Anisotropic Angular Distribution Research Articles

Compact ultrafast neutron sources via bulk acceleration of deuteron ions in an optical trap

A scheme for a quasi-monoenergetic high-flux neutron source with femtosecond duration and highly anisotropic angular distribution is proposed. This scheme is based on bulk acceleration of deuteron ions in an optical trap or density grating formed by two counter-propagating laser pulses at an intensity of ∼1016W/cm2 in a near-critical-density plasma. The deuterons are first pre-accelerated to an energy of tens of keV in the ambipolar fields formed in the optical trap. Their energy is boosted to the MeV level by another one or two laser pulses at an intensity of ∼1020W/cm2, enabling fusion reactions to be triggered with high efficiency. In contrast to previously proposed pitcher–catcher configurations, our scheme can provide spatially periodic acceleration structures and effective collisions between deuterons inside the whole target volume. Subsequently, neutrons are generated directly inside the optical trap. Our simulations show that neutron pulses with energy 2–8 MeV, yield 1018–1019n/s, and total number 106–107 in a duration ∼400 fs can be obtained with a 25 μm target. Moreover, the neutron pulses exhibit unique angularly dependent energy spectra and flux distributions, predominantly along the axis of the energy-boosting lasers. Such microsize femtosecond neutron pulses may find many applications, such as high-resolution fast neutron imaging and nuclear physics research.

Photoelectron Velocity Map Imaging Spectroscopy of the Beryllium Trimer and Tetramer.

Computational studies of small beryllium clusters (BeN) predict dramatic, nonmonotonic changes in the bonding mechanisms and per-atom cohesion energies with increasing N. To date, experimental tests of these quantum chemistry models are lacking for all but the Be2 molecule. In the present study, we report spectroscopic data for Be3 and Be4 obtained via anion photodetachment spectroscopy. The trimer is predicted to have D3h symmetric equilibrium structures for both the neutral molecule and the anion. Photodetachment spectra reveal transitions that originate from the X2A2″ ground state and the 12A1' electronically excited state. The state symmetries were assigned on the basis of anisotropic photoelectron angular distributions. The neutral and anionic forms of Be4 are predicted to be tetrahedral. Franck-Condon diagonal photodetachment was observed with a photoelectron angular distribution consistent with the expected Be4-X2A1 → Be4X1A1 transition. The electron affinities of Be3 and Be4 were determined to be 11363 ± 60 and 13052 ± 50 cm-1, respectively.

Photodissociation dynamics of the ethyl radical via the Ã2A'(3s) state: H-atom product channels and ethylene product vibrational state distribution.

The photodissociation dynamics of jet-cooled ethyl radical (C2H5) via the Ã2A'(3s) states are studied in the wavelength region of 230-260nm using the high-n Rydberg H-atom time-of-flight (TOF) technique. The H + C2H4 product channels are reexamined using the H-atom TOF spectra and photofragment translational spectroscopy. A prompt H + C2H4(X̃1Ag) product channel is characterized by a repulsive translational energy release, anisotropic product angular distribution, and partially resolved vibrational state distribution of the C2H4(X̃1Ag) product. This fast dissociation is initiated from the 3s Rydberg state and proceeds via a H-bridged configuration directly to the H + C2H4(X̃1Ag) products. A statistical-like H + C2H4(X̃1Ag) product channel via unimolecular dissociation of the hot electronic ground-state ethyl (X̃2A') after internal conversion from the 3s Rydberg state is also examined, showing a modest translational energy release and isotropic angular distribution. An adiabatic H + excited triplet C2H4(ã3B1u) product channel (a minor channel) is identified by energy-dependent product angular distribution, showing a small translational energy release, anisotropic angular distribution, and significant internal excitation in the C2H4(ã3B1u) product. The dissociation times of the different product channels are evaluated using energy-dependent product angular distribution and pump-probe delay measurements. The prompt H + C2H4(X̃1Ag) product channel has a dissociation time scale of <10ps, and the upper bound of the dissociation time scale of the statistical-like H + C2H4(X̃1Ag) product channel is <5ns.

