| 1. |
- Khodabakhsh, Amir, 1983-
(författare)
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Fourier transform and Vernier spectroscopy using optical frequency combs
- 2017
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Optical frequency comb spectroscopy (OFCS) combines two previously exclusive features, i.e., wide optical bandwidth and high spectral resolution, enabling precise measurements of entire molecular bands and simultaneous monitoring of multiple gas species in a short measurement time. Moreover, the equidistant mode structure of frequency combs enables efficient coupling of the comb power to enhancement resonant cavities, yielding high detection sensitivities. Different broadband detection methods have been developed to exploit the full potential of frequency combs in spectroscopy, based either on Fourier transform spectroscopy or on dispersive elements.There have been two main aims of the research presented in this thesis. The first has been to improve the performance of mechanical Fourier transform spectrometers (FTS) based on frequency combs in terms of sensitivity, resolution and spectral coverage. In pursuit of this aim, we have developed a new spectroscopic technique, so-called noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS), and achieved a shot-noise-limited sensitivity and low ppb (parts-per-billion, 10−9) CO2 concentration detection limit in the near-infrared range using commercially available components. We have also realized a novel method for acquisition and analysis of comb-based FTS spectra, a so-called sub-nominal resolution method, which provides ultra-high spectral resolution and frequency accuracy (both in kHz range, limited only by the stability of the comb) over the broadband spectral range of the frequency comb. Finally, we have developed an optical parametric oscillator generating a frequency comb in the mid-infrared range, where the strongest ro-vibrational molecular absorption lines reside. Using this mid-infrared comb and an FTS, we have demonstrated, for the first time, comb spectroscopy above 5 μm, measured broadband spectra of several species and reached low ppb detection limits for CH4, NO and CO in 1 s.The second aim has been more application-oriented, focused on frequency comb spectroscopy in combustion environments and under atmospheric conditions for fast and sensitive multispecies detection. We have demonstrated, for the first time, cavity-enhanced optical frequency comb spectroscopy in a flame, detected broadband high temperature H2O and OH spectra using the FTS in the near-infrared range and showed the potential of the technique for flame thermometry. For applications demanding a short measurement time and high sensitivity under atmospheric pressure conditions, we have implemented continuous-filtering Vernier spectroscopy, a dispersion-based spectroscopic technique, for the first time in the mid-infrared range. The spectrometer was sensitive, fast, robust, and capable of multispecies detection with 2 ppb detection limit for CH4 in 25 ms.
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| 2. |
- Andersson, Magnus, 1975-
(författare)
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Construction of force measuring optical tweezers instrumentation and investigations of biophysical properties of bacterial adhesion organelles
- 2007
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Optical tweezers are a technique in which microscopic-sized particles, including living cells and bacteria, can be non-intrusively trapped with high accuracy solely using focused light. The technique has therefore become a powerful tool in the field of biophysics. Optical tweezers thereby provide outstanding manipulation possibilities of cells as well as semi-transparent materials, both non-invasively and non-destructively, in biological systems. In addition, optical tweezers can measure minute forces (< 10-12 N), probe molecular interactions and their energy landscapes, and apply both static and dynamic forces in biological systems in a controlled manner. The assessment of intermolecular forces with force measuring optical tweezers, and thereby the biomechanical structure of biological objects, has therefore considerably facilitated our understanding of interactions and structures of biological systems. Adhesive bacterial organelles, so called pili, mediate adhesion to host cells and are therefore crucial for the initial bacterial-cell contact. Thus, they serve as an important virulence factor. The investigation of pili, both their biogenesis and their expected in vivo properties, brings information that can be of importance for the design of new drugs to prevent bacterial infections, which is crucial in the era of increased bacterial resistance towards antibiotics. In this thesis, an experimental setup of a force measuring optical tweezers system and the results of a number of biomechanical investigations of adhesive bacterial organelles are presented. Force measuring optical tweezers have been used to characterize three different types of adhesive organelles under various conditions, P, type 1, and S pili, which all are expressed by uropathogenic Escherichia coli. A quantitative biophysical force-extension model, built upon the structure and force response, has been developed. It is found, that this model describes the biomechanical properties for all three pili in an excellent way. Various parameters in their energy landscape, e.g., bond lengths and transition barrier heights, are assessed and the difference in behavior is compared. The work has resulted in a method that in a swift way allows us to probe different types of pili with high force and high spatial resolution, which has provided an enhanced understanding of the biomechanical function of these pili.
