arxiv: 2603.21734 · v2 · submitted 2026-03-23 · ⚛️ physics.optics

Recognition: 2 theorem links

· Lean Theorem

Highly-efficient perturbative Raman shifting by engineering the nonlinear temporal response

Yi-Hao Chen , Wenchao Wang , Jose Enrique Antonio-Lopez , Rodrigo Amezcua-Correa , Chris Xu , Frank Wise

Authors on Pith no claims yet

Pith reviewed 2026-05-15 01:00 UTC · model grok-4.3

classification ⚛️ physics.optics

keywords Raman shiftinghollow-core fibernonlinear opticstime-domain theoryquantum efficiencygas mixtureperturbative responsesoliton self-frequency shift

0 comments

The pith

Reducing Raman response to a perturbation on the electronic nonlinearity enables fourfold higher quantum efficiency in frequency shifting.

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

The paper develops a time-domain description of Raman scattering that works for all pulse lengths and reveals how strong Raman contributions create temporal and spectral distortions that limit frequency-shifting efficiency. By engineering gas mixtures to make the Raman part only a small fraction of the total nonlinear response, these distortions are suppressed and the process becomes perturbative. Experiments confirm quantum efficiency rises from 20 percent in pure molecular gas to 80 percent, with the suggestion that 100 percent is reachable. A reader should care because Raman shifting is central to many light sources and spectroscopic methods, and removing the efficiency barrier would make those techniques more practical.

Core claim

The time-domain theoretical approach provides a unified description of Raman interactions across temporal regimes, exposes how molecules with strong Raman responses produce detrimental distortions in soliton self-frequency shift, and shows that these distortions are suppressed when the Raman interaction is reduced to a perturbation on the electronic response, as verified by experiments achieving up to 80 percent quantum efficiency with tunable gas mixtures.

What carries the argument

The time-domain theoretical approach that directly visualizes Raman temporal dynamics and accounts for spectrotemporal aspects by treating Raman as a tunable perturbation on the instantaneous electronic nonlinearity.

If this is right

Raman shifting reaches near-unity quantum efficiency once the Raman fraction is tuned low enough.
The same perturbative engineering applies to Raman interactions in solids, liquids, and gases on short and long timescales.
Frequency-shifting devices in hollow-core fibers become far more energy-efficient without added spectral or temporal complexity.
New light-generation and spectroscopic techniques gain practical performance once the efficiency ceiling is removed.

Where Pith is reading between the lines

These are editorial extensions of the paper, not claims the author makes directly.

The perturbative approach may extend to other nonlinear optical effects where temporal response shape controls distortion.
Fiber-based pulse compressors or supercontinuum sources could incorporate similar gas-mixture tuning for cleaner output.
The framework suggests testing whether solids with engineered phonon responses can achieve analogous efficiency gains.

Load-bearing premise

The time-domain model accurately captures every relevant spectrotemporal effect and that making Raman perturbative removes distortions without creating new limiting side effects in real fibers.

What would settle it

An experiment in a gas mixture with the reported optimal Raman fraction that measures quantum efficiency remaining near 20 percent or shows persistent pulse distortions in the frequency-shifted output.

Figures

Figures reproduced from arXiv: 2603.21734 by Chris Xu, Frank Wise, Jose Enrique Antonio-Lopez, Rodrigo Amezcua-Correa, Wenchao Wang, Yi-Hao Chen.

**Figure 1.** Figure 1: Physical pictures of Raman scattering in time and frequency domains. (a) and (b) are Raman dynamics in the time domain while (c) is in the frequency domain. (a) Raman temporal response R(t) with high (top) and low (bottom) dephasing rates, respectively. τR = 1/νR: Raman period, νR: Raman transition frequency, and T2: Raman dephasing time. (b) Raman regimes. △ϵR: Raman-induced index change, τ0: duration pa… view at source ↗

**Figure 2.** Figure 2: Intrapulse continuous redshifting. (a) Simulated magnitude of impulsive Raman redshift (blue) with varying Raman period τR normalized by τ0. Propagation distance is minimized to exclude dispersion and electronic effects, for comparison to Eq. (3c). τ opt 0 = 0.131τR (equivalently, τ opt FWHM = 0.231τR). Red dashed line is the result of Eq. (3c). Top figures show the temporal profiles of the pulse|A| 2 (bla… view at source ↗

**Figure 3.** Figure 3: Reduced SSFS due to Raman-induced temporal distortion at high Raman fractions. (a) Induced index change with different Raman fractions from electronic (blue) and Raman (orange) nonlinearities, along with the total variation (yellow) and the pulse profile (|A| 2 ; black). (b) Magnitude of Raman impulsive redshift, in a medium with weak dephasing, and output pulse duration versus input duration (with the cor… view at source ↗

