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Optical parametric amplification with periodically poled KTiOPO4Fragemann, Anna January 2005 (has links)
This thesis explores the use of engineered nonlinear crystals from the KTiOPO4 (KTP) family as the gain material in optical parametric amplifiers (OPAs), with the aim to achieve more knowledge about the benefits and limitations of these devices. The work aims further at extending the possible applications of OPAs by constructing and investigating several efficient and well performing amplifiers. An OPA consists of a strong pump source, which transfers its energy to a weak seed beam while propagating through a nonlinear crystal. The crystals employed in this work are members of the KTP family, which are attractive due to their large nonlinear coefficients, high resistance to damage and wide transparency range. The flexibility of OPAs with respect to different wavelength regions and pulse regimes was examined by employing various dissimilar seed and pump sources. The possibility to adapt an OPA to a specific pump and seed wavelength and achieve efficient energy conversion between the beams, originates from quasi-phasematching, which is achieved in periodically poled (PP) nonlinear crystals. Quasi-phasematched samples can be obtained by changing the position of certain atoms in a ferroelectric crystal and thereby reversing the spontaneous polarisation. In this thesis several material properties of PP crystals from the KTP family were examined. The wavelength and temperature dispersion of the refractive index were determined for PP RbTiOPO4, which is essential for future use of this material. Another experiment helped to increase the insight into the volumes close to domain walls in PP crystals Further, several OPAs were built and their ability to efficiently amplify the seed beam without changing its spectral or spatial properties was studied. Small signal gains of up to 55 dB and conversion efficiencies of more than 35 % were achieved for single pass arrangements employing 8 mm long PPKTP crystals. Apart from constructing three setups, which generated powerful nanosecond, picosecond and femtosecond pulses, the possibility to amplify broadband signals was investigated. An increase of the OPA bandwidth by a factor of approximately three was achieved in a noncollinear configuration. / QC 20101013
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Optical parametric amplification with periodically poled KTiOPO<sub>4</sub>Fragemann, Anna January 2005 (has links)
<p>This thesis explores the use of engineered nonlinear crystals from the KTiOPO4 (KTP) family as the gain material in optical parametric amplifiers (OPAs), with the aim to achieve more knowledge about the benefits and limitations of these devices. The work aims further at extending the possible applications of OPAs by constructing and investigating several efficient and well performing amplifiers.</p><p>An OPA consists of a strong pump source, which transfers its energy to a weak seed beam while propagating through a nonlinear crystal. The crystals employed in this work are members of the KTP family, which are attractive due to their large nonlinear coefficients, high resistance to damage and wide transparency range. The flexibility of OPAs with respect to different wavelength regions and pulse regimes was examined by employing various dissimilar seed and pump sources.</p><p>The possibility to adapt an OPA to a specific pump and seed wavelength and achieve efficient energy conversion between the beams, originates from quasi-phasematching, which is achieved in periodically poled (PP) nonlinear crystals. Quasi-phasematched samples can be obtained by changing the position of certain atoms in a ferroelectric crystal and thereby reversing the spontaneous polarisation.</p><p>In this thesis several material properties of PP crystals from the KTP family were examined. The wavelength and temperature dispersion of the refractive index were determined for PP RbTiOPO4, which is essential for future use of this material. Another experiment helped to increase the insight into the volumes close to domain walls in PP crystals</p><p>Further, several OPAs were built and their ability to efficiently amplify the seed beam without changing its spectral or spatial properties was studied. Small signal gains of up to 55 dB and conversion efficiencies of more than 35 % were achieved for single pass arrangements employing 8 mm long PPKTP crystals. Apart from constructing three setups, which generated powerful nanosecond, picosecond and femtosecond pulses, the possibility to amplify broadband signals was investigated. An increase of the OPA bandwidth by a factor of approximately three was achieved in a noncollinear configuration.</p>
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Vysokovýkonný zdroj pikosekundových optických pulzů ve střední infračervené oblasti / High-average power picosecond mid-IR sourceVyvlečka, Michal January 2017 (has links)
1 Title: High-average power picosecond mid-IR source Author: Michal Vyvlečka Department: Department of Chemical Physics and Optics Supervisor: Ing. Ondřej Novák, Ph.D., Hilase centre, Institute of Physics of CAS Abstract: High average power wavelength tunable picosecond mid-IR source based on optical parametric generation (OPG) and optical parametric amplification (OPA) is being developed. The conversion system is pumped by an Yb:YAG thin-disk laser delivering 100 W of average power at 100 kHz repetition rate, 1030 nm wavelength, and 2-3 ps pulse width. Part of this fundamental beam pumps an OPG process in a PPLN crystal. The generated wavelength is determined by PPLN's poling period and temperature. Tunability of the signal wavelength between 1.46 µm and 1.95 µm was achieved, the signal beam of 20 mW was generated at 2 W of pump power, when double pass of the beams through PPLN crystal was used. The corresponding idler wavelengths were in range 2.18-3.50 μm. The signal beam was further amplified by OPA process in two KTP crystals, which was pumped by the fundamental beam. The signal beam was amplified up to 2 W at pumping of 38 W. Tuning of the output wavelength was realized by change of the phase-matching angle in KTP crystals. Tunability between 1.70-1.95 µm for signal and 2.18-2.62 µm for idler was...
