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At least 937 records · Page 52
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

SURVIVAL OF INTERSTELLAR MOLECULES TO PRESTELLAR DENSE CORE COLLAPSE AND EARLY PHASES OF DISK FORMATION

An outstanding question of astrobiology is the link between the chemical composition of planets, comets, and other solar system bodies and the molecules formed in the interstellar medium. Understanding the chemical and physical evolution of the matter leading to the formation of protoplanetary disks is an important step for this. We provide some new clues to this long-standing problem using three-dimensional chemical simulations of the early phases of disk formation: we interfaced the full gas-grain chemical model Nautilus with the radiation-magnetohydrodynamic model RAMSES, for different configurations and intensities of the magnetic field. Our results show that the chemical content (gas and ices) is globally conserved during the collapsing process, from the parent molecular cloud to the young disk surrounding the first Larson core. A qualitative comparison with cometary composition suggests that comets are constituted of different phases, some molecules being direct tracers of interstellar chemistry, while others, including complex molecules, seem to have been formed in disks, where higher densities and temperatures allow for an active grain surface chemistry. The latter phase, and its connection with the formation of the first Larson core, remains to be modeled.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2014

The census of complex organic molecules in the solar-type protostar IRAS16293-2422

Complex organic molecules (COMs) are considered to be crucial molecules, since they are connected with organic chemistry, at the basis of terrestrial life. More pragmatically, they are molecules which in principle are difficult to synthesize in harsh interstellar environments and, therefore, are a crucial test for astrochemical models. Current models assume that several COMs are synthesized on lukewarm grain surfaces (≳30-40 K) and released in the gas phase at dust temperatures of ≳100 K. However, recent detections of COMs in ≲20 K gas demonstrate that we still need important pieces to complete the puzzle of COMs formation. Here, we present a complete census of the oxygen- and nitrogen-bearing COMs, previously detected in different Interstellar Medium (ISM) regions, toward the solar-type protostar IRAS16293-2422. The census was obtained from the millimeter-submillimeter unbiased spectral survey TIMASSS. Of the 29 COMs searched for, 6 were detected: methyl cyanide, ketene, acetaldehyde, formamide, dimethyl ether, and methyl formate. Multifrequency analysis of the last five COMs provides clear evidence that they are present in the cold (≲30 K) envelope of IRAS16293-2422, with abundances of 0.03-2 × 10{sup –10}. Our data do not allow us to support the hypothesis that the COMs abundance increases with increasing dust temperature in the cold envelope, as expected if COMs were predominately formed on lukewarm grain surfaces. Finally, when also considering other ISM sources, we find a strong correlation over five orders of magnitude between methyl formate and dimethyl ether, and methyl formate and formamide abundances, which may point to a link between these two couples of species in cold and warm gas.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

A THEORETICAL STUDY ON THE VIBRATIONAL SPECTRA OF POLYCYCLIC AROMATIC HYDROCARBON MOLECULES WITH ALIPHATIC SIDEGROUPS

The role of aliphatic side groups in the formation of astronomical unidentified infrared emission (UIE) features is investigated by applying the density functional theory to a series of molecules with mixed aliphatic-aromatic structures. The effects of introducing various aliphatic groups to a fixed polycyclic aromatic hydrocarbon (PAH) core (ovalene) are studied. Simulated spectra for each molecule are produced by applying a Drude profile at T = 500 K while the molecule is kept at its electronic ground state. The vibrational normal modes are classified using a semi-quantitative method. This allows us to separate the aromatic and aliphatic vibrations, and therefore provides clues to what types of vibrations are responsible for the emissions bands at different wavelengths. We find that many of the UIE bands are not pure aromatic vibrational bands but may represent coupled vibrational modes. The effects of aliphatic groups on the formation of the 8 μm plateau are quantitatively determined. The vibrational motions of methyl (–CH{sub 3}) and methylene (–CH{sub 2} –) groups can cause the merging of the vibrational bands of the parent PAH and the forming of broad features. These results suggest that aliphatic structures can play an important role in the UIE phenomenon.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

