The spectral resolution of broadband Fourier-transform coherent anti-Stokes Raman spectroscopy is limited by the maximum optical path length difference that can be scanned within a short time in an interferometer. However, alternatives to the Fourier-transform exist which can bypass this limitation with certain assumptions. We apply one such approach to broadband coherent Raman spectroscopy using interferometers with short delay line (low Fourier spectral resolution) and large delay line (high Fourier spectral resolution). With this method, we demonstrate broadband coherent Raman spectroscopy of closely spaced vibrational bands is possible using a short delay line interferometer, with superior spectral resolution to the longer delay line instrument. We discuss how this approach may be particularly useful for more complex Raman spectra, such as those measured from biological samples.
We report on the observation of both stable dissipative solitons and noise-like pulses with the presence of strong Raman scattering in a relatively short all-normal-dispersion Yb-doped fiber laser. We show that Raman scattering can be filtered out by intracavity filter. Furthermore, by appropriate intracavity polarization control, the Raman effect can be utilized to generate broadband noise-like pulses (NLPs) with bandwidth up to 61.4 nm. To the best of our knowledge, this is the broadest NLP achieved in all-normal-dispersion fiber lasers
The noise figure and photon probability distribution are calculated for coherent anti-Stokes Raman scattering (CARS) where an anti-Stokes signal is converted to Stokes. We find that the minimum noise figure is ~ 3dB.
Raman sensing and Raman microscopy are amongst the most specific optical technologies to identify the chemical compounds of unknown samples, and to enable label-free biomedical imaging with molecular contrast. However, the high cost and complexity, low speed, and incomplete spectral information provided by current technology are major challenges preventing more widespread application of Raman systems. To overcome these limitations, we developed a new method for stimulated Raman spectroscopy and Raman imaging using continuous wave (CW), rapidly wavelength swept lasers. Our all-fiber, time-encod…
We present general analytical expressions of Stokes and anti-Stokes spectral photon-flux densities that are spontaneously generated by a single monochromatic pump wave propagating in a single-mode optical fiber. We validate our results by comparing them with experimental data. Limiting cases of the general expressions corresponding to interesting physical situations are discussed.
A high-Q silica whispering-gallery mode microresonator is an attractive platform on which to demonstrate a broad and phase-locked Raman comb in various wavelength regimes. Raman combs can be used for applications such as compact pulse laser sources, sensors, optical clocks, and coherence tomography. However, the formation dynamics of a Raman comb has not been well exploited. Here we study the dynamics of the Raman comb formation in silica rod microresonators, which have cavity free spectral ranges in microwave rates. We generated a Raman comb with a smooth spectral envelope and also observed t…
We show that coherent anti-Stokes Raman lineshapes do not follow known spectral profiles if the time asymmetry of realistic laser pulses is taken into account. Examples are given for nanosecond and picosecond laser pulses commonly employed in frequency-resolved coherent anti-Stokes Raman scattering. More remarkably, the analysis suggests an effect of line narrowing in comparison to the customary approach, based primarily on the Voigt lineshape.
We introduce new lineshapes of coherent anti-Stokes Raman spectra of gases by considering realistic nanosecond laser pulses that deviate from the Gaussian representations of their time and spectral envelopes. The analysis suggests that the contribution to the linewidth caused by the interaction with such laser pulses could be erroneously attributed to the intrinsic Raman width if the customary CARS approach, based primarily on the Voigt lineshape, is assumed.
We have developed an interferometric implementation of coherent anti-Stokes Raman scattering (CARS) which enables broadband coherent Raman spectroscopy free from non-resonant background (NRB), with a signal strength proportional to concentration. Spectra encode mode symmetry information into the amplitude response which can be directly compared to polarised spontaneous Raman spectra. The method requires only passive polarisation optics and is suitable for a wide range of laser linewidths and pulse durations
We show that time-resolved coherent anti-Stokes Raman signals of isolated transitions deviate from the exponential decay whose time constant is nowadays used for measuring Raman linewidths. The deviation is caused by probe pulse-shape effects that can be understood in terms of the spectral filtering created by the necessary action of laser probing. Consequent corrections to recent linewidth measurements on heteronuclear molecules support the unprecedented agreement between theoretical works and experiments.
