Nonlinear Raman Spectroscopy Research Articles

Efficient Raman frequency conversion by coherent feedback at low light intensity

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 efficient conversion process is realized with coherent feedback of both the Raman pump and the frequency-converted fields (Stokes or anti-Stokes). The experimental setup is simple and can be applied easily to produce light sources with larger frequency shifts using other Raman media with long coherence time. They may have potential applications in nonlinear optics, Raman spectroscopy and precision measurement.

Fiber optic probes for linear and nonlinear Raman applications – Current trends and future development

AbstractThis review focuses on fiber optic probes for linear and nonlinear Raman spectroscopy, especially for medical applications. It aims at providing an overview over contemporary technology, recent first clinical trials, and helps identifying future developments necessary to bring the emerging technology to clinical end users. After a short introduction to linear and nonlinear Raman spectroscopic modalities, general design considerations will be discussed and compared to common fiber probe setups. Subsequently, examples for medical applications of fiber optic Raman probes will be given concentrating on probes for linear Raman spectroscopy as these devices are technologically more mature compared to their counterparts based on nonlinear Raman spectroscopy. The review also includes a brief summary of first multimodal fiber optic probes and highlights their benefits for clinical applications. Finally, probes are introduced which employ either nonlinear Raman spectroscopy or surface enhanced spectroscopy.

Recent advances in linear and nonlinear Raman spectroscopy. Part VI

The purpose of this review is to provide a concise overview of recent advances in the broadly defined field of Raman spectroscopy as reflected in part by the many articles published each year in Journal of Raman Spectroscopy as well as in trends across all related journals publishing in this research area. Context for this review is derived from statistical data on article counts obtained from Thomson Reuters ISI Web of Knowledge by year and by subfield of Raman spectroscopy. Additional information is gleaned from presentations featuring Raman spectroscopy presented at the XXIII International Conference on Raman Spectroscopy in Bangalore, India, in August 2012 and at Scientific Exchange 2012 sponsored by the Federation of Analytical Chemistry and Spectroscopy Societies in Kansas City, Missouri, USA, October 2012. Papers published in the Journal of Raman Spectroscopy in 2011 are highlighted in this review and reflect trends at the cutting edge of Raman spectroscopy, a field that is expanding rapidly as a sensitive photonic probe of matter at the molecular level with an ever widening sphere of novel applications. Copyright © 2012 John Wiley & Sons, Ltd.

Recent advances in linear and nonlinear Raman spectroscopy. Part V

The purpose of the review is to provide a concise overview of recent advances in the broadly defined field of Raman spectroscopy as reflected in part by the many articles published each year in JRS as well as in trends across all related journals publishing in this research area. Context for this review is derived from statistical data on article counts obtained from Thomson Reuters ISI Web of Knowledge by year and by subfield of Raman spectroscopy. Additional information is gleaned from presentations featuring Raman spectroscopy presented at the meetings of the Federation of Analytical Chemistry and Spectroscopy Societies 2011 and the Sixth International Conference on Advanced Vibrational Spectroscopy 2011. Papers published in JRS in 2010, as reviewed here, reflect trends at the cutting edge of Raman spectroscopy, which is expanding rapidly as a sensitive photonic probe of matter at the molecular level with an ever‐widening sphere of novel applications. Copyright © 2011 John Wiley & Sons, Ltd.

Intra-operative optical diagnostics with vibrational spectroscopy

Established methods for characterization of tissue and diagnostics, for example histochemistry, magnetic resonance imaging (MRI), X-ray tomography, or positron emission tomography (PET), are mostly not suitable for intra-operative use. However, there is a clear need for an intra-operative diagnostics especially to identify the borderline between normal and tumor tissue. Currently, vibrational spectroscopy techniques (both Raman and infrared) complement the standard methods for tissue diagnostics. Vibrational spectroscopy has the potential for intra-operative use, because it can provide a biochemically based profile of tissue in real time and without requiring additional contrast agents, which may perturb the tissue under investigation. In addition, no electric potential needs to be applied, and the measurements are not affected by electromagnetic fields. Currently, promising approaches include Raman fiber techniques and nonlinear Raman spectroscopy. Infrared spectroscopy is also being used to examine freshly resected tissue ex vivo in the operating theater. The immense volume of information contained in Raman and infrared spectra requires multivariate analysis to extract relevant information to distinguish different types of tissue. The promise and limitations of vibrational spectroscopy methods as intra-operative tools are surveyed in this review.