Electron-neutral collision cross sections for H2O: II. Anisotropic scattering and assessment of the validity of the two-term approximation

This work proposes a complete and consistent set of cross sections (CS) for electron collisions with water gas molecules to be published in the IST-Lisbon database on LXCat. The set is validated by the electron swarm analysis technique. The anisotropic angular distribution of electrons in rotational collisions is considered by means of the Born approximation in a two-term Boltzmann solver (LisbOn KInetics two-term Boltzmann solver (LoKI-B)) and a Monte Carlo simulations code (LoKI-MC), both freely available as open-source codes. The inclusion of electron anisotropic scattering in rotational collisions significantly improves the agreement between calculations and measurements of the electron drift velocity, reduced mobility, characteristic energy, reduced Townsend ionisation coefficient, reduced effective Townsend coefficient and reduced attachment coefficient. The MC simulations are deemed more accurate and shown to yield similar results as LoKI-B with the proposed set. The use of LoKI-MC also validates the set of CSs against parameters that cannot be obtained by LoKI-B, such as the longitudinal diffusion coefficient or the bulk transport coefficients.

Photons production in heavy-ion collisions as a signal of deconfinement phase

The photon production due to conversion of two gluons into a photon, $$gg\rightarrow \gamma $$ , in the presence of the background gauge fields is studied within the specific mean-field approach to QCD vacuum. In this approach, mean field in the confinement phase is represented by the statistical ensemble of almost everywhere homogeneous abelian (anti-)self-dual gluon configurations, while the deconfined phase can be characterized by the purely chromomagnetic fields. The probability of gluon conversion of two gluons into a photon vanishes in the confinement phase due to the randomness of the background field configurations. The anisotropic strong electromagnetic field, generated in the collision of relativistic heavy ions, serves as a catalyst for deconfinement with the appearance of an anisotropic purely chromomagnetic mean field. Respectively, deconfined phase is characterized by nonzero probability of the conversion of two gluons into a photon with strongly anisotropic angular distribution.

Ultraviolet photodissociation of 2-methylallyl radical

Ultraviolet photodissociation dynamics of 2-methylallyl radical from the 3p Rydberg state were investigated in the wavelength region of 226–244 nm using the high-n Rydberg atom time-of-flight (HRTOF) technique. The 2-methylallyl radicals were generated by 193 nm photolysis of 3-chloro-2-methyl-1-propene precursors. The photofragment yield spectrum of H-atom products increases in intensity with decreasing wavelengths in 226–244 nm. The TOF spectra of H-atom products show a bimodal structure. The predominant product channel (with ∼98% branching ratio) has a kinetic energy release peaking at ∼7 kcal/mol, with an average ratio of ET in the total available energy, (fT), of ∼0.18 in 226–244 nm and an isotropic product angular distribution. At the low ET, isotropic component is from statistical unimolecular decomposition of highly vibrationally excited hot 2-methylallyl to the methylenecyclopropane+H products, following internal conversion from the excited electronic state. The minor product channel (with ∼2% branching ratio) has a large kinetic energy peaking at ∼50 kcal/mol, with (fT)≈0.63 and an anisotropic angular distribution (β≈−0.2). At the high ET, anisotropic component is non-statistical and is postulated to be from direct loss of H atom via the 3p Rydberg state or repulsive part of the ground state to the 1,3-butadiene+H products.

Photodissociation dynamics of tetrahydrofuran at 193 nm.

Tetrahydrofuran (THF), a cyclic ether with the chemical formula C4H8O, can be considered the simplest analog of the deoxyribose backbone component of deoxyribonucleic acid (DNA). As such, it provides a useful model for probing the photochemistry of such biomolecular motifs. We present a velocity-map imaging study into the ultraviolet dissociation of THF at a wavelength of 193 nm. Excitation to the S1 state occurs via a 3s ← n transition involving a lone-pair electron on the oxygen atom, and has been shown by other authors to result in rapid ring opening via cleavage of one of the C-O bonds to form a ring-opened C4H8O diradical, followed by C-C bond cleavage over a longer timescale to form either OCH2 + C3H6 products (Channel 1a), HOCH2 + C2H5 products (Channel 1b), or OCH2CH2 + C2H4 products (Channel 2). The C2H4O products formed via Channel 2 are unstable on the timescale of our experiment and dissociate further to form CH3 and CHO. We also observe a number of minor products resulting from H or H2 loss from the primary photofragments. The speed distributions observed for all photofragments are broad, indicating excitation of a range of rotational and vibrational states of the products. The angular distributions of the photofragments show an interesting speed dependence: the slowest products have almost isotropic angular distributions, but the magnitude of the recoil anisotropy increases monotonically with photofragment speed. The fastest products exhibit highly anisotropic angular distributions, with the recoil anisotropy parameter β approaching its limiting value of -1 (-0.75 for Channel 1 and -0.5 for Channel 2). This behaviour is attributed to the range of timescales over which the diradical intermediate dissociates into the observed photofragments. Rapid dissociation leads to fast photofragments which retain the correlation between the transition dipole moment for the S1 ← S0 excitation (which lies perpendicular to the ring) and the photofragment velocities (which lie predominantly in the plane of the ring). Slow dissociation results in a high degree of energy redistribution into internal modes, slower photofragments, and loss of correlation between the photofragment velocities and the transition dipole. The higher barrier associated with dissociation via Channel 2 suggests somewhat longer lifetimes for the diradical intermediate and is consistent with a corresponding reduction in the maximum observed value for β.