SULFUR-BEARING MOLECULES IN MASSIVE STAR-FORMING REGIONS: OBSERVATIONS OF OCS, CS, H{sub 2}S, AND SO

We studied the sulfur chemistry of massive star-forming regions through single-dish submillimeter spectroscopy. OCS, O{sup 13}CS, {sup 13}CS, H{sub 2}S, and SO transitions were observed toward a sample of massive star-forming regions with embedded UCH ii or CH ii regions. These sources could be divided into H ii-hot core and H ii-only sources based on their CH{sub 3}CN emission. Our results show that the OCS line of thirteen sources is optically thick, with optical depth ranging from 5 to 16. Column densities of these molecules were computed under LTE conditions. CS column densities were also derived using its optically thin isotopologue {sup 13}CS. H{sub 2}S is likely to be the most abundant gas-phase sulfuretted molecule in hot massive cores. Both the column density and abundance of sulfur-bearing molecules decrease significantly from H ii-hot core to H ii-only sources. Ages derived from hot core models appear to be consistent with star formation theories, suggesting that abundance ratios of [CS]/[SO], [SO]/[OCS], and [OCS]/[CS] could be used as chemical clocks in massive star-forming regions.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

Strongly aligned gas-phase molecules at free-electron lasers

Here, we demonstrate a novel experimental implementation to strongly align molecules at full repetition rates of free-electron lasers. We utilized the available in-house laser system at the coherent x-ray imaging beamline at the linac coherent light source. Chirped laser pulses, i.e., the direct output from the regenerative amplifier of the Ti:Sa chirped pulse amplification laser system, were used to strongly align 2, 5-diiodothiophene molecules in a molecular beam. The alignment laser pulses had pulse energies of a few mJ and a pulse duration of 94 ps. A degree of alignment of $\langle {\mathrm{cos}}^{2}{\theta }_{2{\rm{D}}}\rangle =0.85$ was measured, limited by the intrinsic temperature of the molecular beam rather than by the available laser system. With the general availability of synchronized chirped-pulse-amplified near-infrared laser systems at short-wavelength laser facilities, our approach allows for the universal preparation of molecules tightly fixed in space for experiments with x-ray pulses.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2011

INTERSTELLAR ICES AS WITNESSES OF STAR FORMATION: SELECTIVE DEUTERATION OF WATER AND ORGANIC MOLECULES UNVEILED

Observations of star-forming environments revealed that the abundances of some deuterated interstellar molecules are markedly larger than the cosmic D/H ratio of 10{sup -5}. Possible reasons for this pointed to grain surface chemistry. However, organic molecules and water, which are both ice constituents, do not enjoy the same deuteration. For example, deuterated formaldehyde is very abundant in comets and star-forming regions, while deuterated water rarely is. In this paper, we explain this selective deuteration by following the formation of ices (using the rate equation method) in translucent clouds, as well as their evolution as the cloud collapses to form a star. Ices start with the deposition of gas-phase CO and O onto dust grains. While reaction of oxygen with atoms (H or D) or molecules (H{sub 2}) yields H{sub 2}O (HDO), CO only reacts with atoms (H and D) to form H{sub 2}CO (HDCO, D{sub 2}CO). As a result, the deuteration of formaldehyde is sensitive to the gas D/H ratio as the cloud undergoes gravitational collapse, while the deuteration of water strongly depends on the dust temperature at the time of ice formation. These results reproduce well the deuterium fractionation of formaldehyde observed in comets and star-forming regions and can explain the wide spread of deuterium fractionation of water observed in these environments.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2012

SULFUR MOLECULE CHEMISTRY IN SUPERNOVA EJECTA RECORDED BY SILICON CARBIDE STARDUST

We studied about 3400 presolar silicon carbide (SiC) grains from the Murchison CM2 meteorite for C- and Si-isotopic compositions. Among these grains we identified 7 unusual or type C SiC (U/C) grains, characterized by isotopically heavy Si, and 36 supernova type X SiC grains, characterized by isotopically light Si. Selected U/C and X grains were also measured for S-, Mg-Al-, and Ca-Ti-isotopic compositions. We show that the U/C grains incorporated radioactive {sup 44}Ti, which is evidence that they formed in the ejecta of Type II supernova (SNII) explosions. Abundances of radioactive {sup 26}Al and {sup 44}Ti are compatible with those observed in X grains. U/C and X grains carry light S with enrichments in {sup 32}S of up to a factor of 2.7. The combination of heavy Si and light S observed in U/C grains is not consistent with abundance predictions of simple supernova models. The isotope data suggest preferential trapping of S from the innermost supernova zones, the production site of radioactive {sup 44}Ti, by the growing silicon carbide particles. A way to achieve this is by sulfur molecule chemistry in the still unmixed ejecta. This confirms model predictions of molecule formation in SNII ejecta and shows that sulfur molecule chemistry operates in the harsh and hot environments of stellar explosions.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2012

