Non-thermal Excitation Research Articles

Current-induced local heating and extractable work in nonthermal vibrational excitation

Current-induced local heating and extractable work in nonthermal vibrational excitation

Spatially inhomogeneous inverse Faraday effect provides tunable nonthermal excitation of exchange dominated spin waves

Abstract We demonstrate optical nonthermal excitation of exchange dominated spin waves of different orders in a magnetophotonic crystal. The magnetophotonic structure consists of a thin magnetic film and a Bragg stack of nonmagnetic layers to provide a proper nonuniform interference pattern of the inverse Faraday effect induced by light in the magnetic layer. We found a phenomenon of the pronounced phase slippage of the inverse Faraday effect distribution when the pump wavelength is within the photonic band gap of the structure. It allows to tune the interference pattern by a slight variation of light wavelength which results in the modification of excitation efficiency of the different order spin waves. The approach can be applied for different magnetic dielectrics expanding their application horizons for spin-wave based devices.

Entangling-gate error from coherently displaced motional modes of trapped ions

Entangling gates in trapped-ion quantum computing have primarily targeted stationary ions with initial motional distributions that are thermal and close to the ground state. However, future systems will likely incur significant non-thermal excitation due to, e.g., ion transport, longer operational times, and increased spatial extent of the trap array. In this paper, we analyze the impact of such coherent motional excitation on entangling-gate error by performing simulations of Molmer-Sorenson (MS) gates on a pair of trapped-ion qubits with both thermal and coherent excitation present in a shared motional mode at the start of the gate. We discover that a small amount of coherent displacement dramatically erodes gate performance in the presence of experimental noise, and we demonstrate that applying only limited control over the phase of the displacement can suppress this error. We then use experimental data from transported ions to analyze the impact of coherent displacement on MS-gate error under realistic conditions.

Heisenberg representation of nonthermal ultrafast laser excitation of magnetic precessions

We derive the Heisenberg representation of the ultrafast inverse Faraday effect that provides the time evolution of magnetic vectors of a magnetic system during its interaction with a laser pulse. We obtain a time-dependent effective magnetic operator acting in the Hilbert space of the total angular momentum that describes a process of nonthermal excitation of magnetic precessions in an electronic system by a circularly polarized laser pulse. The magnetic operator separates the effect of the laser pulse on the magnetic system from other magnetic interactions. The effective magnetic operator provides the equations of motion of magnetic vectors during the excitation by the laser. We show that magnetization dynamics calculated with these equations is equivalent to magnetization dynamics calculated with the time-dependent Schr\"odinger equation, which takes into account the interaction of an electronic system with the electric field of light. We model and compare laser-induced precessions of magnetic sublattices of an easy-plane and an easy-axis antiferromagnetic systems. Using these models, we show how the ultrafast inverse Faraday effect induces a net magnetic moment in antiferromagnets and demonstrate that a crystal field environment and the exchange interaction play essential roles for laser-induced magnetization dynamics even during the action of a pump pulse. Using our approach, we show that light-induced precessions can start even during the action of the pump pulse with a duration several tens times shorter than the period of induced precessions and affect the position of magnetic vectors after the action of the pump pulse.

Investigation of Nonthermal Plasma Jet Excitation Mode and Optical Assessment of Its Electron Concentration

The results of a study of a plasma jet of atmospheric-pressure helium driven by a capacitive discharge using sine and pulsed modes of excitation are presented. The homogeneous discharge of a multi-channel plasma jet at gas temperature of 34 °C and helium flow rate of 0.5 L/min was achieved with short pulse excitation. A digital holography method is proposed to estimate a basic plasma parameter, i.e., its electron concentration. An automated digital holographic interferometry set-up for the observation and study of a nonthermal plasma jet in a pulse mode is developed and described. The synchronization features of recording devices with the generation of plasma pulses are considered. The electron concentration of the plasma jet is also estimated. The disadvantages of the proposed technique and its further application are discussed.

