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All sourcesNASA NTRSDOE OSTI
NASA NTRS1982

A bootstrap approach to bump hunting

An important question in cluster analysis and pattern recognition is the determination of the number of clusters into which a given population should be divided. Frequently, particularly when certain specific clustering methods are being used, the number of clusters is taken to be equal to the number of modes, or local maxima, in the probability density function underlying the given data set. The use of kernal density estimates in mode estimation is discussed. The test statistic to be used is defined and a bootstrap technique for assessing significance is given. An illustrative application is followed by an examination of the asymptotic behavior of the test statistic.

Silverman, B. W.↗
NASA NTRS1986

On statistical searches for filaments

The presence or absence of an excess of filamentary structure in the galaxy distribution has important implications for the origin of such structure. In an attempt to answer this question, many statistics have been devised to quantify the visual impression of filaments seen in galaxy maps, but few of these are at all well understood. Two of these, a quadrupole elongation statistic and a nearest-neighbor alignment statistic, are analyzed in the common language of the irreducible N-point correlation functions of the galaxy distribution, and it is argued that there has as yet been no success in isolating filaments in particular from clustering in general.

Fry, J. N.↗
NASA NTRS2020

Overview and Status of EXCLAIM, the Experiment for Cryogenic Large-Aperture Intensity Mapping

The EXperiment for Cryogenic Large-Aperture Intensity Mapping (EXCLAIM) is a balloon-borne far-infrared telescope that will survey star formation history over cosmological time scales to improve our un-derstanding of why the star formation rate declined at redshiftz <2, despite continued clustering of darkmatter. Specifically, EXCLAIM will map the emission of redshifted carbon monoxide and singly ionized carbon lines in windows over a redshift range0< z <3.5, following an innovative approach known asintensity mapping. Intensity mapping measures the statistics of brightness fluctuations of cumulative lineemissions, as opposed to detecting individual galaxies, thus enabling a blind, complete census of the emittinggas. To detect this emission unambiguously, EXCLAIM will cross-correlate with a rich spectroscopic galaxycatalog. The EXCLAIM mission will use a cryogenic design to cool the telescope optics to approximately1.7K. The telescope will feature a90-cm primary mirror to probe spatial scales on the sky from the linearregime up to shot-noise-dominated scales. The telescope optical elements will couple to six μ-Spec spectrom-eter modules, operating over a420–540-GHz frequency band with a spectral resolution of512and featuringMicrowave Kinetic Inductance Detectors (MKIDs). In the baseline design, the detectors will be read out witha Radio Frequency System-on-Chip (RFSoC). The cryogenic telescope and the sensitive detectors will allowEXCLAIM to reach high sensitivity in spectral windows of low emission in the upper atmosphere. Here, anoverview of the mission design and development status since the start of the EXCLAIM project in early 2019 is presented.

Giuseppe Cataldo↗
NASA NTRS1993

Testing higher-order Lagrangian perturbation theory against numerical simulation. 1: Pancake models

We present results showing an improvement of the accuracy of perturbation theory as applied to cosmological structure formation for a useful range of quasi-linear scales. The Lagrangian theory of gravitational instability of an Einstein-de Sitter dust cosmogony investigated and solved up to the third order is compared with numerical simulations. In this paper we study the dynamics of pancake models as a first step. In previous work the accuracy of several analytical approximations for the modeling of large-scale structure in the mildly non-linear regime was analyzed in the same way, allowing for direct comparison of the accuracy of various approximations. In particular, the Zel'dovich approximation (hereafter ZA) as a subclass of the first-order Lagrangian perturbation solutions was found to provide an excellent approximation to the density field in the mildly non-linear regime (i.e. up to a linear r.m.s. density contrast of sigma is approximately 2). The performance of ZA in hierarchical clustering models can be greatly improved by truncating the initial power spectrum (smoothing the initial data). We here explore whether this approximation can be further improved with higher-order corrections in the displacement mapping from homogeneity. We study a single pancake model (truncated power-spectrum with power-spectrum with power-index n = -1) using cross-correlation statistics employed in previous work. We found that for all statistical methods used the higher-order corrections improve the results obtained for the first-order solution up to the stage when sigma (linear theory) is approximately 1. While this improvement can be seen for all spatial scales, later stages retain this feature only above a certain scale which is increasing with time. However, third-order is not much improvement over second-order at any stage. The total breakdown of the perturbation approach is observed at the stage, where sigma (linear theory) is approximately 2, which corresponds to the onset of hierarchical clustering. This success is found at a considerable higher non-linearity than is usual for perturbation theory. Whether a truncation of the initial power-spectrum in hierarchical models retains this improvement will be analyzed in a forthcoming work.