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| 3. |
- Björnham, Oscar, 1976-
(författare)
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A study of bacterial adhesion on a single-cell level by means of force measuring optical tweezers and simulations
- 2009
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The intriguing world of microbiology is nowadays accessible for detailed exploration at a single–molecular level. Optical tweezers are a novel instrument that allows for non–invasive manipulation of single cells by the sole use of laser light and operates on the nano– and micrometer scale which corresponds to the same length scale as living cells. Moreover, forces within the field of microbiology are typically in the picoNewton range which is in accordance with the capability of force measuring optical tweezers systems. Both these conformabilities imply that force measuring optical tweezers is suitable for studies of single living cells. This thesis focuses on the mechanisms of bacterial attachments to host cells which constitute the first step in bacterial infection processes. Bacteria bind specifically to host receptors by means of adhesins that are expressed either directly on the bacterial membrane or on micrometer–long adhesion organelles that are called pili. The properties of single adhesin–receptor bonds that mediate adherence of the bacterium Helicobacter pylori are first examined at various acidities. Further on, biomechanical properties of P pili expressed by Escherichia coli are presented to which computer simulations, that capture the complex kinetics of the pili structure and precisely replicate measured data, are applied. Simulations are found to be a powerful tool for investigations of adhesive attributes of binding systems and are utilized in the analyses of the specific binding properties of P pili on a single–pilus level. However, bacterial binding systems generally involve a multitude of adhesin–receptor bonds. To explore bacterial attachments, the knowledge from single–pilus studies is brought into a full multipili attachment scenario which is analyzed by means of theoretical treatments and simulations. The results are remarkable in several aspects. Not only is it found that the intrinsic properties of P pili are composed in an optimal combination to promote strong multipili bindings. The properties of the pili structure itself are also found to be optimized with respect to its in vivo environment. Indeed, the true meaning of the attributes derived at a single–pilus level cannot be unraveled until a multipili–binding system is considered. Whereas detailed studies are presented for the helix–like P pili expressed by Gram–negative Escherichia coli, conceptual studies are presented for the open coil–like T4 pili expressed by Gram–positive Streptococcus pneumoniae. The structural and adhesive properties of these two types of pili differ considerably. These dissimilarities have far–reaching consequences on the adhesion possibilities at both single–pilus and multipili levels which are discussed qualitatively. Moreover, error analyses of conventional data processing methods in dynamic force spectroscopy as well as development of novel analysis methods are presented. These findings provide better understanding of how to perform refined force measurements on single adhesion organelles as well as how to improve the analyses of measurement data to obtain accurate parameter values of biomechanical entities. In conclusion, this thesis comprises a study of bacterial adhesion organelles and the way they cooperate to establish efficient attachment systems that can successfully withstand strong external forces that acts upon bacteria. Such systems can resist, for instance, rinsing effects and thereby allow bacteria to colonize their host. By understanding the complexity, and thereby possible weaknesses, of bacterial attachments, new targets for combating bacterial infections can be identified.
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| 4. |
- de Andres Gonzalez, Aitor, 1992-
(författare)
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Enhancement of few-cycle light fields for relativistic nanophotonics
- 2023
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Pulses of light that are both ultrashort and ultraintense are often generated using optical parametric amplifiers (OPA). These are capable of driving highly non-linear interactions with matter, which are interesting when studying the fundamental laws of our universe. Furthermore, they are also used in many scientific and industrial applications, such as particle accelerators, inertial-confinement nuclear fusion, and medical diagnostics and treatment. This thesis explores the diagnostic and optimization of pulses of light with extreme properties and utilizes them to drive electron acceleration.The applied light pulses with very short duration (<5 fs) and high peak power (>10 TW) are sensitive to develop spatio-temporal aberrations. These are color-dependent distortions that can significantly degrade the pulse properties, like peak-intensity, and affect their applicability. Furthermore, in most cases they are not easy to correctly diagnose, with current tools failing to provide widely applicable solutions. In this thesis, we describe a new type of spatio-temporal coupling that is especially relevant for optical parametric synthesizers (OPS), systems that coherently combine multiple OPA stages. To do this, we have contributed to the development of two methods for the characterization of such aberrations, the so-called simplified-INSIGHT and HASO multispectral. These enabled us to further improve the structure of our OPS and laser systems.We also explored the applicability of light pulses to drive relativistic electron acceleration in vacuum. To this end, an injection system using nanotips is presented, capable of inserting electrons spatially in the focus and temporally in the most intense light-cycle. This way, vacuum laser accelerated electrons of up to 14 MeV were detected using a tight focusing configuration (f#1) and their properties characterized. Furthermore, we investigated the dependence of the acceleration process when the focusing geometry is relaxed (f#3). This resulted in the unexpected outcome of similar electron energies in both cases, although the intensity was ten times reduced. This indicates that the decrease in accelerating field strength is compensated by longer acceleration lengths, which is not predicted by currently existing analytical models.
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| 5. |
- Fischer, Peter, 1988-
(författare)
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A sub-5 fs 100 TW optical parametric synthesizer
- 2022
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- State-of-the-art ultrashort light sources in the visible and near-infrared spectral regions provide direct access to the femtosecond realm, thereby enabling understanding and control of electronic processes within matter. On the other hand, ultra-intense light pulses lead to the emergence of relativistic electron motion and many related phenomena, such as electron & ion acceleration and high-order harmonic generation in plasmas. The generation and amplification techniques for those intense short light pulses were developed over the last 60 years. Nowadays, they are unique scientific research tools and the basis of commercial applications. The driving forces behind many of these new optical technologies are second and third order nonlinear ultrashort processes. Optical parametric chirped pulse amplification (OPCPA) is currently the most interesting of these techniques and promises in particular high single-pass gain, broad gain bandwidth, scalability, good high-dynamic range temporal contrast, and tunability. However, OPCPA comes also with a bundle of challenges. The aim of this thesis, by utilizing the advantages and facing these challenges, is to boost a sub-two cycle optical parametric synthesizer (OPS), a two-color-pumped OPCPA, to an unprecedented parameter regime in respect of energy, intensity, contrast and stability.The presented sub-2-optical cycle OPS – the light wave synthesizer (LWS) - is a worldwide unique system, amplifying a spectral bandwidth in three pairs of OPCPA stages. One pair of these stages sequentially amplifies and coherently combines two complementary spectral ranges to an almost octave spanning bandwidth. The amplified spectrum ranges from 580 nm to 1000 nm, which makes Fourier limited pulses with 4.6 fs possible. The present system is a fundamental reconstruction and extension of a former version of LWS that provided peak powers of up to 16 TW. By carefully redesigning of the former OPCPA stages, implementing a new front end and adding two nominally 2.3 J Nd:YAG amplifiers, harmonic generation setups and a third pair of OPCPA stages, the pulse energy has been raised up to 450-500 mJ while keeping the spectral bandwidth. After compression, this corresponds to about the aspired 100 TW peak power.Focus was also laid on various important parameters for such ultra-short and ultra-intense light pulses, such as the temporal contrast, the carrier-envelope phase (CEP) and energy stability. Analysis and optimization of the 16 TW LWS version operation parameters made it possible to optimize the LWS-100 root mean square energy stabilities down to 0.3-0.5% over 100 s, which is significantly lower than previously reported for the former version. For the first time, the CEP-stability for this full system has been demonstrated. Currently, it is limited by slow drifts, but an active feedback system could suppress this to 400 mrad. The influences on the temporal contrast were investigated and prepulses identified and eliminated. Furthermore, hardware and software control for easy handling and reliable operation have been implemented.The LWS-100 pushes the limits for few-cycle laser technology even further. It enables the generation of intense and isolated attosecond pulses beyond 100 eV photon energy, acceleration of attosecond electron bunches to relativistic energies, measurement of nonlinear processes of inner shell electrons via XUV pump-probe experiments and generation of isolated attosecond pulses on plasma mirrors.