Coherent Raman scattering spectroscopy is studied purposely, with the Gaussian ultrashort pulses as a hands-on elucidatory extraction tool of the clean coherent Raman resonant spectra from the overall measured data contaminated with the non-resonant four wave mixing background. The integral formulae for both the coherent anti-Stokes and Stokes Raman scattering are given in the semiclassical picture, and the closed-form solutions in terms of a complex error function are obtained. An analytic form of maximum enhancement of pure coherent Raman spectra at threshold time delay depending on bandwidt…
Due to their high circulating intensities, ultra-high quality factor dielectric whispering-gallery mode resonators have enabled the development of low threshold Raman microlasers. Subsequently, other Raman-related phenomena, such as cascaded stimulated Raman scattering (CSRS) and stimulated anti-Stokes Raman scattering (SARS), were observed. While low threshold frequency conversion and generation have clear applications, CSRS and SARS have been limited by the low Raman gain. In this work, the surface of a silica resonator is modified with an organic monolayer, increasing the Raman gain. Up to …
We propose to use frequency-selective quasi parity-time symmetry to reduce the heat generated by coherent anti-Stokes Raman scattering (CARS) reversed cycles in active Raman media with phase mismatch. This is accomplished using a coupled-waveguide structure, which includes the active Raman waveguide (RW), where the Stokes signal undergoes amplification via stimulated Stokes Raman scattering (SSRS), and a dissipative waveguide (DW), which is tuned to the anti-Stokes wavelength so as to evacuate the corresponding anti-Stokes photons from the RW by coupling. The DW introduces optical loss that pa…
We propose an elegant scheme towards phase locking of two independent degenerate coherent anti-Stokes Raman scattering (CARS) processes. The optical implementation involves a modified Mach-Zehnder interferometer that is utilized to transfer phase coherence from three totally uncorrelated laser beams into two degenerate CARS beams which are independently produced in two distinct Raman active samples. Such a phase-transport interferometer allows for explicit measurement and control of phase differences between the two phase-locked degenerate CARS processes, hence may lead to applications in othe…
We theoretically investigate a scheme in which backward coherent anti-Stokes Raman scattering (CARS) is significantly enhanced by using slow light. Specifically, we reduce the group velocity of the Stokes excitation pulse by introducing a coupling laser that causes electromagnetically induced transparency (EIT). When the Stokes pulse has a spatial length shorter than the CARS wavelength, the backward CARS emission is significantly enhanced. We also investigated the possibility of applying this scheme as a CARS lidar with O2 or N2 as the EIT medium. We found that if nanosecond laser with large …
Single-shot time resolved Coherent Anti-Stokes Raman Scattering (CARS) is presented as a viable method for fast measurements of molecular spectra. The method is based on the short spatial extension of femtosecond pulses and maps time delays between pulses onto the region of intersection between broad beams. The image of the emitted CARS signal contains full temporal information on the field-free molecular dynamics, from which spectral information is extracted. The method is demonstrated on liquid samples of CHBr3 and CHCl3 and the Raman spectrum of the low-lying vibrational states of these mol…
We propose a new technique for comparing two Raman active samples. The method employs optical interference of the signals generated via coherent anti-Stokes Raman scattering (CARS) of broadband laser pulses with noisy spectra. It does not require spectrally resolved detection, and no prior knowledge about either the Raman spectrum of the samples, or the spectrum of the incident light is needed. We study the proposed method theoretically, and demonstrate it in a proof-of-principle experiment on Toluene and ortho-Xylene samples.