Observation of giant quadrupole plasmon resonance in C60 in fast ion collisions

Strong perturbation caused due to the Coulomb interaction with fast highly charged ions has been used to probe the quadrupole plasmon excitation in ${\mathrm{C}}_{60}$ fullerene. The electron-emission spectrum arising from a free ${\mathrm{C}}_{60}$ molecule reveals a double-peak structure due to the decay of the giant plasmon resonance. Using a state-of-the-art theoretical approach describing the electron dynamics by time-dependent density functional theory, with an explicit ionic background these two peaks are unambiguously identified as arising from the dipole and quadrupole modes of the plasmon. Furthermore, the electron angular distribution clearly shows a double-well-type distribution which is well reproduced by quadrupole and plasmon resonances. The dipole and quadrupole excitations combined with a long-range postcollisional Coulomb interaction shows excellent agreement with the observed anisotropic angular distribution. The present paper serves as an independent confirmation of the presence of a substantial quadrupole plasmon contribution in molecular systems.

Simulation of the fission process of the excited compound nuclei Rn210 and Fr215 produced in fusion reactions within the framework of the modified statistical model

In the framework of the modified statistical model there have been simulated fission process of the excited compound nuclei $^{210}\mathrm{Rn}$ and $^{215}\mathrm{Fr}$ produced in $^{16}\mathrm{O}+^{194}\mathrm{Pt}$ and $^{19}\mathrm{F}+^{196}\mathrm{Pt}$ reactions and calculated the evaporation residue cross section, the fission cross section, the fission probability, the average prescission neutron multiplicity, the mean fission time, and the anisotropy of fission fragments angular distribution as a function of excitation energy. The classical collective motion of the excited compound nuclei about the ground state, the temperature dependence of the location, the height of fission transition points, and the projection of the total spin of the compound nucleus onto the symmetry axis $K$ have been considered in the statistical calculations. A constant nuclear dissipation was applied in the statistical calculations. In the statistical calculations, the temperature coefficient of the effective potential $k$ and the scaling factor of the fission-barrier height ${r}_{s}$ were considered as a free parameter and their magnitudes inferred by fitting measured data on the evaporation residue cross section and the fission cross section for the excited compound nuclei $^{210}\mathrm{Rn}$ and $^{215}\mathrm{Fr}$. It was shown that the results of calculations are in good agreement with the experimental data by using appropriate values for these parameters equal to $k=0.0160\ifmmode\pm\else\textpm\fi{}0.0050\phantom{\rule{0.28em}{0ex}}\mathrm{Me}{\mathrm{V}}^{\ensuremath{-}2}$ and ${r}_{s}=1.0030\ifmmode\pm\else\textpm\fi{}0.0020$ for $^{210}\mathrm{Rn}$ and $k=0.0065\ifmmode\pm\else\textpm\fi{}0.0040\phantom{\rule{0.16em}{0ex}}\mathrm{Me}{\mathrm{V}}^{\ensuremath{-}2}$ and ${r}_{s}=1.0040\ifmmode\pm\else\textpm\fi{}0.0015$ for $^{215}\mathrm{Fr}$. Furthermore, by using appropriate values of parameters $k$ and ${r}_{s}$ have been calculated the average prescission neutron multiplicity, the fission probability, the mean fission time, and the anisotropy of fission fragments angular distribution for the nuclei $^{210}\mathrm{Rn}$ and $^{215}\mathrm{Fr}$. Comparison of the theoretical data with the experimental data were shown that the modified statistical model is well able to reproduce different experimental data. Although, at high excitation energies the results of calculations for the anisotropy of fission fragments angular distribution and fission probability are slightly lower than the experimental data.

Two-photon dissociation dynamics of the mercapto radical.

