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DOE OSTI2025

Visible-light H 2 evolution using dye-sensitized TiO 2 : effects of physicochemical properties of TiO 2 on excited carrier dynamics and activity

Dye-sensitized photocatalysts have emerged as promising materials for solar-driven water splitting due to their ability to utilize visible light, in contrast to conventional wide-band-gap semiconductors. However, the relationship between semiconductor properties and charge carrier dynamics remains insufficiently understood. In this study, we investigated Pt/TiO 2 systems sensitized with a visible-light-absorbing Ru(II) polypyridyl complex (RuP), focusing on how the crystal phase and specific surface area of TiO 2 influence excited carrier dynamics and H 2 evolution activity. To isolate the effects of TiO 2 properties, Pt and RuP loadings were standardized across samples. Emission lifetime analysis showed similarly efficient electron injection from RuP to TiO 2 in all cases, suggesting that injection efficiency does not account for observed differences in activity. Transient absorption measurements revealed that back electron transfer (BET) rates depended strongly on the TiO 2 phase, with anatase and P25 exhibiting slower BET and higher activity for H 2 evolution than rutile. The highest apparent quantum yield for H 2 evolution was 12.0% at 450 nm. Among anatase samples, larger surface areas correlated with higher activity, while smaller-area samples exhibited slower BET rates but still low H 2 evolution activity, implying a role for RuP dye–dye interactions in performance loss. This was further supported by improvements in H 2 evolution activity by lowering RuP loading or adding co-adsorbents. Overall, these results demonstrate that both BET suppression and control over RuP dye aggregation are essential for designing efficient dye-sensitized photocatalytic systems.

Harada, Kakeru [Institute of Science Tokyo (Japan)↗
DOE OSTI2024

Perturbative quantum evolution of the gravitational state and dressing in general backgrounds

This paper sets up a perturbative treatment of the evolving quantum state of a gravitational system, in a Schrödinger-like picture, working about a general background. This connects gauge symmetry, the constraints, gravitational dressing, and evolution. Starting with a general time slicing, we give a simple derivation of the relation between the constraints, the Hamiltonian, and its well-known boundary term. Among different approaches to quantization with constraints, we focus on a “gauge-invariant canonical quantization,” which is developed perturbatively in the gravitational coupling. The leading-order solution of the constraints (including the Wheeler-DeWitt equation) for perturbations about the background is given in terms of an explicit construction of gravitational dressings built using certain generalized Green’s functions; different such dressings corresponding to adding propagating gravitational waves to a particular solution of the constraints. Dressed operators commute with the constraints, expressing their gauge invariance, and have an algebraic structure differing significantly from the undressed operators of the underlying field theory. These operators can act on the vacuum to create dressed states, and evolution of general such states is then generated by the boundary Hamiltonian, and alternately may be characterized using other relational observables. This provides a concrete approach to studying perturbative time evolution, including the leading gravitational backreaction, of quantum states of black holes with flat or anti–de-Sitter asymptotics, for example on horizon-crossing slices. This description of evolution in turn provides a starting point for investigating possibly important corrections to quantum evolution, that go beyond quantized general relativity. Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Adiabatic quantum imaginary time evolution

We introduce an adiabatic state preparation protocol which implements quantum imaginary time evolution under the Hamiltonian of the system. Unlike the original quantum imaginary time evolution algorithm, adiabatic quantum imaginary time evolution does not require quantum state tomography during its runtime and, unlike standard adiabatic state preparation, the final Hamiltonian is not the system Hamiltonian. Instead, the algorithm obtains the adiabatic Hamiltonian by integrating a classical differential equation that ensures that one follows the imaginary time evolution state trajectory. We introduce some heuristics that allow this protocol to be implemented on quantum architectures with limited resources. We explore the performance of this algorithm via classical simulations in a one-dimensional spin model and highlight essential features that determine its cost, performance, and implementability for longer times, and compare to the original quantum imaginary time evolution for ground-state preparation. More generally, our algorithm expands the range of states accessible to adiabatic state preparation methods beyond those that are expressed as ground states of simple explicit Hamiltonians. Published by the American Physical Society 2024

