Nonresonant Processes Research Articles

Rotational Dynamics of Quantum State-Selected Symmetric-Top Molecules in Nonresonant Femtosecond Laser Fields.

Rotational dynamics of quantum state selected and unselected CH3I molecules in intense femtosecond laser fields has been studied. The orientation and alignment evolutions are derived from a pump-probe measurement and in good agreement with the numerical results from the time-dependent Schrödinger equation (TDSE) calculation. The different rotational transitions through nonresonant Raman process have been assigned from the Fourier analysis of the orientation and alignment revivals. These revivals are derived from a pump-probe measurement and in good agreement with the numerical results from the TDSE calculation. For the molecules in rotational state |1, ±1, ∓1⟩, the transitions can be assigned to ΔJ = ±1, ±2, while for thermally populated molecules, the transitions are ΔJ = ±2. Our results illustrate that the orientation and alignment revivals of the rotational quantum-state-selected molecules give a deep insight into the rotational excitation pathways for the transition of different rotational states of molecules in ultrafast laser fields.

Theoretical analysis of 1D resonant tunneling behavior in ion-enhanced cold field and thermo-field emission

In cold field and thermo-field emission, positive ions or adsorbates very close to the cathode surface can enhance emission current by both resonant and non-resonant processes. In this paper, resonant tunneling behavior is investigated by solving the one-dimensional Schrödinger equation in the presence of an ion, and the enhancement due to resonant processes is evaluated. Results shows that as the applied electric field increases, the resonant states move from higher to lower energies as the ion energy levels are shifted down. Conversely, as the ion position moves closer to the cathode, the resonant states shift up in energy. Further, through a simplified perturbation analysis, the general scaling of these trends can be predicted. These shifts of resonant states directly impact the emission current density, and they are especially relevant when the applied field is on the order of a few volts per nanometer (∼0.5–3 V/nm) and the ion is a few nanometers (∼0.5–3 nm) away from the cathode. Further, when the energy level for resonant emission coincides with the Fermi level of a metallic cathode, the current density is particularly enhanced. The results of this study suggest that it may be possible to control (augment/inhibit) the resonant emission current by manipulating the supply function of a cathode relative to the operating conditions of the emitter in either ion-enhanced or adsorbate-enhanced field emission, which can be applied to various plasma and electron emission technologies.

Measurements of top-quark pair differential cross-sections in the lepton+jets channel in pp collisions at [Formula: see text] using the ATLAS detector.

Measurements of normalized differential cross-sections of top-quark pair production are presented as a function of the top-quark, tbar{t} system and event-level kinematic observables in proton–proton collisions at a centre-of-mass energy of sqrt{s}=8,mathrm{TeV}. The observables have been chosen to emphasize the tbar{t} production process and to be sensitive to effects of initial- and final-state radiation, to the different parton distribution functions, and to non-resonant processes and higher-order corrections. The dataset corresponds to an integrated luminosity of 20.3 fb^{-1}, recorded in 2012 with the ATLAS detector at the CERN Large Hadron Collider. Events are selected in the lepton+jets channel, requiring exactly one charged lepton and at least four jets with at least two of the jets tagged as originating from a b-quark. The measured spectra are corrected for detector effects and are compared to several Monte Carlo simulations. The results are in fair agreement with the predictions over a wide kinematic range. Nevertheless, most generators predict a harder top-quark transverse momentum distribution at high values than what is observed in the data. Predictions beyond NLO accuracy improve the agreement with data at high top-quark transverse momenta. Using the current settings and parton distribution functions, the rapidity distributions are not well modelled by any generator under consideration. However, the level of agreement is improved when more recent sets of parton distribution functions are used.

Resonant Raman scattering theory for Kitaev models and their Majorana fermion boundary modes

We study the inelastic light scattering response in two- (2D) and three-dimensional (3D) Kitaev spin-liquid models with \ms band structures in the symmetry classes BDI and D leading to protected gapless surface modes. We present a detailed calculation of the resonant Raman/Brillouin scattering vertex relevant to iridate and ruthenate compounds whose low-energy physics is believed to be proximate to these spin-liquid phases. In the symmetry class BDI, we find that while the resonant scattering on thin films can detect the gapless boundary modes of spin liquids, the non-resonant processes do not couple to them. For the symmetry class D, however, we find that the coupling between both types of light-scattering processes and the low-energy surface states is strongly suppressed. Additionally, we describe the effect of weak time-reversal symmetry breaking perturbations on the bulk Raman response of these systems.