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| 6. |
- Hjältén, Adrian, 1988-
(författare)
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Precision molecular spectroscopy in the near- and mid-infrared using frequency comb-based Fourier transform spectrometers
- 2023
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Absorption spectroscopy is a powerful scientific tool for non-invasive and remote sensing applications ranging from atmospheric monitoring to astrophysics. In spectroscopic detection schemes it is necessary to have spectral models for any molecular species to be detected or quantified. Such models are often based on spectroscopic measurements or at the very least require experimental validation. The experimental data need to be accurate in terms of absorption line positions and intensities, but should also cover as many absorption lines as possible, i.e. broadband measurements are highly desirable.Fourier transform spectroscopy (FTS) based on optical frequency combs (OFCs) can supply laboratory data that meet these requirements. OFCs provide a broad optical bandwidth and high spectral brightness, and also revolutionized our ability to measure optical frequencies, which had a profound impact on the frequency accuracy of spectroscopic measurements. The combination of OFCs and FTS, using the recently developed sub-nominal resolution technique, allows for measuring broadband absorption spectra with very high resolution, and a frequency accuracy provided by the OFCs. The aim of the work in this thesis was to expand the application of sub-nominal OFC-FTS to provide the much needed high-accuracy data for validation and development of spectroscopic databases of molecules relevant for a wide range of sensing application.We developed a spectrometer to target the strong molecular absorption bands in the mid-infrared using two OFC sources based on difference frequency generation (DFG) emitting in the 3 μm and 8 μm wavelength ranges. We measured the spectra of iodomethane, CH3I, and dibromomethane, CH2Br2, around 3 μm, fitted Hamiltonian models to several bands using the PGOPHER software, and reported molecular constants. For CH3I we improved on previous models, while for CH2Br2 we presented a new interpretation of the spectrum. We also reported the first assessments of line intensities of CH3I performed using multispectral fitting. At 8 μm, we implemented OFC-FTS based on a fiber-based compact DFG OFC source and measured low pressure spectra of nitrous oxide, N2O, methane, CH4, and formaldehyde, H2CO. After the frequency accuracy was confirmed by excellent agreement with an earlier accurate study of N2O, we compiled extensive line lists for CH4 and H2CO containing hundreds of transition frequencies with a precision improved by one order of magnitude compared to previously available data, and also reported line intensities for most transitions. For CH4 the new data were used to improve a global Hamiltonian model, while the H2CO data were incorporated into an algorithm based on spectroscopic networks to yield better precision in predicted energy levels and transition frequencies.We also further developed a recent implementation of double resonance (DR) spectroscopy where optical pumping by a continuous-wave laser was used to populate selected vibrational energy levels of CH4 not populated at room temperature, and a near-infrared OFC probed sub-Doppler transitions from the pumped states. Such measurements are necessary to validate theoretical predictions of transitions between excited vibrational levels that are relevant for high-temperature environments such as the atmospheres of hot celestial objects. We reported an improved measurement setup using a new pump laser, new enhancement cavity with an updated OFC-cavity locking scheme, and measured transitions between more highly excited rotational levels than was previously reported. The higher rotational excitations lead to a larger number of DR transitions, which could be readily detected in the broadband high-resolution OFC-FTS spectra. We retrieved parameters of 88 lines of which we could assign 79 to theoretically predicted transitions. We found systematic frequency discrepancies with the predictions, that had not been observed earlier for lower rotational levels.These implementations of sub-nominal OFC-FTS thus provided highly accurate line lists and improved spectral models of absorption bands of several molecules in the universally important mid-infrared region, as well as the first detection of 88 transitions between excited vibrational states of CH4 relevant for high-temperature environments. We demonstrated the high potential of these techniques for collecting large amounts of accurate spectroscopic data, that further the scope of applicability of molecular spectroscopy.