Hejazi, Kasra (ORCID:000000032349478X)↗
DOE OSTI2024

Development of a MOOSE-based crystal plasticity model with irradiation defect evolution for irradiation creep in 316

Irradiation creep and irradiation swelling are two of the lifetime limiting factors for structural materials in nuclear reactors. These mechanical effects are driven by irradiation defect evolution and the interaction of those defects with dislocations in the microstructure. We present here a coupled cluster dynamics – crystal plasticity approach to model irradiation swelling and creep behavior in 316 SS. The time-dependent evolution of irradiation defects is calculated with a cluster dynamics approach and passed to the crystal plasticity model to compute the dislocation evolution. We show the impact of the irradiation defect evolution on the stress state in the material, which drives inelastic deformation through dislocation motion. The inelastic deformation in the 316 SS is dependent on the dose rate, where the inelastic deformation driven by the early-stage irradiation defect evolution determines the mechanical behavior of the 316 SS.

316 Stainless Steels↗
NASA NTRS1978

Lunar initial Nd-143/Nd-144 - Differential evolution of the lunar crust and mantle

The Sm-Nd evolution of Apollo 15 green glass is discussed. The ICE age (intercept with chondritic evolution) of 3.8 + or - 0.4 eons overlaps the range of reported (Ar-39)-(Ar-40) ages and implies a distinct source region for green glass, characterized by very low and unfractionated REE abundances. Evidence is presented that LINd (lunar initial Nd) is compatible with a 'chondritic'-type Nd isotopic evolution as observed in the Juvinas meteorite. This normalization is used to study the Sm-Nd system of various lunar rock types. The results obtained from a limited number of rocks clearly indicate differential Sm-Nd evolution for the lunar crust and mantle. High-Ti basalts returned by the Apollo 11 and 17 missions were derived from distinct source regions. The Nd-143 evolution in KREEP requires a source region which is clearly distinct from any mantle reservoir.

Lugmair, G. W.↗
NASA NTRS1981

Organic chemical evolution

The course of organic chemical evolution preceding the emergence of life on earth is discussed based on evidence of processes occurring in interstellar space, the solar system and the primitive earth. Following a brief review of the equilibrium condensation model for the origin and evolution of the solar system, consideration is given to the nature and organic chemistry of interstellar clouds, comets, Jupiter, meteorites, Venus and Mars, and the prebiotic earth. Major issues to be resolved in the study of organic chemical evolution on earth are identified regarding condensation and accretion in the solar nebula, early geological evolution, the origin and evolution of the atmosphere, organic production rates, organic-inorganic interactions, environmental fluctuations, phase separation and molecular selectivity.

Chang, S.↗
NASA NTRS1983

Chemical evolution and the origin of life

A review is presented of recent advances made in the understanding of the formation of carbon compounds in the universe and the occurrence of processes of chemical evolution. Topics discussed include the principle of evolutionary continuity, evolution as a fundamental principle of the physical universe, the nuclear synthesis of biogenic elements, organic cosmochemistry and interstellar molecules, the solar nebula and the solar system in chemical evolution, the giant planets and Titan in chemical evolution, and comets and their interaction with the earth. Also examined are carbonaceous chondrites, environment of the primitive earth, energy sources available on the primitive earth, the synthesis of biochemical monomers and oligomers, the abiotic transcription of nucleotides, unified prebiotic and enzymatic mechanisms, phospholipids and membranes, and protobiological evolution.

Oro, J.↗
NASA NTRS1985

Evolution of the luminosity function of extragalactic objects

A nonparametric procedure for determination of the evolution of the luminosity function of extragalactic objects and use of this for prediction of expected redshift and luminosity distribution of objects is described. The relation between this statistical evolution of the population and their physical evolution, such as the variation with cosmological epoch of their luminosity and formation rate is presented. This procedure when applied to a sample of optically selected quasars with redshifts less than two shows that the luminosity function evolves more strongly for higher luminosities, indicating a larger quasar activity at earlier epochs and a more rapid evolution of the objects during their higher luminosity phases. It is also shown that absence of many quasars at redshifts greater than three implies slowing down of this evolution in the conventional cosmological models, perhaps indicating that this is near the epoch of the birth of the quasar (and galaxies).

