Optimizing the Laser-Pulse Configuration for Coherent Raman Spectroscopy

Pestov, Dmitry; Murawski, Robert K.; Ariunbold, Gombojav O.; Wang, Xi; Zhi, Mingjia; Sokolov, Alexei V.; Sautenkov, Vladimir A.; Rostovtsev, Yuri V.; Dogariu, Arthur; Huang, Yu; Scully, Marlan O.

doi:10.1126/science.1139055

Cited by 320 publications

(253 citation statements)

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“…Considerable effort has been devoted to increasing the sensitivity and eliminating off-resonant background, thus improving the signal-to-noise ratio and enabling the detection of small samples and even single molecules. Pulse shaping (Oron et al, 2002;Pestov et al, 2007) and the combination of broad and narrow band pulses (technique known as Femtosecond Stimulated Raman Spectroscopy (FSRS) (Dietze and Mathies, 2016)) have been employed. Here, we present an Interferometric FSRS (IFSRS) technique that combines quantum entangled light with interferometric detection (Kalachev et al, 2007;Scarcelli et al, 2003;Slattery et al, 2013;Yabushita and Kobayashi, 2004) in order to enhance the resolution and selectivity of Raman signals (Dorfman et al, 2014).…”

Section: Coincidence Detection Of Femtosecond Stimulated Raman Signalsmentioning

confidence: 99%

Nonlinear optical signals and spectroscopy with quantum light

2016

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Conventional nonlinear spectroscopy uses classical light to detect matter properties through the variation of its response with frequencies or time delays. Quantum light opens up new avenues for spectroscopy by utilizing parameters of the quantum state of light as novel control knobs and through the variation of photon statistics by coupling to matter. We present an intuitive diagrammatic approach for calculating ultrafast spectroscopy signals induced by quantum light, focusing on applications involving entangled photons with nonclassical bandwidth properties -known as "time-energy entanglement". Nonlinear optical signals induced by quantized light fields are expressed using time ordered multipoint correlation functions of superoperators in the joint field plus matter phase space. These are distinct from Glauber's photon counting formalism which use normally ordered products of ordinary operators in the field space. One notable advantage for spectroscopy applications is that entangled photon pairs are not subjected to the classical Fourier limitations on the joint temporal and spectral resolution. After a brief survey of properties of entangled photon pairs relevant to their spectroscopic applications, different optical signals, and photon counting setups are discussed and illustrated for simple multi-level model systems.

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Section: Coincidence Detection Of Femtosecond Stimulated Raman Signalsmentioning

confidence: 99%

Nonlinear optical signals and spectroscopy with quantum light

2016

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“…1b(i)). It enables selective excitation [4,15] or selective probing [16,17] of separate vibrational modes on the frequency scale narrower than the overall pulse bandwidth. Selective excitation is based on the coherent control of nonlinear optical processes, while selective probing employs the idea of multiplex CARS in which a small part of the pulse spectrum is modified (in amplitude, phase or polarization) and serves as a narrowband probe.…”