We demonstrate for the first time, Raman random lasing in a continuous-wave (CW) excited, completely biocompatible and biodegradable carrot medium. The Stokes Raman mode of carotene renders carrot as a gain medium whereas random scattering in the natural fibrous cellulose of the carrot structure facilitates random lasing. CW laser induced photoluminescence(PL) threshold and linewidth analysis at the Stokes modes of carotene show a characteristic lasing action with threshold of 130 W/cm2 and linewidth-narrowing with mode Q factors (~1300). Polarization study of output modes reveals that lasing …
We show that the increasingly popular nonlinear optical technique of time-domain coherent anti-Stokes Raman scattering (CARS), which is usually understood in terms of the semiclassical time-dependent third-order polarization, can be equally explained in terms of the time-delayed version of the Yuratich equation so popular in traditional frequency-domain CARS. The method brings out the strong dependence of CARS time traces and time-delayed CARS lineshapes on the spectral envelope of the probe laser electric field. Examples are analytically shown for experimental results that are otherwise treat…
We demonstrate stimulated Raman gain using a broadband LED Stokes source to measure vibrational spectra of aqueous glucose solutions. This versatile and cost-effective method increases Raman signal for a variety of applications. We measured both stimulated Raman and spontaneous Raman spectra of glucose solutions with concentrations up to 10 mM with a photon counter and lock-in amplifier. We built partial least squares regression models based on both stimulated Raman and spontaneous Raman spectral data measured with each instrument for predicting concentrations of the glucose solutions. The sti…
Nonlinear optical methods, such as coherent anti-Stokes Raman scattering (CARS) and stimulated Raman scattering (SRS), are able to perform label free imaging, with chemical bonds specificity. Here, we demonstrate that the use of circularly polarized light allows to retrieve not only the chemical nature but also the symmetry of the probed sample, in a single shot measurement. Our symmetry-resolved scheme offers simple access to the local organization of vibrational bonds and as a result provides enhanced image contrast for anisotropic samples as well as an improved chemical selectivity. We quan…
Nonlinear optical microscopy allows rapid high-resolution microscopy with image contrast generated from intrinsic properties of the sample. Established modalities such as multiphoton excited fluorescence and second/third-harmonic generation can be combined with other nonlinear techniques, such as coherent Raman spectroscopy which typically allow chemical imaging of a single resonant vibrational mode of a sample. Here, we utilize a single ultrafast laser source to obtain broadband coherent Raman spectra on a microscope, together with other nonlinear microscopy approaches on the same instrument.…
As shown in the early 1960s, the gain in stimulated Raman scattering (SRS) is drastically suppressed when the rate of creation of phonons (via pump-to-Stokes conversion) is exactly balanced by the rate of phonon annihilation (via pump-to-anti-Stokes conversion). This occurs when the phonon coherence waves synchronized vibrations of a large population of molecules have identical propagation constants for both processes, i.e., they are phase-velocity matched. As recently demonstrated, hydrogen-filled photonic crystal fiber pumped in the vicinity of its zero dispersion wavelength provides an idea…
We study Raman scattering in active media placed in proximity of different types of metal nanostructures, at wavelengths that display either Fabry-Perot or plasmonic resonances, or a combination of both. We use a semi-classical approach to derive equations of motion for Stokes and anti-Stokes fields that arise from quantum fluctuations. Our calculations suggest that local field enhancement yields Stokes and anti-Stokes conversion efficiencies between five and seven orders of magnitudes larger compared to cases without the metal nanostructure. We also show that to first order in the linear susc…
We propose a full-vectorial numerical study of far field radiation patterns in coherent anti-Stokes Raman scattering (CARS) microscopy. We emphasis the particular role of the Raman depolarisation ratio of the observed medium and show how it modifies the radiation pattern of thin objects.