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| 7. |
- Johansson, Alexandra C., 1987-
(författare)
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Optical Frequency Comb Fourier Transform Spectroscopy
- 2018
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Fourier transform spectroscopy (FTS) based on optical frequency combs is an excellent spectroscopic tool as it provides broadband molecular spectra with high spectral resolution and an absolutely calibrated frequency scale. Moreover, the equidistant comb mode structure enables efficient coupling of the comb to enhancement cavities, yielding high detection sensitivity. This thesis focuses on further advances in comb-based FTS to improve its performance and extend its capabilities for broadband precision spectroscopy, particularly in terms of i) spectral resolution, ii) accuracy and precision of molecular parameters as well as concentrations retrieved from fitting models to spectra, and iii) species selectivity.To improve the spectral resolution we developed a new methodology to acquire and analyze comb-based FTS signals that yields spectra with a resolution limited by the comb linewidth rather than the optical path difference of the FTS, referred to as the sub-nominal resolution method. This method enables measurements of narrow features, e.g. low-pressure absorption spectra and modes of enhancement cavities, with frequency scale accuracy and precision provided by the comb. Using the technique we measured low-pressure spectra of the entire 3ν1+ν3 carbon dioxide (CO2) band at 1575 nm with sufficient signal-to-noise ratio and precision to observe collision narrowing of the absorption lineshape, which was for the first time with a comb-based spectroscopic technique. This allowed retrieval of spectral line parameters for this CO2 band using the speed-dependent Voigt profile.Using the sub-nominal resolution method, we measured the transmission modes of a Fabry-Perot cavity over 15 THz of bandwidth with kHz resolution and characterized the cavity modes in terms of their center frequency, linewidth, and amplitude. From the mode center frequencies, we retrieved the group delay dispersion of cavity mirror coatings and intracavity gas with an unprecedented combination of spectral bandwidth and resolution. By measuring both the mode broadening and frequency shift simultaneously we performed broadband cavity-enhanced complex refractive index spectroscopy (CE-CRIS), which allows for simultaneous and calibration-free assessment of the absorption and dispersion spectra of intracavity gas. In this first demonstration we measured the absorption and dispersion spectra of three combination bands of CO2 in the 1525 to 1620 nm range.Another comb-based FTS technique is noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS), which combines phase modulation and cavity-enhancement to obtain broadband and highly sensitive absorption spectra. In this thesis we improved the NICE-OFCS technique in terms of stability, sensitivity and modeling of the NICE-OFCS signal. We implemented a model of the NICE-OFCS signal with multiline fitting for assessment of gas concentration. We also identified the optimum operating conditions of the NICE-OFCS systems for accurate gas concentration assessment.Finally, to improve the species selectivity we combined comb-based FTS with the Faraday rotation spectroscopy (FRS) technique. In this first demonstration of optical frequency comb Faraday rotation spectroscopy (OFC-FRS), we measured background and interference-free spectra of the entire Q- and R-branches of the fundamental vibrational band of nitric oxide at 5.3 μm showing good agreement with the theoretical model.
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| 8. |
- Lu, Chuang, 1991-
(författare)
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Continuous-filtering Vernier spectroscopy
- 2022
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Continuous-filtering Vernier spectroscopy (CF-VS) is a laser-based detection technique that combines the broad spectral coverage of an optical frequency comb (OFC) with the enhanced interaction length provided by an optical cavity. The resonances of the cavity filter the OFC to a small group of comb modes that probe the transitions of the species present in the cavity. Controlling cavity resonances allows for a fast scanning of the selected comb modes across the full bandwidth of the comb. CF-VS delivers high detection sensitivity through its immunity to the frequency-to-amplitude-noise conversion. Previous works have shown the capability of CF-VS to perform sensitive and broadband measurements of multiple species in both the near-infrared (NIR) and the mid-infrared (MIR) regions. Those implementations required high-bandwidth stabilization via feedback to the comb sources, which resulted in bulky setups and complex operations. Moreover, they provided acquisition rates up to 20 Hz, limited by the mechanical design. Besides, the target species were measured under static conditions 一 CF-VS had not yet been employed to monitor any time-dependent processes.The goal of the thesis was to address these issues. In the first project, we used CF-VS based on an Er:fiber comb to measure consecutive spectra of H2O and OH with 25 ms time resolution in a premixed flame whose fuel/air equivalence ratio was modulated with a square wave to simulate temporal perturbations. The concentrations of both species were retrieved with percent level precision, and their temporal profiles were repeatable in each modulation cycle. The steady-state concentrations were in good agreement with a static flame simulator. This work was the first demonstration of CF-VS and cavity-enhanced comb-based spectroscopy with ms time resolution.In the second project, we implemented a new design of CF-VS that uses a compact Er:fiber comb and a custom-made moving aperture. This removes the requirement for high-bandwidth stabilization and allows acquisition rates up t0 100 Hz. To verify these capabilities, we measured CO2 and CH4 spectra in two spectral ranges. We developed a simple model to account for the influence of the high scanning speed above the adiabatic limit on the absorption signal.The last project aimed to implement a robust and compact CF-VS spectrometer in the MIR region. For that, we improved an existing MIR source based on difference frequency generation (DFG) using a low-noise Yb:fiber pump, delay stabilization, and a novel polarization-maintaining silicon crystal fiber. The MIR comb uses a soliton generated in the fiber as the seed for DFG. We characterized the soliton using the pump laser. The wide tuning range of the soliton allows the idler to emit in the 2.7-4.2 μm range with high brightness. The MIR comb has a simple delay stabilization and a fixed zero-offset frequency and was successfully implemented to measure high-resolution and precision spectra of CH3I using a comb-resolved Fourier transform spectrometer. Finally, we used the source to perform CF-VS by measuring CH4 spectra at around 3.3 μm. We showed that a single-shot spectrum could be successfully retrieved under the robust operation in the fingerprint regime.