Recent advances in linear and nonlinear Raman spectroscopy. Part IV

AbstractThe purpose of the review is to provide a concise overview of recent advances in the broadly defined field of Raman spectroscopy as reflected in part by the many articles published each year in the Journal of Raman Spectroscopy (JRS) as well as in trends across all related journals publishing in this research area. Context for the review is provided by considering statistical data on citations for the Thompson Reuters ISI Web of Science by year and by subfield of Raman spectroscopy. Additional statistics of number of papers and posters presented by category at the XXII International Conference on Raman Spectroscopy (ICORS 2010) is also provided. Papers published in JRS in 2009, as reviewed here, reflect trends at the cutting edge of Raman spectroscopy which is expanding rapidly as a sensitive photonic probe of matter at the molecular level with an ever widening sphere of novel applications. Copyright © 2010 John Wiley & Sons, Ltd.

Analysis of the cytochrome distribution via linear and nonlinear Raman spectroscopy

The cytochrome distribution in hyphal tip cells of Schizophyllum commune was visualized using resonance Raman mapping and CARS microscopy. For comparison, resonance Raman mapping and CARS imaging of cytochrome was also performed during branch formation and in completely developed central hyphae. Cytochrome, as an essential component of the electron transport chain in mitochondria, plays an important role in providing energy to actively growing mycelia. It could be shown that mitochondria at the growing hyphal tips and at branching regions are more active, i.e. contain more cytochrome, as compared to those in older parts of the hyphae. This finding is compatible with the idea of high energy consumption for biosynthesis and intracellular transport at the growing tip, while older hyphae have lower needs for ATP generated via the respiratory chain in mitochondria. To the best of our knowledge this is the first study reporting about the localization and distribution of cytochrome, as an indirect mitochondria localization within S. commune or other basidiomycetous fungi, by means of resonance Raman microspectroscopy and CARS microscopy. These Raman methods bear the potential of label-free in vivo mitochondria localization and investigation.

Ultrafast Raman loss spectroscopy

AbstractThis paper deals with a new form of nonlinear Raman spectroscopy called ‘ultrafast Raman loss spectroscopy (URLS)’. URLS is analogous to stimulated Raman spectroscopy (SRS) but is much more sensitive than SRS. The signals are background (noise) free unlike in coherent anti‐Stokes Raman spectroscopy (CARS) and it provides natural fluorescence rejection, which is a major problem in Raman spectroscopy. In addition, being a self‐phase matching process, the URLS experiment is much easier than CARS, which requires specific phase matching of the laser pulses. URLS is expected to be alternative if not competitive to CARS microscopy, which has become a popular technique in applications to materials, biology and medicine. Copyright © 2009 John Wiley & Sons, Ltd.

Recent advances in linear and nonlinear Raman spectroscopy II

AbstractFollowing the first review on recent advances in linear and nonlinear Raman spectroscopy, the present review summarizes papers mainly published in the Journal of Raman Spectroscopy during 2007. This serves to give a fast overview of recent advances in this research field as well as to provide readers of this journal a quick introduction to the various subfields of Raman spectroscopy. It also reflects the current research interests of the Raman community. Similar reviews of highly active areas of Raman spectroscopy will appear in future issues of this journal. Copyright © 2008 John Wiley & Sons, Ltd.

Hydrogen Clusters that Remain Fluid at Low Temperature

Superfluidity of hydrogen, predicted three decades ago, continues to elude experimental observation, due to the high freezing temperature of H2 at T=13.8 K. Here, large para-H2 clusters are obtained in a cryogenic pulsed free jet expansion and are studied via nonlinear Raman spectroscopy. Clusters formed from neat pH_{2} are solid as evidenced by the characteristic splitting of the rotational S0(0) line. However, clusters formed of highly diluted pH_{2} (< or = 1%) in He have a single S0(0) line and remain liquid at the estimated superfluid transition temperature of T=1-2 K.

Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses

We demonstrate a single-beam, standoff (&amp;gt;10m) detection and identification of various materials including minute amounts of explosives under ambient light conditions. This is obtained by multiplex coherent anti-Stokes Raman scattering spectroscopy (CARS) using a single femtosecond phase-shaped laser pulse. We exploit the strong nonresonant background for amplification of the backscattered resonant CARS signals by employing a homodyne detection scheme. The simple and highly sensitive spectroscopic technique has a potential for hazardous materials standoff detection applications.

ChemInform Abstract: Local Structure Formation in Alkyl‐imidazolium‐Based Ionic Liquids as Revealed by Linear and Nonlinear Raman Spectroscopy

AbstractChemInform is a weekly Abstracting Service, delivering concise information at a glance that was extracted from about 200 leading journals. To access a ChemInform Abstract of an article which was published elsewhere, please select a “Full Text” option. The original article is trackable via the “References” option.

