arXiv subjects

Aleksandra Foltynowicz

Publications and source records attributed to Aleksandra Foltynowicz.

At least 19 recordsLinked to original sources

arXiv2026

Triple-Resonance Spectroscopy Using a Cavity-Enhanced Frequency Comb Probe

Accurate experimentally verified models of molecular hot-band transitions are essential for interpreting high-temperature spectra in environments ranging from exoplanetary atmospheres to combustion systems. However, line-resolved measurements of infrared hot-band transitions reaching highly excited vibrational states above 10000 cm$^{-1}$ are missing because these transitions are too weak to observe at room temperature and become spectrally congested at elevated temperatures. Here, we introduce a nonlinear spectroscopic approach that enables simultaneous measurement of individual infrared hot-band transitions between four vibrational bands up to 12000 cm$^{-1}$ over a broad spectral range with sub-Doppler resolution and sub-MHz frequency accuracy (10$^{-10}$ relative line position accuracy). The methods is based on an all-optical triple-resonance (AOTR) scheme that combines stepwise mid-infrared pumping using an optical-frequency-comb-stabilized, double-seeded continuous-wave optical parametric oscillator with broadband highly sensitive near-infrared probing using a cavity-enhanced optical frequency comb. As a proof of principle, we measure transitions between high polyads (P) of methane - groups of strongly interacting, near-degenerate vibrational energy states arising from couplings between the C-H stretching and bending modes. In a single probe spectrum, we simultaneously resolve sub-Doppler P4$\leftarrow$P0, P6$\leftarrow$P2 and P8$\leftarrow$P4 transitions, reaching the poorly understood polyad P8 near 12000 cm$^{-1}$ and providing the first set of 41 experimentally observed lines in the P8$\leftarrow$P4 spectral region.Comb-based AOTR spectroscopy opens a new route for broadband exploration of highly excited molecular states, delivering extensive high-accuracy spectroscopic data needed to refine molecular models and improve predictions of high-temperature spectra.

physics.optics↗

arXiv2026

Measurement and assignment of $\it{J}$ $\geq$ 10 rotational energy levels in the 9510 to 9810 cm$^{-1}$ and 6590 to 6900 cm$^{-1}$ ranges of methane using optical frequency comb double-resonance spectroscopy

Accurate models of high temperature methane spectra are needed in astrophysics. Previous measurements of methane hot-band transitions in the $\it{P}$6 $\leftarrow$ $\it{P}$2 polyad range have been limited to final rotational numbers of $\it{J}$ $\le$ 9, with theoretical predictions at higher $\it{J}$s remaining unvalidated. Here, we use optical-optical double resonance spectroscopy (OODR) with a 3.3 $μ$m narrow linewidth pump to excite the $ν$${_3}$ P(12, A${_1}$$^{(2)}$) methane transition ($\it{P}$2 $\leftarrow$ $\it{P}$0) and a cavity-enhanced frequency comb centered around 1.68 $μ$m to probe the sub-Doppler ladder-type ($\it{P}$6 $\leftarrow$ $\it{P}$2) and V-type ($\it{P}$4 $\leftarrow$ $\it{P}$0) transitions, as well as Doppler-broadened collision-induced four-level transitions ($\it{P}$6 $\leftarrow$ $\it{P}$2). 49 ladder-type transitions with final rotational states $\it{J}$ = 10-12 in the range of 9510 to 9810 cm$^{-1}$ (i.e., the $\it{P}$6 polyad) were assigned to effective Hamiltonian predictions and the ExoMol database, of which 6 reached vibrational states that had not been observed experimentally before. 19 sub-Doppler V-type transitions with final states $\it{J}$ = 11-13 in the range of 6590 to 6900 cm$^{-1}$ (i.e., the $\it{P}$4 polyad) were observed and assigned to the Hamiltonian and ExoMol, while only 2 of these V-type transitions could be unambiguously assigned to WKLMC and HITRAN line lists. 170 Doppler-broadened four-level double-resonance (4LDR) lines were observed, 7 of which were newly observed compared with our previous work when pumping transitions starting from the $\it{J}$ = 7 level in the ground state [Lehmann et al., J. Chem. Phys. 163, 144304 (2025)]. We could not assign these lines as they did not form combination differences with other observed 4LDR transitions.

