Raman Pump Research Articles

Overtone Excitation of Nitrogen Molecules via Stimulated Raman Pumping.

Nitrogen bond activation is a pivotal process in chemistry, with bond excitation being fundamental to understanding the underlying mechanisms, making the preparation of molecules in specific quantum states crucial. Here we report the first overtone excitation of the N2 molecule from X1Σg+(v = 0, j = 0, 1, and 2) to X1Σg+(v = 2, j = 0, 1, 2, and 3) using the stimulated Raman pumping (SRP) method in a pulsed molecular beam. N2 was detected using 2+1 resonance-enhanced multiphoton ionization through the a″1Σg+ state. An excitation efficiency of 4% was achieved within the excitation region in which the SRP laser intensity was saturated, indicating the low cross-sectional nature of the process. The SRP detuning spectra for different branches were measured, and the excited N2 [X1Σg+(v = 2)] was further used to access various vibrational states of a″1Σg+, enabling the determination of its vibrational constants. This research opens up new opportunities for studying the specific high vibrational excitation of nitrogen in reactions and scattering experiments and contributes additional precise spectral data for the N2 molecule.

Ultra‐Broadband Visible‐DUV Supercontinuum Generation by Non‐Resonant Coherent Raman Scattering in Air

AbstractTo date, supercontinuum light in the visible and near‐infrared ranges is readily realizable by the optical Kerr effect through self‐phase modulation of ultrashort laser pulses in transparent media. However, it is still a challenge to extend the supercontinuum spectrum down to the deep‐ultraviolet (DUV) range, which is particularly needed for exploring ultrafast dynamics in chemistry, materials, and biology. Here, an approach of non‐resonant coherent Raman scattering is developed to generate ultra‐broadband visible‐DUV supercontinuum in ambient air with a spectral range spanning over 250 nm and a wavelength down to 220 nm. A rovibrational coherence is established in air molecules by filamentation of a near‐infrared femtosecond 800 nm pulse and two femtosecond Raman laser pulses at 267 and 400 nm are introduced into the coherent media to induce non‐resonant coherent Stokes and anti‐Stokes Raman scatterings, which serve as the spectral bridges to link the neighboring Raman pump laser spectra, resulting in ultra‐broadband supercontinuum light. The mechanism is further verified by examining the broadening of picosecond N2+ laser lines with narrow bandwidths (10–30 cm−1), which forms a supercontinuum spectrum spanning over 150 nm. The work provides a viable route for the establishment of coherent DUV supercontinuum in the gas media at designed wavelength ranges.

Inverse Design of Incoherent Raman Pump Sources for U-Band WDM Transmission Over 125 km G.652.D Fiber

Inverse Design of Incoherent Raman Pump Sources for U-Band WDM Transmission Over 125 km G.652.D Fiber

Unrepeatered transmission of single-carrier 800 Gb/s over 447.96 km with simplified third-order ROPA system

Abstract To achieve the longest distance of 800 Gb/s unrepeatered transmission, we use commercial 800 Gb/s transceivers with soft-decision FEC, optimized high-order Raman pumps, and enhanced bidirectional ROPA with third-order Raman pumping in this experiment to optimize system performance. Two types of G.654E fibers are also fully characterized and used as span fibers. The improvement of transmission distance is mainly due to the remote pump power for RGU can be increased by nearly 4 dB in G.654E fiber by the third-order Raman pumping. At last, a single 800 Gb/s channel is transmitted over 447.96 km with a span loss of 73.16 dB. As far as we know, this is the longest 800 Gb/s unrepeatered transmission distance ever reported.

Water Solvent Reorganization upon Ultrafast Resonant Stimulated X-ray Raman Excitation of a Metalloporphyrin Dimer.

We propose an X-ray Raman pump-X-ray diffraction probe scheme to follow solvation dynamics upon charge migration in a solute molecule. The X-ray Raman pump selectively prepares a valence electronic wavepacket in the solute, while the probe provides information about the entire molecular ensemble. A combination of molecular dynamics and ab initio quantum chemistry simulations is applied to a Zn-Ni porphyrin dimer in water. Using time-resolved X-ray diffraction and pair distribution functions, we extracted solvation shell dynamics.

Experimental study of rotational relaxation for D2(1,12) in collisions with N2.