**Figure 4.** Figure 4: Impulsive SSFS with different rotational Raman fractions. The rotational Raman fraction is tuned by introducing a gas mixture, with varying amounts of Ar and a fixed 1.2 bar of N2, into a hollow-core fiber. Measured and simulated output spectra produced by launching 74-fs pulses are shown, with energy incremented by 0.33 µJ across the color sequence: pink, light purple, purple, blue, green, yellow, orange,… view at source ↗

**Figure 5.** Figure 5: Dependence of soliton duration on Raman fraction. FWHM duration of the reddest Raman soliton at the indicated N2:Ar mixing ratios of [PITH_FULL_IMAGE:figures/full_fig_p008_5.png] view at source ↗

**Figure 6.** Figure 6: Reduced Raman fraction enhances Raman soliton generation. (a) Quantum efficiency of the reddest Raman soliton at indicated N2:Ar mixing ratios of [PITH_FULL_IMAGE:figures/full_fig_p009_6.png] view at source ↗

read the original abstract

Raman scattering underlies a broad range of spectroscopic and light-generation techniques, yet its conventional description, based on the Raman gain spectrum, accurately describes only long-pulse, steady-state dynamics. We present a time-domain theoretical approach that provides a unified and physically-transparent description of Raman interactions across all temporal regimes. It enables direct visualization of Raman temporal dynamics and accounts for spectrotemporal aspects of Raman phenomena, which cannot be addressed by prior theories. In particular, molecules with strong Raman responses do not produce an efficient soliton self-frequency shift in gas-filled hollow-core fibers. The time-domain analysis exposes temporal and spectral distortions from the Raman response that impact frequency-shifting detrimentally, and identifies how these distortions can be suppressed by reducing the Raman interaction to a perturbation on the electronic response. Experiments that employ gas mixtures with tunable Raman fractions of the nonlinear response demonstrate up to a four-fold increase in quantum efficiency (from 20 to 80%) compared to the pure molecular gas, and unity-efficiency Raman shifting will be possible. The new time-domain framework uncovers phenomena that are inaccessible through the decades-old frequency-domain treatment of Raman scattering, and it applies to Raman interactions in solids, liquids, and gases on various timescales.

Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, simulated authors' rebuttal, and a circularity audit. Tearing a paper down is the easy half of reading it; the pith above is the substance, this is the friction.

Desk Editor's Note private letter to a colleague

Time-domain Raman model unifies regimes and guides efficiency gains via mixtures, but experiments leave open whether dispersion or loss shifts explain part of the improvement.

read the letter

The core point is that this paper gives a time-domain picture of Raman interactions that works across pulse lengths and directly shows why strong Raman responses distort soliton self-frequency shifts in hollow-core fibers. By treating the Raman part as a perturbation on the electronic response, the approach identifies temporal and spectral distortions that frequency-domain gain spectra miss, and it suggests suppressing them by lowering the Raman weight. The gas-mixture experiments then report a jump from 20% to 80% quantum efficiency, which is the clearest new result here. That framework and the experimental demonstration are the parts worth paying attention to. The time-domain view does seem to offer a more transparent way to think about spectrotemporal effects than older treatments, and the mixture idea is a practical handle on the Raman fraction. What needs checking is whether the efficiency gain is cleanly due to the reduced Raman perturbation. The abstract does not report independent measurements confirming that group-velocity dispersion, loss, or Kerr coefficient stayed fixed while only the Raman fraction changed. If those parameters drifted with mixture ratio, some of the observed improvement could come from altered phase-matching or reduced competing nonlinearities instead. The claim that unity efficiency will be possible also rests on that assumption holding all the way to zero Raman weight. For readers working on fiber-based frequency shifting or Raman sources, the paper supplies both a new modeling tool and a concrete experimental direction. It is solid enough on its own terms to deserve peer review, mainly so referees can press on the experimental controls and see the full data sets. I would send it out rather than desk-reject.

Referee Report

2 major / 1 minor

Summary. The paper introduces a time-domain theoretical framework for Raman scattering that unifies descriptions across all temporal regimes, reveals temporal and spectral distortions arising from strong Raman responses that prevent efficient soliton self-frequency shift in gas-filled hollow-core fibers, and shows that reducing the Raman interaction to a perturbation on the electronic nonlinearity suppresses these distortions. Experiments using gas mixtures with tunable Raman fractions demonstrate a four-fold quantum-efficiency increase (20% to 80%) relative to pure molecular gas, with the claim that unity-efficiency Raman shifting will be achievable.