Multimode hollow microcavities in three-dimensional (3D) photonic crystals (PhCs) are designed for achieving enhanced coherent anti-Stokes Raman scattering, which requires a cavity to have three high quality-factor (Q) modes with equally spaced resonant frequencies. Cavities in 3D PhCs allows more flexibility in design and tuning than their 2D slab counterparts, since radiation loss that degrades Q can be suppressed by the 3D photonic band gap. We first tune all the mode frequencies simultaneously by changing the material and geometry of the cavity based on perturbation theory. Spectral spacin…
Compact, power efficient and fiber compatible lasers, wavelength converters and amplifiers are vital ingredients for the future fiber optic systems and networks. Nonlinear optical effects, like Raman scattering and parametric four wave mixing, offer a way to realize such devices. Here we use a single chalcogenide microwire to realize a device that provides the functions of a Stokes Raman parametric laser, a four wave mixing anti Stokes wavelength converter, and an ultra broadband Stokes/anti Stokes Raman amplifier or supercontinuum generator. The device operation relies on ultrahigh Raman and …
Coherent Raman microscopy provide label-free imaging by interrogating the intrinsic vibration of biomolecules. Nevertheless, trade-off between high chemical-specificity and high imaging-speed currently exists in transition from spectroscopy to spectroscopic imaging when capturing dynamics in complex living systems. Here, we present a novel concept in dual-comb scheme to substantially beat this trade-off and facilitate high-resolution broadband coherent anti-Stokes Raman spectroscopic imaging based on down-converted, automatically varying delay-time in spectral focusing excitation. A rapid meas…
A commercial single laser line Raman spectrometer is modified to accommodate multiline and tunable dye lasers, thus combining the high sensitivity of such single monochromator systems with broadband operation. Such instruments rely on high-throughput interference filters that perform both beam alignment and Rayleigh filtering. Our setup separates the dual task of the built-in monochromator into two independent elements: a beam splitter and a long pass filter. Filter rotation shifts the transmission passband, effectively expanding the range of operation. Rotation of the filters has a negligible…
We propose an all-fiber-generated dual-soliton pulses based scheme for the background-free detection of coherent anti-Stokes Raman spectroscopy under the spectral focusing mechanism. Due to the strong birefringence and high nonlinearity of a polarization-maintaining photonic crystal fiber (PM-PCF), two redshifted soliton pulses can be simultaneously generated relying on high-order dispersion and nonlinear effects along two eigenpolarization axes in the anomalous dispersion regime, while allowing feasible tunability of the frequency distance and temporal interval between them. This proposed sch…
Excited-state vibrational dynamics in molecules can be studied by an electronically off-resonant Raman process induced by a probe pulse with variable delay with respect to an actinic pulse. We establish the connection between several variants of the technique that involve either spontaneous or stimulated Raman detection and different pulse configurations. By using loop diagrams in the frequency domain we show that all signals can be described as six wave mixing which depend on the same four point molecular correlation functions involving two transition dipoles and two polarizabilities and acco…
We demonstrate a novel technique of coherent Raman spectroscopy with a femtosecond laser. We apply to a molecular sample a sequence of pairs of ultrashort excitation and probe pulses, with a linearly increasing time delay between the two pulses from one pair to the next. We measure, as a function of the delay, the intensity modulation in the signal resulting from the differential detection of the Stokes and anti-Stokes radiations generated at the sample. The Fourier transform of such time-domain signal reveals the spectrum of the excited vibrational Raman transitions. The experimental proof-of…
Coherent Anti-Stokes Raman Scattering (CARS) processes are ``coherent,'' but the phase of the anti-Stokes radiation is usually lost by most incoherent spectroscopic CARS measurements. We propose a novel Raman microscopy imaging method called Nonlinear Interferometric Vibrational Imaging, which measures Raman spectra by obtaining the temporal anti-Stokes signal through nonlinear interferometry. With a more complete knowledge of the anti-Stokes signal, we show through simulations that a high-resolution Raman spectrum can be obtained of a molecule in a single pulse using broadband radiation. This…