physics.chem-ph↗

arXiv2026

Rotational energy levels in the ground vibrational state of methane with kHz-level accuracy from comb-referenced double-resonance and Lamb-dip spectroscopies

Methane is a key spherical-top molecule, yet restrictive selection rules for one-photon transitions have prevented determination of its ground state (GS) energies with state-of-the-art kHz-level accuracy. We report the GS rotational energy level differences with kHz-level accuracy from two frequency-comb-referenced sub-Doppler methods: optical-optical double-resonance spectroscopy in the $Λ$-type configuration, and Lamb-dip spectroscopy of allowed and forbidden transitions. A Hamiltonian fit to the data yields GS term values with rotational numbers up to $\it{J}$ = 12 with kHz level accuracy.

physics.chem-ph↗

arXiv2026

Optical frequency comb Fourier transform spectroscopy of the CH$_2$$^{79}$Br$^{81}$Br, CH$_2$$^{79}$Br$_2$, and CH$_2$$^{81}$Br$_2$ isotopologues in the 1180-1210 cm$^{-1}$ region

Quantitative spectroscopic detection of dibromomethane, CH$_2$Br$_2$, for environmental monitoring, workplace safety, and exoplanetary studies is limited by the lack of accurate absorption cross-section data and rigorous spectroscopic models. We report the first high-resolution (6.3 MHz point spacing) absorption cross-section of CH$_2$Br$_2$ in the 1180-1210 cm$^{-1}$ region measured using optical frequency comb Fourier transform spectroscopy. This region is dominated by the strong CH$_2$ wagging ($ν$$_8$) fundamental vibration, which is about 50 times stronger than the fundamental C-H stretch around 3077 cm$^{-1}$. The measurements resolve isotopologue-specific rovibrational features of CH$_2$$^{79}$Br$^{81}$Br, CH$_2$$^{79}$Br$_2$, and CH$_2$$^{81}$Br$_2$, and we assign rovibrational transitions of the $ν$$_8$ fundamental and the overlapping $ν$$_4$+$ν$$_8$-$ν$$_4$ hot bands using two methods. First, an empirical non-linear least square fit implemented in PGOPHER provides high-precision line assignment and spectroscopic constants, including accurate band origins, rotational constants, and quartic centrifugal distortion parameters, for the three isotopologues, covering rotational levels up to K$_a$ = 25 and J = 144, with an average RMS residual of 0.00037 cm$^{-1}$ (11.1 MHz). Compared with previously reported band parameters retrieved from a fit to narrowband (1.78 cm$^{-1}$) supersonically cooled spectra (B. E. Brumfield et al., J. Mol. Spectrosc., 2011, 266, 57-62), our fit provides much improved global agreement between measured and simulated spectra. In parallel, an ab initio-based effective Hamiltonian approach was used to model the complete rovibrational polyads, including weak hot-band transitions and polyad interactions inaccessible to purely empirical fits, and provided the first ab initio-based line intensities of CH$_2$Br$_2$ in the 8 $μ$m spectral region.

physics.chem-ph↗

arXiv2026

Optical frequency comb double-resonance spectroscopy of the 9030-9175 cm$^{-1}$ states of ethylene

We use optical-optical double-resonance (OODR) spectroscopy to measure for the first time hot-band transitions of ethylene (C${_2}$H${_4}$) between states in the 3000 cm$^{-1}$ and 9000 cm$^{-1}$ energy ranges. A 3.2 $μ$m continuous wave (CW) pump is used to populate selected states in the $ν$${_9}$ vibrational mode. The sub-Doppler OODR transitions are then probed with two different cavity-enhanced probes tunable around 1.7 $μ$m: a frequency comb probe that allows for broadband measurements and simultaneous detection of many OODR lines, and a CW probe that measures individual lines with higher signal-to-noise ratio and better frequency accuracy. We report center frequencies and relative intensities of 90 ladder-type hot-band transitions from three different states in the $ν$${_9}$ vibrational mode. We exploit combination differences and measurements of polarization-dependent intensity ratios to determine the final state rotational quantum numbers J. Comparison to theoretical predictions from ExoMol allows tentative assignments for 28 transitions. We report improved center frequencies for the three pump transitions in the $ν$${_9}$ band. Furthermore, we observe 18 sub-Doppler V-type transitions from the depleted ground state to the 6000 cm$^{-1}$ region and assign 14 of them to the variational line list of Mraidi et al. [J Quant Spectros Radiat Transfer. 2023;310:108734 doi:10.1016/j.jqsrt.2023.108734].