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| 9. |
- Schmidt, Florian, 1975-
(författare)
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Laser-based absorption spectrometry : development of NICE-OHMS towards ultra-sensitive trace species detection
- 2007
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Laser-based absorption spectroscopy (AS) is a powerful technique for qualitative and quantitative studies of atoms and molecules. An important field of use of AS is the detection of species in trace concentrations, which has applications not only in physics and chemistry but also in biology and medicine, encompassing environmental monitoring, regulation of industrial processes and breath analysis. Although a large number of molecular species can successfully be detected with established AS techniques, there are some applications that require higher sensitivity, selectivity and accuracy, yet robust and compact instrumentation.Various approaches have been made during the years to improve on the performance of AS, usually based on modulation spectrometry or external cavities. The most sensitive absorption technique of today is, however, noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS). This technique elegantly combines several approaches: external cavities (for optical path length enhancement), modulation techniques (for noise reduction) and saturation spectroscopy (for enhanced selectivity). However, due to its complexity, the technique has so far not been applied to practical trace species detection.This thesis provides the background for an understanding of NICE-OHMS and describes the construction of a first compact NICE-OHMS spectrometer based on a narrowband fiber laser. Moreover, it gives theoretical expressions for NICE-OHMS signal lineshapes, measured in various modes of detection, which can be fitted to the experimental data and thereby facilitate the assessment of species concentration. The sensitivity of the instrumentation is demonstrated by detection of acetylene (C2H2) and carbon dioxide (CO2) in the 1.5 μm region. A fractional absorption sensitivity of 3*10-9 (integrated absorption of 5*10-11 cm-1), could be achieved using a cavity with a finesse of 4800 and an acquisition time of 0.7 s. This results in a detection limit for C2H2 of 4.5 ppt (4.5*10-12 atm).In addition, the thesis revives the idea of using an accurate (frequency) measurement of the free-spectral-range (FSR) of an external cavity for sensitive and calibration-free concentration assessment. A theoretical description of the expected signal lineshapes is given, and in a first experimental demonstration the FSR could be measured with a resolution of 5 Hz, resulting in a fractional absorption sensitivity of 1*10-7, and subsequently in a detection limit for C2H2 of 180 ppt (12.5 s acquisition time).The thesis, finally, also contributes to the continuously ongoing development of conventional AS and wavelength modulated AS by addressing concepts related to when the light optically saturates the transition.
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| 10. |
- Wang, Junyang, 1983-
(författare)
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Dicke narrowing and speed-dependent effects in dispersion signals : Influence on assessment of concentration and spectral parameters by noise-immune cavity-enhanced optical heterodyne molecular spectrometry
- 2013
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Laser spectroscopic techniques have, during the last decades, demonstrated an extraordinary capability for sensitive detection of molecular constituents in gas phase. Since spectra from such techniques constitute unique and characteristic signatures for each type of species, these techniques enable investigations of molecular structures as well as detection of the presence of species in a gas mixture. They are therefore used for a variety of application, from fundamental studies to the assessment of gas concentrations. In fact, quantitative assessments of gas concentrations by laser-based techniques are constantly gaining in popularity, primarily due to properties such as high sensitivity and selectivity and an ability to perform non-invasive measurement. Moreover, investigations of isolated molecular transitions under different conditions provide excellent means to obtain a comprehensive understanding of spectral broadening mechanisms, which is of importance for, for example, environmental sciences and remote sensing applications. In fundamental studies, spectroscopic parameters are often retrieved from fits of a model function of the technique used, which in turn is based upon a suitable lineshape function. In order to obtain parameter values with highest possible accuracy, it is of importance to use the lineshape model that most correctly can predict the measured spectra. Even though the Voigt function is the most commonly used lineshape model when both Doppler and collision broadenings are present, it is not always suitable when spectroscopic parameters are to be assessed with high precision.This thesis represents a thorough investigation of Dicke narrowing and speed-dependent effects, which are phenomena that are not accounted for by the conventional Voigt profile. For the first time, it is demonstrated that both these effects take place not only in absorption but also in the dispersion mode of detection. Their dispersion lineshape functions are first theoretically presumed and explicitly given before they are validated experimentally by the noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS). By using the models developed, it is also shown that although the two modes of detection, absorption and dispersion, both can provide good quality of fits, they do not always provide identical spectroscopic parameters. A detailed analysis under which conditions they do so, and subsequent recommendations of their use, are presented.It also describes the instrumental implementation of a distributed-feed-back (DFB) laser-based NICE-OHMS instrumentation, which constitutes an important step towards the further development of this technique. Due to the wide tunability of the DFB laser, the setup is capable of extending the working range of NICE-OHMS into the collision broadening region, which, in turn, allows for precise spectroscopic studies. The use of a fiber-coupled DFB laser also provides a compact NICE-OHMS system. The minimum detectable on-resonance absorption was assessed to 2× 10-10 cm-1 for a 70 s integration time.