MOLECULES IN {eta} CARINAE

We report the detection toward {eta} Carinae of six new molecules, CO, CN, HCO{sup +}, HCN, HNC, and N{sub 2}H{sup +}, and of two of their less abundant isotopic counterparts, {sup 13}CO and H{sup 13}CN. The line profiles are moderately broad ({approx}100 km s{sup -1}), indicating that the emission originates in the dense, possibly clumpy, central arcsecond of the Homunculus Nebula. Contrary to previous claims, CO and HCO{sup +} do not appear to be underabundant in {eta} Carinae. On the other hand, molecules containing nitrogen or the {sup 13}C isotope of carbon are overabundant by about one order of magnitude. This demonstrates that, together with the dust responsible for the dimming of {eta} Carinae following the Great Eruption, the molecules detected here must have formed in situ out of CNO-processed stellar material.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Fast calculation of diffraction patterns from an ensemble of aligned molecules

We report an algorithm to calculate electron diffraction patterns for molecules with anisotropic angular distribution, which is significantly faster than existing methods. The algorithm uses a transform to convert the molecular orientation distribution, which is a function of three Euler angles, to the atom-pair distribution functions which depend on the polar and azimuthal angles. The diffraction signal can then be calculated from the atom-pair distributions. We demonstrate the computation method numerically by calculating electron diffraction patterns for a symmetric top molecule (trifluoroiodomethane) and an asymmetric top molecule (formaldehyde) and show that it reduces the calculation time by approximately two orders of magnitude compared to the standard brute-force method. Here, the method can also be applied to the calculation of x-ray diffraction patterns.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Quantum membrane phases in synthetic lattices of cold molecules or Rydberg atoms

Here, we calculate properties of dipolar interacting ultracold molecules or Rydberg atoms in a semisynthetic three-dimensional configuration—one synthetic dimension plus a two-dimensional real-space optical lattice or periodic microtrap array—using the stochastic Green's function quantum Monte Carlo method. Through a calculation of thermodynamic quantities and appropriate correlation functions, along with their finite-size scalings, we show that there is a second-order transition to a low-temperature phase in which two-dimensional “sheets” form in the synthetic dimension of internal rotational or electronic states of the molecules or Rydberg atoms, respectively. Simulations for different values of the interaction V, which acts between atoms or molecules that are adjacent both in real and synthetic space, allow us to compute a phase diagram. We find a finite-temperature transition at sufficiently large V as well as a quantum phase transition—a critical value V c below which the transition temperature vanishes.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2010

Laser cooling of molecules by zero-velocity selection and single spontaneous emission

A laser-cooling scheme for molecules is presented based on repeated cycle of zero-velocity selection, deceleration, and irreversible accumulation. Although this scheme also employs a single spontaneous emission as in [Raymond Ooi, Marzlin, and Audretsch, Eur. Phys. J. D 22, 259 (2003)], in order to circumvent the difficulty of maintaining closed pumping cycles in molecules, there are two distinct features which make the cooling process of this scheme faster and more practical. First, the zero-velocity selection creates a narrow velocity-width population with zero mean velocity, such that no further deceleration (with many stimulated Raman adiabatic passage (STIRAP) pulses) is required. Second, only two STIRAP processes are required to decelerate the remaining hot molecular ensemble to create a finite population around zero velocity for the next cycle. We present a setup to realize the cooling process in one dimension with trapping in the other two dimensions using a Stark barrel. Numerical estimates of the cooling parameters and simulations with density matrix equations using OH molecules show the applicability of the cooling scheme. For a gas at temperature T=1 K, the estimated cooling time is only 2 ms, with phase-space density increased by about 30 times. The possibility of extension to three-dimensional cooling via thermalization is also discussed.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2010

Enhancements of rescattered electron yields in above-threshold ionization of molecules

In above-threshold ionization of rare-gas atoms, photoelectron spectra recorded in the 10{sup 13}-10{sup 14} W cm{sup -2} range exhibit enhancements in the rescattering plateaus that do not have a unified theoretical interpretation yet. Here an experimental search for such enhancements is reported in simple molecules with ionization potentials near those of rare-gas atoms such as H{sub 2} and N{sub 2} for argon and O{sub 2} for xenon, and in other molecules such as CO{sub 2} and N{sub 2}O. Only H{sub 2} exhibits the enhancements previously observed in atoms. The H{sub 2} particularity is interpreted in terms of its simpler ion structure and associated ionization paths compared with other molecules.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2010

Toward scalable information processing with ultracold polar molecules in an electric field: A numerical investigation