Buchert, T.↗
NASA NTRS2014

The Contribution of z < or Approx. 6 Sources to the Spatial Coherence in the Unresolved Cosmic Near-Infrared and X-Ray Backgrounds

A spatial clustering signal has been established in Spitzer/IRAC measurements of the unresolved cosmic near-infrared background (CIB) out to large angular scales, approx. 1deg. This CIB signal, while significantly exceeding the contribution from the remaining known galaxies, was further found to be coherent at a highly statistically significant level with the unresolved soft cosmic X-ray background (CXB). This measurement probes the unresolved CXB to very faint source levels using deep near-IR source subtraction.We study contributions from extragalactic populations at low to intermediate redshifts to the measured positive cross-power signal of the CIB fluctuations with the CXB. We model the X-ray emission from active galactic nuclei (AGNs), normal galaxies, and hot gas residing in virialized structures, calculating their CXB contribution including their spatial coherence with all infrared emitting counterparts. We use a halo model framework to calculate the auto and cross-power spectra of the unresolved fluctuations based on the latest constraints of the halo occupation distribution and the biasing of AGNs, galaxies, and diffuse emission. At small angular scales (1), the 4.5microns versus 0.5-2 keV coherence can be explained by shot noise from galaxies and AGNs. However, at large angular scales (approx.10), we find that the net contribution from the modeled populations is only able to account for approx. 3% of the measured CIB×CXB cross-power. The discrepancy suggests that the CIB×CXB signal originates from the same unknown source population producing the CIB clustering signal out to approx. 1deg.

unresolved cosmic near infrared background (CIB)↗
NASA NTRS1994

The metallicity of M4: Accurate spectroscopic fundamental parameters for four giants

High-quality spectra, covering the wavelength range 5480 to 7080 A, have been obtained for four giant stars in the intermediate-metallicity CN-bimodal globular cluster M4 (NGC 6121). We have employed a model atmosphere analysis that is entirely independent from cluster parameters, such as distance, age, and reddening, in order to derive accurate values for the stellar parameters effective temperature, surface gravity, and microturbulence, and for the abundance of iron relative to the Sun, (Fe/H), and of calcium, Ca/H, for each of the four stars. Detailed radiative transfer and statistical equilibrium calculations carried out for iron and calcium suggest that departures from local thermodynamic equilibrium are not significant for the purposes of our analysis. The spectroscopically derived effective temperatures for our program stars are hotter by about 200 K than existing photometric calibrations suggest. We conclude that this is due partly to the uncertain reddening of M4 and to the existing photometric temperature calibration for red giants being too cool by about 100 K. Comparison of our spectroscopic and existing photometric temperatures supports the prognosis of a significant east-west gradient in the reddening across M4. Our derived iron abundances are slightly higher than previous high-resolution studies suggested; the differences are most probably due to the different temperature scale and choice of microturbulent velocities adopted by earlier workers. The resulting value for the metallicity of M4 is (Fe/H )(sub M4) = -1.05 + or - 0.15. Based on this result, we suggest that metallicities derived in previous high-dispersion globular cluster abundance analyses could be too low by 0.2 to 0.3 dex. Our calcium abundances suggest an enhancement of calcium, an alpha element, over iron, relative to the Sun, in M4 of (Ca/H) = 0.23.

Drake, J. J.↗
DOE OSTI2023

Linear growth of circuit complexity from Brownian dynamics

How rapidly can a many-body quantum system generate randomness? Using path integral methods, we demonstrate that Brownian quantum systems have circuit complexity that grows linearly with time. In particular, we study Brownian clusters of N spins or fermions with time-dependent all-to-all interactions, and calculate the Frame Potential to characterize complexity growth in these models. In both cases the problem can be mapped to an effective statistical mechanics problem which we study using path integral methods. Within this framework it is straightforward to show that the kth Frame Potential comes within ϵ of the Haar value after a time of order t ~ kN + k log k + log ϵ –1 . Using a bound on the diamond norm, this implies that such circuits are capable of coming very close to a unitary k-design after a time of order t ~ kN. We also consider the same question for systems with a time-independent Hamiltonian and argue that a small amount of time-dependent randomness is sufficient to generate a k-design in linear time provided the underlying Hamiltonian is quantum chaotic. These models provide explicit examples of linear complexity growth that are analytically tractable and are directly applicable to practical applications calling for unitary k-designs.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
NASA NTRS1985