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| 11. |
- Westberg, Jonas, 1983-
(författare)
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Faraday modulation spectroscopy : Theoretical description and experimental realization for detection of nitric oxide
- 2013
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Faraday modulation spectroscopy (FAMOS) is a laser-based spectroscopic dispersion technique for detection of paramagnetic molecules in gas phase. This thesis presents both a new theoretical description of FAMOS and experimental results from the ultra-violet (UV) as well as the mid-infrared (MIR) regions. The theoretical description, which is given in terms of the integrated linestrength and Fourier coefficients of modulated dispersion and absorption lineshape functions, facilitates the description and the use of the technique considerably. It serves as an extension to the existing FAMOS model that thereby incorporates also the effects of lineshape asymmetries primarily originating from polarization imperfections. It is shown how the Fourier coefficients of modulated Lorentzian lineshape functions, applicable to the case with fully collisionally broadened transitions, can be expressed in terms of analytical functions. For the cases where also Doppler broadening needs to be included, resulting in lineshapes of Voigt type, the lineshape functions can be swiftly evaluated (orders of magnitude faster than previous procedures) by a newly developed method for rapid calculation of modulated Voigt lineshapes (the WWA-method). All this makes real-time curve fitting to FAMOS spectra feasible. Two experimental configurations for sensitive detection of nitric oxide (NO) by the FAMOS technique are considered and their optimum conditions are determined. The two configurations target transitions originating from the overlapping Q22(21=2) and QR12(21=2) transitions in the ultra-violet (UV) region (227nm) and the Q3=2(3=2)-transition in the fundamental rotational-vibrational band in the mid-infrared (MIR) region (5.33 µm). It is shown that the implementations of FAMOS in the UV- and MIR-region can provide detection limits in the low ppb range, which opens up the possibility for applications where high detection sensitivities of NO is required.
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| 12. |
- Alrifaiy, Ahmed
(författare)
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Lab on a chip for electrophysiological measurements with control of the oxygen content : optical manipulation and spectroscopic analysis of biological cells
- 2013
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Stroke affects nearly 20 million people around the world every year. Clinically, stroke is a result of brain damage due to the shortage of oxygen delivered to the nerve cells. To minimize suffering and costs related to the disease, extensive research is performed on different levels. The focus of our research is to achieve fundamental understanding on how the lack of oxygen in brain tissue activates intrinsic biomolecular defense mechanisms that may reduce brain damage. More knowledge may hopefully lead to new therapeutic and preventive strategies on the molecular level for individuals in the risk zone for stroke or those who have just suffered a stroke.The area of study is based on the discovery of a hemoprotein called neuroglobin (Ngb), which is found in various regions in the brain, in the islets of Langerhans, and in the retina. Several studies have shown that Ngb seems to have a protective function against hypoxia-related damage. However, until now, it has not been understood how Ngb affects the nerve system and protects neurons from damage.The well-established patch-clamp technique is routinely used to measure and analyze the electrophysiological activity of individual biological cells. To perform accurate patchclamp experiments, it is important to create well-controlled physiological conditions, i.e. different oxygen levels and fast changes of nutrients and other biochemical substances. A promising approach is to apply lab on a chip technologies combined with optical manipulation techniques. These give optimal control over fast changing environmental conditions and enable multiple readouts.The conventional open patch-clamp configuration cannot provide adequate control of the oxygen content. Therefore, the aim of the thesis was to design and test a multifunctional microfluidic system, lab on a chip (LOC), that can achieve normoxic, anoxic and hypoxic conditions. The conventional patch clamp configuration was substituted by a gas-tight LOC system with an integrated patch-clamp micropipette. The system was combined with optical tweezers, optical sensor and optical spectroscopy.Optical tweezers were used to trap and guide single cells through the LOC microchannels towards the fixed micropipette. Optical spectroscopy was essential to investigate the biochemical composition of the biological samples. The developed, gas-tight LOC acted as a multifunctional system for simultaneous electrophysiological and spectroscopic experiments with good control over the oxygen content in the liquid perifusing the cells. The system was tested in series of experiments: optically trapped cells (red blood cells from human and chicken and nerve cells) were steered to the fixed patch-clamp pipette within the LOC system. The oxygen content within the microfluidic channels was measured to ∼ 1% compared to the usual 4-7% found in open system. The trapping dynamics were monitored in real-time while the spectroscopic measurements were performed simultaneously to acquire absorption spectra of the trapped cell under varying environments. To measure the effect of the laser tweezers on the sample, neurons from rats in a Petri dish were optically trapped and steered towards the patch-clamp micropipette where electrophysiological investigations were performed. The optical tweezers had no effect on the electrophysiological measurements.The future aim is to perform complete protocols of patch-clamp electrophysiological investigations while simultaneously monitoring the biochemical composition of the sample by optical spectroscopy. The straightforwardness and stability of the microfluidic chip have shown excellent potential to be applied for various biomedical applications. The subsequent ambition is to use this system as a mini laboratory that has benefits in cell sorting, patch-clamp and fertilization experiments where the gaseous and the biochemical content is of importance.The long-term goal is to study the response of individual neurons and defense mechanisms under hypoxic conditions that may establish new ways to understand cell behavior related to Ngb for various diseases such as stroke, Alzheimer’s and Parkinson’s.