Time-resolving molecular vibration for microanalytics: single laser beam nonlinear Raman spectroscopy in simulation and experiment

A single-beam implementation of coherent anti-Stokes Raman scattering (CARS) allows experimentally very much simplified and flexible approaches to time-resolved vibrational spectroscopy, with the additional benefit of microscopic spatial resolution. To achieve this, a broadband femtosecond laser is combined with a pulse shaper creating tailored pulse sequences by computer control. We discuss the theoretical foundations and technical issues of the technique in detail and show the successful implementation of different schemes for truly femtosecond time-resolved vibrational spectroscopy. Hereby, we elaborate all the details of the method shown earlier in a proof-of-principle study [Von Vacano and Motzkus, Opt. Comm., 2006, 264, 488] and greatly extend it by novel approaches relying on the use of identical double pulses or additional polarization control for background-free spectroscopy with superior robustness and signal-to-noise ratio. Perspectives and applications of the presented schemes for chemical microanalysis and high-contrast chemical imaging are examined.

Recent Advances in linear and nonlinear Raman spectroscopy I

AbstractRaman spectroscopy has advanced considerably in the last several years due to rapid developments in instrumentation and the availability of theoretical methods for accurate calculation of Raman spectra, thus enormously facilitating the interpretation of Raman data. This review is restricted to cover papers mainly published in the Journal of Raman Spectroscopy, which serve to give a fast overview of recent advances in this research field as well as to provide readers of this journal a quick introduction to the various subfields of Raman spectroscopy. It also reflects the current research interests of the Raman community. Similar reviews of highly active areas of Raman spectroscopy will appear in future issues of this journal. Copyright © 2007 John Wiley &amp; Sons, Ltd.

Local Structure Formation in Alkyl-imidazolium-Based Ionic Liquids as Revealed by Linear and Nonlinear Raman Spectroscopy

We show several pieces of Raman spectroscopic evidence that are indicative of local structure formation in imidazolium-based ionic liquids. Low-frequency Raman spectra of C n mimX, where C n mim stands for 1-alkyl(C n H 2 n+1 )-3-methylimidazolium cation and X represents the anion, exhibit broad bands assignable to collective modes of local structures. Spatial distributions of coherent anti-Stokes Raman scattering (CARS) signals from C n mim[PF 6] are consistent with local structures whose size increases with increasing n. Picosecond Raman spectra of S 1 trans-stilbene as a "picosecond Raman thermometer" show microscopic thermal inhomogeneity ascribable to local structure formation in C 2mimTf 2N and C 4mimTf 2N. We also describe two novel phenomena that we believe are relevant to extraordinary nanoenvironments generated by local structures in a magnetic ionic liquid C 4mim[FeCl 4].

Characterizing the Formation of Organic Layers on the Surface of Inorganic/Aqueous Aerosols by Raman Spectroscopy

We demonstrate that nonlinear Raman spectroscopy coupled with aerosol optical tweezers can be used to probe the evolving phase partitioning in mixed organic/inorganic/aqueous aerosol droplets that adopt a core-shell structure in which the aqueous phase is coated in an organic layer. Specifically, we demonstrate that the characteristic fingerprint of wavelengths at which stimulated Raman scattering is observed can be used to assess the phase behavior of multiphase decane/aqueous sodium chloride droplets. Decane is observed to form a layer on the surface of the core aqueous droplet, and from the spectroscopic signature the aqueous core size can be determined with nanometer accuracy and the thickness of the decane layer with an accuracy of +/-8 nm. Further, the presence of the organic layer is observed to reduce the rate at which water evaporates from the core of the droplet with an increasing rate of evaporation observed with diminishing layer thickness.

S05I6 非線形ラマン分光法による生細胞の分子振動イメージング(振動分光法が拓く生命科学;分子から細胞まで,シンポジウム,第45回日本生物物理学会年会)

S05I6 非線形ラマン分光法による生細胞の分子振動イメージング(振動分光法が拓く生命科学;分子から細胞まで,シンポジウム,第45回日本生物物理学会年会)