The rotational relaxation behavior of D2(1,12) in a D2-N2 mixture was investigated using coherent anti-Stokes Raman scattering (CARS) technique. The rovibrational level v = 1 and J = 12 of D2 was selectively excited through stimulated Raman pumping while monitoring the temporal evolution of population for D2(1, J ≤ 12) molecules using time-resolved CARS spectroscopy. The results demonstrate that the rotational relaxation processes of D2(1,12) encompass both multi-quantum relaxation and continuous single-quantum relaxation. When α, the molar ratio of N2, is less than 0.5, D2(1,12) predominantly undergoes a single quantum relaxation process transition. However, when α ≥ 0.5, the multi-quantum relaxation mechanism gradually predominates. The total rotational relaxation rate coefficients of D2(1,12) collisions with N2 and D2 at 295K were determined to be 3.974 × 10-14 and 1.179 × 10-14cm3s-1, respectively. The temperature dependence of rotational relaxation rate of D2(1,12) was investigated within the temperature range of 295-453K. With increasing temperature, the dominant relaxation process exhibited an accelerated behavior, while the minor relaxation process remained largely unaffected. The rotational temperature of the D2molecule at various N2 molar ratios was determined through the utilization of Boltzmann plots. The rotational temperature undergoes a rapid decline within 2 μs, corresponding to the near-resonant rotation-vibration relaxation process of D2(1,12) collisions with N2. The system reaches a quasi-equilibrium state when the delay time is 3 μs. The findings of this study can serve as a valuable empirical basis for further validation of the kinetic theory and simulation.

OSNR enhancement of Rayleigh-assisted Brillouin-Raman fiber laser via double pass configuration.

We propose and demonstrate a 10 GHz spacing multi-wavelength Brillouin-Raman fiber laser (MBRFL) with wide bandwidth and an outstanding optical signal-to-noise ratio (OSNR). This is achieved by utilizing loop mirror at one end of the laser cavity through a symmetrical bi-directional Raman pumping scheme. The setup is arranged in a double pass configuration by employing different lengths of dispersion compensating fibers (DCF). The attainment of MBRFL with outstanding performance necessitates the optimization of Raman pump power, Brillouin pump wavelength, and DCF length. By employing an 11 km DCF, when setting the Brillouin pump wavelength at 1531.4 nm, 504 Stoke lines are produced with a channel spacing of 0.08 nm. All the counted laser lines have less than a 1-dB peak amplitude variation and are spread across a 40.4 nm bandwidth that covers from 1531.4 to 1571.8 nm wavelength. In this case, the Raman pump power is fixed at 900 mW which results in average OSNR and Stokes peak amplitude level of 28 dB and -7 dBm respectively. To date, this is the simplest cavity design with the widest bandwidth and flattest spectrum together with outstanding OSNR attained in 10 GHz spacing multi-wavelength fiber lasers that incorporate a single low-power Raman pump unit.

Power evolution prediction of bidirectional Raman amplified WDM system based on PINN.

We propose using physical-informed neural network (PINN) for power evolution prediction in bidirectional Raman amplified WDM systems with Rayleigh backscattering (RBS). Unlike models based on data-driven machine learning, PINN can be effectively trained without preparing a large amount of data in advance and can learn the potential rules of power evolution. Compared to previous applications of PINN in power prediction, our model considers bidirectional Raman pumping and RBS, which is more practical. We experimentally demonstrate power evolution prediction of 200 km bidirectional Raman amplified wavelength-division multiplexed (WDM) system with 47 channels and 8 pumps using PINN. The maximum prediction error of PINN compared to experimental results is only 0.38 dB, demonstrating great potential for application in power evolution prediction. The power evolution predicted by PINN shows good agreement with the results simulated by traditional numerical method, but its efficiency is more suitable for establishing models and calculating noise, providing convenience for subsequent power configuration optimization.

Tunable broadband multi-wavelength Brillouin-Raman random fiber laser based on high-order Raman pump

Tunable broadband multi-wavelength Brillouin-Raman random fiber laser based on high-order Raman pump

Enhanced Total Vibrational Excitation Yield in a Slow Narrow-Pulsed Hydrogen Molecular Beam.

High-efficiency excitation of a molecular beam is critical for investigating state-selected chemistry. However, achieving vibrational excitation of the entire beam for Raman-active molecules such as H2 proves extremely challenging, primarily because laser pulses are much shorter than the molecular beam. In this study, we achieve a total excitation efficiency of over 20% by employing stimulated Raman pumping (SRP) in a slow, narrow-pulsed molecular beam. Through optimizing the intensity and spot shape of the SRP lasers, we attain saturated excitation within the laser crossing region. Furthermore, by reducing the beam velocity and narrowing the beam pulse using a cold valve and a fast chopper, we significantly enhance the total excitation yield. COMSOL simulation and a newly developed model reveal that a critical velocity allows the chopper to block unexcited molecules and reserve most of the excited ones from the beam, resulting in the highest overall excitation yield. This innovative setup opens new possibilities for state-selected experiments in surface science and ion-molecule reaction dynamics, particularly involving weak transitions and pulsed lasers.