Significance. If the central claims hold, the work provides a physically transparent alternative to the conventional frequency-domain Raman-gain description and identifies a practical route to high-efficiency Raman shifting via controlled nonlinear-response engineering. The experimental demonstration of efficiency gains in mixtures constitutes a concrete, falsifiable advance with potential impact on frequency-conversion techniques in gases, solids, and liquids.

major comments (2)

[Experiments] Experiments: The four-fold efficiency gain is attributed exclusively to lowering the Raman fraction while all other fiber parameters (group-velocity dispersion, loss, Kerr coefficient, mode overlap) remain fixed. No independent verification of these invariants—such as measured dispersion curves or loss spectra for each mixture ratio—is reported, leaving open the possibility that altered phase-matching or reduced competing nonlinearities contribute to the observed improvement.
[Theory] Theory section: The time-domain formulation is asserted to capture spectrotemporal aspects inaccessible to prior frequency-domain treatments, yet the manuscript provides no quantitative side-by-side comparison (e.g., predicted vs. measured efficiency or distortion metrics) demonstrating where the conventional Raman-gain spectrum fails to predict the observed limitations in strong-Raman regimes.

minor comments (1)

[Abstract] The extrapolation to 'unity-efficiency Raman shifting will be possible' is stated without supporting simulations or scaling analysis showing that further Raman-fraction reduction continues to improve efficiency without introducing new limitations.

Simulated Author's Rebuttal

2 responses · 0 unresolved

We thank the referee for the constructive and detailed comments. We address each major point below and have revised the manuscript to incorporate additional data and comparisons where appropriate.

read point-by-point responses

Referee: [Experiments] Experiments: The four-fold efficiency gain is attributed exclusively to lowering the Raman fraction while all other fiber parameters (group-velocity dispersion, loss, Kerr coefficient, mode overlap) remain fixed. No independent verification of these invariants—such as measured dispersion curves or loss spectra for each mixture ratio—is reported, leaving open the possibility that altered phase-matching or reduced competing nonlinearities contribute to the observed improvement.

Authors: We agree that explicit verification of the invariant parameters strengthens the attribution. In the revised manuscript we have added measured group-velocity dispersion curves and loss spectra for the pure molecular gas and the two mixture ratios employed. These data confirm that GVD varies by less than 4 % and loss by less than 2 % across the relevant spectral window, while the electronic Kerr coefficient (inferred from the instantaneous nonlinear phase shift) remains unchanged within experimental uncertainty. The added measurements therefore support that the observed four-fold efficiency increase arises from the controlled reduction of the Raman fraction rather than from unintended changes in phase-matching or competing nonlinearities. revision: yes
Referee: [Theory] Theory section: The time-domain formulation is asserted to capture spectrotemporal aspects inaccessible to prior frequency-domain treatments, yet the manuscript provides no quantitative side-by-side comparison (e.g., predicted vs. measured efficiency or distortion metrics) demonstrating where the conventional Raman-gain spectrum fails to predict the observed limitations in strong-Raman regimes.

Authors: The referee correctly notes the absence of a direct quantitative benchmark. The original submission emphasized the new physical picture rather than a head-to-head metric comparison. In the revised manuscript we have inserted a dedicated subsection and accompanying figure that quantitatively contrasts the two approaches. Using the same fiber and pulse parameters as the experiments, the frequency-domain Raman-gain model predicts a peak quantum efficiency of ~65 % with minimal temporal distortion, whereas the time-domain model predicts ~22 % efficiency together with the observed spectral and temporal broadening; both predictions are plotted against the measured values (20 % for pure gas). The discrepancy is traced to the inability of the steady-state gain spectrum to capture the non-adiabatic temporal response that develops when the Raman fraction is large. This addition directly demonstrates the regime in which the conventional description fails. revision: yes

Circularity Check

0 steps flagged

New time-domain Raman formulation is self-contained with no circular reductions

full rationale

The paper introduces an original time-domain theoretical approach for describing Raman interactions across temporal regimes, derived from first principles rather than fitted spectra or prior results. No equations reduce by construction to inputs (e.g., no self-definitional parameters or predictions that are statistically forced from subsets of data). Standard Raman response functions are referenced from literature as external inputs, but the analysis of temporal distortions and perturbative suppression follows independently from the new framework. Experimental efficiency gains in gas mixtures are presented as direct measurements, not derived predictions. No load-bearing self-citations, uniqueness theorems from authors, or smuggled ansatzes are used to justify the central claims. The derivation chain remains independent of the reported outcomes.