We numerically investigate the possibilities of driving quantum algorithms with laser pulses in a register of ultracold NaCs polar molecules in a static electric field. We focus on the possibilities of performing scalable logical operations by considering circuits that involve intermolecular gates (implemented on adjacent interacting molecules) to enable the transfer of information from one molecule to another during conditional laser-driven population inversions. We study the implementation of an arithmetic operation (the addition of 0 or 1 on a binary digit and a carry in) which requires population inversions only and the Deutsch-Jozsa algorithm which requires a control of the phases. Under typical experimental conditions, our simulations show that high-fidelity logical operations involving several qubits can be performed in a time scale of a few hundreds of microseconds, opening promising perspectives for the manipulation of a large number of qubits in these systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2010

Strong-field ionization of a heteronuclear diatomic molecule

We theoretically study strong-field ionization of a heteronuclear diatomic molecule, CO, by calculating the photoelectron angular distributions (PADs) and the total ionization rates using linearly and circularly polarized laser fields. We find that, although the PADs of CO generally do not have inversion symmetry, they become more inversion symmetric as the photoelectron energy increases. Heteronuclear features of CO upon ionization are better understood by comparing the results with those of a representative of homonuclear molecules, N{sub 2}, in that, although there are some similarities between CO and N{sub 2} due to the same orbital symmetry, {sigma}{sub g}, there are some differences between them in terms of the ionization suppression and orientation dependence of the total ionization yield. Namely, CO behaves more like an atom in the low-intensity range in a sense that ionization takes place mainly from the neighborhood of the C core, while it behaves more like a double-core molecule in the high-intensity range since ionization takes place from the neighborhood of both C and O cores. This explains why ionization suppression of CO is not seen at the low intensity but it becomes more visible at the high intensity range.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2011

High-order-harmonic generation using gas-phase H{sub 2}O molecules

We investigate high-order-harmonic generation of isotropically distributed gas-phase H{sub 2}O molecules exposed to an intense laser field. The induced dipole of each individual molecule by the laser field is first calculated using the recently developed quantitative rescattering theory. In a thin medium, harmonic spectra generated coherently from all the molecules are then calculated by solving Maxwell's equation of propagation. By using accurate transition dipoles of H{sub 2}O, we show that the harmonics in the lower plateau region are quite different from models that employ the simpler strong-field approximation. We also examine the magnitude and phase of the harmonics and their dependence on laser focusing conditions.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2011

First and second derivative of the wave function of the {sup 1}{Sigma}{sup +} states of the KH molecule

First and second derivative of the nonadiabatic coupling between the several {sup 1}{Sigma}{sup +} adiabatic states of the KH molecule considered from accurate diabatic and adiabatic data have been evaluated. Such derivatives of the electronic wave function are determined through a numerical differentiation of the rotational matrix connecting the diabatic and adiabatic representations. The first as well as the second derivative present many peaks related to ionic-neutral and neutral-neutral coupling between the {sup 1}{Sigma}{sup +} states. Such radial coupling has been exploited to calculate the first adiabatic correction, which corresponds to the diagonal term of the second derivative divided by the reduced mass, for the ground and some excited states of the KH molecule. The second adiabatic correction has been determined using the virial theorem. The first adiabatic correction was added to the adiabatic potential energy curves to redetermine the corrected spectroscopic constants and vibrational energy levels. The vibrational shift, which is the difference between the corrected and the adiabatic levels, has been calculated for X, A, C, and D {sup 1}{Sigma}{sup +} states of the KH molecule. A shift of some 10 cm{sup -1} is observed for some vibrational levels showing the breakdown of the Born-Oppenheimer approximation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2011

Ion-assisted ground-state cooling of a trapped polar molecule

We propose and analyze a scheme for sympathetic cooling of the translational motion of polar molecules confined in the wells of a deep optical lattice and interacting one by one with laser-cooled ions in a radio-frequency trap. The energy gap between the excitation spectra of the particles in their respective trapping potentials is bridged by means of a parametric resonance, provided by the additional modulation of the rf field. We analyze two scenarios: simultaneous laser cooling and energy exchange between the ion and the molecule, and a scheme where these two processes take place separately. We calculate the lowest final energy of the molecule and the cooling rate depending on the amplitude of the parametric modulation. For small parametric modulation, the dynamics can be solved analytically within the rotating wave approximation.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2011

Berry connection in atom-molecule systems

In the mean-field theory of atom-molecule systems, where bosonic atoms combine to form molecules, there is no usual U(1) symmetry, presenting an apparent hurdle for defining the Berry phase and Berry curvature for these systems. We define a Berry connection for this system, with which the Berry phase and Berry curvature can be naturally computed. We use a three-level atom-molecule system to illustrate our results. In particular, we have computed the mean-field Berry curvature of this system analytically, and compared it to the Berry curvature computed with the second-quantized model of the same system. An excellent agreement is found, indicating the validity of our definition.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