Nonthermal excitation effects mediated by sub-terahertz radiation on hydrogen exchange in ubiquitin

Water dynamics in the hydration layers of biomolecules play crucial roles in a wide range of biological functions. A hydrated protein contains multiple components of diffusional and vibrational dynamics of water and protein, which may be coupled at ∼0.1-THz frequency (10-ps timescale) at room temperature. However, the microscopic description of biomolecular functions based on various modes of protein-water-coupled motions remains elusive. A novel approach for perturbing the hydration dynamics in the subterahertz frequency range and probing them at the atomic level is therefore warranted. In this study, we investigated the effect of klystron-based, intense 0.1-THz excitation on the slow dynamics of ubiquitin using NMR-based measurements of hydrogen-deuterium exchange. We demonstrated that the subterahertz irradiation accelerated the hydrogen-deuterium exchange of the amides located in the interior of the protein and hydrophobic surfaces while decelerating this exchange in the amides located in the surface loop and short 310 helix regions. This subterahertz-radiation-induced effect was qualitatively contradictory to the increased-temperature-induced effect. Our results suggest that the heterogeneous water dynamics occurring at the protein-water interface include components that are nonthermally excited by the subterahertz radiation. Such subterahertz-excited components may be linked to the slow function-related dynamics of the protein.

Insights into the Formation of Hydroxyl Radicals with Nonthermal Vibrational Excitation in the Meinel Airglow.

To understand night time airglow in the Meinel bands and heat conversion from the highly excited OH radicals in the upper atmosphere via the important atmospheric reaction H + O3 → OH + O2, we report here a quasi-classical trajectory study of the reaction dynamics on a recently developed full-dimensional potential energy surface (PES). Our results indicate that the reaction energy of this highly exoergic reaction is almost exclusively channeled into the vibration of the OH product, underscoring an extreme departure from the statistical limit. The calculated OH vibrational distribution is highly inverted and peaks near the highest accessible vibrational state, in excellent agreement with experimental observations, validating the accuracy of the PES. More importantly, the dynamical origin of the nonthermal excitation of the OH vibrational mode is identified by its large projection onto the reaction coordinate at a small potential barrier in the entrance channel, which controls the energy flow into various degrees of freedom in the products.

A Theoretical Argument for Extended Interpulse Delays in Therapeutic High-Frequency Irreversible Electroporation Treatments.

We sought to determine whether modifications to the delays within H-FIRE bursts could yield a more desirable clinical outcome in terms of ablation volume versus extent of tissue excitation. We used a modified spatially extended nonlinear node (SENN) nerve fiber model to evaluate excitation thresholds for H-FIRE bursts with varying delays. We then calculated non-thermal tissue ablation, thermal damage, and excitation in a clinically relevant numerical model. Excitation thresholds were maximized by shortening d1, and extension of d2 up to 1,000 μs increased excitation thresholds by at least 60% versus symmetric bursts. In the ablation model, long interpulse delays lowered the effective frequency of burst waveforms, modulating field redistribution and reducing heat production. Finally, we demonstrate mathematically that variable delays allow for increased voltages and larger ablations with similar extents of excitation as symmetric waveforms. Interphase and interpulse delays play a significant role in outcomes resulting from H-FIRE treatment. Waveforms with short interphase delays (d1) and extended interpulse delays (d2) may improve therapeutic efficacy of H-FIRE as it emerges as a clinical tissue ablation modality.

Helium-rich Superluminous Supernovae from the Zwicky Transient Facility

Abstract Helium is expected to be present in the massive ejecta of some hydrogen-poor superluminous supernovae (SLSN-I). However, until now only one event has been identified with He features in its photospheric spectra (PTF10hgi). We present the discovery of a new He-rich SLSN-I, ZTF19aawfbtg (SN2019hge), at z = 0.0866. This event has more than 10 optical spectra at phases from −41 to +103 days relative to the peak, most of which match well with that of PTF10hgi. Confirmation comes from a near-IR spectrum taken at +34 days, revealing He i features with P-Cygni profiles at 1.083 and 2.058 μm. Using the optical spectra of PTF10hgi and SN2019hge as templates, we examined 70 other SLSNe-I discovered by Zwicky Transient Facility in the first two years of operation and found five additional SLSNe-I with distinct He-features. The excitation of He i atoms in normal core-collapse supernovae requires nonthermal radiation, as proposed by previous studies. These He-rich events cannot be explained by the traditional 56Ni mixing model because of their blue spectra, high peak luminosities, and long rise timescales. Magnetar models offer a possible solution since pulsar winds naturally generate high-energy particles, potential sources of nonthermal excitation. An alternative model is the interaction between the ejecta and dense H-poor circumstellar material, which may be supported by observed undulations in the light curves. These six SLSNe-Ib have relatively low-peak luminosities (rest frame M g = −20.06 ± 0.16).

