Line Shape Studies Research Articles

A comprehensive study of non-Lorentzian resonant lineshapes in nested ring resonators for quantum and photonic applications

Microring resonators are pivotal in photonic and quantum technologies. Enhancing their versatility for various applications often involves integrating additional elements to modify their resonant lineshapes. In this regard, Nested Ring Resonators (NRRs) offer a novel approach to generate a variety of lineshapes without the need for supplementary components. The coupled resonant architecture of NRRs can induce phenomena such as Electromagnetically Induced Absorption, Electromagnetically Induced Transparency, Fano resonance, and double Fano resonance. This study comprehensively analyzes the different resonant lineshapes achievable with NRRs, highlighting their broad applicability. We identify the specific conditions required for each resonant phenomenon and closely examine their characteristics. The theoretical insights from our research enable the autonomous design and realization of various resonance lineshapes within an NRR, eliminating the need for additional components while maintaining device compactness for a wide range of practical applications.

CRDS line-shape study of the (7–0) band of CO

We present the results of the spectral line-shape study of the first measurement of the extremely weak (7–0) band of the 12C16O molecule. Measurements were done with a highly sensitive cavity ring-down spectrometer. Collisional narrowing, analyzed in terms of speed-dependent effects, was observed for the first time for transitions with line intensities below 2⋅10−29 cm/molecule at 296 K. We provide a full set of line-shape parameters of the speed-dependent and regular Voigt profile analysis for 14 transitions from P and R branches. Experimental verification of a strong vibrational dependence of the pressure shifting described by the Hartmann model (Hartmann, 2009) is extended up to the sixth overtone highly sensitive to the model parameter.

Line-shape study of CO perturbed by N2 with mid-infrared frequency comb-based Fourier-transform spectroscopy

We developed a mid-infrared optical frequency comb-based Fourier-transform spectrometer and performed a line-shape study of the fundamental vibrational band of CO perturbed by N2, which is crucial for atmospheric science and astronomical observations. The comb-based FTS enabled us to measure the whole vibrational band with high resolution and precision at several pressures between 10 and 400 Torr. Observed absorption profiles were fitted with the speed-dependent Voigt profile. Collisional broadening, speed-dependent collisional width and shift coefficients are derived. The reliability of our results is established from considerations of systematic errors and comparison with previous studies.

A stimulated Raman loss spectrometer for metrological studies of quadrupole lines of hydrogen isotopologues

We discuss layout and performance of a high-resolution Stimulated Raman Loss spectrometer that has been newly developed for accurate studies of spectral lineshapes and line centre frequencies of hydrogen isotopologues and in general of Raman active transitions. Thanks to the frequency comb calibration of the detuning between pump and Stokes lasers and to an active alignment of the two beams, the frequency accuracy is at a level of 50 kHz. Over the vertical axis the spectrometer benefits from shot-noise limited detection, signal enhancement via multipass cell, active flattening of the spectral baseline and measurement times of few seconds over spectral spans larger than 10 GHz. Under these conditions an efficient averaging of Raman spectra is possible over long measurement times with minimal distortion of spectral lineshapes. By changing the pump laser, transitions can be covered in a very broad frequency span, from 50 to 5000 cm−1, including both vibrational and rotational bands. The spectrometer has been developed for studies of fundamental and collisional physics of hydrogen isotopologues and has been recently applied to the metrology of the Q(1) 1–0 line of H2.

Novel correlated {D}^0{overline{D}}^0 systems for c/b physics and tests of T/CPT

Decays of charmonia(-like) particles with definite JPC (e.g. χc1(3872)) to a {D}^0{overline{D}}^0 system and any combination of C-definite decay particles, are sources of quantum-correlated {D}^0{overline{D}}^0 systems with C = P = ±1. Several b-hadron decays also produce quantum-correlated {D}^0{overline{D}}^0 systems. Advantages of isolating these systems in their C = +1 components for amplitude analyses and studies of lineshapes are discussed. Methods to separate the C = ±1 {D}^0{overline{D}}^0 components from χc1(3872) decay samples are presented. Studies of T and CPT conservation in C = +1 {D}^0{overline{D}}^0 systems can be performed with more easily reconstructible final states, when compared to C = −1 {D}^0{overline{D}}^0 systems. Experimental mechanisms that can produce C = ±1 {D}^0{overline{D}}^0 systems are described in an appendix.