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| 13. |
- Ehlers, Patrick, 1981-
(författare)
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Further development of NICE-OHMS : – an ultra-sensitive frequency-modulated cavity-enhanced laser-based spectroscopic
technique for detection of molecules in gas phase
- 2014
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Noise-immune cavity-enhanced optical heterodyne molecular spectroscopy, NICE-OHMS, is a laser-based spectroscopic detection technique that comprises the concepts of frequency modulation (FM, for reduction of 1/f-noise by detecting the signal at a high frequency) and cavity enhancement (CE, for a prolongation of the optical path length) in a unique way. Properly designed, this gives the technique an intrinsic immunity against the frequency-to-noise conversion that limits many other types of CE techniques. All this gives it an exceptionally high sensitivity for detection of molecular species. Although originally developed for frequency standard purposes in the late 1990s, soon thereafter development of the technique towards molecular spectroscopy and trace gas detection was initiated. This thesis focuses on the further development of Doppler- broadened NICE-OHMS towards an ultra-sensitive detection technique. A number of concepts have been addressed. A few of these are: i) The detection sensitivity of fiber-laser-based NICE- OHMS has been improved to the 10−12 cm−1 range, which for detection of C2H2 corresponds to a few ppt (parts-per-trillion, 1:1012) in gas phase, by improving the locking of the laser to a cavity mode by use of an acousto-optic modulator. ii) It is shown that the system can be realized with a more compact footprint by implementation of a fiber-optic circulator. iii) A systematic and thorough investigation of the experimental conditions that provide maximum signals, referred to as the optimum conditions, e.g. modulation and demodulation conditions and cavity length, has been performed. As a part of this, an expression for the NICE-OHMS line shape beyond the conventional triplet formalism has been proposed and verified. iv) To widen the applicability of NICE-OHMS for detection of pressure broadened signals, also a setup based upon a distributed-feedback (DFB) laser has been realized. v) In this regime, the Voigt profile cannot model signals with the accuracy that is needed for a proper assessment of analyte concentrations. Therefore, the thesis demonstrates the first implementations of line profiles encompassing Dicke narrowing and speed-dependent effects to NICE-OHMS. While such profiles are well-known for absorption, there were no expressions available for their dispersion counterparts. Such expressions have been derived and validated by accompanying experiments. vi) The applicability of the technique for elemental detection, then referred to as NICE-AAS, has been prophesied.
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| 14. |
- Forssén, Clayton, 1991-
(författare)
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Fabry-Pérot based refractometry : development of a transportable refractometer for assessment of gas pressure
- 2023
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- A unified description of physical phenomena through measurement science is one of the foundational pillars in a global society. The International System of Units (SI) is the most widely used system of units and since its redefinition in 2019, all units encompassed by it are based on fundamental physical constants. The units of the SI, such as the second, metre, and kilogram, are realized by the use of primary standards which are used, through calibration chains, to certify the accuracy of measuring devices in our society. Its redefinition enabled the realization of the SI-unit for pressure (pascal) in a novel way; instead of force per area (N/m2), it can alternatively be defined as an energy density (J/m3). Subsequently, this opened up for the use of optical realizations of the pascal (Pa). It has been prophesied that a possible means to do this is by assessing refractivity through the use of Fabry-Pérot (FP) refractometry. Although such instrumentation indeed can assess refractivity, it has unfortunately been found that they in practice are affected by various types of disturbances that aggravate assessments with the required uncertainty.This thesis describes the development of FP-based refractometers utilizing a novel measurement methodology, denoted gas modulation refractometry (GAMOR). By the use of rapid gas modulation and baseline interpolation, GAMOR has the ability to significantly reduce the influence of various types of disturbances, not least drifts and fluctuations. From this, two FP-based refractometers have been developed; one stationary, denoted the SOP, capable of assessing pressure with an uncertainty of [(10 mPa)2 + (10 × 10−6·P)2]1/2, and one transportable, denoted the TOP, with an uncertainty of [(16 mPa)2 + (28 × 10−6·P)2]1/2. Furthermore, it was shown that their mutual short-term precision is excellent, with a deviation of only 0.04 ppm when simultaneously assessing a pressure of 16 kPa.A major part of this thesis was devoted to the construction of the TOP and an investigation of its transportability and performance. It was used in a ring comparison with various pressure standards at four European national metrology institutes. It was concluded that, despite being transported, the performance remained virtually unchanged, and that, in the 10 – 90 kPa range, all the standards agreed within their uncertainties.These results indicate that FP-based refractometers utilizing the GAMOR methodology have the potential to act as transportable standards based on fundamental physical constants and paves the way for future research within the field.
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| 15. |
- Hausmaninger, Thomas, 1987-
(författare)
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Mid- and near-infrared NICE-OHMS : techniques for ultra-sensitive detection of molecules in gas phase
- 2018
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS) is a technique for ultra-sensitive detection of molecular absorption and dispersion. For highest performance, the technique combines cavity enhancement (CE) with frequency modulation (FM); while the former increases the effective interaction length between the light and the analyte by several orders of magnitudes, the latter removes the in-coupling of 1/f noise and makes the signals background free. The combination of CE and FM also gives the technique an immunity to amplitude noise caused by the jitter of the laser frequency relative to the cavity resonance frequencies. All these properties make the technique suitable for ultra sensitive trace gas detection in the sub-parts-per-trillion (ppt) range. The aim of this thesis is to improve the performance of the NICE-OHMS technique and to increase its range of applications.The work in this thesis can be divided into three areas:Firstly, a mid-infrared (MIR)-NICE-OHMS instrumentation was developed. In a first realization an unprecedented white-noise equivalent absorption limit for Doppler broadened (Db) detection in the MIR of 3×10-9 cm-1Hz-1/2was demonstrated. This was subsequently improved to 2.4×10-10 cm-1Hz-1/2allowing for detection methane and its two main isotopologues (CH3D and 13CH4) at their natural abundance.Secondly, further development of an existing near-infrared NICE-OHMS system was performed. This resulted in an improved longtime stability and the first shot-noise limited NICE-OHMS system for Db detection with a noise equivalent absorption limit of 2.3×10-14 cm-1detected over 200 s. Thirdly, models and theoretical descriptions of NICE-OHMS signals under strong absorption conditions and from methane under high laser power were developed. It was experimentally verified that the models allow for a more accurate evaluation of NICE-OHMS signals under a wide range of conditions.