Sunquake with a second bounce, other sunquakes, and emission associated with the X9.3 flare of 6 September 2017

In this paper we present the interpretation of the observations of the flare from 6 September 2017 reported in Paper I. These include gamma-ray (GR), hard X-ray (HXR), soft X-rays, Lyαline, extreme ultraviolet (EUV), Hα, and white light (WL) emission, which were recorded during the two flaring events 1 (FE1) and 2 (FE2) that occurred at 11:55:37 UT (FE1) and 12:06:40 UT (FE2). Paper I also reported the first detection of the sunquake with first and second bounces of seismic waves combined with four other sunquakes in different locations supported with the observations of HXR, GR, EUV, Hα, and WL emission with strongly varying spatial resolution and temporal coverage. In the current paper, we propose some likely scenarios for heating of flaring atmospheres in the footpoints with sunquakes which were supported with EUV and Hαemission. We used a range of parameters derived from the HXR, EUV, and Hαline observations to generate hydrodynamic models, which can account for the blueshifts derived from the EUV emission and the redshifts observed with the EUV Imaging Spectrometer in the He II line and by the CRisp Imaging Spectro-Polarimeter in the Swedish Solar Telescope in Hαline emission. The parameters of hydrodynamic shocks produced by different beams in flaring atmospheres were used as the initial conditions for another type of hydrodynamic models that were developed for acoustic wave propagation in the solar interior. These models simulate the sets of acoustic waves produced in the interior by the hydrodynamic shocks from atmospheres above deposited in different footpoints of magnetic loops. The Hαline profiles with large redshifts in three kernels (two in FE1 and one in FE2) were interpreted with the full non-local thermodynamic equilibrium radiative simulations in all optically thick transitions (Lyman lines and continuum Hα, Hβ, and Pα) applied for flaring atmospheres with fast downward motions while considering thermal and non-thermal excitation and ionisation of hydrogen atoms by energetic power-law electron beams. The observed Hαline profiles in three kernels were fit with the simulate blue wing emission of the Hαline profiles shifted significantly (by 4–6 Å) towards the line red wings, because of strong downward motions with velocities about 300 km s−1by the shocks generated in flaring atmospheres by powerful beams. The flaring atmosphere associated with the largest sunquake (seismic source 2 in FE1) is found consistent with being induced by a strong hydrodynamic shock produced by a mixed beam deposited at an angle of −30° from the local vertical. We explain the occurrence of a second bounce in the largest sunquake by a stronger momentum delivered by the shock generated in the flaring atmosphere by a mixed beam and deeper depths of the interior where this shock was deposited. Indeed, the shock with mixed beam parameters is found deposited deeply into the interior beneath the flaring atmosphere under the angle to the local vertical that would allow the acoustic waves generated in the direction closer to the surface to conserve enough energy for the second bounces from the interior layers and from the photosphere. The wave characteristics of seismic sources 1 and 3 (in FE1) were consistent with those produced by the shocks generated by similar mixed beams deposited at the angles −(0 − 10)° (seismic source 1) and +30° (seismic source 3) to the local vertical. The differences of seismic signatures produced in the flares of 6 September 2011 and 2017 are also discussed.

Time- and momentum-resolved tunneling spectroscopy of pump-driven nonthermal excitations in Mott insulators

We present a computational technique to calculate time and momentum resolved non-equilibrium spectral density of correlated systems using a tunneling approach akin scanning tunneling spectroscopy. The important difference is that our probe is extended, basically a copy of the sample, allowing one to extract the momentum information of the excitations. We illustrate the method by measuring the spectrum of a Mott-insulating extended Hubbard chain after a sudden quench with the aid of time-dependent density matrix renormalization group (tDMRG) calculations. We demonstrate that the system realizes a non-thermal state that is an admixture of spin and charge density wave states, with corresponding signatures that are recognizable as in-gap sub-bands. In particular, we identify a band of excitons and one of stable anti-bound states at high energies that gains enhanced visibility after the pump. We do not appreciate noticeable relaxation within the time-scales considered, which is attributed to the lack of decay channels due to spin-charge separation. These ideas can be readily applied to study transient dynamics and spectral signatures of correlation-driven non-equilibrium processes.

Direct observation of picosecond melting and disintegration of metallic nanoparticles

Despite more than a century of study, the fundamental mechanisms behind solid melting remain elusive at the nanoscale. Ultrafast phenomena in materials irradiated by intense femtosecond laser pulses have revived the interest in unveiling the puzzling processes of melting transitions. However, direct experimental validation of various microscopic models is limited due to the difficulty of imaging the internal structures of materials undergoing ultrafast and irreversible transitions. Here we overcome this challenge through time-resolved single-shot diffractive imaging using X-ray free electron laser pulses. Images of single Au nanoparticles show heterogeneous melting at the surface followed by density fluctuation deep inside the particle, which is directionally correlated to the polarization of the pumping laser. Observation of this directionality links the non-thermal electronic excitation to the thermal lattice melting, which is further verified by molecular dynamics simulations. This work provides direct evidence to the understanding of irreversible melting with an unprecedented spatiotemporal resolution.