Study of EIT line shape in optically thin and thick media using 87Rb D1 and D2 lines: theory and experiment

In this work, we have presented the variation of the amplitude of electromagnetically induced transparency (EIT) resonances with the density of the atom in a V-type system using 87Rb D1 and D2 lines both theoretically and experimentally. Up to the value of atomic density 18.1 × 1010 cm−3, the amplitude of the EIT resonance gradually increases with the increase of atomic density and then it decreases with the increase of the density of the atom. We have also found the radiation trapping effect in this experiment. We observe the effect of the atomic density on the electromagnetically induced transparency when the systems act as a thin optical media as well as thick optical media. We have found that the amplitude of EIT also depends on pump laser Rabi frequency. Numerical simulations are agreed well with the experimental observations.

Al27 NMR local study of the Al0.5TiZrPdCuNi alloy in high-entropy alloy and metallic glass forms

We report a $^{27}\mathrm{Al}$ nuclear magnetic resonance (NMR) local spectroscopic study of the NMR lineshape and Knight shift of a six-component ${\mathrm{Al}}_{0.5}\mathrm{TiZrPdCuNi}$ metallic alloy that can be prepared either as a crystalline high-entropy alloy (HEA) or as an amorphous metallic glass (MG) at the same chemical composition. For both structural modifications of the material (HEA and MG), we have determined the distribution of electric-field-gradient (EFG) tensors and the local electronic density of states (DOS) $g({\ensuremath{\varepsilon}}_{\mathrm{F}})$ at the Fermi level at the position of $^{27}\mathrm{Al}$ nuclei. A theoretical $I=\frac{5}{2}$ quadrupole-perturbed NMR spectrum, pertinent to both cubic HEAs and amorphous MGs, has been derived using the Gaussian isotropic model of the EFG tensor distribution, and excellent fits of the experimental spectra were obtained. The EFG distribution function of the MG state is about twice broader than that of the HEA state, reflecting the existence of a (distorted) crystal lattice in the latter and its absence in the former. The ${T}^{2}$ dependence of the Knight shift indicates that the DOS is changing rapidly with energy within the Fermi level region for both structural modifications. The local DOS at the $^{27}\mathrm{Al}$ sites of the HEA sample is $\ensuremath{\sim}10%$ larger than that of the MG state, indicating comparable degrees of disorder.

High-Temperature Quantum Tunneling and Hydrogen Bonding Rearrangements Characterize the Solid-Solid Phase Transitions in a Phosphonium-Based Protic Ionic Liquid.

We report the complex phase behavior of the glass forming protic ionic liquid (PIL) d3‐octylphosphonium bis(trifluoromethylsulfonyl)imide [C8H17PD3][NTf2] by means of solid‐state NMR spectroscopy. Combined line shape and spin relaxation studies of the deuterons in the PD3 group of the octylphosphonium cation allow to map and correlate the phase behavior for a broad temperature range from 71 K to 343 K. In the solid PIL at 71 K, we observed a static state, characterized by the first deuteron quadrupole coupling constant reported for PD3 deuterons. A transition enthalpy of about 12 kJ mol−1 from the static to the mobile state with increasing temperature suggests the breaking of a weak, charge‐enhanced hydrogen bond between cation and anion. The highly mobile phase above 100 K exhibits an almost disappearing activation barrier, strongly indicating quantum tunneling. Thus, we provide first evidence of tunneling driven mobility of the hydrogen bonded P−D moieties in the glassy state of PILs, already at surprisingly high temperatures up to 200 K. Above 250 K, the mobile phase turns from anisotropic to isotropic motion, and indicates strong internal rotation of the PD3 group. The analyzed line shapes and spin relaxation times allow us to link the structural and dynamical behavior at molecular level with the phase behavior beyond the DSC traces.

Lineshape study of optical force spectra on resonant structures.

Understanding the frequency spectrum of the optical force is important for controlling and manipulating micro- and nano-scale objects using light. Spectral resonances of these objects can significantly influence the optical force spectrum. In this paper, we develop a theoretical formalism based on the temporal coupled-mode theory that analytically describes the lineshapes of force spectra and their dependencies on resonant scatterers for arbitrary incident wavefronts. We obtain closed-form formulae and discuss the conditions for achieving symmetric as well as asymmetric lineshapes, pertaining, respectively, to a Lorentzian and Fano resonance. The relevance of formalism as a design tool is exemplified for a conceptual scheme of the size-sorting mechanism of small particles, which plays a role in biomedical diagnosis.