Petrosian, V.↗
NASA NTRS1988

The isotopic and chemical evolution of planets: Mars as a missing link

The study of planetary bodies has advanced to a stage where it is possible to contemplate general models for the chemical and physical evolution of planetary interiors, which might be referred to as UMPES (Unified Models of Planetary Evolution and Structure). UMPES would be able to predict the internal evolution and structure of a planet given certain input parameters such as mass, distance from the sun, and a time scale for accretion. Such models are highly dependent on natural observations because the basic material properties of planetary interiors, and the processes that take place during the evolution of planets are imperfectly understood. The idea of UMPES was particularly unrealistic when the only information available was from the earth. However, advances have been made in the understanding of the general aspects of planetary evolution now that there is geochemical and petrological data available for the moon and for meteorites.

Depaolo, D. J.↗
NASA NTRS1988

MEVTV Workshop on Early Tectonic and Volcanic Evolution of Mars

Although not ignored, the problems of the early tectonic and volcanic evolution of Mars have generally received less attention than those later in the evolution of the planet. Specifically, much attention was devoted to the evolution of the Tharsis region of Mars and to the planet itself at the time following the establishment of this major tectonic and volcanic province. By contrast, little attention was directed at fundamental questions, such as the conditions that led to the development of Tharsis and the cause of the basic fundamental dichotomy of the Martian crust. It was to address these and related questions of the earliest evolution of Mars that a workshop was organized under the auspices of the Mars: Evolution of Volcanism, Tectonism, and Volatiles (MEVTV) Program. Four sessions were held: crustal dichotomy; crustal differentiation/volcanism; Tharsis, Elysium, and Valles Marineris; and ridges and fault tectonics.

Frey, H.↗
NASA NTRS1991

Frontiers of stellar evolution

The present conference discusses theoretical and observational views of star formation, spectroscopic constraints on the evolution of massive stars, very low mass stars and brown dwarfs, asteroseismology, globular clusters as tests of stellar evolution, observational tests of stellar evolution, and mass loss from cool evolved giant stars. Also discussed are white dwarfs and hot subdwarfs, neutron stars and black holes, supernovae from single stars, close binaries with evolved components, accretion disks in interacting binaries, supernovae in binary systems, stellar evolution and galactic chemical evolution, and interacting binaries containing compact components.

Lambert, David L.↗
NASA NTRS1993

Luminosity segregation in galaxy clusters as an indication of dynamical evolution

Theoretical models describing the dynamical evolution of self-gravitating systems predict a spatial mass segregation for more evolved systems, with the more massive objects concentrated toward the center of the configuration. From the observational point of view, however, the existence of mass segregation in galaxy clusters seems to be a matter of controversy. A special problem in this connection is the formation of cD galaxies in the centers of galaxy clusters. The most promising scenarios of their formation are galaxy cannibalism (merger scenario) and growing by cooling flows. It seems to be plausible to consider the swallowing of smaller systems by a dominant galaxy as an important process in the evolution of a cD galaxy. The stage of the evolution of the dominant galaxy should be reflected by the surrounding galaxy population, especially by possible mass segregation effects. Assuming that mass segregation is tantamount to luminosity segregation we analyzed luminosity segregation in roughly 40 cD galaxy clusters. Obviously there are three different groups of clusters: (1) clusters with luminosity segregation, (2) clusters without luminosity segregation, and (3) such objects exhibiting a phenomenon which we call antisegregation in luminosity, i.e. a deficiency of bright galaxies in the central regions of clusters. This result is interpreted in the sense of different degrees of mass segregation and as an indication for different evolution stages of these clusters. The clusters are arranged in the three segregation classes 2, 1, and 0 (S2 = strong mass segregation, S1 = moderate mass segregation, S0 = weak or absent mass segregation). We assume that a galaxy cluster starts its dynamical evolution after virialization without any radial mass segregation. Energy exchange during encounters of cluster members as well as merger processes between cluster galaxies lead to an increasing radial mass segregation in the cluster (S1). If a certain degree of segregation (S2) has been established, an essential number of slow-moving and relative massive cluster members in the center will be cannibalized by the initial brightest cluster galaxy. This process should lead to the growing of the predominate galaxy, which is accompanied by a diminution of the mass segregation (transition to S1 and S0, respectively) in the neighborhood of the central very massive galaxy. An increase of the areal density of brighter galaxies towards the outer cluster regions (antisegregation of luminosity), i.e. an extreme low degree of mass segregation was estimated for a substantial percentage of cD clusters. This result favors the cannibalism scenario for the formation of cD galaxies.