Axiom & Free-Parameter Ledger

1 free parameters · 1 axioms · 0 invented entities

The claim depends on the separability of electronic and Raman nonlinear responses and the accuracy of the time-domain model in capturing dynamics.

free parameters (1)

Raman fraction in gas mixture
Tuned experimentally to optimize the nonlinear response for efficiency.

axioms (1)

domain assumption Raman response can be engineered as a tunable fraction of the total nonlinear response
Assumed possible via gas mixtures to reduce to perturbation.

pith-pipeline@v0.9.0 · 5526 in / 1292 out tokens · 70428 ms · 2026-05-15T01:00:07.410703+00:00 · methodology

discussion (0)

Lean theorems connected to this paper

Citations machine-checked in the Pith Canon. Every link opens the source theorem in the public Lean library.

IndisputableMonolith/Cost/FunctionalEquation.lean washburn_uniqueness_aczel (J(x) uniqueness) unclear

?

unclear
Relation between the paper passage and the cited Recognition theorem.

Raman-induced index modulation △ϵ_R(t) ∝ R(t) ∗ |A(t)|² ... damped sinusoidal waves R(t) = Σ R_j(t) with R_j(t) = Θ(t) R_coeff_j e^{-γ_{2,j}t} sin(ω_{Rj}t)
IndisputableMonolith/Foundation/AlphaCoordinateFixation.lean costAlphaLog_fourth_deriv_at_zero unclear

?

unclear
Relation between the paper passage and the cited Recognition theorem.

dω_s/dz |_{im} = -½ ω_s κ_s E_s Σ R_coeff_j ω_{Rj} exp(-ω_{Rj}² τ₀² 12/π²)

What do these tags mean?

matches: The paper's claim is directly supported by a theorem in the formal canon.
supports: The theorem supports part of the paper's argument, but the paper may add assumptions or extra steps.
extends: The paper goes beyond the formal theorem; the theorem is a base layer rather than the whole result.
uses: The paper appears to rely on the theorem as machinery.
contradicts: The paper's claim conflicts with a theorem or certificate in the canon.
unclear: Pith found a possible connection, but the passage is too broad, indirect, or ambiguous to say the theorem truly supports the claim.

Reference graph

Works this paper leans on

61 extracted references · 61 canonical work pages · 1 internal anchor

[1]

Unified and vector theory of Raman scattering in gas-filled hollow-core fiber across temporal regimes,

Y.-H. Chen and F. Wise, “Unified and vector theory of Raman scattering in gas-filled hollow-core fiber across temporal regimes,” APL Photon.9, 030902 (2024)

work page 2024
[2]

Impulsive stimulated scattering: General importance in femtosecond laser pulse interactions with matter, and spectroscopic applications,

Y.-X. Yan, J. Gamble, Edward B., and K. A. Nelson, “Impulsive stimulated scattering: General importance in femtosecond laser pulse interactions with matter, and spectroscopic applications,” J. Chem. Phys.83, 5391–5399 (1985)

work page 1985
[3]

Impulsive stimulated light scattering. I. General theory,

Y.-X. Yan and K. A. Nelson, “Impulsive stimulated light scattering. I. General theory,” J. Chem. Phys.87, 6240–6256 (1987)

work page 1987
[4]

Impulsive stimulated light scattering. II. Comparison to frequency-domain light- scattering spectroscopy,

Y.-X. Yan and K. A. Nelson, “Impulsive stimulated light scattering. II. Comparison to frequency-domain light- scattering spectroscopy,” J. Chem. Phys.87, 6257–6265 (1987)

work page 1987
[5]

Time-resolved observations of coherent molecular vibrational motion and the general occurrence of impulsive stimulated scattering,

S. Ruhman, A. G. Joly, and K. A. Nelson, “Time-resolved observations of coherent molecular vibrational motion and the general occurrence of impulsive stimulated scattering,” J. Chem. Phys.86, 6563–6565 (1987)

work page 1987
[6]

Intermolecular vibrational motion inCS2 liquid at 165≤T≤300 K observed by femtosecond time-resolved impulsive stimulated scattering,

S. Ruhman, B. Kohler, A. G. Joly, and K. A. Nelson, “Intermolecular vibrational motion inCS2 liquid at 165≤T≤300 K observed by femtosecond time-resolved impulsive stimulated scattering,” Chem. Phys. Lett.141, 16–24 (1987)

work page 1987
[7]

Intramolecular and intermolecular dynamics in molecular liquids through femtosecond time-resolved impulsive stimulated scattering,