The evolution of large-scale structure in a universe dominated by cold dark matter

The results of numerical simulations of nonlinear gravitational clustering in universes dominated by weakly interacting, 'cold' dark matter are presented. The numerical methods used and the way in which initial conditions were generated are described, and the simulations performed are catalogued. The evolution of the fundamental statistical properties of the models is described and their comparability with observation is discussed. Graphical comparisons of these open models with the observed galaxy distribution in a large redshift survey are made. It is concluded that a model with a cosmological density parameter omega equal to one is quite unacceptable if galaxies trace the mass distribution, and that models with omega of roughly two, while better, still do not provide a fully acceptable match with observation. Finally, a situation in which galaxy formation is suppressed except in sufficiently dense regions is modelled which leads to models which can agree with observation quite well even for omega equal to one.

Davis, M.↗
NASA NTRS2014

Spatiotemporal Organization of Energy Release Events in the Quiet Solar Corona

Using data from the STEREO and SOHO spacecraft, we show that temporal organization of energy release events in the quiet solar corona is close to random, in contrast to the clustered behavior of flaring times in solar active regions. The locations of the quiet-Sun events follow the meso- and supergranulation pattern of the underling photosphere. Together with earlier reports of the scale-free event size statistics, our findings suggest that quiet solar regions responsible for bulk coronal heating operate in a driven self-organized critical state, possibly involving long-range Alfvenic interactions.

sun activity↗
DOE OSTI2022

Long- and short-term temporal variability in cloud condensation nuclei spectra over a wide supersaturation range in the Southern Great Plains site

Abstract. When aerosol particles seed the formation of liquid water droplets in the atmosphere, they are called cloud condensation nuclei (CCN). Different aerosols will act as CCN under different degrees of water supersaturation (relative humidity above 100 %), depending on their size and composition. In this work, we build and analyze a best-estimate CCN spectrum product, tabulated at ∼ 45 min resolution, generated using high quality data from seven independent instruments at the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) Southern Great Plains site. The data product spans a large supersaturation range, from 0.0001 % to ∼ 30 %, and time period of 5 years, from 2009–2013, and is available on the ARM data archive. We leverage this added statistical power to examine relationships that are unclear in smaller datasets. Our analysis is performed in three main areas. First, probability distributions of many aerosol and CCN metrics are found to exhibit skewed log-normal distribution shapes. Second, clustering analyses of CCN spectra reveal that the primary drivers of CCN differences are aerosol number size distributions, rather than hygroscopicity or composition, especially at supersaturations above 0.2 %, while also allowing for a simplified understanding of seasonal and diurnal variations in CCN behavior. The predictive ability of using limited hygroscopicity data with accurate number size distributions to estimate CCN spectra is investigated, and the uncertainties of this approach are estimated. Third, the dynamics of CCN spectral clusters and concentrations are examined with cross-correlation and autocorrelation analyses. We find that CCN concentrations change rapidly on the timescale of 1–3 h, with some conservation beyond that which is greatest for the lower supersaturation region of the spectrum.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1994

Stellar density enhancements associated with IRAS sources in L1641

We obtained H and K' images of 59 Infrared Astronomical Satellite (IRAS) sources associated with dense molecular gas in L1641. Some of the sources were also imaged in narrow-band L and M. Using these near-IR images and photometry, we are able to identify the near-IR counterparts for most of the IRAS sources. The spectral energy distributions of the sources suggest that all of them are young stellar objects (class I and II sources). Most importantly, we find in this study that 14 IRAS sources are associated with small (but statistically significant) groupings of bright near-IR sources defined as stellar density enhancements (SDEs). The spatial distribution of young stars in the Orion A molecular cloud can be characterized by a range of stellar densities, from the Trapezium Cluster, to the SDEs, to individual stars. We conjecture that the SDEs are regions of continuous star formation within or around dense molecular cores and that they may represent an important mode of star formation in L1641. If true, adjustments to the standard star formation model may be required.