Section: Pacs Numbersmentioning

confidence: 99%

Noise autocorrelation spectroscopy with coherent Raman scattering

Konorov

Hepburn

et al. 2007

Nature Phys

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Ultrafast lasers have become one of the most powerful tools in coherent nonlinear optical spectroscopy. Short pulses enable direct observation of fast molecular dynamics [1,2], whereas broad spectral bandwidth offers ways of controlling nonlinear optical processes [3,4] by means of quantum interferences [5]. Special care is usually taken to preserve the coherence of laser pulses as it determines the accuracy of a spectroscopic measurement. Here we present a new approach to coherent Raman spectroscopy based on deliberately introduced noise, which increases the spectral resolution, robustness and efficiency. We probe laser induced molecular vibrations using a broadband laser pulse with intentionally randomized amplitude and phase. The vibrational resonances result in and are identified through the appearance of intensity correlations in the noisy spectrum of coherently scattered photons. Spectral resolution is neither limited by the pulse bandwidth, nor sensitive to the quality of the temporal and spectral profile of the pulses. This is particularly attractive for the applications in microscopy[6], biological imaging [7] and remote sensing [8], where dispersion and scattering properties of the medium often undermine the applicability of ultrafast lasers. The proposed method combines the efficiency and resolution of a coherent process with the robustness of incoherent light. As we demonstrate here, it can be implemented by simply destroying the coherence of a laser pulse, and without any elaborate temporal scanning or spectral shaping commonly required by the frequency-resolved spectroscopic methods with ultrashort pulses. PACS numbers:We apply our method to coherent anti-Stokes Raman scattering (CARS), which has become the method of choice in nonlinear optical spectroscopy and microscopy [6,9] after the advent of powerful ultrafast lasers. As a third-order nonlinear process, femtosecond CARS exhibits high efficiency at low average laser power. High sensitivity to molecular structure enables detection of small quantities of complex molecules[10] and non-invasive biological imaging [7]. In CARS, pump and Stokes photons of frequencies ω p and ω S , respectively, excite molecular vibrations at frequency Ω = ω p − ω S (Fig. 1a). A probe photon at ω 0 is scattered off the coherent vibrations generating the anti-Stokes signal at frequency ω = (ω 0 +Ω). Temporal and spectral resolution of CARS spectroscopy is typically limited by the duration of the excitation pulses and their frequency bandwidth, respectively. Broadband femtosecond pulses, though advantageous for time-resolved CARS spectroscopy[2, 11], offer poor spectral resolution. The latter can be improved by means of the pulse shaping technique [12,13] which modifies the amplitudes and phases of the spectral constituents of the pulse [14] (Fig. 1b(i)). It enables selective excitation [4,15] or selective probing [16,17] of separate vibrational modes on the frequency scale narrower than the overall pulse bandwidth. Selective excitation is based on the coherent control...

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“…98 Recently, femtosecond adaptive spectroscopic technique via coherent anti-Stokes Raman spectroscopy (FAST-CARS) has been used for bacterial system identification. 99 The remote sensing of medicinal plants, in addition to drug plants, will be of vital significance in the future for gauging the illicit collection of plants and the optimum collection time for medicinal plant harvesting once active (or at least marker) compounds have been identified.…”

Section: Location and Detection Techniquesmentioning

confidence: 99%

Sustainable drugs and global health care

Cordell¹

2009

Quím. Nova

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Each day, Earth's finite resources are being depleted for energy, for material goods, for transportation, for housing, and for drugs. As we evolve scientifically and technologically, and as the population of the world rapidly approaches 7 billion and beyond, among the many issues with which we are faced is the continued availability of drugs for future global health care. Medicinal agents are primarily derived from two sources, synthetic and natural, or in some cases, as semi-synthetic compounds, a mixture of the two. For the developed world, efforts have been initiated to make drug production "greener", with milder reagents, shorter reaction times, and more efficient processing, thereby using less energy, and reactions which are more atom efficient, and generate fewer by-products. However, most of the world's population uses plants, in either crude or extract form, for their primary health care. There is relatively little discussion as yet, about the long term effects of the current, non-sustainable harvesting methods for medicinal plants from the wild, which are depleting these critical resources without concurrent initiatives to commercialize their cultivation. To meet future public health care needs, a paradigm shift is required in order to adopt new approaches using contemporary technology which will result in drugs being regarded as a sustainable commodity, irrespective of their source. In this presentation, several approaches to enhancing and sustaining the availability of drugs, both synthetic and natural, will be discussed, including the use of vegetables as chemical reagents, and the deployment of integrated strategies involving information systems, biotechnology, nanotechnology, and detection techniques for the development of medicinal plants with enhanced levels of bioactive agents.

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Optimizing the Laser-Pulse Configuration for Coherent Raman Spectroscopy

Cited by 320 publications

References 24 publications

Nonlinear optical signals and spectroscopy with quantum light

Nonlinear optical signals and spectroscopy with quantum light

Noise autocorrelation spectroscopy with coherent Raman scattering

Sustainable drugs and global health care

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