Electro-optic Crystal Research Articles

Phonon-Suppressing Intermolecular Adhesives: Catechol-Based Broadband Organic THz Generators.

Solid‐state molecular phonons play a crucial role in the performance of diverse photonic and optoelectronic devices. In this work, new organic terahertz (THz) generators based on a catechol group that acts as a phonon suppressing intermolecular adhesive are developed. The catechol group is widely used in mussel‐inspired mechanical adhesive chemistry. Newly designed organic electro‐optic crystals consist of catechol‐based nonlinear optical 4‐(3,4‐dihydroxystyryl)‐1‐methylpyridinium (DHP) cations and 4‐(trifluoromethyl)benzenesulfonate anions (TFS), which both have multiple interionic interaction capability. Interestingly, compared to benchmark organic crystals for THz generators, DHP‐TFS crystals concomitantly achieve top level values of the lowest void volume and the highest crystal density, resulting in an exceptionally small amplitude of solid‐state molecular phonons. Simultaneously achieving small molecular phonon amplitude, large optical nonlinearity and good phase matching at infrared optical pump wavelengths, DHP‐TFS crystals are capable of generating broadband THz waves of up to 16 THz with high optical‐to‐THz conversion efficiency; one order of magnitude higher than commercial inorganic THz generators.

Terahertz-slicing - an all-optical synchronization for 4th generation light sources.

A conceptually new approach to synchronizing accelerator-based light sources and external laser systems is presented. The concept is based on utilizing a sufficiently intense accelerator-based single-cycle terahertz pulse to slice a thereby intrinsically synchronized femtosecond-level part of a longer picosecond laser pulse in an electro-optic crystal. A precise synchronization of the order of 10 fs is demonstrated, allowing for real-time lock-in amplifier signal demodulation. We demonstrate successful operation of the concept with three benchmark experiments using a 4th generation accelerator-based terahertz light source, i.e. (i) far-field terahertz time-domain spectroscopy, (ii) terahertz high harmonic generation spectroscopy, and (iii) terahertz scattering-type scanning near-field optical microscopy.

Propagation dynamics of optically generated unipolar electromagnetic pulses

It was recently predicted [M. I. Bakunov, A. V. Maslov, and M. V. Tsarev, Phys. Rev. A 95, 063817 (2017)] that an ultrashort laser pulse producing multiphoton ionization in an electro-optic crystal can generate a quasistatic unipolar electromagnetic precursor propagating ahead of the laser pulse. Here we study the propagation dynamics of such a precursor outside the generating crystal. Our analysis is based on a specially developed semianalytical model that represents the precursor generation as radiation from sequentially switched discrete current-carrying ribbons distributed along the laser path. The model allows for calculating the precursor spatiotemporal structure at an arbitrarily long distance behind the crystal. The calculations reveal the complex propagation dynamics of the precursor. Starting as a unipolar pulse, it becomes quasiunipolar after some distance, which depends on the precursor transverse size, and then bipolar preserving a constant transverse size and maximum field strength. These findings are important for the experimental observation of the precursors and their practical use.

Inhomogeneous spatial distribution of residual amplitude modulation in optical phase modulation using a bulk electro-optic crystal.

Residual amplitude modulation is one of the major sources of instability in many precision measurements using frequency modulation techniques. Although a transverse and inhomogeneous distribution of residual amplitude modulation has long been observed, the underlying mechanism is not well understood. We perform measurement and analysis of this spatial inhomogeneity using several electro-optic crystals of different types. Two distinct components are identified in the spatial distributions, and their detailed properties, some of which are previously unnoticed, are mapped out and analyzed, showing that the spatial inhomogeneity can be explained by acousto-optic interaction inside the crystal. Moreover, this spatial inhomogeneity can be further suppressed, improving the 1000-s stability of residual amplitude modulation to 3×10-7 (8×10-8) at modulation frequency of 11 MHz (120 kHz), corresponding to a frequency instability of 1×10-17 (3×10-18), estimated for a cavity-stabilized laser using a Pound-Drever-Hall discrimination slope of 1×10-4 V/Hz.

Ferroelectric crystals with giant electro-optic property enabling ultracompact Q-switches.