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| 16. |
- Lathdavong, Lemthong, 1964-
(författare)
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Development of diode laser-based absorption and dispersion spectroscopic techniques for sensitive and selective detection of gaseous species and temperature
- 2011
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The main aim of this thesis has been to contribute to the ongoing work with development of new diode-laser-based spectroscopic techniques and methodologies for sensitive detection of molecules in gas phase. The techniques under scrutiny are tunable diode laser absorption spectrometry (TDLAS) and Faraday modulation spectrometry (FAMOS). Conventional distributed-feedback (DFB) telecommunication diode lasers working in the near-infrared (NIR) region have been used for detection of carbon monoxide (CO) and temperature in hot humid media whereas a unique frequency-quadrupled external-cavity diode laser producing mW powers of continuous-wave (cw) light in the ultra violet (UV) region have been used for detection of nitric oxide (NO). A methodology for assessment of CO in hot humid media by DFB-TDLAS has been developed. By addressing a particular transition in its 2nd overtone band, and by use of a dual-fitting methodology with a single reference water spectrum for background correction, % concentrations of CO can be detected in media with tens of percent of H2O (≤40%) at T≤1000 °C with an accuracy of a few %. Moreover, using an ordinary DFB laser working in the C-band, a technique for assessment of the temperature in hot humid gases (T≤1000 °C) to within a fraction of a percent has been developed. The technique addresses two groups of lines in H2O that have a favorable temperature dependence and are easily accessed in a single scan, which makes it sturdy and useful for industrial applications. A technique for detection of NO on its strong electronic transitions by direct absorption spectrometry (DAS) using cw UV diode laser light has been developed. Since the electronic transitions are ca. two or several orders of magnitude stronger than of those at various rotational-vibrational bands, the system is capable of detecting NO down to low ppb∙m concentrations solely using DAS. Also the FAMOS technique has been further developed. A new theoretical description expressed in terms of both the integrated line strength of the transition and 1st Fourier coefficients of a magnetic-field-modulated dispersive lineshape functions is presented. The description has been applied to both ro-vib Q-transitions and electronic transitions in NO. Simulations under different pressures and magnetic field conditions have been made that provide the optimum conditions for both cases. A first demonstration and characterization of FAMOS of NO addressing its electronic transitions in the UV-region has been made, resulting in a detection limit of 10 ppb∙m. The characterization indicates that the technique can be significantly improved if optimum conditions can be obtained, which demonstrates the high potential of the UV-FAMOS technique.
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| 17. |
- Silander, Isak, 1980-
(författare)
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Cavity enhanced optical sensing
- 2015
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- An optical cavity comprises a set of mirrors between which light can be reflected a number of times. The selectivity and stability of optical cavities make them extremely useful as frequency references or discriminators. With light coupled into the cavity, a sample placed inside a cavity will experience a significantly increased interaction length. Hence, they can be used also as amplifiers for sensing purposes. In the field of laser spectroscopy, some of the most sensitive techniques are therefore built upon optical cavities. In this work optical cavities are used to measure properties of gas samples, i.e. absorption, dispersion, and refractivity, with unprecedented precision.The most sensitive detection technique of all, Doppler-broadened noise-immune cavity enhanced optical heterodyne molecular spectrometry (Db NICE-OHMS), has in this work been developed to an ultra-sensitive spectroscopic technique with unprecedented detection sensitivity. By identifying limiting factors, realizing new experimental setups, and determining optimal detection conditions, the sensitivity of the technique has been improved several orders of magnitude, from 8 × 10-11 to 9 × 10-14 cm-1. The pressure interval in which NICE-OHMS can be applied has been extended by derivation and verification of dispersions equations for so-called Dicke narrowing and speed dependent broadening effects. The theoretical description of NICE-OHMS has been expanded through the development of a formalism that can be applied to the situations when the cavity absorption cannot be considered to be small, which has expanded the dynamic range of the technique. In order to enable analysis of a large number of molecules at their most sensitive transitions (mainly their fundamental CH vibrational transitions) NICE-OHMS instrumentation has also been developed for measurements in the mid-infrared (MIR) region. While it has been difficult to realize this in the past due to a lack of optical modulators in the MIR range, the system has been based on an optical parametric oscillator, which can be modulated in the near-infrared (NIR) range.As the index of refraction can be related to density, it is possible to retrieve gas density from measurements of the index of refraction. Two such instrumentations have been realized. The first one is based on a laser locked to a measurement cavity whose frequency is measured by compassion with an optical frequency comb. The second one is based on two lasers locked to a dual-cavity (i.e. one reference and one measurement cavity). By these methods changes in gas density down to 1 × 10-9 kg/m3 can be detected.All instrumentations presented in this work have pushed forward the limits of what previously has been considered measurable. The knowledge acquired will be of great use for future ultrasensitive cavity-based detection methods.
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