Accumulation and Pulse Electron Paramagnetic Resonance Spectroscopic Investigation of the 4-Oxidobenzyl Radical Generated in the Radical S-Adenosyl-l-methionine Enzyme HydG.

The radical S-adenosyl-l-methionine (SAM) enzyme HydG cleaves tyrosine to generate CO and CN- ligands of the [FeFe] hydrogenase H-cluster, accompanied by the formation of a 4-oxidobenzyl radical (4-OB•), which is the precursor to the HydG p-cresol byproduct. Native HydG only generates a small amount of 4-OB•, limiting detailed electron paramagnetic resonance (EPR) spectral characterization beyond our initial EPR lineshape study employing various tyrosine isotopologues. Here, we show that the concentration of trapped 4-OB• is significantly increased in reactions using HydG variants, in which the "dangler Fe" to which CO and CN- bind is missing or substituted by a redox-inert Zn2+ ion. This allows for the detailed characterization of 4-OB• using high-field EPR and electron nuclear double resonance spectroscopy to extract its g-values and 1H/13C hyperfine couplings. These results are compared to density functional theory-predicted values of several 4-OB• models with different sizes and protonation states, with a best fit to the deprotonated radical anion configuration of 4-OB•. Overall, our results depict a clearer electronic structure of the transient 4-OB• radical and provide new insights into the radical SAM chemistry of HydG.

Study of UV Ne II line shapes in the cathode sheath of an abnormal glow discharge

We report results of an experimental and theoretical study of complex UV line shapes of Ne II 369.421 nm, Ne II 370.962 nm, Ne II 371.308 nm, and.Ne II 372.711 nm lines in the cathode sheath (CS) region of an abnormal DC glow discharge in pure neon. Two sets of experimental profiles and electric field distributions, one for discharge with tungsten and the other with titanium cathode, were obtained by means of the optical emission spectroscopy (OES) and theoretically studied by the iterative CS kinetic model. It is shown that our theoretical model enables the determination of the most important CS parameters (e.g. the thickness of the CS region, and the theoretical distributions of electric field and gas temperature) and thereupon based accurate theoretical predictions of the experimentally observed profiles of the studied lines.

Spectral asymmetry of phonon sideband luminescence in monolayer and bilayer WSe2

We report an experimental study of temperature-dependent spectral line shapes of phonon sideband emission stemming from dark excitons in monolayer and bilayer WSe2. Using photoluminescence spectroscopy in the range from 4 to 100 K, we observe a pronounced asymmetry in the phonon-assisted luminescence from momentum-indirect exciton reservoirs. We demonstrate that the corresponding spectral profiles are distinct from those of bright excitons with direct radiative decay pathways. The line-shape asymmetry reflects thermal distribution of exciton states with finite center-of-mass momenta, characteristic for phonon sideband emission. The extracted temperature of the exciton reservoirs is found to generally follow that of the crystal lattice, with deviations reflecting overheated populations. The latter are most pronounced in the bilayer case and at lowest temperatures. Our results add to the understanding of phonon-assisted recombination of momentum-dark excitons and, more generally, establish means to access the thermal distribution of finite-momentum excitons in atomically thin semiconductors with indirect band gaps.Received 21 May 2021Revised 28 September 2021Accepted 30 September 2021DOI:https://doi.org/10.1103/PhysRevResearch.3.L042019Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasExcitonsPhysical SystemsTransition metal dichalcogenidesTechniquesPhotoluminescenceCondensed Matter, Materials & Applied Physics

Theoretical study of CH3Cl-N2 line shapes in the ν1 band. Line mixing effects in QR doublets and QQk sub-branches

Line coupling and line mixing effects of CH3Cl lines in the ν1 band perturbed by N2 have been investigated. We have taken into account the non-diagonality of the exp(−S2) operator within specified line spaces as well as the k-degeneracy of the transitions (due to the double degeneracy of the j,k levels with k ≠ 0). These transitions should be considered as doublets coupled by the line mixing process. A new problem appears in the calculation when the atom-atom potential model is introduced. In order to overcome this difficulty, a pragmatic approach is proposed. Comparisons of theoretically calculated matrix elements of W with measurements of QR(j,k) doublets as well as some QQk sub-branches, which are strongly affected by line mixing, have been made. The results show that the formalism improved in this way leads to rather accurate predictions.