Chen, Hua↗
NASA NTRS2012

Calculation of the Frequency Distribution of the Energy Deposition in DNA Volumes by Heavy Ions

Radiation quality effects are largely determined by energy deposition in small volumes of characteristic sizes less than 10 nm representative of short-segments of DNA, the DNA nucleosome, or molecules initiating oxidative stress in the nucleus, mitochondria, or extra-cellular matrix. On this scale, qualitatively distinct types of molecular damage are possible for high linear energy transfer (LET) radiation such as heavy ions compared to low LET radiation. Unique types of DNA lesions or oxidative damages are the likely outcome of the energy deposition. The frequency distribution for energy imparted to 1-20 nm targets per unit dose or particle fluence is a useful descriptor and can be evaluated as a function of impact parameter from an ions track. In this work, the simulation of 1-Gy irradiation of a cubic volume of 5 micron by: 1) 450 (1)H(+) ions, 300 MeV; 2) 10 (12)C(6+) ions, 290 MeV/amu and 3) (56)Fe(26+) ions, 1000 MeV/amu was done with the Monte-Carlo simulation code RITRACKS. Cylindrical targets are generated in the irradiated volume, with random orientation. The frequency distribution curves of the energy deposited in the targets is obtained. For small targets (i.e. <25 nm size), the probability of an ion to hit a target is very small; therefore a large number of tracks and targets as well as a large number of histories are necessary to obtain statistically significant results. This simulation is very time-consuming and is difficult to perform by using the original version of RITRACKS. Consequently, the code RITRACKS was adapted to use multiple CPU on a workstation or on a computer cluster. To validate the simulation results, similar calculations were performed using targets with fixed position and orientation, for which experimental data are available [5]. Since the probability of single- and double-strand breaks in DNA as function of energy deposited is well know, the results that were obtained can be used to estimate the yield of DSB, and can be extended to include other targeted or non-target effects.

Plante, Ianik↗
NASA NTRS2014

Investigation of Spiral Bevel Gear Condition Indicator Validation Via AC-29-2C Using Damage Progression Tests

This report documents the results of spiral bevel gear rig tests performed under a NASA Space Act Agreement with the Federal Aviation Administration (FAA) to support validation and demonstration of rotorcraft Health and Usage Monitoring Systems (HUMS) for maintenance credits via FAA Advisory Circular (AC) 29-2C, Section MG-15, Airworthiness Approval of Rotorcraft (HUMS) (Ref. 1). The overarching goal of this work was to determine a method to validate condition indicators in the lab that better represent their response to faults in the field. Using existing in-service helicopter HUMS flight data from faulted spiral bevel gears as a "Case Study," to better understand the differences between both systems, and the availability of the NASA Glenn Spiral Bevel Gear Fatigue Rig, a plan was put in place to design, fabricate and test comparable gear sets with comparable failure modes within the constraints of the test rig. The research objectives of the rig tests were to evaluate the capability of detecting gear surface pitting fatigue and other generated failure modes on spiral bevel gear teeth using gear condition indicators currently used in fielded HUMS. Nineteen final design gear sets were tested. Tables were generated for each test, summarizing the failure modes observed on the gear teeth for each test during each inspection interval and color coded based on damage mode per inspection photos. Gear condition indicators (CI) Figure of Merit 4 (FM4), Root Mean Square (RMS), +/- 1 Sideband Index (SI1) and +/- 3 Sideband Index (SI3) were plotted along with rig operational parameters. Statistical tables of the means and standard deviations were calculated within inspection intervals for each CI. As testing progressed, it became clear that certain condition indicators were more sensitive to a specific component and failure mode. These tests were clustered together for further analysis. Maintenance actions during testing were also documented. Correlation coefficients were calculated between each CI, component, damage state and torque. Results found test rig and gear design, type of fault and data acquisition can affect CI performance. Results found FM4, SI1 and SI3 can be used to detect macro pitting on two more gear or pinion teeth as long as it is detected prior to progressing to other components or transitioning to another failure mode. The sensitivity of RMS to system and operational conditions limit its reliability for systems that are not maintained at steady state. Failure modes that occurred due to scuffing or fretting were challenging to detect with current gear diagnostic tools, since the damage is distributed across all the gear and pinion teeth, smearing the impacting signatures typically used to differentiate between a healthy and damaged tooth contact. This is one of three final reports published on the results of this project. In the second report, damage modes experienced in the field will be mapped to the failure modes created in the test rig. The helicopter CI data will then be re-processed with the same analysis techniques applied to spiral bevel rig test data. In the third report, results from the rig and helicopter data analysis will be correlated. Observations, findings and lessons learned using sub-scale rig failure progression tests to validate helicopter gear condition indicators will be presented.

