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Optical phonons and temperature dependent phase transitions in paraelectric antimony and ferroelectric sulfoiodide semiconductors, using polarized IR and Raman spectra measurements
Laser diode pumped mid-IR wavelength sources include at least one high power, near-IR wavelength, injection and/or sources wherein one or both of such sources may be tunable providing a pump wave output beam to a quasi-phase matched (QPM) nonlinear frequency mixing (NFM) device. The NFM device may be a difference frequency mixing (DFM) device or an optical parametric oscillation (OPO) device. Wavelength tuning of at least one of the sources advantageously provides the ability for optimizing pump or injection wavelengths to match the QPM properties of the NFM device enabling a broad range of mid-IR wavelength selectivity. Also, pump powers are gain enhanced by the addition of a rare earth amplifier or oscillator, or a Raman/Brillouin amplifier or oscillator between the high power source and the NFM device. Further, polarization conversion using Raman or Brillouin wavelength shifting is provided to optimize frequency conversion efficiency in the NFM device.
Laser diode pumped mid-IR wavelength systems include at least one high power, near-IR wavelength, injection and/or sources wherein one or both of such sources may be tunable providing a pump wave output beam to a quasi-phase matched (QPM) nonlinear frequency mixing (NFM) device. The NFM device may be a difference frequency mixing (DFM) device or an optical parametric oscillation (OPO) device. Wavelength tuning of at least one of the sources advantageously provides the ability for optimizing pump or injection wavelengths to match the QPM properties of the NFM device enabling a broad range of mid-IR wavelength selectivity. Also, pump powers are gain enhanced by the addition of a rare earth amplifier or oscillator, or a Raman/Brillouin amplifier or oscillator between the high power source and the NFM device. Further, polarization conversion using Raman or Brillouin wavelength shifting is provided to optimize frequency conversion efficiency in the NFM device.
Laser diode pumped mid-IR wavelength sources include at least one high power, near-IR wavelength, injection and/or sources wherein one or both of such sources may be tunable providing a pump wave output beam to a quasi-phase matched (QPM) nonlinear frequency mixing (NFM) device. The NFM device may be a difference frequency mixing (DFM) device or an optical parametric oscillation (OPO) device. Wavelength tuning of at least one of the sources advantageously provides the ability for optimizing pump or injection wavelengths to match the QPM properties of the NFM device enabling a broad range of mid-IR wavelength selectivity. Also, pump powers are gain enhanced by the addition of a rare earth amplifier or oscillator, or a Raman/Brillouin amplifier or oscillator between the high power source and the NFM device. Further, polarization conversion using Raman or Brillouin wavelength shifting is provided to optimize frequency conversion efficiency in the NFM device.
An intrinsic antiferromagnetic topological insulator MnBi 2 Te 4 arises when intercalating a Mn-Te bilayer chain in a topological insulator, Bi 2 Te 3 . We present observations on the inter- and intralayer phonon modes of the generalized MnBi 2n Te 3n+1 (n=1,2,3,4) family using cryogenic low-frequency Raman spectroscopy with various polarization configurations. Two peaks at 66 and 112 cm –1 show abnormal perturbation in Raman linewidths below magnetic transition temperature due to spin-phonon coupling. In MnBi 4 Te 7 , B i2 Te 3 layers induce Davydov splitting of the A1g mode around 137 cm –1 at 5 K. The out-of-plane interlayer force constant estimated using the linear chain model was (3.98±0.14)×10 19 N/m 3 , three times weaker than that of Bi 2 Te 3 . Adding more Bi 2 Te 3 layers, such as MnBi 6 Te 10 and MnBi 8 Te 13 , makes Bi 2 Te 3 properties more dominant than magnetic properties. Our work experimentally and theoretically discovers the dynamics of phonon modes of MnBi 2n Te 3n+ 1 family, facilitating utilization of magnetic topological heterostructures.