Baier, F. W.↗
NASA NTRS1995

Evolution of magnetized protoplanetary disks

We investigate the global evolution of a turbulent protoplanetary disk in its viscous stage, incorporating the effects of Maxwell stress due to a large-scale magnetic field permeating disk. We assume that the viscous stress is given by an alpha model. A magnetic field is produced contemporaneously by an alpha omega dynamo mechanism and the resultant Maxwell stress assists the viscous stress in providing the means for disk evolution. The aim of this work is to compare the evolution of magnetized and nonmagnetized disks driven by turbulent viscosity of the same magnitude and thus assess the effects of a self-generated magnetic field on the structure and dynamical evolution of protoplanetary disks. Two illustrative examples corresponding to two different initial conditions are considered: a high-mass case that starts with a disk of 0.245 solar mass and angular momentum of 5.6 x 10(exp 52)g sq cm/s, and a low-mass that case starts with a disk of 0.11 solar mass and angular momentum of 1.8 x 10(exp 52)g sq cm/s. For each of these two cases the radial development of a disk is calculated numerically assuming a fiducial value of the dimensionless viscosity parameter alpha(sub ss) = 0.01, as well as alpha(sub ss) = 2 x 10(exp -3). In all cases the central star has a mass equal to 1 solar mass. The most striking feature of magnetized disk evolution is the presence of the surface density bulge located in the region of the disk where the dynamo mechanism cannot support a magnetic field. The bulge persists for a time of the order of 10(exp 5)-10(exp 6) yr. The presence and persistence of the surface density bulge may have important implications for the process of planet formation and the overall characteristics of resultant planetary systems.

Reyes-Ruiz, Mauricio↗
NASA NTRS1994

Cluster evolution and microwave source counts

We present the modeled counts for the expected Sunyaev-Zel'dovich microwave sources associated with clusters of galaxies, predicted for experiments with arcminute-scale spatial resolution, assuming self-similar cluster evolution, for different spectra of the primordial density fluctuations and values of the cosmological density parameter Omega. Our simulations show that the source counts should be a powerful test of the evolution of very high redshift clusters. Experiments with 1 - 2 min spatial resolution, with moderate sensitivity but covering a large area of the sky, would be most effective for studying the SZ source population. Recent arcminute-scale radio experiments, the Owens Valley Radio Observatory (OVRO) RING experiment and VLA deep imaging, achieved sensitivity and sky coverage close to that needed for the detection of negative sources associated with very distant clusters. From the absence of cluster detections in these experiments, we rule out, with 90% confidence, models with Omega less than 0.3 and n = +1 as predicting too many bright sources; or there is no hot gas in clusters more distant than z(sub max) = 5 in such models. If the single negative source detected in the RING experiment is a distant cluster, the Omega = 1, n = -2 model also may be ruled out as it predicts too few sources. The new generation of telescopes, including the new SUZIE and Ryle instruments, will soon be able to detect distant clusters. The cluster population in the past has been modeled by scaling the observed present-day sample of X-ray clusters back to high redshifts, an approach which makes the best use of the observed cluster gas parameters, and makes the simulations robust to the assumed evolution at very early epochs. Although the pure self-similar model may be incompatible with the variety of observed evolutionary effects, we show that reasonable modifications to the intracluster gas history in that model, proposed to reconcile the self-similar evolution of cluster mass and the observed evolution of their X-ray luminosity, do not considerably change our microwave predictions made using the pure self-similar model. That is, the results of our simulations are applicable to the wide class of evolutionary models in which the cluster gas mass times gas temperature evolves as the dark mass times cluster virial temperature.

