to quantum chaos in the form of six-point scrambling in an out-of time ordered correlator. Interestingly, the global block does not contribute to the scrambling mode of this correlator, implying that, to leading order, six-point scrambling is insensitive to the three-point graviton coupling in the bulk dual. Finally, we compare our findings with a different OPE channel, called the comb channel, and find the same result for the chaos exponent in this decomposition.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

How do mirror charge radii constrain density dependence of the symmetry energy?

It has recently been suggested that differences in the charge radii of mirror nuclei (Δ$R^{mirr}_{ch}$) are strongly correlated with the neutron-skin thickness ($R_{skin}$) of neutron-rich nuclei and with the slope of the symmetry energy ($L$). To test this assumption, we present ab initio calculations of $R_{skin}$ in 48 Ca and 208 Pb, Δ$R^{mirr}_{ch}$ in 36 Ca$-$ 36 S, 38 Ca$-$ 38 Ar, 41 Sc$-$ 41 Ca, 48 Ni$-$ 48 Ca, 52 Ni$-$ 52 Cr, and 54 Ni$-$ 54 Fe mirror pairs, and $L$. Employing the recently developed 34 chiral interaction samples, identified by the history matching approach, we conduct rigorous statistical analysis of correlations among Δ$R^{mirr}_{ch}$, $R_{skin}$ and $L$, accounting for quantified uncertainties from low-energy constants of chiral interaction, chiral effective field theory truncation and many-body method approximation. The ab initio results reveal an appreciable Δ$R^{mirr}_{ch}$ $-$ $L$ correlation in $fp$-shell mirror pairs. However, contrary to previous studies, the present calculation finds that the studied $sd$-shell mirror pairs do not exhibit any Δ$R^{mirr}_{ch}$ $-$ $L$ correlation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Anyon superconductivity from topological criticality in a Hofstadter–Hubbard model

We argue that the combination of strong repulsive interactions and high magnetic fields can generate electron pairing and superconductivity. Inspired by the large lattice constants of moiré materials, which make large flux per unit cell accessible at laboratory fields, we study the triangular lattice Hofstadter-Hubbard model at one-quarter flux quantum per plaquette, where previous literature has argued that a chiral spin liquid separates a weak-coupling integer quantum Hall phase and a strong-coupling topologically trivial antiferromagnetic insulator at a density of one electron per site. We argue that topological superconductivity emerges upon doping in the vicinity of the integer quantum Hall to chiral spin liquid transition. We employ exact diagonalization and density matrix renormalization group methods to examine this theoretical scenario and find that electronic pairing indeed occurs on both sides of criticality over a remarkably broad range of interaction strengths. On the chiral spin liquid side, our results provide a concrete model realization of the long-hypothesized mechanism of anyon superconductivity. Our study thus establishes a beyond-Bardeen-Cooper-Schrieffer route to electron pairing in a well-controlled limit, relying crucially on the interplay between electron correlations and band topology.

Hubbard model↗
DOE OSTI2024

Proton deflectometry analysis in magnetized plasmas: Magnetic field reconstruction in one dimension

Proton deflectometry is used in magnetized high-energy-density plasmas to observe electromagnetic fields. Here we describe a reconstruction algorithm to recover the electromagnetic fields from proton fluence data in 1-D. The algorithm is verified against analytic solutions and applied to example data. Next, we study the role of source fluence uncertainty for 1-D reconstructions. We show that reconstruction boundary conditions can be used to constrain the source fluence profile and use this to develop a reconstruction using a specified pair of boundary conditions on the magnetic field. From these considerations, we experimentally demonstrate a hybrid mesh-fluence reconstruction technique where fields are reconstructed from fluence data in an interior region with boundary conditions supplied by direct mesh measurements at the boundary.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Topological superconductivity from forward phonon scatterings

Searching for topological superconductors with non-Abelian states has been attracting broad interest. The most commonly used recipe for building topological superconductors utilizes the proximity effect, which significantly limits the working temperature. Here, we propose a mechanism to attain topological superconductivity via forward phonon scatterings. Our crucial observation is that electron-phonon interactions with small momentum transfers favor spin-triplet Cooper pairing under an applied magnetic field. This process facilitates the formation of chiral topological superconductivity even without Rashba spin-orbit coupling. As a proof of concept, we propose an experimentally feasible heterostructure to systematically study the entangled relationship among forward-phonon scatterings, Rashba spin-orbit coupling, pairing symmetries, and the topological property of the superconducting state. This theory not only deepens our understanding of the superconductivity induced by the electron-phonon interaction but also sheds light on the critical role of the electron-phonon coupling in pursuing non-Abelian Majorana quasiparticles.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Nematicity and superconductivity: Competition versus cooperation

Electronic nematic behavior has been identified and studied in iron-based superconductors for some time, particularly in the well-known BaFe 2 As 2 system, where it is well known to compete with superconductivity. On the other hand, it has been shown recently that FeSe displays a negligible effect of nematicity on superconductivity near the superconducting transition, and actual cooperation between the two orders when the system is doped with S. Recently it has also been proposed that LiFeAs undergoes a nematic transition in the superconducting state itself. Generally, we expect superconductivity to be anisotropic when it coexists with nematic order, but it is not clear under what circumstances the two orders compete or cooperate, nor how the anisotropy of the superconducting state correlates with that in the nematic state. To address this, we study a simple mean-field model of a d-wave Pomeranchuk instability together with a mixed s,d pairing interaction, and identify when nematicity is enhanced or suppressed by superconductivity. Here, we show that the competition or cooperation depends significantly on the distortion of the Fermi surface due to nematicity relative to the anisotropy of the superconducting gap function. Further, we discuss the implications of our results for FeSe and LiFeAs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Data and scripts associated with a manuscript investigating impacts of solid phase extraction on freshwater organic matter optical signatures and mass spectrometry pairing