Ion temperature anisotropy due to perpendicular heating by Alfvén wave propagating along magnetic field lines

The perpendicular heating and acceleration of ions by linearly polarized Alfvén wave, which is propagating along constant background magnetic field, is studied. The perpendicular diffusion coefficient of ions is calculated through the autocorrelation function based on linear perturbation theory, which unambiguously demonstrates that ion heating is attained by non-resonant wave-particle interaction. It is found that the perpendicular heating and acceleration of ions occur by the Alfvén wave during a relatively short time interval, i.e., approximately 20 ion gyro period (Ωi0t) even though the perturbation amplitude is quite low. Also, it is shown that the temperature anisotropy of ions A, where A=T⊥/T∥−1, increases with the increasing perturbation amplitude while the parallel ion heating does not occur. Test particle simulation is also carried out in order to investigate the non-resonant perpendicular heating process.

Intermolecular Vibrational Energy Transfers in Melts and Solutions

Resonant and nonresonant intermolecular vibrational energy transfers in Gdm-SCN/KSCN=1/1, GdmSCN/KS13CN=1/1 and GdmSCN/KS13C15N=1/1 mixed crystals in melts and in aqueous solutions are studied with the two dimensional infrared spectroscopy. The energy transfers in the samples are slower with a larger energy donor/acceptor gap, independent of the Raman spectra. The energy gap dependences of the nonresonant energy transfers cannot be described by the phonon compensation mechanism. Instead, the experimental energy gap dependences can be quantitatively described by the dephasing mechanism. Temperature dependences of resonant and nonresonant energy transfer rates in the melts are also consistent with the prediction of the dephasing mechanism. The series of results suggest that the dephasing mechanism can be dominant not only in solutions, but also in melts (pure liquids without solvents), only if the molecular motions (translations and rotations) are much faster than the nonresonant energy transfer processes.

Thermally Tunable Absorption‐Induced Transparency by a Quasi 3D Bow‐Tie Nanostructure for Nonplasmonic and Volumetric Refractive Index Sensing at Mid‐IR

A nonresonant transmission process namely absorption‐induced transparency (AIT) is demonstrated in a quasi 3D bow‐tie nanostructure at mid‐IR spectrum for the first time. The quasi 3D structure is formed by self‐aligning two metasurfaces obtained by the Babinet's principle which are linked to each other through a patterned layer of PMMA. It is shown that the vibrational absorption of poly(methyl methacrylate) (PMMA) at 5.79 μm can strongly influence the propagation characteristics of the quasi 3D structure and generate the absorption‐induced transmission peak. A detailed parametric study is conducted on the process and its nonplasmonic characteristics are confirmed. Later, the usefulness of the quasi 3D nanochannels of the geometry is addressed and volumetric refractive index sensing (refractive index unit (RIU) shift of 123.33 nm) by the AIT effect is experimentally demonstrated for the first time. Lastly, the thermal responsiveness of the metal–dielectric hybrid platform is exploited and a thermal tuning up to 25 nm for a moderate range of temperature increase (100°) is obtained. It is believed that the hybrid system with 3D nanochannels assisted transparency can be a new avenue for volumetric plasmonic sensing and stimuli responsive device operating solely on the principle of changing molecular conformation of material.

Interference asymmetry of molecular frame photoelectron angular distributions in bichromatic UV ionization processes

We investigate molecular photoionization by ultrafast bichromatic linearly polarized UV laser pulses at frequencies perpendicular to the internuclear axis R involving π orbital excitation. Results from numerical solutions of time dependent Schrödinger equations for aligned show that molecular frame photoelectron angular distributions (MFPADs) exhibit signatures of asymmetry perpendicular to the molecular symmetry axis, arising from interference of coherent electron wave packets created by respectively one and two-photon absorption. A resonant excitation process between the ground state and the excited state is triggered by the pulse. The asymmetry of MFPADs varies periodically with pulse intensity I0 and duration T, which we attribute to coherent resonant Rabi oscillations in electronic state population. A perturbative model is adopted to qualitatively describe and analyze these effects in both resonant and nonresonant photoionization processes.

Gate-Dependent Electronic Raman Scattering in Graphene.

We report the direct observation of polarization resolved electronic Raman scattering in a gated monolayer graphene device. The evolution of the electronic Raman scattering spectra with gate voltage and its polarization dependence are in full agreement with theoretical expectations for nonresonant Raman processes involving interband electron-hole excitations across the Dirac cone. We further show that the spectral dependence of the electronic Raman scattering signal can be simply described by the dynamical polarizability of graphene in the long wavelength limit. The possibility to directly observe Dirac fermion excitations in graphene opens the way to promising Raman investigations of electronic properties of graphene and other 2D crystals.