Widely-tunable, multi-band Raman laser based on dispersion-managed thin-film lithium niobate microring resonators

Stimulated Raman scattering is an attractive way to extend the operation spectral range of optical sources. However, the spectral extension range of a tunable Raman laser is limited by the Raman frequency shift and pump tuning bandwidth. This makes it challenging to realize chip-scale, widely tunable Raman lasers, as on-chip lasers only provide limited pump power and tuning bandwidth. Here, we tackle this by dispersion engineering of a thin-film lithium niobate microring resonator, where its high-quality factor ( ~ 2.5 million) ensures a sub-milli-watt (0.8 mW) threshold for Raman lasing while its strong normal dispersion with suppressed avoided mode crossing restrains the competing Kerr comb generation process. Combining the multi-wavelength Raman gain response of lithium niobate and cascaded Raman lasing, we demonstrate a widely tunable Raman laser covering 1592–1955 nm, showing a 335-nm spectral extension range from a 94-nm-tuning-bandwidth pump laser. Our demonstration paves the way to realize chip-scale, widely-tunable Raman lasers.

Broadband multi-wavelength Brillouin-Raman fiber laser with frequency switching

We purpose and demonstrate the switchable multi-wavelength Brillouin–Raman fiber laser (MBRFL) through a bi-directional Raman pumping scheme. The laser structure is arranged in a linear cavity by including a physical mirror at one side of the cavity. The switching operation for MBRFL with single- and double-wavelength spacing is implemented by optimizing the Raman power distribution through a variable optical coupler. This effect on feedback power of the physical mirror provides the difference between odd- and even-order Stoke lines’ maximum power on different sides of the cavity with 10 GHz and 20 GHz spacing. A 90/10 coupler is found to be the optimal. Up to 460 flat-amplitude lines within only a 0.5-dB flatness range, average −5 dBm Stokes peak power (SPP), 10 GHz frequency spacing, and an average optical signal-to-noise ratio (OSNR) of 26 dB are observed. All the counted laser lines are spread across a 37 nm bandwidth. Simultaneously, 170 Stoke lines with overall −2 dBm SPP, 28 dB OSNR, and 20 GHz frequency spacing are attained on other side of the cavity. These are achieved when the Raman pump power is set only at 900 mW. To date, this is the simplest cavity design with the flattest spectrum and highest output power for both wavelength spacing and excellent OSNR achieved in multi-wavelength fiber lasers that incorporate a single low-power Raman pump unit.

O-band tunable multiwavelength Brillouin-Raman fiber laser based on a wavelength-agile Raman pump.

Multiwavelength Brillouin-Raman fiber laser (MBRFL) features broadband multiwavelength generation with flat-amplitude and high optical signal to noise ratio (OSNR), which has great potential in optical fiber communication applications. Till now, the spectral regions of MBRFLs are mostly concentrated at conventional C- and L-band and the tunability of MBRFL is limited by using the Raman pump with fixed wavelength. Here, by utilizing wavelength-agile random fiber laser which can emit tunable lasing at 1.2 µm band as the Raman pump, we experimentally demonstrate the tunable MBRFL in the O-band for the first time, to the best of our knowledge. At Raman and Brillouin pump powers of 920 mW and -3 dBm, respectively, up to 90 Stokes lines with 0.13 nm wavelength spacing and >13 dB OSNR can be obtained when the Raman and Brillouin pump wavelength are set at 1231 nm and 1300 nm, respectively. Moreover, by tuning the wavelength of Brillouin pump from 1295 nm to 1330 nm, tunable MBRFL can be achieved with similar multiwavelength generation bandwidth by simultaneously tuning the Raman pump wavelength, and the number of Stokes lines are beyond 85 across the tuning range. The bandwidth of the demonstrated O-band MBRFL is also the widest wavelength span ever reported for multiwavelength Brillouin fiber lasers at 1.3 µm band. Our work indicates that the use of wavelength-agile random fiber laser as Raman pump in MBRFL can provide an effective way to extend the spectral regions of MBRFL and also improve the tunability performance of MBRFL.