Relaxor-lead titanate (PbTiO3) crystals, which exhibit extremely high piezoelectricity, are believed to possess high electro-optic (EO) coefficients. However, the optical transparency of relaxor-PbTiO3 crystals is severely reduced as a result of light scattering and reflection by domain walls, limiting electro-optic applications. Through synergistic design of a ferroelectric phase, crystal orientation, and poling technique, we successfully removed all light-scattering domain walls and achieved an extremely high transmittance of 99.6% in antireflection film-coated crystals, with an ultrahigh EO coefficient r33 of 900 picometers per volt (pm V-1), >30 times as high as that of conventionally used EO crystals. Using these crystals, we fabricated ultracompact EO Q-switches that require very low driving voltages, with superior performance to that of commercial Q-switches. Development of these materials is important for the portability and low driving voltage of EO devices.

Experimental observation of optically generated unipolar electromagnetic precursors.

It was recently predicted [Phys. Rev. A95(6), 063817 (2017) 10.1103/PhysRevA.95.063817] that an intense femtosecond laser pulse propagating in an electro-optic crystal and producing free carriers via multiphoton ionization can generate a unipolar electromagnetic precursor propagating ahead of the laser pulse. Here we report the experimental observation of this phenomenon in a GaP crystal excited by an amplified Ti:sapphire laser.

Inverse-Designed Narrowband THz Radiator for Ultrarelativistic Electrons.

THz radiation finds various applications in science and technology. Pump–probe experiments at free-electron lasers typically rely on THz radiation generated by optical rectification of ultrafast laser pulses in electro-optic crystals. A compact and cost-efficient alternative is offered by the Smith–Purcell effect: a charged particle beam passes a periodic structure and generates synchronous radiation. Here, we employ the technique of photonic inverse design to optimize a structure for Smith–Purcell radiation at a single wavelength from ultrarelativistic electrons. The resulting design is highly resonant and emits narrowbandly. Experiments with a 3D-printed model for a wavelength of 900 μm show coherent enhancement. The versatility of inverse design offers a simple adaption of the structure to other electron energies or radiation wavelengths. This approach could advance beam-based THz generation for a wide range of applications.

Passive repetition-rate stabilization for a mode-locked fiber laser by electro-optic modulation.

We report a passive stabilization of the repetition rate for a mode-locked fiber laser by using an electro-optic modulator in a phase-biased nonlinear amplifying loop mirror. The underlying mechanism, in contrast to active feedback operations, lies in the cross-phase modulation between electrical and optical pulses within an electro-optic crystal. The resulting spectral shift can automatically compensate for the cavity-length drift via the group velocity dispersion. Consequently, the artificial actuator enables a capture range up to 2.3 mm, much longer than that achieved by index changes of the modulator. A robust and tight locking for the repetition rate is then realized with a standard deviation as low as 9 μHz with a 1-s sample time over 11 hours, corresponding to a fractional instability of 4.3 × 10-13. Furthermore, a dynamic optical sampling by repetition-rate tuning has been manifested with a fast refresh rate at 100 kHz and a broad scanning range over 305 ps. The demonstrated passive servo action may provide a simple yet effective way to stabilize the repetition rate with high precision, large bandwidth, and wide tunability.

Electro-Optic Modulation of Higher-Order Poincaré Beam Based on Nonlinear Optical Crystal

Vector beams (VBs) have spatially inhomogeneous polarization states distribution and have been widely used in many fields. In this paper, we proposed a method to modulate polarization states of higher-order Poincaré (HOP) beams and designed a system based on Mach-Zehnder interferometers, in which polarization state (include azimuth and ellipticity) of generated HOP beams were modulated by linear electro-optic (EO) effect of nonlinear optical crystals. Using this method, the polarization state of generated HOP beams could be controlled by voltage signal applied on EO crystals, which makes the process of the polarization state change with no optical element moving and mechanical vibrations. Besides, due to the flexibility of the voltage signal, the polarization state could be switched directly and immediately.

Approach to the Design of a Polarization Maintaining Fiber Electric Field Probe for High Signal-to-Noise Ratio

We propose an approach to elevate the signal-to-noise ratio (SNR) in a microwave electric field sensor system with a polarization maintaining fiber (PMF) probe incorporated with an electro-optic (EO) crystal. The optimal probe parameters were determined to obtain the best SNR based on the suggested approach, which was validated experimentally. Using a newly fabricated PMF probe with parameters close to the optimal design, an SNR improvement of 2.5 dB compared to our previous probe was successfully demonstrated in microwave electric field measurements.