Role of Λ(1670) in the γp → K+ ηΛ reaction near threshold

The role of the $\Lambda(1670)$ resonance in the $\gamma p \to K^+ \eta \Lambda$ reaction near threshold is studied within an effective Lagrangian approach. We perform a calculation for the total and differential cross section of the $\gamma p \to K^+ \eta \Lambda$ reaction by including the contributions from the $\Lambda(1670)$ intermediate state decaying into $\eta \Lambda$ dominated by $K^-$ and $K^{*-}$ mesons exchanges, the nucleon pole and $N^*(1535)$ resonance decaying into $K^+ \Lambda$ dominated by exchanges of $\omega$ and $K^-$ mesons. Besides, the non-resonance process and contact terms to keep the total scattering amplitude gauge invariant are also considered. With our model parameters, the total cross section of this reaction is of the order of $1$ nanobarn at photon beam energy $E_{\gamma} \sim 2.5$ GeV. It is expected that our model predictions could be tested by future experiments.

Resonant Auger-decay induced fragmentation of glycine molecule

SynopsisWe investigated the fragmentation of glycine molecule induced by resonant Auger-decay following core-shell ionization at different atomic sites by synchrotron light. We show that the dissociation pathways as well as the charge state distributions are modified due to core-level photoionization followed by Auger-decay at the different target atomic sites. The initial states for the dissociation are associated with vacancies in valence or inner-valence shells that are not localized as in core shells. We also compare the molecular dissociation following resonant and non-resonant Auger decay processes to gain insight into the influence on bond cleavage by different ionization mechanisms.

Dual Fano and Lorentzian line profile properties of autoionizing states

Photon absorption spectroscopy is a powerful tool for uncovering the structure of atoms, molecules, and solids. Symmetric Lorentzian and asymmetric Fano line shapes are fundamental spectroscopic signatures related to the structural and dynamical properties. Recently, Ott et al. [Science 340, 716 (2013)] successfully transferred Fano profile into Lorentzian line shape using an intense infrared laser, after excitation of autoionizing states in helium by attosecond XUV pulse. This is a very important step forward in quantum phase control. However, here we show experimentally that an autoionizing state can have both Fano and Lorentzian behavior naturally, depending on the process involved. This study utilized the inverse process of photon absorption ionization, i.e., electron ion recombination with photon emission, making sure the resonant autoionizing state is not modified or decorated by the laser fields. Our result implies that excitation of the state through different paths\char22{}for example, one photon versus multiphoton excitation, or even one step versus multistep excitation\char22{}can lead to different Fano profiles for the same resonant state. We also report an experimental determination of the energy shifts in the recombination photon-intensity peaks due to the interference between the resonant and nonresonant processes.

Non-resonant Higgs-pair production in the $$b\overline{b}$$ b b ¯ $$b\overline{b}$$ b b ¯ final state at the LHC

We present a particle-level study of the Standard Model non-resonant Higgs-pair production process in the $b\bar{b}b\bar{b}$ final state, at the Large Hadron Collider at $\sqrt{s}=14$ TeV. Each Higgs boson is reconstructed from a pair of close-by jets formed with the anti-$k_t$ jet clustering algorithm, with radius parameter $R=0.4$. Given the kinematic properties of the produced Higgs bosons, this Higgs reconstruction approach appears to be more suitable than the use of large-radius jets that was previously proposed in the literature. We find that the sensitivity for observing this final state can be improved significantly when the full set of uncorrelated angular and kinematic variables of the $4b$ system is exploited, leading to a statistical significance of 1.8 per experiment with an integrated luminosity of 3 ab$^{-1}$.

Molecular photoelectron angular distribution rotations in multi-photon resonant ionization of H2(+) by circularly polarized ultraviolet laser pulses.

We study effects of pulse durations on molecular photoelectron angular distributions (MPADs) in ultrafast circular polarization ultraviolet resonant ionization processes. Simulations performed on aligned H2 (+) by numerically solving time dependent Schrödinger equations show rotations of MPADs with respect to the molecular symmetry axes. It is found that in multi-photon resonant ionization processes, rotation angles are sensitive to pulse durations, which we attribute to the coherent resonant excitation between the ground state and the intermediate excited electronic state induced by Rabi oscillations. Multi-photon nonresonant and single photon ionization processes are simulated and compared which exhibit a constant rotation angle. An asymmetry parameter is introduced to describe the pulse duration sensitivity by perturbation theory models. Influence of pulse frequency detunings on MPADs is also investigated where oscillations of rotations are absent at long pulse durations due to nonresonance excitation.

Resonant and nonresonant multiphoton ionization processes in the mass spectrometry of explosives.

Multiphoton ionization processes were studied for three types of explosives using a line-tunable ultraviolet femtosecond laser. When peroxides such as triacetone triperoxide (TATP) and hexamethylene triperoxide diamine (HMTD) were ionized through a nonresonant two-photon process, a molecular ion was dominantly observed by reducing the excess energy remaining in the ion. However, an aromatic nitro compound such as 2,4,6-trinitrotoluene (TNT) produced large signals arising from molecular and fragment ions by resonant two-photon ionization. In addition, only fragment ions were produced from a nonaromatic nitro compound such as 1,3,5-trinitroperhydro-1,3,5-triazine (RDX), even when a resonant two-photon ionization process was employed, suggesting that a further reduction in excess energy would be necessary if a molecular ion were to be observed.