This data package is associated with the publication “Investigating the impacts of solid phase extraction on dissolved organic matter optical signatures and the pairing with high-resolution mass spectrometry data in a freshwater system” submitted to “Limnology and Oceanography: Methods.” This data is an extension of the River Corridor and Watershed Biogeochemistry SFA’s Spatial Study 2021 (https://doi.org/10.15485/1898914). Other associated data and field metadata can be found at the link provided. The goal of this manuscript is to assess the impact of solid phase extraction (SPE) on the ability to pair ultra-high resolution mass spectrometry data collected from SPE extracts with optical properties collected on ambient stream samples. Forty-seven samples collected from within the Yakima River Basin, Washington were analyzed dissolved organic carbon (DOC, measured as non-purgeable organic carbon, NPOC), absorbance, and fluorescence. Samples were subsequently concentrated with SPE and reanalyzed for each measurement. The extraction efficiency for the DOC and common optical indices were calculated. In addition, SPE samples were subject to ultra-high resolution mass spectrometry and compared with the ambient and SPE generated optical data. Finally, in addition to this cross-platform inter-comparison, we further performed and intra-comparison among the high-resolution mass spectrometry data to determine the impact of sample preparation on the interpretability of results. Here, the SPE samples were prepared at 40 milligrams per liter (mg/L) based on the known DOC extraction efficiency of the samples (ranging from ~30 to ~75%) compared to the common practice of assuming the DOC extraction efficiency of freshwater samples at 60%. This data package folder consists of one main data folder with one subfolder (Data_Input). The main data folder contains (1) readme; (2) data dictionary (dd); (3) file-level metadata (flmd); (4) final data summary output from processing script; and (5) the processing script. The R-markdown processing script (SPE_Manuscript_Rmarkdown_Data_Package.rmd) contains all code needed to reproduce manuscript statistics and figures (with the exception of that stated below). The Data_Input folder has two subfolders: (1) FTICR and (2) Optics. Additionally, the Data_Input folder contains dissolved organic carbon (DOC, measured as non-purgeable organic carbon, NPOC) data (SPS_NPOC_Summary.csv) and relevant supporting Solid Phase Extraction Volume information (SPS_SPE_Volumes.csv). Methods information for the optical and FTICR data is embedded in the header rows of SPS_EEMs_Methods.csv and SPS_FTICR_Methods.csv, respectively. In addition, the data dictionary (SPS_SPE_dd.csv), file level metadata (SPS_SPE_flmd.csv), and methods codes (SPS_SPE_Methods_codes.csv) are provided. The FTICR subfolder contains all raw FTICR data as well as instructions for processing. In addition, post processed FTICR molecular information (Processed_FTICRMS_Mol.csv) and sample data (Processed_FTICRMS_Data.csv) is provided that can be directly read into R with the associated R-markdown file. The Optics subfolder contains all Absorbance and Fluorescence Spectra. Fluorescence spectra have been blank corrected, inner filter corrected, and undergone scatter removal. In addition, this folder contains Matlab code used to make a portion of Figure 1 within the manuscript, derive various spectral parameters used within the manuscript, and used for parallel factor analysis (PARAFAC) modeling. Spectral indices (SPS_SpectralIndices.csv) and PARAFAC outputs (SPS_PARAFAC_Model_Loadings.csv and SPS_PARAFAC_Sample_Scores.csv) are directly read into the associated R-markdown file. We acknowledge the Yakama Nation as owners and caretakers of the lands where we collected some of these data. We thank the Confederated Tribes and Bands of the Yakama Nation Tribal Council and Yakama Nation Fisheries for working with us to facilitate sample collection and optimization of data usage according to their values and worldview.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Understanding the nature of mean-field semiclassical light-matter dynamics: An investigation of energy transfer, electron-electron correlations, external driving, and long-time detailed balance

Semiclassical electrodynamics (with quantum matter plus classical electrodynamics fields) is an appealing approach for studying light-matter interactions, especially for realistic molecular systems. However, there is no unique semiclassical scheme. On the one hand, intermolecular interactions can be described instantaneously by static two-body interactions connecting two different molecules, while a classical transverse E field acts as a spectator at short distance; we will call this Hamiltonian no. I. On the other hand, intermolecular interactions can also be described as effects that are mediated exclusively through a classical one-body Ε field without any quantum effects at all (assuming we ignore electronic exchange); we will call this Hamiltonian no. II. Moreover, one can also mix these two different Hamiltonians into a third, hybrid Hamiltonian, which preserves quantum electron-electron correlations for lower excitations but describes higher excitations in a mean-field way. To investigate which semiclassical scheme is most reliable for practical use, here we study the real-time dynamics of a minimalistic many-site model—a pair of identical two-level systems (TLSs)—undergoing either resonance energy transfer (RET) or collectively driven dynamics. While both approaches (no. 1 and no. 2) perform reasonably well when there is no strong external excitation, we find that no single approach is perfect for all conditions (and all methods fail when a strong external field is applied). Each method has its own distinct problems: Hamiltonian no. I performs best for RET but behaves in a complicated manner for driven dynamics; Hamiltonian no. II is always stable, but obviously fails for RET at short distances. One key finding is that, for externally driven dynamics, a full configuration-interaction description of Hamiltonian no. I strongly overestimates the long-time electronic energy, highlighting the not obvious fact that, if one plans to merge quantum molecules with classical light, a full, exact treatment of electron-electron correlations can actually lead to worse results than a simple mean-field electronic structure treatment. Future work will need to investigate (i) how these algorithms behave in the context of more than a pair of TLSs and (ii) whether or not these algorithms can be improved in general by including crucial aspects of spontaneous emission.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