Spectroscopic studies of the size and composition of single aerosol droplets

The characterization of aerosol properties and processes, non-intrusively and directly, poses a severe analytical challenge. In order to understand the role of aerosols in often complex environments, it is necessary to probe the particles in situ and without perturbation. Sampling followed by end-of-line analysis can lead to perturbations in particle composition, morphology and size, particularly when analysing liquid aerosol droplets containing volatile components. Optical spectroscopy can provide a strategy for the direct assessment of particle size, composition and phase. We review here the application of linear and non-linear Raman spectroscopies in the characterization of liquid aerosol droplets. Spontaneous Raman scattering can allow the unambiguous identification of chemical components and the determination of droplet composition. Stimulated Raman spectroscopy can allow the determination of droplet size with nanometre accuracy and can allow the characterization of near-surface composition. When combined, the mixing state and homogeneity in droplet composition can be investigated. We highlight some applications of these spectroscopic techniques in studies of the kinetics of particle transformation, the equilibrium composition of aqueous aerosol droplets, and the coagulation and mixing state of organic and aqueous aerosol components. Specifically, we examine the heat and mass transfer accompanying the evaporation of volatile components from liquid droplets, the equilibrium size of aqueous/sodium chloride droplets with varying relative humidity, and the mixing of the immiscible decane and water components during droplet coagulation. We conclude by considering the potential of these techniques for improving our understanding of aerosol properties and processes.

Enhancement of Raman modes by coherent control in β-carotene

The enhancement of vibrational modes by phase-shaped femtosecond laser pulses is studied under resonant and non-resonant conditions in an open loop coherent control experiment using non-linear Raman spectroscopy. Applying multipulse sequences matching the periodicity of single vibrations, the modes of β-carotene solvated in cylcohexane were not only specifically excited, but under resonant conditions also enhanced compared to the Fourier-limited case. This effect is attributed to an increased population transfer to the excited state and stronger coherences created and demonstrates the feasibility to selectively amplify ground state Raman modes by coherent control.

Modern Raman spectroscopy: a practical approach

Preface. Acknowledgements. CHAPTER 1: INTRODUCTION, BASIC THEORY AND PRINCIPLES. 1.1 Introduction. 1.2 Basic Theory. 1.3 Molecular Vibrations. 1.4 Summary. CHAPTER 2: THE RAMAN EXPERIMENT - RAMAN INSTRUMENTATION, SAMPLE PRESENTATION, DATA HANDLING AND PRACTICAL ASPECTS OF INTERPRETATION. 2.1 Introduction. 2.2 Choice of Instrument. 2.3 Visible Excitation. 2.4 NIR Excitation. 2.5 Raman Sample Preparation and Handling. 2.6 Sample Mounting Accessories. 2.7 Microscopy. 2.8 Calibration. 2.9 Data Handling, Manipulation and Quantitation. 2.10 Approach to Qualitative Interpretation. 2.11 Summary. CHAPTER 3: THE THEORY OF RAMAN SPECTROSCOPY. 3.1 Introduction. 3.2 Absorption and Scattering. 3.3 States of a System and Hooke's Law. 3.4 The Nature of Polarizability and the Measurement of Polarization. 3.5 The Basic Selection Rule. 3.6 Number and Symmetry of Vibrations. 3.7 Symmetry Elements and Point Groups. 3.8 The Mutual Exclusion Rule. 3.9 The Kramer Heisenberg Dirac Expression. 3.10 Lattice Modes. 3.11 Conclusions. CHAPTER 4: RESONANCE RAMAN SCATTERING. 4.1 Introduction. 4.2 Theoretical Aspects. 4.3 Practical Aspects. 4.4 Examples of the Use of Resonance Raman Scattering. 4.5 Conclusions. CHAPTER 5: SURFACE-ENHANCED RAMAN SCATTERING AND SURFACE-ENHANCED RESONANCE RAMAN SCATTERING. 5.1 Introduction. 5.2 Theory. 5.3 Electromagnetic and Charge Transfer Enhancement. 5.4 Selection Rules. 5.5 Applications of SERS. 5.6 Applications of SERRS. 5.7 The Basic Method. CHAPTER 6: APPLICATIONS. 6.1 Introduction. 6.2 Inorganics and Minerals. 6.3 Art and Archaeology. 6.4 Polymers and Emulsions. 6.5 Colour. 6.6 Electronics Applications. 6.7 Biological and Pharmaceutical Applications. 6.8 Forensic Applications. 6.9 Plant Control and Reaction Following. 6.10 Summary. CHAPTER 7: MORE ADVANCED RAMAN SCATTERING TECHNIQUES. 7.1 Flexible Optics. 7.2 Tuneable Lasers, Frequency Doubling and Pulsed Lasers. 7.3 Spatially Resolved Systems. 7.4 Nonlinear Raman Spectroscopy. 7.5 Time Resolved Scattering. 7.6 Raman Optical Activity. 7.7 UV Excitation. 7.8 Conclusions. Index.