gears↗
NASA NTRS2016

Landslides in West Coast Metropolitan Areas: The Role of Extreme Weather Events

Rainfall-induced landslides represent a pervasive issue in areas where extreme rainfall intersects complex terrain. A farsighted management of landslide risk requires assessing how landslide hazard will change in coming decades and thus requires, inter alia, that we understand what rainfall events are most likely to trigger landslides and how global warming will affect the frequency of such weather events. We take advantage of 9 years of landslide occurrence data compiled by collating Google news reports and of a high-resolution satellite-based daily rainfall data to investigate what weather triggers landslide along the West Coast US. We show that, while this landslide compilation cannot provide consistent and widespread monitoring everywhere, it captures enough of the events in the major urban areas that it can be used to identify the relevant relationships between landslides and rainfall events in Puget Sound, the Bay Area, and greater Los Angeles. In all these regions, days that recorded landslides have rainfall distributions that are skewed away from dry and low-rainfall accumulations and towards heavy intensities. However, large daily accumulation is the main driver of enhanced hazard of landslides only in Puget Sound. There, landslide are often clustered in space and time and major events are primarily driven by synoptic scale variability, namely "atmospheric rivers" of high humidity air hitting anywhere along the West Coast, and the interaction of frontal system with the coastal orography. The relationship between landslide occurrences and daily rainfall is less robust in California, where antecedent precipitation (in the case of the Bay area) and the peak intensity of localized downpours at sub-daily time scales (in the case of Los Angeles) are key factors not captured by the same-day accumulations. Accordingly, we suggest that the assessment of future changes in landslide hazard for the entire the West Coast requires consideration of future changes in the occurrence and intensity of atmospheric rivers, in their duration and clustering, and in the occurrence of short-duration (sub-daily) extreme rainfall as well. Major regional landslide events, in which multiple occurrences are recorded in the catalog for the same day, are too rare to allow a statistical characterization of their triggering events, but a case study analysis indicates that a variety of synoptic-scale events can be involved, including not only atmospheric rivers but also broader cold- and warm-front precipitation. That a news-based catalog of landslides is accurate enough to allow the identification of different landslide/ rainfall relationships in the major urban areas along the US West Coast suggests that this technology can potentially be used for other English-language cities and could become an even more powerful tool if expanded to other languages and non-traditional news sources, such as social media.

landslides↗
DOE OSTI2023

Mechanism of Stoichiometrically Governed Titanium Oxide Brownian Tree Formation on Stepped Au(111)

Previously observed formation of substoichiometric titanium oxide dendritic structures across terraces of Au(111) is computationally studied and shown to follow the classical fractal formation mechanism of diffusion-limited aggregation (DLA). Globally optimized gas-phase oxide cluster structures are sampled in a variety of landing formations on gold surfaces and shown to favor isomers driving polymerization to Brownian tree fractal structures. Mobility of Ti 3 O 5 monomers is shown to be extremely high, with diffusion barriers of 0.21 eV or less. Through bonding stabilization, polymerization of these monomers is energetically favorable and irreversible on the 111 terrace but geometrically impossible to propagate along the step edge. Simulated scanning tunneling microscopy (STM) images show strong similarity to experiment. By contrast, observation of Ti 3 O 6 aggregating as wires along step edges is explained by the affinity of oxygen to step edges and statistical arguments for aggregation entropy at the step, in addition to low barriers for monomer diffusion and polymerization.

36 MATERIALS SCIENCE↗
NASA NTRS2019

Statistical Hypothesis Testing in Wavelet Analysis: Theoretical Developments and Applications to Indian Rainfall