On the Competition Between Electron Autodetachment and Dissociation of Molecular Anions

We treat the competition between autodetachment of electrons and unimolecular dissociation of excited molecular anions as a rigid-/loose-activated complex multichannel reaction system. To start, the temperature and pressure dependences under thermal excitation conditions are represented in terms of falloff curves of separated single-channel processes within the framework of unimolecular reaction kinetics. Channel couplings, caused by collisional energy transfer and “rotational channel switching” due to angular momentum effects, are introduced afterward. The importance of angular momentum considerations is stressed in addition to the usual energy treatment. Non-thermal excitation conditions, such as typical for chemical activation and complex-forming bimolecular reactions, are considered as well. The dynamics of excited SF6− anions serves as the principal example. Other anions such as CF3− and POCl3− are also discussed.

Underlying Physical Process for the Unusual Spectral Quality of Double Pulse Laser Spectroscopy in He Gas.

This study is aimed at elucidating the physical processes responsible for the excellent spectral qualities in terms of full width at half-maximum (fwhm) and signal-to-noise (S/N) ratio shown in a special double pulse laser-induced spectroscopy. Apart from the use of atmospheric He ambient gas, the achievement is due to the first laser for generating He gas plasma and the subsequent use of the second laser pulse for target ablation, in opposite order of the two-laser operations in conventional double pulse LIBS. This setup allows adjustments of the many experimental parameters to yield the optimal condition resulting in 0.03 nm fwhm and around 1000× S/N ratio of Cu I 521.8 nm and far surpasses the spectral qualities obtained by other techniques. This is obtained by allowing the crucial separation of the target plasma from the He gas plasma and thereby enabling the He-assisted excitation (HAE) to play its full and unique role of nonthermal excitation, taking advantage of metastable excited He atoms in the He plasma and the Penning-like energy transfer process. This excellent performance is further verified by its successful application analysis of Cr in low alloy steel samples, with the presence of smooth linear calibration lines, signifying the absence of the self-absorption effect well-known in ordinary LIBS.

Monte-Carlo methods for NLTE spectral synthesis of supernovae

We present JEKYLL, a new code for modelling of supernova (SN) spectra and lightcurves based on Monte-Carlo (MC) techniques for the radiative transfer. The code assumes spherical symmetry, homologous expansion and steady state for the matter, but is otherwise capable of solving the time-dependent radiative transfer problem in non-local-thermodynamic-equilibrium (NLTE). The method used was introduced in a series of papers by Lucy, but the full time-dependent NLTE capabilities of it have never been tested. Here, we have extended the method to include non-thermal excitation and ionization as well as charge-transfer and two-photon processes. Based on earlier work, the non-thermal rates are calculated by solving the Spencer-Fano equation. Using a method previously developed for the SUMO code, macroscopic mixing of the material is taken into account in a statistical sense. To save computational power a diffusion solver is used in the inner region, where the radiation field may be assumed to be thermalized. In addition, a statistical Markov-chain model is used to sample the emission frequency more efficiently, and we introduce a method to control the sampling of the radiation field, which is used to reduce the noise in the radiation field estimators. Except for a description of JEKYLL, we provide comparisons with the ARTIS, SUMO and CMFGEN codes, which show good agreement in the calculated spectra as well as the state of the gas. In particular, the comparison with CMFGEN, which is similar in terms of physics but uses a different technique, shows that the Lucy method does indeed converge in the time-dependent NLTE case. Finally, as an example of the time-dependent NLTE capabilities of JEKYLL, we present a model of a Type IIb SN, taken from a set of models presented and discussed in detail in an accompanying paper. Based on this model we investigate the effects of NLTE, in particular those arising from non-thermal excitation and ionization, and find strong effects even on the bolometric lightcurve. This highlights the need for full NLTE calculations when simulating the spectra and lightcurves of SNe.

Magnetoelastic excitation of single nanomagnets for optical measurement of intrinsic Gilbert damping

We report an alternative all-optical technique to drive and probe the spin dynamics of single nanomagnets. Optically generated surface acoustic waves (SAWs) drive the magnetization precession in nanomagnets via magnetoelastic (MEL) coupling. We investigate the field-swept dynamics of isolated Ni nanomagnets at various SAW frequencies and show that this method can be used to accurately determine the intrinsic Gilbert damping of nanostructured magnetic materials. This technique opens a new avenue for studying the spin dynamics of nanoscale devices using nonthermal (``cold'') excitation, enabling direct observation of the MEL driven dynamics.