A novel technique for extracting Q-branch Raman signals scattered by a diatomic species from the emission spectrum resulting from the irradiation of combustion products using a broadband excimer laser has been developed. This technique is based on the polarization characteristics of vibrational Raman scattering and can be used for both single-shot Raman extraction and time-averaged data collection. The Q-branch Raman signal has a unique set of polarization characteristics which depend on the direction of the scattering while fluorescence signals are unpolarized. For the present work, a calcite crystal is used to separate the horizonal component of a collected signal from the vertical component. The two components are then sent through a UV spectrometer and imaged onto an intensified CCD camera separately. The vertical component contains both the Raman signal and the interfering fluorescence signal. The horizontal component contains the fluorescence signal and a very weak component of the Raman signal; hence, the Raman scatter can be extracted by taking the difference between the two signals. The separation of the Raman scatter from interfering fluorescence signals is critically important to the interpretation of the Raman for cases in which a broadband ultraviolet (UV) laser is used as an excitation source in a hydrogen-oxygen flame and in all hydrocarbon flames. The present work provides a demonstration of the separation of the Raman scatter from the fluorescence background in real time.
The application of tunable excimer lasers in combustion and flow diagnostics is almost routine nowadays. The properties of this laser system that enable density and temperature measurements in supersonic and hypersonic flow fields to be conducted are its high power, high repetition rate, and high spectral brightness. The limitation imposed by this system on these measurements is the paucity of lines in the wavelength region, the vacuum-ultraviolet, where species of interest, such as OH, N2, O2, H2, H2O, CO, NO, etc., are susceptible to electronic excitation to high-lying states. To circumvent this problem one normally resorts to nonlinear optical techniques such as frequency conversion via stimulated Raman scattering (SRS), more commonly known as Raman shifting or Raman mixing, to extend these nonintrusive and nonperturbing techniques to the shorter wavelengths in the VUV region and, for that matter, to longer wavelengths in the infrared region, if the need arises. The theoretical basis of SRS and its application are well documented in the literature. In essence, the Raman shift is a consequence of the inelastic scattering of the incident radiation by the sample. Most of the scattered radiation from the molecules of the sample is unchanged in frequency. However, a small fraction of the incident radiation is changed in frequency. This shift is a result of the fact that some of the incident photons on colliding with the molecules of the sample give up some of their energy and emerge with a lower energy resulting in the lower-frequency Stokes radiation. Other incident photons may increase their energy by colliding with the vibrationally excited molecules of the medium and emerge as higher-frequency antistokes radiation. The generation of the latter is the main objective of this project. The process, however, depends on several factors, including the beam quality of the pump laser, the cross-section of the gaseous medium, the gas pressure, and the ambient temperature of the gas near the focal region. Furthermore, since the Raman shifting process is polarization sensitive, it is necessary to have all of the laser energy in a single polarization. These factors were taken into consideration in the execution of the project. The implementation of the Raman shift was accomplished by focusing the 193 nm output of an ArF excimer laser (Lamda-Physik LPX 150) into a 1-meter long high pressure recirculating Raman cell filled with H2 gas. The laser system was modified in order to improve the mode quality of the pump beam to enhance the Raman shifting. To accomplish this feat, a prism beam expander and grating on the oscillator discharge provided wavelength tuning over the excimer gain profile. Furthermore, a triple-pass configuration, as opposed to unstable resonator optics, was employed in the operation of the amplifier cavity so that when the oscillator output radiation, focused by a 51-cm focal length fused silica lens through a 50 micron pinhole (serving as a spatial filter) and recollimated with a 25-cm focal length lens, was fed into the amplifier, it was injection locked, thereby providing tunable radiation with relatively low divergence. The forward scattered radiation emanating from the impingement of the modified pump beam on the Raman cell was detected using an energy meter after the latter had been separated from it using a dispersing prism.