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Feasibility study of optical parametric amplification using CMOS compatible ring resonatorsJazayerifar, Mahmoud, Namdari, Meysam, Hamerly, Ryan, Gray, Dodd, Rogers, Christopher, Jamshidi, Kambiz 05 September 2019 (has links)
In this paper, we analytically describe the parametric amplification in ring resonators using silicon and silicon nitride waveguides. Achievable gain and bandwidth of the ring-based amplifiers are studied taking into account the Kerr nonlinearity for silicon nitride and Kerr nonlinearity as well as two photon absorption and free carrier absorption for silicon waveguides. Both telecom and 2-μm wavelengths are investigated in case of silicon. An approach for obtaining the optimum amplifier design without initiating the comb generation has been introduced. It is shown that there is a trade-off between the input pump and amplifier bandwidth. It is estimated that using optimum designs an amplifier with a gain and bandwidth of 10 dB and 10 GHz could be feasible with silicon ring resonators in 2 μm.
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Applications of Quantum Electro-Optic Control and Squeezed LightLam, Ping Koy, Ping.Lam@anu.edu.au January 1999 (has links)
In this thesis, we report the observations of optical squeezing from second harmonic generation (SHG), optical parametric oscillation (OPO) and optical parametric amplification (OPA). Demonstrations and proposals of applications involving the squeezed light and electro-optic control loops are presented.
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In our SHG setup, we report the observation of 2.1 dB of intensity squeezing on the second harmonic (SH) output. Investigations into the system show that the squeezing performance of a SHG system is critically affected by the pump noise and a modular theory of noise propagation is developed to describe and quantify this effect. Our experimental data has also shown that in a low-loss SHG system, intra-cavity nondegenerate OPO modes can simultaneously occur. This competition of nonlinear processes leads to the optical clamping of the SH output power and in general can degrade the SH squeezing. We model this competition and show that it imposes a limit to the observable SH squeezing. Proposals for minimizing the effect of competition are presented.
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In our OPO setup, we report the observation of 7.1 dB of vacuum squeezing and more than 4 dB of intensity squeezing when the OPO is operating as a parametric amplifier. We present the design criteria and discuss the limits to the observable squeezing from the OPO.We attribute the large amount of squeezing obtained in our experiment to the high escape efficiency of the OPO. The effect of phase jitter on the squeezing of the vacuum state is modeled.
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The quantum noise performance of an electro-optic feedforward control loop is investigated. With classical coherent inputs, we demonstrate that vacuum fluctuations introduced at the beam splitter of the control loop can be completely cancelled by an optimum amount of positive feedforward. The cancellation of vacuum fluctuations leads to the possibility of noiseless signal amplification with the feedforward loop. Comparison shows that the feedforward amplifier is superior or at least comparable in performance with other noiseless amplification schemes. When combined with an injection-locked non-planar ring Nd:YAG laser, we demonstrate that signal and power amplifications can both be noiseless and independently variable.
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Using squeezed inputs to the feedforward control loop, we demonstrate that information carrying squeezed states can be made robust to large downstream transmission losses via a noiseless signal amplification. We show that the combination of a squeezed vacuum meter input and a feedforward loop is a quantum nondemolition (QND) device, with the feedforward loop providing an additional improvement on the transfer of signal. In general, the use of a squeezed vacuum meter input and an electro-optic feedforward loop can provide pre- and post- enhancements to many existing QND schemes.
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Finally, we proposed that the quantum teleportation of a continuous-wave optical state can be achieved using a pair of phase and amplitude electro-optic feedforward loops with two orthogonal quadrature squeezed inputs. The signal transfer and quantum correlation of the teleported optical state are analysed. We show that a two dimensional diagram, similar to the QND figures of merits, can be used to quantify the performance of a teleporter.