Markevitch, M.↗
NASA NTRS1995

Magnetic field evolution in white dwarfs: The hall effect and complexity of the field

We calculate the evolution of the magnetic fields in white dwarfs, taking into account the Hall effect. Because this effect depends nonlinearly upon the magnetic field strength B, the time dependences of the various multipole field components are coupled. The evolution of the field is thus significantly more complicated than has been indicated by previous investigations. Our calculations employ recent white dwarf evolutionary sequences computed for stars with masses 0.4, 0.6, 0.8, and 1.0 solar mass. We show that in the presence of a strong (up to approximately 10(exp 9) G) internal toroidal magnetic field; the evolution of even the lowest order poloidal modes can be substantially changed by the Hall effect. As an example, we compute the evolution of an initially weak quadrupole component, which we take arbitrarily to be approximately 0.1%-1% of the strength of a dominant dipole field. We find that coupling provided by the Hall effect can produce growth of the ratio of the quadrupole to the dipole component of the surface value of the magnetic field strength by more than a factor of 10 over the 10(exp 9) to 10(exp 10) year cooling lifetime of the white dwarf. Some consequences of these results for the process of magnetic-field evolution in white dwarfs are briefly discussed.

Muslimov, A. G.↗
NASA NTRS1995

Multiple rings around Wolf-Rayet evolution

We present optical narrow-band imaging of multiple rings existing around galactic Wolf-Rayet (WR) stars. The existence of multiple rings of material around Wolf-Rayet stars clearly illustrates the various phases of evolution that massive stars go through. The objects presented here show evidence of a three stage evolution. O stars produce an outer ring with the cavity being partially filled by ejecta from a red supergiant of luminous blue variable phase. A wind from the Wolf-Rayet star then passes into the ejecta materials. A simple model is presented for this three stage evolution. Using observations of the size and dynamics of the rings allows estimates of time scales for each stage of the massive star evolution. These are consistent with recent theoretical evolutionary models. Mass estimates for the ejecta, from the model presented, are consistent with previous ring nebula mass estimates from IRAS data, showing a number of ring nebulae to have large masses, most of which must in be in the form of neutral material. Finally, we illustrate how further observations will allow the determination of many of the parameters of the evolution of massive stars such as total mass loss, average mass loss rates, stellar abundances, and total time spent in each evolutionary phase.

Marston, A. P.↗
NASA NTRS1989

Cometary Evolution: Clues on Physical Properties from Chondritic Interplanetary Dust Particles