physics.chem-ph↗

arXiv2025

Measurement and assignment of E-symmetry states in the 6010-6110 cm$^{-1}$ and 8940-9150 cm$^{-1}$ ranges of methane using optical frequency comb double-resonance spectroscopy

We use sub-Doppler optical-optical double-resonance (OODR) spectroscopy with a 3.3 $μ$m single-frequency pump and a cavity-enhanced 1.65 $μ$m comb probe to measure 33 ladder-type (3$ν$${_3}$ ${\leftarrow}$ $ν$${_3}$) and 8 V-type (2$ν$${_3}$) transitions in the 5880-6090 cm$^{-1}$ range of methane, reaching states with rotational E symmetry in the region of the P6 and P4 polyads, respectively. We assign the ladder-type transitions using new Hamiltonian predictions and the ExoMol line list, and the V-type transitions using the new Hamiltonian, ExoMol, HITRAN2020, and the WKLMC line lists. While 7 of the states in the 3$ν$${_3}$ range have been previously observed either in earlier OODR work (without cavity enhancement) with 1.5 MHz accuracy or in FTIR measurements of cold bands with 150 MHz resolution, the states reported here have uncertainties down to 150 kHz (5 $\times$ 10$^{-6}$ cm$^{-1}$). The E-symmetry states exhibit first-order Stark splitting, which will be reported in our future work.

physics.chem-ph↗

arXiv2025

Data availability and requirements relevant for the Ariel space mission and other exoplanet atmosphere applications

The goal of this white paper is to provide a snapshot of the data availability and data needs primarily for the Ariel space mission, but also for related atmospheric studies of exoplanets and brown dwarfs. It covers the following data-related topics: molecular and atomic line lists, line profiles, computed cross-sections and opacities, collision-induced absorption and other continuum data, optical properties of aerosols and surfaces, atmospheric chemistry, UV photodissociation and photoabsorption cross-sections, and standards in the description and format of such data. These data aspects are discussed by addressing the following questions for each topic, based on the experience of the "data-provider" and "data-user" communities: (1) what are the types and sources of currently available data, (2) what work is currently in progress, and (3) what are the current and anticipated data needs. We present a GitHub platform for Ariel-related data, with the goal to provide a go-to place for both data-users and data-providers, for the users to make requests for their data needs and for the data-providers to link to their available data. Our aim throughout the paper is to provide practical information on existing sources of data whether in databases, theoretical, or literature sources.

astro-ph.IM↗

arXiv2025

Combined frequency comb and continuous wave cavity-enhanced optical-optical double-resonance spectrometer in the 1.7 $μ$m range

We present an optical-optical double-resonance (OODR) spectrometer based on a 3.3 $μ$m continuous wave pump and two cavity-enhanced probes: a frequency comb tunable in the 1.64 - 1.8 $μ$m range, and a comb-referenced continuous wave (CW) laser tunable in the 1.6 - 1.75 $μ$m range. The comb probe provides broad spectral coverage (bandwidth up to 7 THz) for simultaneous detection of many sub-Doppler OODR transitions with sub-MHz line position accuracy, while the CW probe allows targeting individual transitions with kHz accuracy and higher signal-to-noise ratio in shorter time. Using the pump stabilized to the frequency of the R(0) transition in the $ν$${_3}$ band of methane and the comb probe covering the 5550 to 6070 cm$^{-1}$ interval, we detect 37 ladder-type transitions in the 3$ν$${_3}$ $\leftarrow$ $ν$${_3}$ band region and 6 V-type transitions in the 2$ν$${_3}$ band region and assign them using available theoretical predictions. Using the CW probe, we measure selected ladder- and V-type transitions with much higher precision. We also detect Lamb dips in the R(0)- R(3) transitions of the 2$ν$${_3}$ band and report their center frequencies with kHz level accuracy. The synergy effects of the comb- and CW-OODR open new possibilities in precision spectroscopy of levels that cannot be reached from the ground state.