Форма лінії дислокації в полі стохастичних зсувних напружень

The shape of the dislocation line in the stochastic shear stress field in the glide plane was studied using the method of discrete dislocation dynamics. Stochastic shear stresses can occur due to the distortion of the crystal lattice. Such distortion may exist, for example, in a solid solution. Different atoms in a solid solution induce atomic size misfit and elastic modulus misfit into crystal lattice. These misfits result in crystal lattice distortions which varies spatially. The distortions are the origin of internal stresses in the lattice. Such internal stress in certain location has stochastic value normally distributed. The particular case of such stresses is shear stress distribution in the glide plane. The special method was developed to model such stress distribution. The stochastic shear stress field results in movement of different segments of dislocation line to form its equilibrium shape. The important characteristic parameters of the equilibrium shape can be measured by numerical methods. This shape also includes a "long-wavelength" component that has a non-zero amplitude and was formed without thermal activation. The shape of the dislocation line determines to some extent the yield strength of the material. Thus, the study of dislocation line shape and modeling its formation in the field of stochastic shear stresses can help to determine the yield strength of multicomponent alloys, especially multi-principal element alloys. Keywords: dislocation, discrete dislocation dynamics, shear stresses.

Stark-Broadening of Ar K-Shell Lines: A Comparison between Molecular Dynamics Simulations and MERL Results

Analysis of Stark-broadened spectral line profiles is a powerful, non-intrusive diagnostic technique to extract the electron density of high-energy-density plasmas. The increasing number of applications and availability of spectroscopic measurements have stimulated new research on line broadening theory calculations and computer simulations, and their comparison. Here, we discuss a comparative study of Stark-broadened line shapes calculated with computer simulations using non-interacting and interacting particles, and with the multi-electron radiator line shape MERL code. In particular, we focus on Ar K-shell X-ray line transitions in He- and H-like ions, i.e., Heα, Heβ and Heγ in He-like Ar and Lyα, Lyβ and Lyγ in H-like Ar. These lines have been extensively used for X-ray spectroscopy of Ar-doped implosion cores in indirect- and direct-drive inertial confinement fusion (ICF) experiments. The calculations were done for electron densities ranging from 1023 to 3×1024 cm−3 and a representative electron temperature of 1 keV. Comparisons of electron broadening only and complete line profiles including electron and ion broadening effects, as well as Doppler, are presented. Overall, MERL line shapes are narrower than those from independent and interacting particles computer simulations performed at the same conditions. Differences come from the distinctive treatments of electron broadening and are more pronounced in α line transitions. We also discuss the recombination broadening mechanism that naturally emerges from molecular dynamics simulations and its influence on the line shapes. Furthermore, we assess the impact of employing either molecular dynamics or MERL line profiles on the diagnosis of core conditions in implosion experiments performed on the OMEGA laser facility.

Complex UV Ne II line shapes in the cathode sheath of an abnormal glow discharge

We report results of an experimental and theoretical study of complex UV line shapes of Ne II 369.421 nm, Ne II 371.308 nm and Ne II 372.711 nm lines in the cathode sheath (CS) region of an abnormal glow discharge in pure neon. The experimental profiles were studied by means of the optical emission spectroscopy (OES) in conjunction with an iterative CS kinetic model. It is shown that our theoretical model describes the experimental line shapes and that, with the aid of the measured Stark shifts of atomic neon lines, it can be used for the determination of the most important CS parameters (e.g. the thickness of the CS region, distribution of electric field, and the gas temperature). We draw attention to the possibility of determining the electric field strength in CS from the width of the pedestal of the complex line profiles.

Optical frequency comb-based cavity-enhanced Fourier-transform spectroscopy: Application to collisional line-shape study

Direct-comb spectroscopy techniques uses optical frequency combs (OFCs) as spectroscopic light source. They deliver high sensitivity, high frequency resolution and precision in a broad spectral range. Due to these features, the field has burgeoned in recent years. In this work we constructed an OFC-based cavity-enhanced Fourier-transform spectrometer in the near-infrared region and used it for a line-shape study of rovibrational transitions of CO perturbed by Ar. The highly sensitive measurements spanned the wavenumber range from 6270 cm−1 to 6410 cm−1, which covered both P and R branch of the second overtone band of CO. The spectrometer delivers high-resolution surpassing the Fourier-transform resolution limit determined by interferogram length, successfully removing ringing and broadening effects caused by instrumental line shape function. The instrumental-line-shape-free method and high signal-to-noise ratio in the measurement allowed us to observe collisional effects beyond those described by the Voigt profile. We retrieved collisional line-shape parameters by fitting the speed-dependent Voigt profile and found good agreement with the values given by precise cavity ring-down spectroscopy measurements that used a continuous-wave laser referenced to a stabilized OFC. The results demonstrate that OFC-based cavity-enhanced Fourier-transform spectroscopy is a strong tool for accurate line-shape studies that will be crucial for future spectral databases.