Au-Ag nanoalloy molecule-like clusters for enhanced quantum efficiency emission of Er³⁺ ions in silica.

The occurrence of a very efficient non-resonant energy transfer process forming ultrasmall Au-Ag nanoalloy clusters and Er(3+) ions is investigated in silica. The enhancement of the room temperature Er(3+) emission efficiency by an order of magnitude is achieved by coupling rare-earth ions to molecule-like (Au(x)Ag(1-x))N alloy nanoclusters with N = 10-15 atoms and x = 0.6 obtained by optimized sequential ion implantation on Er-implanted silica. For comparison, AuN nanoclusters obtained by the same approach and with the same size and numerical density showed an enhancement by only a factor of 2 with respect to pure Er emission, demonstrating the beneficial effect of using nanoalloyed clusters. The temperature evolution of the energy transfer process is investigated by photoluminescence and exhibits a maximum efficiency at about 600 °C, where the clusters reach the optimal size and the silica matrix completely recovers the implantation damage. The nanoalloy cluster composition and size have been studied by EXAFS analysis, which indicated a stronger Ag-O interaction with respect to the Au-O one and a preferential location of the Ag atoms at the nanoalloy cluster surface.

Assessment of optimal control mechanism complexity by experimental landscape Hessian analysis: fragmentation of CH2BrI

Optimally shaped femtosecond laser pulses can often be effectively identified in adaptive feedback quantum control experiments, but elucidating the underlying control mechanism can be a difficult task requiring significant additional analysis. We introduce landscape Hessian analysis (LHA) as a practical experimental tool to aid in elucidating control mechanism insights. This technique is applied to the dissociative ionization of CH2BrI using shaped fs laser pulses for optimization of the absolute yields of ionic fragments as well as their ratios for the competing processes of breaking the C–Br and C–I bonds. The experimental results suggest that these nominally complex problems can be reduced to a low-dimensional control space with insights into the control mechanisms. While the optimal yield for some fragments is dominated by a non-resonant intensity-driven process, the optimal generation of other fragments maa difficult task requiring significant additionaly be explained by a non-resonant process coupled to few level resonant dynamics. Theoretical analysis and modeling is consistent with the experimental observations.

Parametric interference electron–muon scattering in the field of two pulse laser waves

The nonresonant process of electron scattering at the muon in the two pulse field circularly polarized moderately strong electromagnetic waves in the interference region has been studied theoretically. Such a region occurs if an electron (and a muon) is scattered in the plane formed by the initial electron (and muon) momentum and the wave vector. In such geometry, the stimulated emission and absorption of photons by first and second waves get correlated. A significant increase of the partial scattering cross section of the process is found for non-relativistic electrons even in the case of moderate laser pulse intensities. The received results can be tested at the FAIR project.

Low-energy electron-induced ‘‘oxygen fixation’’ to DNA SAMs studied by stimulated anion desorption

Reactions of 18O2 with self-assembled monolayer films of thiolated DNA oligomers are studied by the electron stimulated desorption of anions. Electrons with energies < 20 eV initiate dehydrogenation of the DNA by resonant and non-resonant processes, to form radical sites for oxygenation. This damage mechanism may underlie the ‘‘oxygen fixation’’ process of radiobiology.

Experiments with an ion-neutral hybrid trap: cold charge-exchange collisions

Due to their large trap depths (∼1 eV or 10,000 K), versatility, and ease of construction, Paul traps have important uses in high-resolution spectroscopy, plasma physics, and precision measurements of fundamental constants. An ion-neutral hybrid trap consisting of two separate but spatially concentric traps [a magneto-optic trap (MOT) for the neutral species and a mass-selective linear Paul trap for the ionic species] is an ideal apparatus for sympathetic cooling. However, over the past few years, hybrid traps have proven most useful in measuring elastic and charge-exchange rate constants of ion-neutral collisions over a wide temperature range from kilo-Kelvin to nano-Kelvin. We report some initially surprising results from a hybrid trap system in our laboratory where we have loaded the Paul trap with Ca+ ions in the presence of a Na MOT (localized dense gas of cold Na atoms). We find a strong loss of Ca+ ions with MOT exposure, attributed to an exothermic, non-resonant ion-neutral charge-exchange process with an activation barrier, which leads to the formation of Na+ ions. We propose a detailed mechanism for this process. We obtain an estimated measure of the rate constant for this charge exchange of ∼2 × 10−11 cm3/s, much less than the Langevin rate, which suggests that the Langevin assumption of unit efficiency in the reaction region is not correct in this case.