physics.optics↗

arXiv2025

Assignment of collision-induced four-level double-resonance transitions in the 3$ν$${_3}$ ${\Leftarrow}$ $ν$${_3}$ spectral region of methane

Optical-optical double-resonance (OODR) spectroscopy using a narrow-linewidth pump and a frequency comb probe has previously been used to measure and assign sub-Doppler transitions in the 3$ν$${_3}$ ${\Leftarrow}$ $ν$${_3}$ spectral region [J. Chem. Phys. 161, 124311 (2024)] when pumping from the J = (7, A${_2}$) ground state. Doppler-broadened double-resonance transitions were also observed in those OODR spectra. In this paper, 68 of these Doppler-broadened transitions are assigned to four-level double-resonance transitions involving collisional transfer from the pumped A${_1}$ symmetry state to other A${_1}$ and A${_2}$ symmetry (I = 2 meta nuclear spin) levels of the $ν$${_3}$ fundamental state. Assignments are made using combination differences and comparison with the term values and intensities of lines predicted by a new effective Hamiltonian, the accuracy of which has been validated by the sub-Doppler transitions.

physics.chem-ph↗

arXiv2024

Precision frequency comb spectroscopy of the $^{14}$N$_{2}$O, $^{14}$N$^{15}$NO, $^{15}$N$^{14}$NO, and $^{15}$N$_{2}$O isotopocules in the 3300-3550 cm$^{-1}$ range

Nitrous oxide is a long-lived greenhouse gas. Its isotopic composition provides valuable insights into sources and sinks, and about the mechanism of formation. A major challenge in the spectroscopic analysis of the isotopocule compositions is the availability of accurate spectroscopic parameters, particularly for the minor $^{15}$N isotopocules. In this work, we introduce high-resolution spectroscopic measurements of four isotopocules of nitrous oxide: $^{14}$N$_{2}$O, $^{14}$N$^{15}$NO, $^{15}$N$^{14}$NO, and $^{15}$N$_{2}$O in the mid-infrared range of 3300 - 3550 cm$^{-1}$, using a frequency comb-based Fourier transform spectrometer. The nitrous oxide samples were obtained from a chemical synthesis involving acid-catalyzed amine-borane reduction of equimolar amounts of $^{15}$N isotopically enriched sodium nitrite and $^{14}$N sodium nitrite. The high-resolution spectra, measured in a temperature-controlled single-pass absorption cell, were used to retrieve line center frequencies and relative intensities for a total of 426 rovibrational transitions of the $ν$$_{1}$ + $ν$$_{3}$ band of the four isotopocules, and of the one order of magnitude weaker 2$ν$$_{2}$ + $ν$$_{3}$ and $ν$$_{1}$ + $ν$$_{2}$ + $ν$$_{3}$ - $ν$$_{2}$ bands in the same spectral region. We compare the determined line center frequencies and relative intensities with spectroscopic parameters available in high-resolution molecular databases. For $^{14}$N$_{2}$O, $^{14}$N$^{15}$NO and $^{15}$N$^{14}$NO we find good agreement with the HITRAN database. The $^{15}$N$_{2}$O isotopocule is missing in HITRAN, and we find that its line center frequencies in the GEISA database, the Institute of Atmospheric Optics database, as well as the Ames-1 line list deviate severely from the comb measurements.

physics.chem-ph↗

arXiv2024

Sub-Doppler optical-optical double-resonance spectroscopy using a cavity-enhanced frequency comb probe