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Trijų ir keturių bangų parametrinių sąveikų taikymas ultratrumpųjų impulsų generacijai ultravioletiniame, artimajame ir viduriniajame infraraudonajame spektro ruože / Three and four wave parametric interactions for ultrashort pulse generation in the ultraviolet, near and mid-infrared spectral rangeDarginavičius, Julius 25 September 2013 (has links)
Pagrindinis šios disertacijos tikslas – sukurti efektyvius trijų ir keturių bangų sąveikomis paremtus metodus ultratrumpiesiems ultravioletinės (UV), artimosios bei vidurinės infraraudonosios (IR) spektro srities impulsams generuoti. Pademonstruota efektyvi Nd:stiklo lazerio harmonikų generacija nekolinearaus keturbangio skirtuminio dažnio žadinimo metodu izotropinėse terpėse. Disertacijoje taip pat eksperimentiškai ir teoriškai nagrinėjama galimybė stiprinti 10 fs trukmės UV impulsus. Pateikėme du metodus derinamo bangos ilgio IR impulsams generuoti naudojant komercinę Ti:safyro lazerio ir nekolinearaus optinio parametrinio stiprintuvo sistemą. Pirmasis metodas remiasi keturių bangų sąveikomis ir leidžia generuoti 20 μJ energijos, <30 fs trukmės impulsus 1−1.5 μm spektro ruože. Antrojo šaltinio veika remiasi skirtuminio dažnio generacijos bei optinio parametrinio stiprinimo sąveikomis BBO kristaluose. Sukurtas stiprintuvas, generuojantis dviejų optinių ciklų trukmės, stabilios gaubtinės fazės, 2 μm bangos ilgio impulsus ir pademonstruotas jo taikymas itin plataus spektro superkontinuumo generacijai plačios draustinės juostos kietojo kūno terpėse. Galiausiai, ištirta vienalaikė trečiosios harmonikos ir superkontinuumo generacija skaidriose dielektrinėse terpėse, bei pasiūlyta netiesinio f-3f interferometro schema impulso gaubtinės fazes fliuktuacijoms matuoti. / In this thesis we investigated and developed three- and four-wave interaction-based frequency conversion methods for ultrashort pulse generation in the ultraviolet (UV), near and mid-infrared (IR) spectral ranges. In particular, efficient generation of Nd:glass laser harmonics was demonstrated experimentally, through noncollinear four-wave difference-frequency mixing in isotropic media. Also, broadband optical parametric amplification in the UV was investigated theoretically and achieved experimentally. The results suggest, that pulses as short as 10 fs could be amplified. We have also developed two methods based on three- and four-wave mixing, that extend the tuning range of a commercial Ti:sapphire laser-NOPA system in the IR. The first method relies on four wave frequency down-conversion, and can achieve up to 20 μJ, sub-30-fs pulses tunable in the 1−1.5 μm range. The second method considers frequency conversion, based on difference frequency generation and optical parametric amplification in BBO crystals. The presented setup delivers two optical-cycle, carrier-envelope phase (CEP)-stable pulses at 2 μm. And finally, we demonstrated supercontinuum generation by filamentation of 20 fs pulses at 2 μm in wide-bandgap solids in the regime of anomalous group velocity dispersion. We also proposed the practical use of intrinsic third harmonic generation, for the CEP stability measurements.