We investigate slow-light via stimulated Brillouin scattering in a room temperature optical fiber that is pumped by a spectrally broadened laser. Broadening the spectrum of the pump field increases the linewidth $Δω_p$ of the Stokes amplifying resonance, thereby increasing the slow-light bandwidth. One physical bandwidth limitation occurs when the linewidth becomes several times larger than the Brillouin frequency shift $Ω_B$ so that the anti-Stokes absorbing resonance cancels out substantially the Stokes amplifying resonance and hence the slow-light effect. We find that partial overlap of the…
We report the observations of spontaneous Raman scattering in silicon photonic crystal waveguides. Continuous-wave measurements of Stokes emission for both wavelength and power dependence is reported in single line-defect waveguides in hexagonal lattice photonic crystal silicon membranes. By utilizing the Bragg gap edge dispersion of the TM-like mode for pump enhancement and the TE-like fundamental mode-onset for Stokes enhancement, the Stokes emission was observed to increase by up to five times in the region of slow group velocity. The results show explicit nonlinear enhancement in a silicon…
Expressions for the two-dimensional Stimulated x-ray Raman Spectroscopy (2D-SXRS) signal obtained using attosecond x-ray pulses are derived. The 1D- and 2D-SXRS signals are calculated for trans-N-methyl acetamide (NMA) with broad bandwidth (FWHM ~14.2eV, 181 as) pulses tuned to the oxygen and nitrogen K-edges. Crosspeaks in 2D signals reveal electronic Franck-Condon overlaps between valence orbitals and relaxed orbitals in the presence of the core hole.
Optical refrigeration of solids holds tremendous promise for applications in thermal management. It can be achieved through multiple mechanisms including inelastic anti-Stokes Brillouin and Raman scattering. However, engineering of these mechanisms remains relatively unexplored. The major challenge lies in the natural unfavorable imbalance in transition rates for Stokes and anti-Stokes scattering. We consider the influence of anisotropic photonic density of states on Raman scattering and derive expressions for cooling in such systems. We demonstrate optimization of the Raman cooling figure of …
We investigate the evolution of coherence property of noise-seeded Stokes wave in short (< 1 ps) and long pulse (> 1 ps) regimes. Nonlinear equations expressing the evolution of pump and Stokes wave are solved numerically for both the regions. The simulations include quantum noise by incorporating noise seed in the pump field where one photon per mode with random phase. The spectral phase fluctuations of the Stokes wave for both the regions, are characterized by performing multiple simulations and finally, the degrees of first-order mutual coherence are calculated as a function of wavelength f…
We experimentally demonstrate efficient Raman conversion to respective Stokes and anti-Stokes fields in both pulsed and continuous modes with a Rb-87 atomic vapor cell. The conversion efficiency is about 40-50% for the Stokes field and 20-30% for the anti-Stokes field, respectively. This conversion process is realized with feedback of both the Raman pump and the frequency-converted fields (Stokes or anti-Stokes). The experimental setup is very simple and can be applied easily to produce the light source with larger frequency difference using other Raman media. They may have wide applications i…
Nonstationary molecular states which contain electronic coherences can be impulsively created and manipulated by using recently-developed ultrashort optical and X-ray pulses via photoexcitation, photoionization and Auger processes. We propose several stimulated-Raman detection schemes that can monitor the phase-sensitive electronic and nuclear dynamics. Three detection protocols of an X-ray broadband probe are compared - frequency dispersed transmission, integrated photon number change, and total pulse energy change. In addition each can be either linear or quadratic in the X-ray probe intensi…
We study a generalized notion of two-mode squeezing for the Stokes and anti-Stokes fields in a model of a cavity Raman laser, which leads to a significant reduction in decoherence or quantum noise. The model comprises a loss-less cavity with classical pump, unsaturated medium and arbitrary homogeneous broadening and dispersion. Allowing for arbitrary linear combinations of the two modes in the definition of quadrature variables, we find that there always exists a combination of the two output modes which exhibits quadrature squeezing with noise reduction below the vacuum level. The number of n…
Using a high-Q diamond microresonator (Q > 300,000) interfaced with high-power-handling directly-written doped-glass waveguides, we demonstrate a Raman laser in an integrated platform pumped in the near-visible. Both TM-to-TE and TE-to-TE lasing is observed, with a Raman lasing threshold as low as 20 mW and Stokes power of over 1 mW at 120 mW pump power. Stokes emission is tuned over a 150 nm (60 THz) bandwidth around 875 nm wavelength, corresponding to 17.5% of the center frequency.