Accurate parameters of molecular hot-band transitions, i.e., those starting from vibrationally excited levels, are needed to accurately model high-temperature spectra in astrophysics and combustion, yet laboratory spectra measured at high temperatures are often unresolved and difficult to assign. Optical-optical double-resonance (OODR) spectroscopy allows the measurement and assignment of individual hot-band transitions from selectively pumped energy levels without the need to heat the sample. However, previous demonstrations lacked either sufficient resolution, spectral coverage, absorption sensitivity, or frequency accuracy. Here we demonstrate OODR spectroscopy using a cavity-enhanced frequency comb probe that combines all these advantages. We detect and assign sub-Doppler transitions in the spectral range of the 3$ν$${_3}$${\leftarrow}$$ν$${_3}$ resonance of methane with frequency precision and sensitivity more than an order of magnitude better than before. This technique will provide high-accuracy data about excited states of a wide range of molecules that is urgently needed for theoretical modeling of high-temperature data and cannot be obtained using other methods.

physics.chem-ph↗

arXiv2024

Measurement and assignment of J = 5 to 9 rotational energy levels in the 9070-9370 cm$^{-1}$ range of methane using optical frequency comb double-resonance spectroscopy

We use optical-optical double-resonance (OODR) spectroscopy with a continuous wave (CW) pump and a cavity-enhanced frequency comb probe to measure high rotational energy levels of methane in the upper part of the triacontad polyad (P6). A high-power CW optical parametric oscillator, tunable around 3000 cm$^{-1}$, is consecutively locked to the P(7, A$_2$), Q(7, A$_2$), R(7, A$_2$), and Q(6, F$_2$) transitions in the $ν$$_3$ band, and a comb covering the 5800-6100 cm$^{-1}$ range probes sub-Doppler ladder-type transitions from the pumped levels with J' = 6 to 8, respectively. We report 118 probe transitions in the 3$ν$$_3$ $\leftarrow$ $ν$$_3$ spectral range with uncertainties down to 300 kHz (1 x 10$^{-5}$ cm$^{-1}$), reaching 84 unique final states in the 9070-9370 cm$^{-1}$ range with rotational quantum numbers J between 5 and 9. We assign these states using combination differences and by comparison to theoretical predictions from a new ab initio-based effective Hamiltonian and dipole moment operator. This is the first line-by-line experimental verification of theoretical predictions for these hot-band transitions, and we find a better agreement of transition wavenumbers with the new calculations compared to the TheoReTS/HITEMP and ExoMol databases. We also compare the relative intensities and find an overall good agreement with all three sets of predictions. Finally, we report the wavenumbers of 27 transitions in the 2$ν$$_3$ spectral range, observed as V-type transitions from the ground state, and compare them to the new Hamiltonian, HITRAN2020, ExoMol and the WKMLC line lists.

physics.chem-ph↗

arXiv2023

Optical frequency comb Fourier transform spectroscopy of formaldehyde in the 1250 to 1390 cm$^{-1}$ range: experimental line list and improved MARVEL analysis

We use optical frequency comb Fourier transform spectroscopy to record high-resolution, low-pressure, room-temperature spectra of formaldehyde (H$_2$$^{12}$C$^{16}$O) in the range of 1250 to 1390 cm$^{-1}$. Through line-by-line fitting, we retrieve line positions and intensities of 747 rovibrational transitions: 558 from the $ν_6$ band, 129 from the $ν_4$ band, and 14 from the $ν_3$ band, as well as 46 from four different hot bands. We incorporate the accurate and precise line positions (0.4 MHz median uncertainty) into the MARVEL (measured active vibration-rotation energy levels) analysis of the H$_2$CO spectrum. This increases the number of MARVEL-predicted energy levels by 82 and of rovibrational transitions by 5382, and substantially reduces uncertainties of MARVEL-derived H$_2$CO energy levels over a large range: from pure rotational levels below 200 cm$^{-1}$ up to multiply excited vibrational levels at 6000 cm$^{-1}$. This work is an important step toward filling the gaps in formaldehyde data in the HITRAN database.

physics.chem-ph↗

arXiv2023

Line positions and intensities of the $ν_1$ band of $^{12}$CH$_3$I using mid-infrared optical frequency comb Fourier transform spectroscopy