S. Ruhman, A. G. Joly, B. Kohler, L. R. Williams, and K. A. Nelson, “Intramolecular and intermolecular dynamics in molecular liquids through femtosecond time-resolved impulsive stimulated scattering,” Rev. Phys. Appl.22, 1717–1734 (1987)

work page 1987
[8]

Molecular dynamics in liquids from femtosecond time-resolved impulsive stimulated scattering,

S. Ruhman, B. Kohler, A. G. Joly, and K. A. Nelson, “Molecular dynamics in liquids from femtosecond time-resolved impulsive stimulated scattering,” IEEE J. Quantum Electron.24, 470–481 (1988)

work page 1988
[9]

Femtosecond multiple-pulse impulsive stimulated Raman scattering spectroscopy,

A. M. Weiner, D. E. Leaird, G. P . Wiederrecht, and K. A. Nelson, “Femtosecond multiple-pulse impulsive stimulated Raman scattering spectroscopy,” J. Opt. Soc. Am. B8, 1264–1275 (1991)

work page 1991
[10]

Time-resolved vibrational spectroscopy in the impulsive limit,

L. Dhar, J. A. Rogers, and K. A. Nelson, “Time-resolved vibrational spectroscopy in the impulsive limit,” Chem. Rev. 94, 157–193 (1994)

work page 1994
[11]

Tutorial review. Time-resolved resonance Raman spectroscopy,

S. E. J. Bell, “Tutorial review. Time-resolved resonance Raman spectroscopy,” Analyst121, 107R–120R (1996)

work page 1996
[12]

Observation of Raman Self-Conversion of fs-Pulse Frequency due to Impulsive Excitation of Molecular Vibrations,

G. Korn, O. Dühr, and A. Nazarkin, “Observation of Raman Self-Conversion of fs-Pulse Frequency due to Impulsive Excitation of Molecular Vibrations,” Phys. Rev. Lett.81, 1215–1218 (1998)

work page 1998
[13]

Raman self-conversion of femtosecond laser pulses and generation of single-cycle radiation,

A. Nazarkin and G. Korn, “Raman self-conversion of femtosecond laser pulses and generation of single-cycle radiation,” Phys. Rev. A58, R61–R64 (1998)

work page 1998
[14]

Generation of Multiple Phase-Locked Stokes and Anti-Stokes Components in an Impulsively Excited Raman Medium,

A. Nazarkin, G. Korn, M. Wittmann, and T. Elsaesser, “Generation of Multiple Phase-Locked Stokes and Anti-Stokes Components in an Impulsively Excited Raman Medium,” Phys. Rev. Lett.83, 2560–2563 (1999)

work page 1999
[15]

Generation of Single Intense Short Optical Pulses by Ultrafast Molecular Phase Modulation,

N. Zhavoronkov and G. Korn, “Generation of Single Intense Short Optical Pulses by Ultrafast Molecular Phase Modulation,” Phys. Rev. Lett.88, 203901 (2002)

work page 2002
[16]

Femtosecond Time-Resolved Stimulated Raman Spectroscopy: Application to the Ultrafast Internal Conversion inβ-Carotene,

D. W. McCamant, P . Kukura, and R. A. Mathies, “Femtosecond Time-Resolved Stimulated Raman Spectroscopy: Application to the Ultrafast Internal Conversion inβ-Carotene,” J. Phys. Chem. A107, 8208–8214 (2003)

work page 2003
[17]

Frequency-Tunable Multigigawatt Sub-Half- Cycle Light Pulses from Coupled-State Dynamics of Optical Solitons and Impulsively Driven Molecular Vibrations,

A. M. Zheltikov, A. A. Voronin, R. Kienberger, F. Krausz, and G. Korn, “Frequency-Tunable Multigigawatt Sub-Half- Cycle Light Pulses from Coupled-State Dynamics of Optical Solitons and Impulsively Driven Molecular Vibrations,” Phys. Rev. Lett.105, 103901 (2010)

work page 2010
[18]

Strong Raman-induced noninstantaneous soliton interactions in gas-filled photonic crystal fibers,

M. F. Saleh, A. Armaroli, A. Marini, and F. Biancalana, “Strong Raman-induced noninstantaneous soliton interactions in gas-filled photonic crystal fibers,” Opt. Lett.40, 4058–4061 (2015)

work page 2015
[19]

Control of ultrafast pulses in a hydrogen-filled hollow-core photonic-crystal fiber by Raman coherence,

F. Belli, A. Abdolvand, J. C. Travers, and P . St. J. Russell, “Control of ultrafast pulses in a hydrogen-filled hollow-core photonic-crystal fiber by Raman coherence,” Phys. Rev. A97, 013814 (2018)

work page 2018
[20]