International Conference on Spectral Lines Shapes

List of Scope, Invited Speakers, International Programme, Local Organising Committee are available in this pdf.24th International Conference on Spectral Line Shapes (ICSLS 2018)It is commonly accepted that the Europhysics Study Conference on Spectral Line Broadening and Related Topics which was held in Meudon in 1973 was the first in the current series of ICSLS meetings. The ICSLS is a bi-annual conference series and to date has been held at alternating European and North-American conference venues. It is proposed that it move to other continents in future. The most recent venues were Paris, France (2004), Auburn, USA (2006), Valladolid, Spain (2008), St. John’s, Canada (2010), St. Petersburg, Russia (2012), Tullahoma, Tennessee, USA (2014) and Torun, Poland (2016). The 2018 (24th) ICSLS conference took place in Dublin during June 17 - 22, 2018.The ICSLS covers a broad range of topics related to spectral line shape studies, including: line shapes of atomic and molecular transitions in neutral gaseous mixtures, single and multi-photoionisation ionisation processes, high and low temperature plasmas, clusters and helium droplets, nanophotonic processes, spectroscopy of stellar atmospheres and interstellar media, spectroscopy of planetary atmospheres and exoplanets, cold atoms and molecules, collision-induced spectra, processes in laser fields, innovative techniques of line shape applications for diagnostic purposes and fundamental studies with narrow optical resonances along with applications in e.g., industrial, environmental, medical and all other potential domains of interest. The conference includes a mix of invited talks, talks selected from submitted abstracts and poster presentations.List of Conference Photograph and Sponsors are available in this pdf.

Prediction of line shape parameters and their temperature dependences for CO2-N2 using molecular dynamics simulations.

We show in this paper that requantized classical molecular dynamics simulations (rCMDSs) are capable of predicting various refined spectral-shape parameters of absorption lines of CO2 broadened by N2 with high precision. Combining CMDSs and a requantization procedure, we computed the auto-correlation function of the CO2 dipole moment responsible for the absorption transition. Its Fourier-Laplace transform directly yields the spectrum. Calculations were made for two temperatures, 200 and 296 K, at 1 atm and for a large range of Doppler widths, from the near-Doppler to the collision-dominant regimes. For each temperature and each line, the spectra calculated for various Doppler widths were simultaneously fit with the Hartmann-Tran (HT) profile. This refined profile, which takes into account the effects of the speed dependent collisional line broadening, the Dicke narrowing, and the collisional line mixing, was recommended as a reference model to be used in high-resolution spectroscopy (instead of the simplified Voigt model). The HT parameters retrieved from the rCMDS-calculated spectra were then directly compared with those deduced from high-precision measurements [J. S. Wilzewski et al., J. Quant. Spectrosc. Radiat. Transfer 206, 296-305 (2018)]. The results show a very good agreement, even for those parameters whose influence on the spectra is very small. Good agreement is also obtained between measured and predicted temperature dependences of these parameters. This demonstrates that rCMDS is an excellent tool, highly competitive with respect to high quality measurements for precise line-shape studies.

Temperature-dependent line parameter study of acetylene transitions near 3 µm

Knowledge of the acetylene spectrum is important for astrophysics, atmospheric, and combustion chemistry research. Twelve acetylene transitions across eleven bands have been studied between 3335.0 and 3336.5 cm−1 with a tunable interband cascade laser. Linestrengths and temperature-dependent lineshape parameters, including collisional broadening and narrowing, are reported through Voigt, Rautian, and Galatry lineshape fits to two strong cold band transitions. Measurements were made in pure acetylene, as well as with diluents argon, nitrogen, and methane, over a temperature range of 296–637 K and pressures of 5–90 Torr. Linestrengths and temperature-dependent self-broadening coefficients are also reported for ten weak hot band transitions through Voigt lineshape fits, measured between 296–513 K and 5–20 Torr. Line parameter measurements are found to be in good agreement with the literature and extend experimental lineshape studies of acetylene into new rovibrational bands, a sparsely-studied temperature regime, and a new perturber: methane.