We present a new scheme for a laser cooled Raman optical fiber amplifier. The heat generated in the process of stimulated Raman scattering is compensated for with laser cooling provided by anti-Stokes fluorescence of ytterbium ions doped in the core of the fiber. The device is pumped with two pump sources. One of the pump sources provides Raman amplification of the signal and does not interact with the ytterbium ions in the core of the fiber. The second pump provides laser cooling of the fiber with anti-Stokes fluorescence of the Yb3+ ions. The proper arrangement of Yb3+distribution can provid…
The operator solution of a completely quantum mechanical Hamiltonian of the Raman processes is used here to investigate the possibility of obtaining intermodal entanglement between different modes involved in the Raman processes (e.g. pump mode, Stokes mode, vibration (phonon) mode and anti-Stokes mode). Intermodal entanglement is reported between a) pump mode and anti-Stokes mode, b) pump mode and vibration (phonon) mode c) Stokes mode and vibration phonon mode, d) Stokes mode and anti-stokes mode in the stimulated Raman processes for the variation of the phase angle of complex eigenvalue $α_…
We report stimulated Raman spectroscopy of the G phonon in both single and multi-layer graphene, through Coherent anti-Stokes Raman Scattering (CARS). The signal generated by the third order nonlinearity is dominated by a vibrationally non-resonant background (NVRB), which obscures the Raman lineshape. We demonstrate that the vibrationally resonant CARS peak can be measured by reducing the temporal overlap of the laser excitation pulses, suppressing the NVRB. We model the observed spectra, taking into account the electronically resonant nature of both CARS and NVRB. We show that CARS can be us…
Light's polarisation contains information about its source and interactions, from distant stars to biological samples. Polarimeters can recover this information, but reliance on birefringent or rotating optical elements limits their wavelength range and stability. Here we present a static, single-shot polarimeter based on a Fresnel cone - the direct spatial analogue to the popular rotating quarter-wave plate approach. We measure the average angular accuracy to be 2.9 (3.6) degrees for elliptical(linear) polarisation states across the visible spectrum, with the degree of polarisation determined…
Many reports on stimulated Raman scattering in mixtures of Raman-active and noble gases indicate that the addition of a dispersive buffer gas increases the phase-mismatch to higher-order Stokes and antiStokes sidebands, resulting in preferential conversion to the first few Stokes lines, accompanied by a significant reduction in Raman gain due to collisions with buffer gas molecules. Here we report that, provided the dispersion can be precisely controlled, the effective Raman gain in gas-filled hollow-core photonic crystal fiber (PCF) can actually be significantly enhanced when a buffer gas is …
We present an improvement on the signal-to-background of single-beam coherent anti-Stokes Raman scattering (SB-CARS) spectroscopy measurements for systems employing ultrafast supercontinuum sources based on all-normal dispersion photonic crystal fibers. Improvements to the signal-to-background arise in the use of a new pulse-reconstruction algorithm based on temporal ptychography, I$^2$PIE. A simple SB-CARS strategy is used to measure the spectrum of para-xylene, where the supercontinuum pulses used are compressed using multiphoton intrapulse interference phase scan (MIIPS) and, for the first …
Coherent anti-Stokes Raman scattering (CARS) microspectroscopy has demonstrated significant potential for biological and materials imaging. To date, however, the primary mechanism of disseminating CARS spectroscopic information is through pseudocolor imagery, which explicitly neglects a vast majority of the hyperspectral data. Furthermore, current paradigms in CARS spectral processing do not lend themselves to quantitative sample-to-sample comparability. The primary limitation stems from the need to accurately measure the so-called nonresonant background (NRB) that is used to extract the chemi…