We present a new spectral analysis of the $ν_1$ and $ν_3$+$ν_1$-$ν_3$ bands of $^{12}$CH$_3$I around 2971 cm$^{-1}$ based on a high-resolution spectrum spanning from 2800 cm$^{-1}$ to 3160 cm$^{-1}$, measured using an optical frequency comb Fourier transform spectrometer. From this spectrum, we previously assigned the $ν_4$ and $ν_3$+$ν_4$-$ν_3$ bands around 3060 cm$^{-1}$ using PGOPHER, and the line list was incorporated in the HITRAN database. Here, we treat the two fundamental bands, $ν_1$ and $ν_4$, together with the perturbing states, 2$ν_2$+$ν_3$ and $ν_2$+2$ν_6$$^{\pm2}$, as a four-level system connected via Coriolis and Fermi interactions. A similar four-level system is assumed to connect the $ν_3$+$ν_1$-$ν_3$ and $ν_3$+$ν_4$-$ν_3$ hot bands, which appear due to the population of the low-lying $ν_3$ state at room temperature, with the 2$ν_2$+2$ν_3$ and $ν_2$+$ν_3$-$ν_6$$^{\pm2}$ perturbing states. This treatment provides a good global agreement of the simulated spectra with experiment, and hence accurate line lists and band parameters of the four connected vibrational states in each system. Overall, we assign 4665 transitions in the fundamental band system, with an average error of 0.00071 cm$^{-1}$, a factor of two better than earlier work on the $ν_1$ band using conventional Fourier transform infrared spectroscopy. The $ν_1$ band shows hyperfine splitting, resolvable for transitions with J $\le$ 2 x K. Finally, the spectral intensities of 65 lines of the $ν_1$ band and 7 lines of the $ν_3$+$ν_1$-$ν_3$ band are reported for the first time using the Voigt line shape as a model in multispectral fitting.

physics.chem-ph↗

arXiv2022

A methane line list with sub-MHz accuracy in the 1250 to 1380 cm-1 range from optical frequency comb Fourier transform spectroscopy

We use a Fourier transform spectrometer based on a difference frequency generation optical frequency comb to measure high-resolution, low-pressure, room-temperature spectra of methane in the 1250 - 1380 cm$^{-1}$ range. From these spectra, we retrieve line positions and intensities of 678 lines of two isotopologues: 157 lines from the $^{12}$CH${_4}$ $ν$${_4}$ fundamental band, 131 lines from the $^{13}$CH${_4}$ $ν$${_4}$ fundamental band, as well as 390 lines from two $^{12}$CH${_4}$ hot bands, $ν$${_2}$ + $ν$${_4}$ - $ν$${_2}$ and 2$ν$${_4}$ - $ν$${_4}$. For another 165 lines from the $^{12}$CH${_4}$ $ν$${_4}$ fundamental band we retrieve line positions only. The uncertainties of the line positions range from 0.19 to 2.3 MHz, and their median value is reduced by a factor of 18 and 59 compared to the previously available data for the $^{12}$CH${_4}$ fundamental and hot bands, respectively, obtained from conventional FTIR absorption measurements. The new line positions are included in the global models of the spectrum of both methane isotopologues, and the fit residuals are reduced by a factor of 8 compared to previous absorption data, and 20 compared to emission data. The experimental line intensities have relative uncertainties in the range of 1.5 - 7.7%, similar to those in the previously available data; 235 new $^{12}$CH${_4}$ line intensities are included in the global model.

physics.chem-ph↗

arXiv2021

Optical Frequency Comb Fourier Transform Spectroscopy of $^{14}$N$_2$$^{16}$O at 7.8 μm