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Three and four wave parametric interactions for ultrashort pulse generation in the ultraviolet, near and mid-infrared spectral range / Trijų ir keturių bangų parametrinių sąveikų taikymas ultratrumpųjų impulsų generacijai ultravioletiniame, artimajame ir viduriniajame infraraudonajame spektro ruožeDarginavičius, Julius 25 September 2013 (has links)
In this thesis we investigated and developed three- and four-wave interaction-based frequency conversion methods for ultrashort pulse generation in the ultraviolet (UV), near and mid-infrared (IR) spectral ranges. In particular, efficient generation of Nd:glass laser harmonics was demonstrated experimentally, through noncollinear four-wave difference-frequency mixing in isotropic media. Also, broadband optical parametric amplification in the UV was investigated theoretically and achieved experimentally. The results suggest, that pulses as short as 10 fs could be amplified. We have also developed two methods based on three- and four-wave mixing, that extend the tuning range of a commercial Ti:sapphire laser-NOPA system in the IR. The first method relies on four wave frequency down-conversion, and can achieve up to 20 μJ, sub-30-fs pulses tunable in the 1−1.5 μm range. The second method considers frequency conversion, based on difference frequency generation and optical parametric amplification in BBO crystals. The presented setup delivers two optical-cycle, carrier-envelope phase (CEP)-stable pulses at 2 μm. And finally, we demonstrated supercontinuum generation by filamentation of 20 fs pulses at 2 μm in wide-bandgap solids in the regime of anomalous group velocity dispersion. We also proposed the practical use of intrinsic third harmonic generation, for the CEP stability measurements. / Pagrindinis šios disertacijos tikslas – sukurti efektyvius trijų ir keturių bangų sąveikomis paremtus metodus ultratrumpiesiems ultravioletinės (UV), artimosios bei vidurinės infraraudonosios (IR) spektro srities impulsams generuoti. Pademonstruota efektyvi Nd:stiklo lazerio harmonikų generacija nekolinearaus keturbangio skirtuminio dažnio žadinimo metodu izotropinėse terpėse. Disertacijoje taip pat eksperimentiškai ir teoriškai nagrinėjama galimybė stiprinti 10 fs trukmės UV impulsus. Pateikėme du metodus derinamo bangos ilgio IR impulsams generuoti naudojant komercinę Ti:safyro lazerio ir nekolinearaus optinio parametrinio stiprintuvo sistemą. Pirmasis metodas remiasi keturių bangų sąveikomis ir leidžia generuoti 20 μJ energijos, <30 fs trukmės impulsus 1−1.5 μm spektro ruože. Antrojo šaltinio veika remiasi skirtuminio dažnio generacijos bei optinio parametrinio stiprinimo sąveikomis BBO kristaluose. Sukurtas stiprintuvas, generuojantis dviejų optinių ciklų trukmės, stabilios gaubtinės fazės, 2 μm bangos ilgio impulsus ir pademonstruotas jo taikymas itin plataus spektro superkontinuumo generacijai plačios draustinės juostos kietojo kūno terpėse. Galiausiai, ištirta vienalaikė trečiosios harmonikos ir superkontinuumo generacija skaidriose dielektrinėse terpėse, bei pasiūlyta netiesinio f-3f interferometro schema impulso gaubtinės fazes fliuktuacijoms matuoti.
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Infrared Few-Cycle Pulse Optical Parametric Amplifier / Kelių optinių ciklų trukmės impulsų parametrinis stiprinimas infraraudonojoje srityjeAlišauskas, Skirmantas 01 October 2010 (has links)
Main objective of this thesis is to generate and amplify few cycle pulses in the infrared region. In this thesis, two approaches were introduced for few cycle pulse parametric amplification at 800 nm and 1.5 μm. First approach is dedicated for prospects for increasing average power of OPCPA via multi-beam pumping; the second approach is dedicated for generation of carrier-envelope-phase (CEP) stable high energy (up to tens of millijoules) few-cycle pulses at 1.5 μm.
An experimental investigation of two or three beams-pumped OPCPA system based on type I BBO crystal is presented. The 2nd OPA stage was pumped by two or three pump beams derived from independent Nd:YAG laser amplifiers. The efficiency of interaction was shown to be comparable to that of single-beam pumped OPA and diminishes only slightly due to cascaded parametric diffraction of interacting waves. The effect was observed and its impact on efficiency of parametric amplification process was shown to decrease at larger intersecting angles of pump. In the prospect, the use of multiple lasers for OPA pumping has an appeal for increasing the repetition rate and consequently the average power of an ultrashort pulse laser system. Finally, the concept and realization of hybrid system based on type II KTP OPCPA and filamentation are described. A CEP-stable 1.5 μm OPCPA system with pulse energies up to 12.5 mJ after 4 OPA stages is demonstrated. Furthermore, self-compression of CEP-stable 2.2 mJ, 74.4 fs, 1.57 μm input... [to full text] / Disertacijos darbo tikslas – suformuoti ir parametriškai stiprinti kelių optinių ciklų trukmės impulsus infraraudonojoje srityje Šioje disertacijoje buvo tirtos dvi moduliuotosios fazės („čirpuotų“) impulsų parametrinio stiprinimo sistemos, stiprinančios ypač plataus spektro impulsus 800 nm bei 1,5 μm srityse. Pirmoji sistema skirta tirti galimybę didinti lazerinės spinduliuotės vidutinę galią keliais pluoštais kaupinamame parametriniame stiprintuve; antroji sistema skirta kelių optinių ciklų trukmės stabilios fazės impulsų formavimui 1,5 μm srityje.