Two-photon dissociation dynamics of the SH/SD radicals are investigated using the high-n Rydberg atom time-of-flight (HRTOF) technique. The H/D(2S) + S(1D) and H/D(2S) + S(1S) products are observed in the dissociation of the SH/SD radicals on the 22Π and B2Σ+ repulsive states, from sequential two-photon excitation via the A2Σ+ (v' = 0, J' = 0.5-2.5) state. The angular distributions of both H/D(2S) + S(1D) and H/D(2S) + S(1S) product channels are anisotropic. The anisotropy parameter (β) of the H(2S) + S(1D) products is ∼-0.8 ± 0.1 (-0.9 ± 0.05 for SD), and that of the H(2S) + S(1S) products is ∼1.3 ± 0.3 (1.2 for SD). The anisotropic angular distributions indicate that the SH/SD radicals promptly dissociate on the repulsive 22Π and B2Σ+ potential energy curves (PECs) along with some non-adiabatic crossings, leading to the H/D(2S) + S(1D) and H/D(2S) + S(1S) products, respectively. The bond dissociation energy of the ground-state X2Π3/2 SH/SD to the ground-state H/D(2S) + S(3P2) products is measured to be D0(S-H) = 29 253 ± 20 cm-1 and D0(S-D) = 29 650 ± 20 cm-1, respectively. The dissociation energy of the A2Σ+ state SH/SD to the H/D(2S) + S(1D) products is derived to be D0[S-H(A)] = 7659 ± 20 cm-1 and D0[S-D(A)] = 7940 ± 20 cm-1.

Photodissociation dynamics of methyl vinyl ketone oxide: A four-carbon unsaturated Criegee intermediate from isoprene ozonolysis.

The electronic spectrum of methyl vinyl ketone oxide (MVK-oxide), a four-carbon Criegee intermediate derived from isoprene ozonolysis, is examined on its second π* ← π transition, involving primarily the vinyl group, at UV wavelengths (λ) below 300nm. A broad and unstructured spectrum is obtained by a UV-induced ground state depletion method with photoionization detection on the parent mass (m/z 86). Electronic excitation of MVK-oxide results in dissociation to O (1D) products that are characterized using velocity map imaging. Electronic excitation of MVK-oxide on the first π* ← π transition associated primarily with the carbonyl oxide group at λ > 300nm results in a prompt dissociation and yields broad total kinetic energy release (TKER) and anisotropic angular distributions for the O (1D) + methyl vinyl ketone products. By contrast, electronic excitation at λ ≤ 300nm results in bimodal TKER and angular distributions, indicating two distinct dissociation pathways to O (1D) products. One pathway is analogous to that at λ > 300nm, while the second pathway results in very low TKER and isotropic angular distributions indicative of internal conversion to the ground electronic state and statistical unimolecular dissociation.

Correlations between fission fragment and neutron anisotropies in neutron-induced fission

Several sources of angular anisotropy for fission fragments and prompt neutrons have been studied in neutron-induced fission reactions. These include kinematic recoils of the target from the incident neutron beam and the fragments from the emission of the prompt neutrons, preferential directions of the emission of the fission fragments with respect to the beam axis due to the population of particular transition states at the fission barrier, and forward-peaked angular distributions of pre-equilibrium neutrons which are emitted before the formation of a compound nucleus. In addition, there are several potential sources of angular anisotropies that are more difficult to disentangle: the angular distributions of prompt neutrons from fully accelerated fragments or from scission neutrons, and the emission of neutrons from fission fragments that are not fully accelerated. In this work, we study the effects of the first group of anisotropy sources, particularly exploring the correlations between the fission fragment anisotropy and the resulting neutron anisotropy. While kinematic effects were already accounted for in our Hauser-Feshbach Monte Carlo code, $\mathtt{CGMF}$, anisotropic angular distributions for the fission fragments and pre-equilibrium neutrons resulting from neutron-induced fission on $^{233,234,235,238}$U, $^{239,241}$Pu, and $^{237}$Np have been introduced for the first time. The effects of these sources of anisotropy are examined over a range of incident neutron energies, from thermal to 20 MeV, and compared to experimental data from the Chi-Nu liquid scintillator array. The anisotropy of the fission fragments is reflected in the anisotropy of the prompt neutrons, especially as the outgoing energy of the prompt neutrons increases, allowing for an extraction of the fission fragment anisotropy to be made from a measurement of the neutrons.