BCS superconductors: The out-of-equilibrium response to a laser pulse

The dynamics of a 2D d-wave BCS superconductor driven out-of-equilibrium by a perpendicularly-impinging polarized laser pulse is analyzed on varying the laser pulse characteristics. The observed effects include: oscillations both in the amplitude and in the phase of the superconducting order parameter, suppression of the superconductivity, but also its enhancement with a strong dependence on all varying parameters and, in particular, on the polarization in plane of the applied vector potential and on the value of its frequency. This study opens up the possibility to distinguish very clearly the behavior of the nodal and anti-nodal non-thermal excitations and to tackle some of the puzzling results of the current experimental scenario in the field.

Ultrafast hot-electron induced quenching of Tb 4f magnetic order

We have investigated ultrafast quenching of the Tb4f magnetic order in Co74Tb26 alloys, induced by femtosecond hot-electrons pulses. The hot-electron pulses were produced in specific non-magnetic capping layers by infrared fs laser pulses. Our experimental results show that sub-picosecond dynamics of Tb4f magnetic moments can be induced by non-thermal and thermal hot-electrons. We further demonstrate that the demagnetization efficiencies of non-thermal and thermal hot electrons are similar. However, the characteristic demagnetization times show values of 0.35 ps for non-thermal hot-electrons excitations and 1.2 ps for thermal hot-electrons excitations. We explain this temporal elongation by the propagation time of thermal hot-electrons through the 15 nm thick CoTb film.

Emission characteristics of 6.78-MHz radio-frequency glow discharge plasma in a pulsed mode

This paper investigated Boltzmann plots for both atomic and ionic emission lines of iron in an argon glow discharge plasma driven by 6.78-MHz radio-frequency (RF) voltage in a pulsed operation, in order to discuss how the excitation/ionization process was affected by the pulsation. For this purpose, a pulse frequency as well as a duty ratio of the pulsed RF voltage was selected as the experimenter parameters. A Grimm-style radiation source was employed at a forward RF power of 70W and at an argon pressures of 670Pa. The Boltzmann plot for low-lying excited levels of iron atom was on a linear relationship, which was probably attributed to thermal collisions with ultimate electrons in the negative glow region; in this case, the excitation temperature was obtained in a narrow range of 3300–3400K, which was hardly affected by the duty ratio as well as the pulse frequency of the pulsed RF glow discharge plasma. This observation suggested that the RF plasma could be supported by a self-stabilized negative glow region, where the kinetic energy distribution of the electrons would be changed to a lesser extent. Additional non-thermal excitation processes, such as a Penning-type collision and a charge-transfer collision, led to deviations (overpopulation) of particular energy levels of iron atom or iron ion from the normal Boltzmann distribution. However, their contributions to the overall excitation/ionization were not altered so greatly, when the pulse frequency or the duty ratio was varied in the pulsed RF glow discharge plasma.

Optically excited structural transition in atomic wires on surfaces at the quantum limit.

Transient control over the atomic potential-energy landscapes of solids could lead to new states of matter and to quantum control of nuclear motion on the timescale of lattice vibrations. Recently developed ultrafast time-resolved diffraction techniques combine ultrafast temporal manipulation with atomic-scale spatial resolution and femtosecond temporal resolution. These advances have enabled investigations of photo-induced structural changes in bulk solids that often occur on timescales as short as a few hundred femtoseconds. In contrast, experiments at surfaces and on single atomic layers such as graphene report timescales of structural changes that are orders of magnitude longer. This raises the question of whether the structural response of low-dimensional materials to femtosecond laser excitation is, in general, limited. Here we show that a photo-induced transition from the low- to high-symmetry state of a charge density wave in atomic indium (In) wires supported by a silicon (Si) surface takes place within 350 femtoseconds. The optical excitation breaks and creates In-In bonds, leading to the non-thermal excitation of soft phonon modes, and drives the structural transition in the limit of critically damped nuclear motion through coupling of these soft phonon modes to a manifold of surface and interface phonons that arise from the symmetry breaking at the silicon surface. This finding demonstrates that carefully tuned electronic excitations can create non-equilibrium potential energy surfaces that drive structural dynamics at interfaces in the quantum limit (that is, in a regime in which the nuclear motion is directed and deterministic). This technique could potentially be used to tune the dynamic response of a solid to optical excitation, and has widespread potential application, for example in ultrafast detectors.