Disertacijoje aprašomas I tipo parametrinis stiprintuvas, kurio 2-oji pakopa buvo kaupinama dviem arba trimis nepriklausomų lazerinių šaltinių pluoštais. Nustatyta, kad parametrinį stiprintuvą kaupinant keliais pluoštais stebimas naujų erdvinių komponentų atsiradimas, kuriuos sąlygoja parametrinė pakopinė difrakcija, o tai mažina bendrą sistemos energetinio keitimo efektyvumą.. Darbo metu pademonstruota galimybė mažinti parametrinės difrakcijos sąlygotus nuostolius parametriniame stiprintuve derinant kampus tarp kaupinimo pluoštų. Taip pat pristatomas alternatyvus būdas formuoti didelės energijos (kelių dešimčių milidžaulių) kelių optinių ciklų trukmės stabilios fazės impulsus 1,5 μm srityje. Būdas paremtas sąlyginai siauro spektro 1,5 μm srityje stiprinimu II tipo KTP kristale bei spektro plėtra inertinėse dujose po stiprinimo. 4 pakopų parametriniame stiprintuve pasiekta iki šiol didžiausia 12,5 mJ impulso energija 1,5 μm... [toliau žr. visą tekstą]
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Kelių optinių ciklų trukmės impulsų parametrinis stiprinimas infraraudonojoje srityje / Infrared Few-Cycle Pulse Optical Parametric AmplifierAlišauskas, Skirmantas 01 October 2010 (has links)
Disertacijos darbo tikslas – suformuoti ir parametriškai stiprinti kelių optinių ciklų trukmės impulsus infraraudonojoje srityje Šioje disertacijoje buvo tirtos dvi moduliuotosios fazės („čirpuotų“) impulsų parametrinio stiprinimo sistemos, stiprinančios ypač plataus spektro impulsus 800 nm bei 1,5 μm srityse. Pirmoji sistema skirta tirti galimybę didinti lazerinės spinduliuotės vidutinę galią keliais pluoštais kaupinamame parametriniame stiprintuve; antroji sistema skirta kelių optinių ciklų trukmės stabilios fazės impulsų formavimui 1,5 μm srityje.
Disertacijoje aprašomas I tipo parametrinis stiprintuvas, kurio 2-oji pakopa buvo kaupinama dviem arba trimis nepriklausomų lazerinių šaltinių pluoštais. Nustatyta, kad parametrinį stiprintuvą kaupinant keliais pluoštais stebimas naujų erdvinių komponentų atsiradimas, kuriuos sąlygoja parametrinė pakopinė difrakcija, o tai mažina bendrą sistemos energetinio keitimo efektyvumą.. Darbo metu pademonstruota galimybė mažinti parametrinės difrakcijos sąlygotus nuostolius parametriniame stiprintuve derinant kampus tarp kaupinimo pluoštų. Taip pat pristatomas alternatyvus būdas formuoti didelės energijos (kelių dešimčių milidžaulių) kelių optinių ciklų trukmės stabilios fazės impulsus 1,5 μm srityje. Būdas paremtas sąlyginai siauro spektro 1,5 μm srityje stiprinimu II tipo KTP kristale bei spektro plėtra inertinėse dujose po stiprinimo. 4 pakopų parametriniame stiprintuve pasiekta iki šiol didžiausia 12,5 mJ impulso energija 1,5 μm... [toliau žr. visą tekstą] / Main objective of this thesis is to generate and amplify few cycle pulses in the infrared region. In this thesis, two approaches were introduced for few cycle pulse parametric amplification at 800 nm and 1.5 μm. First approach is dedicated for prospects for increasing average power of OPCPA via multi-beam pumping; the second approach is dedicated for generation of carrier-envelope-phase (CEP) stable high energy (up to tens of millijoules) few-cycle pulses at 1.5 μm.