Three-beam rotational coherent anti-Stokes Raman scattering (CARS) measurements performed in highly scattering environments are susceptible to contamination by two-beam CARS signals generated by the pump–probe and Stokes–probe interactions at the measurement volume. If this occurs, differences in the Raman excitation bandwidth between the two-beam and three-beam CARS signals can add significant errors to the spectral analysis. This interference to the best of our knowledge has not been acknowledged in previous three-beam rotational CARS experiments, but may introduce measurement errors up to 25% depending on the temperature, amount of scattering, and differences between the two-beam and three-beam Raman excitation bandwidths. Here, the presence of two-beam CARS signal contamination was experimentally verified using a femtosecond–picosecond rotational CARS instrument in two scattering environments: (1) a fireball generated by a laboratory-scale explosion that contained particulate matter, metal fragments, and soot, and (2) a flow of air and small liquid droplets. A polarization scheme is presented to overcome this interference. By rotating the pump and Stokes polarizations +55° and –55° from the probe, respectively, the two-beam and three-beam CARS signals are orthogonally polarized and can be separated using a polarization analyzer. Using this polarization arrangement, the Raman-resonant three-beam CARS signal amplitude is reduced by a factor of 2.3 compared to the case where all polarizations are parallel. This method is successfully demonstrated in both scattering environments. A theoretical model is presented, and the temperature measurement error is studied for different experimental conditions. The criteria for when this interference may be present are discussed.
van der Waals (vdW) magnets have rapidly emerged as a fertile playground for fundamental physics and exciting applications. Despite the impressive developments over the past few years, technical limitations pose a severe challenge to many other potential breakthroughs. High on the list is the lack of suitable experimental tools for studying spin dynamics on atomically thin samples. Here, Raman scattering techniques are employed to directly observe the low-lying magnon (~1 meV) even in bilayer NiPS 3 . Further, the advantage is that it offers excellent energy resolutions far better on low-energy sides than most inelastic neutron spectrometers can offer. More importantly, with appropriate theoretical analysis, the polarization dependence of the Raman scattering by those low-lying magnons also provides otherwise hidden information on the dominant spin-exchange scattering paths for different magnons. By comparing with high-resolution inelastic neutron scattering data, these low-energy Raman modes are confirmed to be indeed of magnon origin. Because of the different scattering mechanisms involved in inelastic neutron and Raman scattering, this information is fundamental in pinning down the final spin Hamiltonian. This work demonstrates the capability of Raman spectroscopy to probe the genuine two-dimensional spin dynamics in atomically thin vdW magnets, which can provide insights that are obscured in bulk spin dynamics.
Abstract One of the primary basic plasma parameters within transient nonequilibrium plasmas is the reduced electric field strength, roughly understood as the ratio of the electrical energy given to the charged species between two collisions. While physical probes have historically been used for electric field measurements, recent advances in high intensity lasers and sensitive detection methods have allowed for non-invasive optical electric field determination in nearly any discharge configuration with time-resolution up to the sub-nanosecond range and sub-millimeter spatial resolution. This topical review serves to highlight several non-invasive methods for in situ electric field strength determination in transient plasmas ranging from high vacuum environments to atmospheric pressure and above. We will discuss the advantages and proper implementation of (i) laser induced fluorescence dip spectroscopy for measurements in low pressure RF discharges, (ii) optical emission spectroscopy based methods for nitrogen, helium or hydrogen containing discharges, (iii) electric field induced coherent Raman scattering, and (iv) electric field induced second harmonic generation. The physical mechanism for each method will be described as well as basic implementation and highlighting recent results.
In spin-1/2 Mott insulators, nonmagnetic quantum liquid phases are often argued to arise when the system shows no magnetic ordering, but identifying positive signatures of these phases or related spinon quasiparticles can be elusive. Here, we use Raman scattering to provide three signatures for spinons in a possible spin-orbit quantum liquid material Ba 4 Ir 3 O 10 : (1) a broad hump, which we show can arise from Luttinger liquid spinons in Raman with parallel photon polarizations normal to one-dimensional chains; (2) strong phonon damping from phonon-spin coupling via the spin-orbit interaction; and (3) the absence of (1) and (2) in the magnetically ordered phase that is produced when 2% of Ba is substituted by Sr [(Ba 0.98 Sr 0.02 ) 4 Ir 3 O 10 ]. Furthermore, the phonon damping via itinerant spinons seen in this quantum liquid insulator suggests a mechanism for enhancing thermoelectricity in strongly correlated conductors, through a neutral quantum liquid that need not affect electronic transport.