Ultra-Wide Bandwidth Brillouin-Raman Random Fiber Laser With Augmented Synergistic Nonlinearity

We propose a Brillouin-Raman random fiber laser with enhanced synergistic nonlinearity for ultra-wide bandwidth Brillouin comb generation. The augmented synergistic nonlinearity, including enhanced Rayleigh scattering (RS) effect, stimulated Brillouin scattering (SBS) and stimulated Raman scattering (SRS), is achieved in a hybrid fiber (a fiber combination of a 7.2-km dispersion compensation fiber and a 10-km single-mode fiber) under a strong Raman pumping condition. Under the strong Raman pumping condition, more Stokes lines are generated due to the enhanced RS-induced oscillations of Brillouin Stokes lines at short wavelength band, thus suppressing self-lasing cavity mode oscillations at long wavelength band. In the experiments, the multi-wavelength Brillouin comb with an ultra-wide bandwidth of 63.5 nm (1513 nm-1576.5 nm) with frequency spacing of double Brillouin frequency shift, which is the largest bandwidth from Brillouin fiber lasers, to the best of our knowledge, has been achieved. The proposed ultra-wide bandwidth Brillouin-Raman fiber laser has potential applications in optical communication, optical wavelength division multiplexing, and fiber sensing.

A New Gas Analysis Method Based on Single-Beam Excitation Stimulated Raman Scattering in Hollow Core Photonic Crystal Fiber Enhanced Raman Spectroscopy.

We previously developed a hollow-core photonic crystal fiber (HCPCF) based Raman scattering enhancement technique for gas/human breath analysis. It enhances photon-gas molecule interactions significantly but is still based on CW laser excitation spontaneous Raman scattering, which is a low-probability phenomenon. In this work, we explored nanosecond/sub-nanosecond pulsed laser excitation in HCPCF based fiber enhanced Raman spectroscopy (FERS) and successfully induced stimulated Raman scattering (SRS) enhancement. Raman measurements of simple and complex gases were performed using the new system to assess its feasibility for gas analysis. We studied the gas Raman scattering characteristics, the relationship between Raman intensities and pump energies, and the energy threshold for the transition from spontaneous Raman scattering to SRS. H2, CO2, and propene (C3H6) were used as test gases. Our results demonstrated that a single-beam pulsed pump combined with FERS provides an effective Raman enhancement technique for gas analysis. Furthermore, an energy threshold for SRS initiation was experimentally observed. The SRS-capable FERS system, utilizing a single-beam pulsed pump, shows great potential for analyzing complex gases such as propene, which is a volatile organic compound (VOC) gas, serving as a biomarker in human breath for lung cancer and other human diseases. This work contributes to the advancement of gas analysis and opens alternative avenues for exploring novel Raman enhancement techniques.

Hybrid amplifier placement in mesh DWDM networks using integer linear programming models

Hybrid erbium-doped fiber (EDF)/Raman amplifiers (HFAs) can be utilized to improve the performance of specific fiber spans in dense wavelength division multiplexing (DWDM) networks, aiming to extend the reach and/or increase the capacity of optical channels, thereby reducing the total number of line interfaces required to satisfy a given set of traffic demands. However, HFAs are costlier than simpler EDF amplifiers (EDFAs) since they include Raman pumps in addition to an EDFA. Consequently, it is paramount to place them only at selected fiber spans of the network so as to maximize their impact while keeping their number limited. It has been shown that HFA placement can be a complex task in mesh DWDM networks in view of optical channel diversity, with each fiber span traversed by multiple channels with different source and destination nodes. Building on the approximation that noise adds up incoherently along the transmission path, this paper proposes optimal methods to solve the problem of placing hybrid amplifiers in mesh networks. Particularly, it describes two integer linear programming models, one to determine the minimum number and location of HFAs required to reach a target set of feasible optical channels (i.e., without intermediate 3R regenerators) and another to maximize the number of feasible optical channels given a limited number of HFAs to be deployed. A comprehensive set of network simulations using three reference optical network topologies is reported, providing insight into the effectiveness of the proposed models when compared to existing approaches.

Flatness enhancement of multi-wavelength Brillouin-Raman fiber laser with 10 GHz spacing utilizing Raman pump power distribution.