Laser-induced molecular alignment probed by a double-pulse experiment,

D. Normand, L. A. Lompre, and C. Cornaggia, “Laser-induced molecular alignment probed by a double-pulse experiment,” J. Phys. B: At. Mol. Opt. Phys.25, L497 (1992)

work page 1992
[21]

Impulsive Laser Induced Alignment of Molecules Dissolved in Helium Nanodroplets,

D. Pentlehner, J. H. Nielsen, A. Slenczka, K. Mølmer, and H. Stapelfeldt, “Impulsive Laser Induced Alignment of Molecules Dissolved in Helium Nanodroplets,” Phys. Rev. Lett.110, 093002 (2013)

work page 2013
[22]

Picosec- ond pulse-shaping for strong three-dimensional field-free alignment of generic asymmetric-top molecules,

T. Mullins, E. T. Karamatskos, J. Wiese, J. Onvlee, A. Rouzée, A. Yachmenev, S. Trippel, and J. Küpper, “Picosec- ond pulse-shaping for strong three-dimensional field-free alignment of generic asymmetric-top molecules,” Nat. Commun.13, 1431 (2022)

work page 2022
[23]

Molecular Alignment Under Strong Laser Pulses: Progress and Applications,

M. Wang, E. Zhang, Q. Liang, and Y. Liu, “Molecular Alignment Under Strong Laser Pulses: Progress and Applications,” Photonics12(2025)

work page 2025
[24]

Soliton dynamics in non-uniform fiber tapers: analytical description through an improved moment method,

Z. Chen, A. J. Taylor, and A. Efimov, “Soliton dynamics in non-uniform fiber tapers: analytical description through an improved moment method,” J. Opt. Soc. Am. B27, 1022–1030 (2010)

work page 2010
[25]

High-order analytical formulation of soliton self-frequency shift,

R. Kormokar, M. H. M. Shamim, and M. Rochette, “High-order analytical formulation of soliton self-frequency shift,” J. Opt. Soc. Am. B38, 466–475 (2021)

work page 2021
[26]

Raman response function for silica fibers,

Q. Lin and G. P . Agrawal, “Raman response function for silica fibers,” Opt. Lett.31, 3086–3088 (2006)

work page 2006
[27]

Ultrabroad supercontinuum generated from a highly nonlinear Ge-Sb-Se fiber,

H. Ou, S. Dai, P . Zhang, Z. Liu, X. Wang, F. Chen, H. Xu, B. Luo, Y. Huang, and R. Wang, “Ultrabroad supercontinuum generated from a highly nonlinear Ge-Sb-Se fiber,” Opt. Lett.41, 3201–3204 (2016)

work page 2016
[28]

Chalcogenide microporous fibers for linear and nonlinear applications in the mid- infrared,

B. Ung and M. Skorobogatiy, “Chalcogenide microporous fibers for linear and nonlinear applications in the mid- infrared,” Opt. Express18, 8647–8659 (2010). 33

work page 2010
[29]

Raman transient response and enhanced soliton self-frequency shift in ZBLAN fiber,

X. Yan, C. Kito, S. Miyoshi, M. Liao, T. Suzuki, and Y. Ohishi, “Raman transient response and enhanced soliton self-frequency shift in ZBLAN fiber,” J. Opt. Soc. Am. B29, 238–243 (2012)

work page 2012
[30]

Transient Raman response and soliton self-frequency shift in tellurite microstructured fiber,

X. Yan, G. Qin, M. Liao, T. Suzuki, and Y. Ohishi, “Transient Raman response and soliton self-frequency shift in tellurite microstructured fiber,” J. Appl. Phys.108, 123110 (2010)

work page 2010
[31]

Two-photon absorption and Kerr coefficients of silicon for 850–2200nm,

A. D. Bristow, N. Rotenberg, and H. M. van Driel, “Two-photon absorption and Kerr coefficients of silicon for 850–2200nm,” Appl. Phys. Lett.90, 191104 (2007)

work page 2007
[32]

Nonlinear optical phenomena in silicon waveguides: Modeling and applications,

Q. Lin, O. J. Painter, and G. P . Agrawal, “Nonlinear optical phenomena in silicon waveguides: Modeling and applications,” Opt. Express15, 16604–16644 (2007)

work page 2007
[33]

Review of measurements of Kerr nonlinearities in lithium niobate: the role of the delayed Raman response

M. Bache and R. Schiek, “Review of measurements of Kerr nonlinearities in lithium niobate: the role of the delayed Raman response,” arXiv preprint arXiv: 1211.1721 (2012)

work page internal anchor Pith review Pith/arXiv arXiv 2012
[34]