A standard photon counting technique and an argon-ion laser with 4545, 4579, 4727, 4765, 4880, 4965, 5017 and 5145-A lasing lines, providing a measurable Raman spectrum from NOCl, were used in the measurement of the Raman scattering cross section of NOCl at a Raman shift of 334.4 plus or minus 1.6/cm in relation to the N2 Raman cross section. A polarization analyzer and a quartz wedge were placed in front of the entrance slit of the double monochromator for depolarization measurements. Diagrams are plotted to show the scattering cross section and depolarization measurement results.
Perfect circular dichroism has been observed in Raman scattering by optical phonons in single chiral domain NiCo 2 TeO 6 crystals. The selection rules for optical phonons are determined by the combination of the chiral structure C and electric polarization P along the c axis. These two symmetry operations are equivalent to the ferroaxial order (C·P) = A, so the observed optical phonons are referred to as ferroaxial. For a given Raman scattering geometry, the observed effect may also be described as a perfect nonreciprocal propagation of the ferroaxial optical phonons, whose preferable q-vector direction is determined by the sign of A. Here, the combination of Raman scattering and polarization plane rotation of the transmitted white light allows for identification of the direction of electric polarization P in monodomain chiral crystals. In addition to the ferroaxial selection rules for optical phonons, a weaker ferroaxial dichroism was observed for the magnon peak at 18 cm −1 .
Black phosphorus (BP) is unique among layered materials because of its homonuclear lattice and strong structural anisotropy. While recent investigations on few-layer BP have extensively explored the in-plane (a, c) anisotropy, much less attention has been given to the out-of-plane direction (b). Here, the optical response from bulk BP is probed using polarization-resolved photoluminescence (PL), photoluminescence excitation (PLE), and resonant Raman scattering along the zigzag, out-of-plane, and armchair directions. An unexpected b-polarized luminescence emission is detected in the visible, far above the fundamental gap. PLE indicates that this emission is generated through b-polarized excitation at 2.3 eV. The same electronic resonance is observed in resonant Raman with the enhancement of the A g phonon modes scattering efficiency. These experimental results are fully consistent with DFT calculations of the permittivity tensor elements and demonstrate the remarkable extent to which the anisotropy influences the optical properties and carrier dynamics in black phosphorus.
A tunable-bandwidth filter system (TBFS), now undergoing development, is intended to be part of a remote sensing multispectral imaging system that will operate in the visible and near infrared spectral region (wavelengths from 400 to 900 nm). Attributes of the TBFS include rapid tunability of the pass band over a wide wavelength range and high transmission efficiency. The TBFS is based on a unique integration of two pairs of broadband Raman reflection holographic filters with two rotating spherical lenses. In experiments, a prototype of the TBFS, was shown to be capable of spectral sampling of images in the visible range over a 200 nm spectral range with a spectral resolution of 30 nm. The figure depicts the optical layout of a prototype of the TBFS as part of a laboratory multispectral imaging system for the spectral sampling of color test images in two orthogonal polarizations. Each pair of broadband Raman reflection holographic filters is mounted at an equatorial plane between two halves of a spherical lens. The two filters in each pair are characterized by steep spectral slopes (equivalently, narrow spectral edges), no ripple or side lobes in their pass bands, and a few nanometers of non-overlapping wavelength range between their pass bands. Each spherical lens and thus the filter pair within it is rotated in order to rapidly tune its pass band. The rotations of are effected by electronically controlled, programmable, high-precision rotation stages. The rotations are coordinated by electronic circuits operating under overall supervision of a personal computer in order to obtain the desired variation of the overall pass bands with time. Embedding the filters inside the spherical lenses increases the range of the hologram incidence angles, making it possible to continuously tune the pass and stop bands of the filters over a wider wavelength range. In addition, each spherical lens also serves as part of the imaging optics: The telephoto lens focuses incoming light to a field stop that is also a focal point of each spherical lens. A correcting lens in front of the field stop compensates for the spherical aberration of the spherical lenses. The front surface of each spherical lens collimates the light coming from the field stop. After the collimated light passes through the filter in the spherical lens, the rear surface of the lens focuses the light onto a charge-coupled-device image detector.