A simple high flat amplitude multi-wavelength Brillouin-Raman fibre laser (MBRFL) with 10 GHz spacing and excellent optical signal-to-noise ratio (OSNR) in C-Band spectral region is demonstrated. The laser consists of a linear cavity in which 12 km dispersion compensating fiber (DCF) in addition to 49 cm Bismuth-oxide Erbium doped fiber (Bi-EDF) are employed as a gain medium for amplification. The impact of Raman pump power distribution through changes in coupling ratio on amplitude flatness is carried out by comparing the peak power discrepancy between odd- and even-order Brillouin Stoke lines. This is the main property that allows the efficient controlling of gain propagation between lasing lines that is vital for Stokes flattening initiation and other output spectra characteristics. The attainment of MBRFL with outstanding OSNR necessitates the utilizing of Bi-EDF as a noise suppressor. By utilizing a 50/50 coupler, 354 identical channels together with uniform Brillouin Stokes linewidth within only 0.3-dB maximum power difference between adjacent channels is generated. The average OSNR and Stokes power are 28 dB and -5 dBm respectively when the RPP is set at 1300 mW. To date, this is the highest flatness 10 GHz spacing MBRFL with outstanding OSNR attained in MBRFL that incorporate only a single Raman pump unit.

Photogrammetry of Ultrafast Excited-State Intramolecular Proton Transfer Pathways in the Fungal Pigment Draconin Red.

Proton transfer processes of organic molecules are key to charge transport and photoprotection in biological systems. Among them, excited-state intramolecular proton transfer (ESIPT) reactions are characterized by quick and efficient charge transfer within a molecule, resulting in ultrafast proton motions. The ESIPT-facilitated interconversion between two tautomers (PS and PA) comprising the tree fungal pigment Draconin Red in solution was investigated using a combination of targeted femtosecond transient absorption (fs-TA) and excited-state femtosecond stimulated Raman spectroscopy (ES-FSRS) measurements. Transient intensity (population and polarizability) and frequency (structural and cooling) dynamics of -COH rocking and -C=C, -C=O stretching modes following directed stimulation of each tautomer elucidate the excitation-dependent relaxation pathways, particularly the bidirectional ESIPT progression out of the Franck-Condon region to the lower-lying excited state, of the intrinsically heterogeneous chromophore in dichloromethane solvent. A characteristic overall excited-state PS-to-PA transition on the picosecond timescale leads to a unique "W"-shaped excited-state Raman intensity pattern due to dynamic resonance enhancement with the Raman pump-probe pulse pair. The ability to utilize quantum mechanics calculations in conjunction with steady-state electronic absorption and emission spectra to induce disparate excited-state populations in an inhomogeneous mixture of similar tautomers has broad implications for the modeling of potential energy surfaces and delineation of reaction mechanisms in naturally occurring chromophores. Such fundamental insights afforded by in-depth analysis of ultrafast spectroscopic datasets are also beneficial for future development of sustainable materials and optoelectronics.

Mitigating probe pulse deformation in Raman amplification in OTDR fiber sensing systems.

We report the numerical and experimental study of probe pulse deformation in a forward-pumped distributed Raman amplifier on a 40-km standard single mode fiber. Distributed Raman amplification can improve the range of OTDR-based sensing systems, but it could result in pulse deformation. A smaller Raman gain coefficient can be used to mitigate pulse deformation. The sensing performance can still be maintained by compensating for the decrease in the Raman gain coefficient by increasing the pump power. The tunability of the Raman gain coefficient and pump power levels are predicted while keeping the probe power below the modulation instability limit.

190km Φ-OTDR with bidirectional Raman and relay erbium-doped fiber hybrid amplification

In this paper, a long-distance coherent detection phase-sensitive optical time-domain reflectometer (Φ-OTDR) scheme with bidirectional Raman and relay erbium-doped fiber hybrid amplification is proposed. The bidirectional Raman pump light acting on the erbium-doped fiber (EDF) can realize the passive amplification of pulsed signal light and Rayleigh backward scattering (RBS) light at the same time. The scheme utilizes bidirectional 1455 nm pumps as the pump source of relay amplification to achieve a longer sensing distance. Experimental results demonstrate that, an ultra-long Φ-OTDR system with 190 km sensing distance and 22 m spatial resolution is realized. Multi-point vibration signals are located and restored at 69.67 km, 120.13 km and 190.79 km, respectively. The average signal-to-noise ratio (SNR) of positioning curve is 10.32 dB, the average SNR of demodulated phase signal is 26.02 dB, and the frequency response range is from 5 Hz to 150 Hz. Furthermore, the sensing system has good linear characteristics of phase demodulation with a correlation coefficient of 0.997. The actual disturbance events are also detected at the far-end of sensing fiber. To the best of our knowledge, this system achieves the longest-distance Φ-OTDR without relay power supply. This passive hybrid amplification method can avoid the intermediate power supply along sensing fiber, which provides a reference for long-distance vibration monitoring of Φ-OTDR system.