Dynamic generation of vortex beam based on partial phase modulation of electro-optical crystal plate

With the increasing demand for potential applications of vortex beams in various fields of modern optics, the generation of optical vortex beams has attracted great interest. Based on a flat plate made of an electro-optical crystal, a method to generate optical vortex beams assisted by the Pockels effect is proposed. This method allows an orbital-angular-momentum-tunable range of <inline-formula><tex-math id="M2">\begin{document}$ \pm 2\hbar$\end{document}</tex-math><alternatives><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="20-20220835_M2.jpg"/><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="20-20220835_M2.png"/></alternatives></inline-formula> with a finite phase-modulated region. We simulate the propagation of optical beams transmitted from the flat plate and investigate the orbital-angular-momentum-mode spectra of the transmitted optical beams. The mode spectra accord well with the simulation results. The proposed method will be applied to fields where tunable optical vortex beams are required, such as optical communication and optical manipulation.

Experimental verification of electro-optical effect in LBO crystal based on nonlinear optical process

Lithium triborate (LBO) crystal is a widely used nonlinear crystal and a potential electro-optic (EO) crystal, but there was no report on experimental verification of its EO characteristics. We verified the linear EO effect of LBO crystal experimentally by designing a second harmonic generation (SHG) experiment. In the experiment, the direction of applied voltage was determined by the analysis of LBO EO tensor matrix. By measuring the curve of voltage-tuning SHG efficiency with different angle detuning, the linear EO effect was verified, and the linear EO coefficient was calculated by the slope of phase mismatch with respect to voltage.

Real-Time Data Acquisition and Processing System for MHz Repetition Rate Image Sensors

An electro-optic detector is one of the diagnostic setups used in particle accelerators. It employs an electro-optic crystal to encode the longitudinal beam charge profile in the spectrum of a light pulse. The charge distribution is then reconstructed using data captured by a fast spectrometer. The measurement repetition rate should match or exceed the machine bunching frequency, which is often in the range of several MHz. A high-speed optical line detector (HOLD) is a linear camera designed for easy integration with scientific experiments. The use of modern FPGA circuits helps in the efficient collection and processing of data. The solution is based on Xilinx 7-Series FPGA circuits and implements a custom latency-optimized architecture utilizing the AXI4 family of interfaces. HOLD is one of the fastest line cameras in the world. Thanks to its hardware architecture and a powerful KALYPSO sensor from KIT, it outperforms the fastest comparable commercial devices.

Organic crystal-based THz source for complex refractive index measurements of window materials using single-shot THz spectroscopy

We employed N-benzyl-2-methyl-4-nitroaniline (BNA) crystals bonded on substrates of different thermal conductivity to generate THz radiation by pumping with 800 nm laser pulses. Crystals bonded on sapphire substrate provided four times more THz yield than glass substrate. A pyrodetector and a single-shot electro-optic (EO) diagnostic were employed for measuring the energy and temporal characterisation of the THz pulse. Systematic studies were carried out for the selection of a suitable EO crystal, which allowed accurate determination of the emitted THz spectrum from both substrates. Subsequently, the THz source and single-shot electro-optic detection scheme were employed to measure the complex refractive index of window materials in the THz range.

Heterogeneous Wafer Bonding Technology and Thin-Film Transfer Technology-Enabling Platform for the Next Generation Applications beyond 5G.

Wafer bonding technology is one of the most effective methods for high-quality thin-film transfer onto different substrates combined with ion implantation processes, laser irradiation, and the removal of the sacrificial layers. In this review, we systematically summarize and introduce applications of the thin films obtained by wafer bonding technology in the fields of electronics, optical devices, on-chip integrated mid-infrared sensors, and wearable sensors. The fabrication of silicon-on-insulator (SOI) wafers based on the Smart CutTM process, heterogeneous integrations of wide-bandgap semiconductors, infrared materials, and electro-optical crystals via wafer bonding technology for thin-film transfer are orderly presented. Furthermore, device design and fabrication progress based on the platforms mentioned above is highlighted in this work. They demonstrate that the transferred films can satisfy high-performance power electronics, molecular sensors, and high-speed modulators for the next generation applications beyond 5G. Moreover, flexible composite structures prepared by the wafer bonding and de-bonding methods towards wearable electronics are reported. Finally, the outlooks and conclusions about the further development of heterogeneous structures that need to be achieved by the wafer bonding technology are discussed.