A tunable-bandwidth filter system (TBFS), now undergoing development, is intended to be part of a remote-sensing multispectral imaging system that will operate in the visible and near infrared spectral region (wavelengths from 400 to 900 nm). Attributes of the TBFS include rapid tunability of the pass band over a wide wavelength range and high transmission efficiency. The TBFS is based on a unique integration of two pairs of broadband Raman reflection holographic filters with two rotating spherical lenses. In experiments, a prototype of the TBFS was shown to be capable of spectral sampling of images in the visible range over a 200-nm spectral range with a spectral resolution of .30 nm. The figure depicts the optical layout of a prototype of the TBFS as part of a laboratory multispectral imaging system for the spectral sampling of color test images in two orthogonal polarizations. Each pair of broadband Raman reflection holographic filters is mounted at an equatorial plane between two halves of a spherical lens. The two filters in each pair are characterized by steep spectral slopes (equivalently, narrow spectral edges), no ripple or side lobes in their pass bands, and a few nanometers of non-overlapping wavelength range between their pass bands. Each spherical lens and thus the filter pair within it is rotated in order to rapidly tune its pass band. The rotations of the lenses are effected by electronically controlled, programmable, high-precision rotation stages. The rotations are coordinated by electronic circuits operating under overall supervision of a personal computer in order to obtain the desired variation of the overall pass bands with time. Embedding the filters inside the spherical lenses increases the range of the hologram incidence angles, making it possible to continuously tune the pass and stop bands of the filters over a wider wavelength range. In addition, each spherical lens also serves as part of the imaging optics: The telephoto lens focuses incoming light to a field stop that is also a focal point of each spherical lens. A correcting lens in front of the field stop compensates for the spherical aberration of the spherical lenses. The front surface of each spherical lens collimates the light coming from the field stop. After the collimated light passes through the filter in the spherical lens, the rear surface of the lens focuses the light onto a charge-coupled-device image detector.
A critical factor in achieving tunability in DESs is varying the type of hydrogen bond acceptors (HBAs) and donors (HBDs). Choline halides (ChX), such as ChCl and ChBr, have been studied to investigate the effect of the choline anion on DESs. However, ChF-based DESs have been underrepresented in scientific research. ChF has excellent potential, such as high electron affinity, ionization potential, and strong hydrogen bond interactions. Moreover, ChF-based DES can lead to a deeper understanding of DESs due to the NMR-active 19F nuclear spin nature. We report the first synthesis and characterization of choline fluoride-EG (1:2, ChF:EG) DES, which we named “EthalineF.” We studied this mixture using various spectroscopic techniques, including NMR, FT-IR, Raman, and UV–vis spectroscopies. Polarity, density, viscosity, and conductivity measurements were collected as well. Transient absorption spectroscopy (TAS) was used to study the solvation dynamics of EthalineF. 19F NMR indicated that some fluoride anions (~15%) are coordinated to the choline cation. In EthalineF, the new type of observed fluoride anions is proposed to be a tight-binding choline-fluoride ion pair. Further, EthalineF has a larger solvodynamic radius than Ethaline. This can explain the lower conductivity for EthalineF compared to Ethaline despite the higher fluidity and solvation dynamics for EthalineF.
We present a polarization-resolved, high-resolution Raman scattering study of the three consecutive charge density wave (CDW) regimes in 1T - TaS 2 single crystals, supported by ab initio calculations. Our analysis of the spectra within the low-temperature commensurate (C-CDW) regime shows P$\bar3$ symmetry of the system, thus excluding the previously proposed triclinic stacking of the “star-of-David” structure, and promoting trigonal or hexagonal stacking instead. The spectra of the high-temperature incommensurate (IC-CDW) phase directly project the phonon density of states due to the breaking of the translational invariance, supplemented by sizable electron-phonon coupling. Between 200 and 352 K, our Raman spectra show contributions from both the IC-CDW and the C-CDW phases, indicating their coexistence in the so-called nearly commensurate (NC-CDW) phase. The temperature dependence of the symmetry-resolved Raman conductivity indicates the stepwise reduction of the density of states in the CDW phases, followed by a Mott transition within the C-CDW phase. We determine the size of the Mott gap to be Ω gap ≈ 170 – 190 meV, and track its temperature dependence.