An experimental investigation of two or three beams-pumped OPCPA system based on type I BBO crystal is presented. The 2nd OPA stage was pumped by two or three pump beams derived from independent Nd:YAG laser amplifiers. The efficiency of interaction was shown to be comparable to that of single-beam pumped OPA and diminishes only slightly due to cascaded parametric diffraction of interacting waves. The effect was observed and its impact on efficiency of parametric amplification process was shown to decrease at larger intersecting angles of pump. In the prospect, the use of multiple lasers for OPA pumping has an appeal for increasing the repetition rate and consequently the average power of an ultrashort pulse laser system. Finally, the concept and realization of hybrid system based on type II KTP OPCPA and filamentation are described. A CEP-stable 1.5 μm OPCPA system with pulse energies up to 12.5 mJ after 4 OPA stages is demonstrated. Furthermore, self-compression of CEP-stable 2.2 mJ, 74.4 fs, 1.57 μm input... [to full text]
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Development of ultra-broadband ultrafast infrared sources and applications to nonlinear vibrational spectroscopy of interfacesIsaienko, Oleksandr January 2011 (has links)
Interfaces play a crucial role in the exchange of energy and matter in various physical, chemical and biological systems. A particular interest has been to study interfaces between aqueous phases and various minerals because of their importance in understanding geochemical phenomena as well as for applications such as enhanced oil recovery. The nonlinear optical technique of vibrational sum-frequency generation (SFG) spectroscopy, introduced over 20 years ago, has become a powerful tool to investigate various surfaces, in particular, mineral-water interfaces. One of the challenges of the SFG spectroscopy of aqueous surfaces is the need to tune the central frequency of relatively narrowband IR lasers through the broad range of the OH-stretch frequencies of water molecules (3000 - 4000 cm-1). We have developed a novel ultrabroadband IR laser source that generates infrared pulses in the ~2800-6000 cm-1 range (lambda~3300-1800 nm) with bandwidths Delta(nu)>1000 cm-1, and bandwidths >2000 cm-1 in the near-IR range (lambda~1000-2000 nm). Pulse front tilt of signal pulse has been corrected allowing for compression of signal pulses down to 25 fsec. Such ultrabroadband IR pulses allow us to perform SFG spectroscopy of aqueous surfaces over the entire frequency range of water molecule spectrum (extending from ~2900 cm -1 to ~3800 cm -1) simultaneously, without tuning the laser ("in one shot"). We have used this novel ultrabroadband IR source to investigate the vibrational SFG spectra of silica/water interfaces. The high signal-to-noise ratio of our spectroscopic setup has allowed us to study low-intensity features that were not studied in detail, or recognized previously in the SFG-spectroscopy investigations, including: 1) non-hydrogen bonded OH vibrations at hydrophilic silica/water interfaces; 2) combination [stretch+bend] bands of water at the silica surface appearing at ~5000-5200 cm -1. 3) Overtones of water stretching modes at silica/water interfaces. The most important conclusions from these studies are outlined below. 1. Non-hydrogen bonded hydroxyls at silica/water interface. Typically SFG-studies of mineral/water interfaces (in particular, silica/water) have focused on the most pronounced features - peaks of H-bonded hydroxyls at ~3150 and ~3450 cm -1. We have been able to systematically observe and study a weaker peak at ~3670 - 3700 cm -1. This peak becomes more pronounced as the pH of aqueous phase decreases, as well as the ionic strength increases, indicating that the hydroxyls corresponding to this spectral feature are situated in a very close proximity to the surface. Isotopic dilution experiments indicate that the 3700 cm -1 feature is not due to asymmetric OH stretches as was suggested before. Based on our results, we suggest that this spectral feature corresponds to hydroxyls of water molecules at the silica surface that cannot hydrogen bond with silanol groups because of the lower density of silanols compared to H2O. We believe this to be the first surface-specific study of non-hydrogen bonded hydroxyls at silica, a surface widely accepted as hydrophilic. 2. SFG spectroscopy of [ν(OH)+δ(HOH)] combination bands of water at silica surface. We have extended SFG spectroscopy of the interfacial hydroxyls at mineral/water surfaces into the near-IR frequency range. The studies of overtones of interfacial OH(OD) groups will provide information on the anharmonicity of such species, and thus on the energy of dissociation. In addition, the positions of the overtone frequencies of the hydroxyls are more sensitive to interactions with the environment than the fundamental stretch frequencies. Our particular focus has been to study the stretch+bend combination band nu comb nu;(OH)+delta;(HOH) of liquid water which occurs in the near-IR spectral range at ~5000-5200 cm -1. It is typically much weaker in the FTIR absorption spectra than the fundamental transitions of the OH stretches or HOH bending, similar to overtones of these modes. We have performed, what we believe to be, the first surface-specific vibrational SFG spectroscopic measurements of combination bands of water molecules at silica surfaces. SFG spectroscopy of water combination band allows access to the water bending mode (delta~1600 cm -1), which still has not been observed in sum-frequency. / Chemistry
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