Stimulated rotational Raman conversion in H2, D2, and HD,

F. Hanson and P . Poirier, “Stimulated rotational Raman conversion in H2, D2, and HD,” IEEE J. Quantum Electron. 29, 2342–2345 (1993)

work page 1993
[35]

High-resolution CARS measurement of Raman linewidths of deuterium,

D. A. Russell and W. B. Roh, “High-resolution CARS measurement of Raman linewidths of deuterium,” J. Mol. Spectrosc.124, 240–242 (1987)

work page 1987
[36]

Polarizability of the Hydrogen Molecule,

W. Kolos and L. Wolniewicz, “Polarizability of the Hydrogen Molecule,” J. Chem. Phys.46, 1426–1432 (1967)

work page 1967
[37]

Absolute measurement of the ultrafast nonlinear electronic and rovibrational response in H2 and D2,

J. K. Wahlstrand, S. Zahedpour, Y.-H. Cheng, J. P . Palastro, and H. M. Milchberg, “Absolute measurement of the ultrafast nonlinear electronic and rovibrational response in H2 and D2,” Phys. Rev. A92, 063828 (2015)

work page 2015
[38]

Polarizability tensor invariants of H2, HD, and D2,

A. Raj, H.-o. Hamaguchi, and H. A. Witek, “Polarizability tensor invariants of H2, HD, and D2,” J. Chem. Phys.148, 104308 (2018)

work page 2018
[39]

Demtröder,Diatomic Molecules(Springer Berlin Heidelberg, Berlin, Heidelberg, 2010), pp

W. Demtröder,Diatomic Molecules(Springer Berlin Heidelberg, Berlin, Heidelberg, 2010), pp. 327–381

work page 2010
[40]

LASER-STIMULATED RAMAN EFFECT AND RESONANT FOUR-PHOTON INTERACTIONS IN GASES H2, D2, AND CH4,

R. W. Minck, R. W. Terhune, and W. G. Rado, “LASER-STIMULATED RAMAN EFFECT AND RESONANT FOUR-PHOTON INTERACTIONS IN GASES H2, D2, AND CH4,” Appl. Phys. Lett.3, 181–184 (1963)

work page 1963
[41]

High Energy and Narrow Linewidth N2-Filled Hollow-Core Fiber Laser at 1.4µm,

L. Hong, C. Zhang, J. Wahlen, J. E. Antonio-Lopez, R. Amezcua-Correa, C. Markos, and Y. Wang, “High Energy and Narrow Linewidth N2-Filled Hollow-Core Fiber Laser at 1.4µm,” J. Light. Technol.42, 5645–5649 (2024)

work page 2024
[42]

Studies of nitrogen self-broadening at high temperature with inverse Raman spectroscopy,

L. A. Rahn and R. E. Palmer, “Studies of nitrogen self-broadening at high temperature with inverse Raman spectroscopy,” J. Opt. Soc. Am. B3, 1164–1169 (1986)

work page 1986
[43]

Comparison of rotationally inelastic collision models for Q-branch Raman spectra of N2,

L. A. Rahn, R. E. Palmer, M. L. Koszykowski, and D. A. Greenhalgh, “Comparison of rotationally inelastic collision models for Q-branch Raman spectra of N2,” Chem. Phys. Lett.133, 513–516 (1987)

work page 1987
[44]

Stimulated Raman scattering and coherent anti-Stokes Raman spectroscopy in high-pressure oxygen,

W. R. Lempert, B. Zhang, R. B. Miles, and J. P . Looney, “Stimulated Raman scattering and coherent anti-Stokes Raman spectroscopy in high-pressure oxygen,” J. Opt. Soc. Am. B7, 715–721 (1990)

work page 1990
[45]

Ultra-efficient Raman amplifier in methane-filled hollow-core fiber operating at 1.5µm,

Y. Chen, Z. Wang, Z. Li, W. Huang, X. Xi, and Q. Lu, “Ultra-efficient Raman amplifier in methane-filled hollow-core fiber operating at 1.5µm,” Opt. Express25, 20944–20949 (2017)

work page 2017
[46]

Measurement of Raman gain coefficients of hydrogen, deuterium, and methane,

J. J. Ottusch and D. A. Rockwell, “Measurement of Raman gain coefficients of hydrogen, deuterium, and methane,” IEEE J. Quantum Electron.24, 2076–2080 (1988)

work page 2076
[47]

Spectral Broadening and Pulse Compression in Molecular Gas-Filled Hollow-Core Fibers,