We use a Fourier transform spectrometer based on a compact mid-infrared difference frequency generation comb source to perform broadband high-resolution measurements of nitrous oxide, $^{14}$N$_2$$^{16}$O, and retrieve line center frequencies of the $ν$$_1$ fundamental band and the $ν$$_1$ + $ν$$_2$ - $ν$$_2$ hot band. The spectrum spans 90 cm$^{-1}$ around 1285 cm$^{-1}$ with a sample point spacing of 3 ${\times}$ 10$^{-4}$ cm$^{-1}$ (9 MHz). We report line positions of 72 lines in the $ν$$_1$ fundamental band between P(37) and R(38), and 112 lines in the $ν$$_1$ + $ν$$_2$ - $ν$$_2$ hot band (split into two components with e/f rotationless parity) between P(34) and R(33), with uncertainties in the range of 90-600 kHz. We derive upper state constants of both bands from a fit of the effective ro-vibrational Hamiltonian to the line center positions. For the fundamental band, we observe excellent agreement in the retrieved line positions and upper state constants with those reported in a recent study by AlSaif et al. using a comb-referenced quantum cascade laser [J Quant Spectrosc Radiat Transf, 2018;211:172-178]. We determine the origin of the hot band with precision one order of magnitude better than previous work based on FTIR measurements by Toth [http://mark4sun.jpl.nasa.gov/n2o.html], which is the source of the HITRAN2016 data for these bands.

physics.chem-ph↗

arXiv2021

Dual-wavelength pumped highly birefringent microstructured silica fiber for widely tunable soliton self-frequency shift

We report the design of a microstructured silica-based fiber for widely tunable soliton self-frequency shift, suitable for pumping with two most common fiber laser wavelengths: 1.04 μm and 1.55 μm. Depending on the pump source, the output spectrum can be continuously tuned up to 1.67 μm (pump at 1.04 μm) or 1.95 μm (pump at 1.55 μm) in the same 1.5 m-long fiber sample, with pump-to-soliton conversion efficiency higher than 20%. The fiber is highly birefringent, which results in an excellent polarization extinction ratio of the soliton, reaching 26 dB. The shifted solitons have a high degree of coherence confirmed by pulse-to-pulse interference measurement. The available soliton tuning range covers the wavelengths inaccessible for fiber lasers, e.g., 1.3 μm and 1.7 μm, highly important for multi-photon microscopy and imaging. Our work shows that it is possible to design and fabricate one universal optical fiber that supports soliton shift when pumped at two different wavelengths separated by over 500 nm.

physics.optics↗

arXiv2020

Line Positions and Intensities of the ν$_4$ Band of Methyl Iodide Using Mid-Infrared Optical Frequency Comb Fourier Transform Spectroscopy

We use optical frequency comb Fourier transform spectroscopy to measure high-resolution spectra of iodomethane, CH$_3$I in the C-H stretch region from 2800 to 3160 cm$^{-1}$. The fast-scanning Fourier transform spectrometer with auto-balanced detection is based on a difference frequency generation comb with repetition rate, f$_{rep}$, of 125 MHz. A series of spectra with sample point spacing equal to f$_{rep}$ are measured at different f$_{rep}$ settings and interleaved to yield sampling point spacing of 11 MHz. Iodomethane is introduced into a 76 m long multipass absorption cell by its vapor pressure at room temperature. The measured spectrum contains three main ro-vibrational features: the parallel vibrational overtone and combination bands centered around 2850 cm$^{-1}$, the symmetric stretch $ν_1$ band centered at 2971 cm$^{-1}$, and the asymmetric stretch $ν_4$ band centered at 3060 cm$^{-1}$. The spectra of the $ν_4$ band and the nearby $ν_3$+$ν_4$-$ν_3$ hot band are simulated using PGOPHER and a new assignment of these bands is presented. The resolved ro-vibrational structures are used in a least square fit together with the microwave data to provide the upper state parameters. We assign 2603 transitions to the $ν_4$ band with standard deviation (observed - calculated) of 0.00034 cm$^{-1}$, and 831 transitions to the $ν_3$+$ν_4$-$ν_3$ hot band with standard deviation of 0.00084 cm$^{-1}$. The hyperfine splittings due to the ${^{127}}$I nuclear quadrupole moment are observed for transitions with J$\leq$2xK. Finally, intensities of 157 isolated transitions in the $ν_4$ band are reported for the first time using the Voigt line shape as a model in multispectral fitting.

physics.chem-ph↗