Generalized Kompaneets formalism for inelastic neutrino-nucleon scattering in supernova simulations

Based on the Kompaneets approximation, we develop a robust methodology to calculate spectral redistribution via inelastic neutrino-nucleon scattering in the context of core-collapse supernova simulations. The resulting equations conserve lepton number to machine precision and scale linearly, not quadratically, with number of energy groups. The formalism also provides an elegant means to derive the rate of energy transfer to matter which, as it must, automatically goes to zero when the neutrino radiation field is in thermal equilibrium. Furthermore, we derive the next-higher-order in {\epsilon}/mc2 correction to the neutrino Kompaneets equation. Unlike other Kompaneets schema, ours also generalizes to the case of anisotropic angular distributions, while retaining the conservative form that is a hallmark of the classical Kompaneets equation. Our formalism enables immediate incorporation into supernova codes that follow the spectral angular moments of the neutrino radiation fields.

Photodissociation dynamics of the tert-butyl perthiyl radical.

The photodissociation dynamics of the tert-butyl perthiyl (t-BuSS) radical are investigated by fast-beam coincidence translational spectroscopy. A fast (6 keV-8 keV) beam of neutral t-BuSS radicals is produced via photodetachment of the corresponding anion, followed by photodissociation at 248 nm (5.00 eV) or 193 nm (6.42 eV) and coincident detection of the neutral products. Photofragment mass and translational energy distributions are obtained at both wavelengths. At 248 nm, the dominant product channel (90%) is found to be S loss, with a product translational energy distribution that peaks close to the maximum available energy and an anisotropic photofragment angular distribution, indicating dissociation along a repulsive excited state. A minor channel (10%) leading to the formation of S2 + t-Bu is also observed. At 193 nm, both two- and three-body dissociation are observed. The formation of S2 + t-Bu is the dominant two-body product channel, with multiple electronic states of the S2 molecule produced via excited-state dissociation processes. The formation of S + t-BuS is a minor two-body channel at this dissociation energy. The three-body channels are S2 + H + isobutene, S2 + CH3 + propene, and S + SH + isobutene. The first two of these channels result from a sequential dissociation process in which the loss of S2 from t-BuSS results in ground-state t-Bu with sufficient internal energy to undergo secondary fragmentation. The third three-body channel, S + SH + isobutene, is attributed to the loss of internally excited HS2 from t-BuSS, which then rapidly dissociates to form S + SH in an asynchronous concerted dissociation process.

Effect of recoil-induced internal excitation on the Auger transition energy

A recent investigation of nitrogen $1s$ ionization in ${\mathrm{N}}_{2}$ by 40-keV photons has shown that only 70% of the recoil-induced internal energy appears as kinetic energy of the two nitrogen ions that are produced following the Auger decay of the core-ionized molecule. It has been concluded that the remaining 30% appears as part of the Auger transition energy. Presented here is an investigation using both classical and quantum mechanical models of how this unexpected result might come about. With these models, and the assumption of an isotropic distribution of the recoil momentum with respect to the molecular axis, it is possible to account for as much as 16% of the internal excitation contributing to the Auger transition energy, but within this framework there does not seem to be an obvious mechanism for producing a contribution as high as 30%. Consideration of refinements to the simple models does not improve this disagreement between prediction and observation. Assumption of a sufficiently anisotropic angular distribution can bring prediction and experiment into agreement, but such anisotropy is not consistent with other experimental results or theoretical expectations.

Two-photon dissociation dynamics of hydroxyl radical

Two-photon dissociation dynamics of the OH radical is studied using the high-n Rydberg atom time-of-flight (HRTOF) technique. The H(2S)+O(1D) and H(2S)+O(1S) product channels are observed in the dissociation of the OH radical on the 22Π and B2Σ+ repulsive states, respectively, from sequential two-photon excitation via the A2Σ+ (v′=2, J′=0.5−2.5) state. Both H+O product channels have anisotropic angular distributions, with β=−0.97 for H(2S)+O(1D) and 1.97 for H(2S)+O(1S). The anisotropic angular distributions are consistent with a mechanism of OH direct dissociation on the repulsive potential energy curves (PECs) leading to the H+O products. The OH bond dissociation energy D0(O−H) is determined to be 35580±15 cm−1.

Ionic Angular Distributions Induced by Strong-Field Ionization of Tri-Atomic Molecules* *Supported by the National Natural Science Foundation of China (Grant Nos. 11534004, 11874179, and 11704149), and the Natural Science Foundation of Jilin Province (Grant Nos. 20180101289JC and 20190103045JH).