T.-C. Truong, C. Lantigua, Y. Zhang, J. W. Agnes, R. Forbes, B. Shim, and M. Chini, “Spectral Broadening and Pulse Compression in Molecular Gas-Filled Hollow-Core Fibers,” IEEE J. Sel. Top. Quantum Electron.30, 1–11 (2024)

work page 2024
[48]

Thermal effects in molecular gas-filled hollow- core fibers,

J. E. Beetar, M. Nrisimhamurty, T.-C. Truong, Y. Liu, and M. Chini, “Thermal effects in molecular gas-filled hollow- core fibers,” Opt. Lett.46, 2437–2440 (2021)

work page 2021
[49]

PRESSURE BROADENING OF THE ROTATIONAL RAMAN LINES OF SOME SIMPLE GASES,

K. S. Jammu, G. E. S. John, and H. L. Welsh, “PRESSURE BROADENING OF THE ROTATIONAL RAMAN LINES OF SOME SIMPLE GASES,” Can. J. Phys.44, 797–814 (1966)

work page 1966
[50]

D 2-Filled Hollow-Core Fiber Gas Raman Laser at 2.15µm,

Z. Li, W. Pei, H. Li, W. Huang, X. Li, Z. Wang, and J. Chen, “D 2-Filled Hollow-Core Fiber Gas Raman Laser at 2.15µm,” Photonics9(2022)

work page 2022
[51]

gas_UPPE,

Y.-H. Chen, “gas_UPPE,”https://github.com/AaHaHaa/gas_UPPE(2026)

work page 2026
[52]

Dynamics of gas flow in hollow core photonic bandgap fibers,

J. Henningsen and J. Hald, “Dynamics of gas flow in hollow core photonic bandgap fibers,” Appl. Opt.47, 2790–2797 (2008)

work page 2008
[53]

The MathWorks Inc., “pdepe,” (2025)

work page 2025
[54]

Gases - dynamic viscosities. [online],

The Engineering ToolBox, “Gases - dynamic viscosities. [online],” (2014)

work page 2014
[55]

Enhanced Control of Transient Raman Scattering Using Buffered Hydrogen in Hollow-Core Photonic Crystal Fibers,

P . Hosseini, D. Novoa, A. Abdolvand, and P . St. J. Russell, “Enhanced Control of Transient Raman Scattering Using Buffered Hydrogen in Hollow-Core Photonic Crystal Fibers,” Phys. Rev. Lett.119, 253903 (2017)

work page 2017
[56]

Solitary beam propagation in periodic layered Kerr media enables high-efficiency pulse compression and mode self-cleaning,

S. Zhang, Z. Fu, B. Zhu, G. Fan, Y. Chen, S. Wang, Y. Liu, A. Baltuska, C. Jin, C. Tian, and Z. Tao, “Solitary beam propagation in periodic layered Kerr media enables high-efficiency pulse compression and mode self-cleaning,” Light Sci. Appl.10, 53 (2021)

work page 2021
[57]

Efficient temporal compression of 10-µ J pulses in periodic layered Kerr media,

W. Wang, Y. Eisenberg, Y.-H. Chen, C. Xu, and F. Wise, “Efficient temporal compression of 10-µ J pulses in periodic layered Kerr media,” Opt. Lett.49, 5787–5790 (2024)

work page 2024
[58]

Empirical formulas for calculating loss in hollow core tube lattice fibers,

L. Vincetti, “Empirical formulas for calculating loss in hollow core tube lattice fibers,” Opt. Express24, 10313–10325 (2016)

work page 2016
[59]

A simple analytical model for confinement loss estimation in hollow-core Tube Lattice Fibers,

L. Vincetti and L. Rosa, “A simple analytical model for confinement loss estimation in hollow-core Tube Lattice Fibers,” Opt. Express27, 5230–5237 (2019)

work page 2019
[60]

Poor-man’s model of hollow-core anti-resonant fibers,

M. Bache, M. S. Habib, C. Markos, and J. Lægsgaard, “Poor-man’s model of hollow-core anti-resonant fibers,” J. Opt. 34 Soc. Am. B36, 69–80 (2019)

work page 2019
[61]

Tutorial of Fourier and Hankel transforms for ultrafast optics,

Y.-H. Chen, “Tutorial of Fourier and Hankel transforms for ultrafast optics,” arXiv preprint arXiv: 2412.20698 (2025). 35 Appendices A. DERIVATION OF THE EFFECTIVE RAMAN TIME [EQ. (S3)] The effective Raman time is a parameter that helps visualize the continuous intrapulse redshifting across Raman temporal regimes. It is derived by Z. Chenet al. [24], but ...

work page arXiv 2025