Statistical hypothesis tests in wavelet analysis are methods that assess the degree to which a wavelet quantity(e.g., power and coherence) exceeds background noise. Commonly, a point-wise approach is adopted in which a wavelet quantity at every point in a wavelet spectrum is individually compared to the critical level of the point-wise test. However, because adjacent wavelet coefficients are correlated and wavelet spectra often contain many wavelet quantities, the point-wise test can produce many false positive results that occur in clusters or patches. To circumvent the point-wise test drawbacks, it is necessary to implement the recently developed area-wise, geometric, cumulative area-wise, and topological significance tests, which are reviewed and developed in this paper. To improve the computational efficiency of the cumulative area-wise test, a simplified version of the testing procedure is created based on the idea that its output is the mean of individual estimates of statistical significance calculated from the geometric test applied at a set of point-wise significance levels. Ideal examples are used to show that the geometric and cumulative area-wise tests are unable to differentiate wavelet spectral features arising from singularity-like structures from those associated with periodicities. A cumulative arc-wise test is therefore developed to strictly test for periodicities by using normalized arc length, which is defined as the number of points composing a cross section of a patch divided by the wavelet scale in question. A previously proposed topological significance test is formalized using persistent homology profiles (PHPs) measuring the number of patches and holes corresponding to the set of all point-wise significance values. Ideal examples show that the PHPs can be used to distinguish time series containing signal components from those that are purely noise. To demonstrate the practical uses of the existing and newly developed statistical methodologies, a first comprehensive wavelet analysis of Indian rainfall is also provided. An R software package has been written by the author to implement the various testing procedures.

Wind speed↗
NASA NTRS2002

Companions to isolated elliptical galaxies: revisiting the Bothun-Sullivan (1977) sample using the NASA/IPAC extragalactic database

We investigate the number of physical companion galaxies for a sample of relatively isolated elliptical galaxies. The NASA/IPAC Extragalactic Database (NED) has been usedto reinvestigate the incidence of satellite galaxies for a sample of 34 elliptical galaxies, firstinvestigated by Bothun & Sullivan (1977) using a visual inspection of Palomar Sky Survey prints out to a projected search radius of 75 kpc. We have repeated their original investigation usingdata cataloged data in NED. Nine of these ellipticals appear to be members of galaxy clusters:the remaining sample of 25 galaxies reveals an average of +1.0 f 0.5 apparent companions per galaxy within a projected search radius of 75 kpc, in excess of two equal-area comparisonregions displaced by 150-300 kpc. This is nearly an order of magnitude larger than the +0.12+/- 0.42 companions/galaxy found by Bothun & Sullivan for the identical sample. Making use of published radial velocities, mostly available since the completion of the Bothun-Sullivan study,identifies the physical companions and gives a somewhat lower estimate of +0.4 companions per elliptical. This is still a factor of 3x larger than the original statistical study, but giventhe incomplete and heterogeneous nature of the survey redshifts in NED, it still yields a firmlower limit on the number (and identity) of physical companions. An expansion of the searchradius out to 300 kpc, again restricted to sampling only those objects with known redshifts in NED, gives another lower limit of 4.3 physical companions per galaxy. (Excluding fiveelliptical galaxies in the Fornax cluster this average drops to 3.5 companions per elliptical.)These physical companions are individually identified and listed, and the ensemble-averagedradial density distribution of these associated galaxies is presented. For the ensemble, the radial density distribution is found to have a fall-off consistent with p c( R^-0.5 out to approximately150 kpc. For non-Fornax cluster companions the fall-off continues out to the 300-kpc limit of thesurvey. The velocity dispersion of these companions is found to be constant with projected radial distance from the central elliptical, holding at a value of approximately +/- 300-350 km/sec overall.

NED NASA/IPAC Extragalactic Database↗
DOE OSTI2022

Transferability of data-driven, many-body models for CO 2 simulations in the vapor and liquid phases

Here, extending on the previous work by Riera et al. [J. Chem. Theory Comput. 16, 2246–2257 (2020)], we introduce a second generation family of data-driven many-body MB-nrg models for CO 2 and systematically assess how the strength and anisotropy of the CO 2 –CO 2 interactions affect the models’ ability to predict vapor, liquid, and vapor–liquid equilibrium properties. Building upon the many-body expansion formalism, we construct a series of MB-nrg models by fitting one-body and two-body reference energies calculated at the coupled cluster level of theory for large monomer and dimer training sets. Advancing from the first generation models, we employ the charge model 5 scheme to determine the atomic charges and systematically scale the two-body energies to obtain more accurate descriptions of vapor, liquid, and vapor–liquid equilibrium properties. Challenges in model construction arise due to the anisotropic nature and small magnitude of the interaction energies in CO 2 , calling for the necessity of highly accurate descriptions of the multidimensional energy landscape of liquid CO 2 . These findings emphasize the key role played by the training set quality in the development of transferable, data-driven models, which, accurately representing high-dimensional many-body effects, can enable predictive computer simulations of molecular fluids across the entire phase diagram.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