Angular distributions of fragment ions from ionization of several tri-atomic molecules (CO 2, OCS, N 2 O and NO 2 ) by strong 800-nm laser fields are investigated via a time-of-flight mass spectrometer. Anisotropic angular distributions of fragment ions, especially those of atomic ions, are observed for all of the molecules studied. These anisotropic angular distributions are mainly due to the geometric alignment of molecules in the strong field ionization. Distinct different patterns in ionic angular distributions for different molecules are observed. It is indicated that both molecular geometric structure and ionization channels have effects on the angular distributions of strong field ionization/fragmentation.

Effects of isospin and dissipation coefficient of the K coordinate in simulation of fission dynamics of excited compound nuclei

A stochastic approach based on four-dimensional (4D) dynamical model has been used to simulate the fission process of the excited compound nuclei [Formula: see text]Fr, [Formula: see text]Fr and [Formula: see text]Fr produced in fusion reactions. Effects of isospin and dissipation coefficient of the [Formula: see text] coordinate, [Formula: see text], on estimation of the evaporation residue (ER) cross-section, the prescission neutron multiplicity, the variance of the mass and energy distributions of fission fragments and the anisotropy of fission fragments angular distribution have been investigated for the excited compound nuclei [Formula: see text]Fr, [Formula: see text]Fr and [Formula: see text]Fr. Three collective shape coordinates [Formula: see text] plus the projection of total spin of the compound nucleus to the symmetry axis, [Formula: see text], were considered in the 4D dynamical model. In the 4D dynamical model, the magnitude of the dissipation coefficient of [Formula: see text], [Formula: see text], was considered as a free parameter and its magnitude inferred by fitting measured data on the ER cross-section. Results of the extracted dissipation coefficients of [Formula: see text] for different isotopes of Fr were shown that the magnitude of the dissipation coefficient of [Formula: see text] increases with decreasing isospin of fissioning compound nucleus. It was also shown that the prescission neutron multiplicity and the anisotropy of fission fragments angular distribution increase with increasing isospin whereas the variance of the mass and energy distributions of fission fragments decrease with increasing isospin of fissioning compound nucleus. Furthermore, it was shown that the calculated values of prescission neutron multiplicity and the variance of the mass distribution of fission fragments for the excited compound nuclei [Formula: see text]Fr, [Formula: see text]Fr and [Formula: see text]Fr decrease with the dissipation strength of [Formula: see text], whereas the variance of the energy distribution of fission fragments and the anisotropy of fission fragments angular distribution increase with the dissipation strength of [Formula: see text].

Study of a data analysis method for the angle resolving silicon telescope

A new data analysis method is developed for the angle resolving silicon telescope introduced at the neutron time of flight facility n_TOF at CERN. The telescope has already been used in measurements of several neutron induced reactions with charged particles in the exit channel. The development of a highly detailed method is necessitated by the latest joint measurement of the 12C(n,p) and 12C(n,d) reactions from n_TOF. The reliable analysis of these data must account for the challenging nature of the involved reactions, as they are affected by the multiple excited states in the daughter nuclei and characterized by the anisotropic angular distributions of the reaction products. The unabridged analysis procedure aims at the separate reconstruction of all relevant reaction parameters—the absolute cross section, the branching ratios and the angular distributions—from the integral number of the coincidental counts detected by the separate pairs of silicon strips. This procedure is tested under the specific conditions relevant for the 12C(n,p) and 12C(n,d) measurements from n_TOF, in order to assess its direct applicability to these experimental data. Based on the reached conclusions, the original method is adapted to a particular level of uncertainties in the input data.

Ultraviolet photodissociation dynamics of DNCO + hν → D + NCO: Two competitive pathways

Photodissociation dynamics of DNCO + hν → D + NCO at photolysis wavelengths between 200 and 235 nm have been studied using the D-atom Rydberg tagging time-of-flight technique. Product translational energy distributions and angular distributions have been determined. Nearly statistical distribution of the product translational energy with nearly isotropic angular distribution was observed at 210–235 nm, which may come from the predissociation pathway of internal conversion from S1 to S0 state followed by decomposition on S0 surface. At shorter photolysis wavelengths, in addition to the statistical distribution, another feature with anisotropic angular distribution appears at high translational energy region, which can be attributed to direct dissociation on S1 surface. Compared with HNCO, the direct dissociation pathway for DNCO photodissociation opens at higher excitation energy. According to our assignment of the NCO internal energy distribution, dominantly bending and a little stretching excited NCO was produced via both dissociation pathways.