Absolute detection of atmospheric temperature by using a scanning Fabry-Pérot interferometer in high spectral resolution lidar

In order to achieve a high signal-to-noise ratio by using small laser energy and telescope aperture, we present a detection method based on Rayleigh-Brillouin scattering (RBS) for the measurement of atmospheric temperature without response functions and calibration procedures by using high spectral resolution lidar (HSRL). Different from the traditional HSRL, a Fabry-Pérot interferometer (FPI) with a continuous tunable cavity and polarization optical scheme are employed in a high spectral resolution filter. In order to continuously change the resonant frequency of the FPI, an electro-optical crystal of potassium dideuterium phosphate (DKDP) with two ring electrodes is used as a continuous tunable cavity in the FPI. At each scanned frequency point corresponded with the resonant frequency of the FPI, the received signals of four discrete points on RBS are obtained. Atmospheric temperature is inverted by using a RBS model. The polarization optical scheme is used to suppress the solar background light, and improve the utilization of return signals. In detection experiment of atmospheric temperature, the detection height is 2 km at night and 1.5 km during the day by using a pulsed energy of 30 mJ and telescope diameter of 250 mm. The results are in good agreement with the data detected by radiosonde.

In Situ Optical Characterization of Twinning in Liquid Crystalline Blue Phases.

Crystal twinning is an intergrowth of two or more single crystals of the same species with specific crystallographic relations in their orientations. Here, we perform microscopic optical characterization of (211) twins in the three-dimensional liquid crystalline phase known as the blue phase (BP), with I4132 space group symmetry. We describe the effect of twinning on the optical diffraction pattern-Kossel pattern-of blue phases and analyze the patterns to deduce structural information such as the twin elements and the previously unnoticed deviations from the perfect cubic structure at zero electric field. Further, we obtain in situ observations as a field is applied along the [110] direction of the twinning crystals and find that the twin boundary shows a pinning effect that defines the orientation of the twinned pair through the cubic-to-orthogonal structure transformation. Our findings not only provide important insights for the application of BPs as electro-optic crystals but also present a step in understanding the hierarchical structures that are crystallographic.

Construction Features of The High-Precision Laser Rangefinder Light Modulator

The issues related to the development of a light modulator operating on the electro-optical effect of laser rangefinders by the modulation method are considered. To reduce the modulation power, it is proposed to lower the modulation frequency to 750-800 MHz, while simultaneously increasing the modulation quality to Q = 1000. The study of the phase determination error of a high-precision laser rangefinder depending on temperature showed that it is rational to construct the light modulator by radial installation of the KDP electro-optical crystal, with separated modulation and demodulation channels, while on combined resonators.

Pure modulation and accurate measurement of optical beam's tilt and displacement.

We developed a tilt modulation technique of a laser beam with a wedged crystal. Combined with a phase-compensating crystal, a pure tilt modulation with a wide bandwidth (actually determined by the bandwidth of electro-optic crystals) is realized. By Fourier transformation with a lens, the tilt signal is transformed into displacement. With homodyne detection using a local oscillator of the first-order Hermite-Gauss mode (HG10) and a 4F phase-monitoring system, we measure the displacement and tilt of a laser probe beam. This technique can be used in metrology, such as Newtonian gravitational constant determination and gravitational wave detection, or the calibration of a spatial sensor, such as tilt/displacement sensors.

Electrically switchable and optically tunable liquid crystal/ silicone oil based non-aqueous emulsions for electro-optical device applications

Liquid crystal/silicone oil based emulsions have been prepared and characterized for interfacial interactions, optical and electro-optical behaviour. Emulsions are stabilized without any surface-active agent via non-covalent interactions, surface alignment and anchoring conditions. Emulsions are characterized by polarizing optical microscopy. Distinct mesomorphic phases, droplet geometries (radial, hedgehog, bipolar) and transitions viz. radial to bipolar and bipolar to broken bipolar are observed as a function of varying silicone oil concentration in liquid crystal. These emulsions are quite stable and show reversible characteristics as a function of time and temperature. The stability of these emulsions has been explained considering hydrophobic interactions, decrease in internal surface tension and anchoring energy etc. Further, the liquid crystal/silicone oil devices have been fabricated and tested for switching and electro-optical behaviour. The emulsion contains 25% silicone oil in liquid crystal matrix shows the best switching characteristics at low deriving voltage 5 V, about 87% enhancement in optical transmission, 8.3 dB contrast and lower Frederiks threshold ~65%. Such switchable and optically tuneable surfactant-free emulsions with controlled morphological dynamics can provide a new door to design novel functional soft material platform for better optical, electro-optical, photonics, sensing and liquid crystals elastomer applications. • Surfactant-free, electrically switchable and optical tuneable liquid crystals/silicone oil emulsions. • 87% enhancement in transmission, 8.3 dB contrast and lower Fredrick's threshold ~65% has been achieved in emulsion systems. • Tuning of optical and electro-optical parameters depends on the boundary conditions, topological deformations.