The degree of diversity or similarity detected in comets depends primarily on the lifetimes of the individual cometary nuclei at the time of analysis. It is inherent in our understanding of cometary orbital dynamics and the seminal model of comet origins by Oort that cometary evolution is the natural order of events in our Solar System. Thus, predictions of cometary behaviour in terms of bulk physical, mineralogical or chemical parameters should contain an appreciation of temporal variation(s). Previously, Rietmeijer and Mackinnon developed mineralogical bases for the chemical evolution of cometary nuclei primarily with regard to the predominantly silicate fraction of comet nuclei. We suggested that alteration of solids in cometary nuclei should be expected and that indications of likely reactants and products can be derived from judicious comparison with terrestrial diagenetic environments which include hydrocryogenic and low-temperature aqueous alterations. In a further development of this concept, Rietmeijer provides indirect evidence for the formation of sulfides and oxides in comet nuclei. Furthermore, Rietmeijer noted that timescales for hydrocryogenic and low-temperature reactions involving liquid water are probably adequate for relatively mature comets, e.g. P/comet Halley. In this paper, we will address the evolution of comet nuclei physical parameters such as solid particle grain size, porosity and density. In natural environments, chemical evolution (e.g. mineral reactions) is often accompanied by changes in physical properties. These concurrent changes are well-documented in the terrestrial geological literature, especially in studies of sediment diagenesis and we suggest that similar basic principles apply within the upper few meters of active comet nuclei. The database for prediction of comet nuclei physical parameters is, in principle, the same as used for the proposition of chemical evolution. We use detailed mineralogical studies of chondritic interplanetary dust particles (IDPS) as a guide to the likely constitution of mature comets traversing the inner Solar System. While there is, as yet, no direct proof that a specific sub-group or type of chondritic IDP is derived from a specific comet, it is clear that these particles are extraterrestrial in origin and that a certain portion of the interplanetary flux received by the Earth is cometary in origin. Two chondritic porous (CP) MPs, sample numbers W7010A2 and W7029Cl, from the Johnson Space Center Cosmic Dust Collection have been selected for this study of putative cometary physical parameters. This particular type of particle is considered a likely candidate for a cometary origin on the basis of mineralogy, bulk composition and morphology. While many IDPs have been subjected to intensive study over the past decade, we can develop a physical parameter model on only these two CP IDPs because few others have been studied in sufficient detail.

Rietmeijer, Frans J. M.↗
NASA NTRS1997

Cometary Evolution: Clues on Physical Properties from Chondritic Interplanetary Dust Particles

The degree of diversity or similarity detected in comets depends primarily on the lifetimes of the individual cometary nuclei at the time of analysis. It is inherent in our understanding of cometary orbital dynamics and the seminal model of comet origins that cometary evolution is the natural order of events in our Solar System. Thus, predictions of cometary behaviour in terms of bulk physical, mineralogical or chemical parameters should contain an appreciation of temporal variation(s). Previously, Rietmeijer and Mackinnon [1987] developed mineralogical bases for the chemical evolution of cometary nuclei primarily with regard to the predominantly silicate fraction of comet nuclei. We suggested that alteration of solids in cometary nuclei should be expected and that indications of likely reactants and products can be derived from judicious comparison with terrestrial diagenetic environments which include hydrocryogenic and low-temperature aqueous alterations. In a further development of this concept, Rietmeijer [1988] provides indirect evidence for the formation of sulfides and oxides in comet nuclei. Furthermore, Rietmeijer [1988] noted that timescales for hydrocryogenic and low-temperature reactions involving liquid water are probably adequate for relatively mature comets, e.g. P/comet Halley. In this paper, we will address the evolution of comet nuclei physical parameters such as solid particle grain size, porosity and density. In natural environments, chemical evolution (e.g. mineral reactions) is often accompanied by changes in physical properties. These concurrent changes are well-documented in the terrestrial geological literature, especially in studies of sediment diagenesis and we suggest that similar basic principles apply within the upper few meters of active comet nuclei. The database for prediction of comet nuclei physical parameters is, in principle, the same as used for the proposition of chemical evolution. We use detailed mineralogical studies of chondritic interplanetary dust particles (IDPS) as a guide to the likely constitution of mature comets traversing the inner Solar System. While there is, as yet, no direct proof that a specific sub-group or type of chondritic IDP is derived from a specific comet, it is clear that these particles are extraterrestrial in origin and that a certain portion of the interplanetary flux received by the Earth is cometary in origin. Two chondritic porous (CP) IDPS, sample numbers W701OA2 and W7029CI, from the Johnson Space Center Cosmic Dust Collection have been selected for this study of putative cometary physical parameters. This particular type of particle is considered a likely candidate for a cometary origin on the basis of mineralogy, bulk composition and morphology. While many IDPs have been subjected to intensive study over the past decade, we can develop a physical parameter model on only these two CP IDPs because few others have been studied in sufficient detail.

Reitmeijer, Frans J. M.↗