Comprehensive Characterization of Terahertz Generation with the Organic Crystal BNA
Isaac C. Tangen, Gabriel A. Valdivida-Berroeta, Larry K. Heki, Zachary B. Zaccardi, Erika W. Jackson, Charles B. Bahr, David J. Michaelis, Jeremy A. Johnson
We characterize the terahertz (THz) generation of N-benzyl-2-methyl-4-nitroaniline (BNA), with crystals ranging in thickness from 123-700 μm. We compare excitation using 800-nm and 1250 to 1500-nm wavelengths. Pumping BNA with 800-nm wavelengths and longer near-infrared wavelengths results in a broad spectrum, producing out to 6 THz using a 100-fs pump, provided the BNA crystal is thin enough. ~200 μm or thinner crystals are required to produce a broad spectrum with an 800-nm pump, whereas ~300 μm thick crystals are optimal for broadband THz generation using the longer wavelengths. We report the favorable THz generation and optical characteristics of our BNA crystals that make them attractive for broadband, high-field THz generation, and we also find significant differences to BNA results reported in other works.
We are reporting on terahertz generation from organic crystal BNA using a 1.15 to 1.55 um near infrared pump. We observed a very large emission spectrum extending up to 7 THz, compared to 2.5 THz from Ti:Sa pump in previous reports. The maximum optical-to-THz conversion efficiency in our experiment was 0.8% at 1 kHz repetition rate and without saturation leading to a peak electric field of 1 GV/m. Our results show pronounced phase matching privilege for intense terahertz generation using a pump in the 1.15 to 1.25 um range where high energy near infrared pump sources operate.
In this work, we demonstrate BNAs high potential for efficient generation of high power THz using ytterbium laser wavelengths. We study the generation theoretically and experimentally using laser wavelength of 960-1150 nm. Broadband pulses of 0-7 THz and high efficiency of 0.6% are demonstrated.
We report on high energy terahertz pulses by optical rectification (OR) in the organic crystal N-benzyl-2-methyl-4-nitroaniline (BNA) directly pumped by a conventional Ti:Sapphire (Ti:Sa) amplifier. The simple scheme provides an optical to terahertz conversion efficiency of 0.25% when pumped by a collimated laser pulses with duration of 50 fs and central wavelength of 800nm. The generated radiation spans frequencies between 0.2 and 3 THz. We measured the damage threshold as well as the dependency of the conversion efficiency on the pump fluence, pump wavelength, and pulse duration.
We demonstrate a 13.3 MHz repetition rate, broadband THz source with milliwatt-average power, obtained by collinear optical rectification of a high-power Yb-doped thin-disk laser in the organic crystal BNA (N-benzyl-2-methyl-4-nitroaniline). Our source reaches a maximum THz average power of 0.95 mW with an optical-to-THz efficiency of 4e-4 and a spectral bandwidth spanning up to 6 THz at -50 dB, driven by 2.4 W average power (after an optical chopper with duty cycle of 10%), 85 fs-pulses. This high average power excitation was possible without damaging the crystal by using a diamond-heatsinked…
The organic terahertz (THz) generation crystal BNA has recently gained traction as a valuable source to produce broadband THz pulses. Even when pumped with 800-nm light, thin BNA crystals can produce relatively high electric fields with frequency components out to 5 THz. However, the THz output when pumped with 800-nm light is limited by the damage threshold of the organic crystal. Here we report that the damage threshold of BNA can be significantly improved by physically bonding BNA to a high-thermal conductivity sapphire window. When pumped with 800-nm light from an amplified Ti:sapphire las…
Terahertz radiation by optical rectification has been observed at room temperature in a hydrogen-bonded organic molecular ferroelectric crystal, 2-phenyl malondialdehyde (PhMDA). The radiated electromagnetic wave consisted of a single-cycle terahertz pulse with a temporal width of $\sim$ 0.5 ps. The terahertz radiation amplitude divided by the sample thickness in PhMDA was nearly equivalent to that in a typical terahertz wave emitter ZnTe. This is attributable to a long coherence length in the range of 130 $\sim$ 800 $μ$m for the terahertz radiation from PhMDA. We also discussed the possibilit…
Broadband THz spectroscopy system beyond 25 THz using BNA crystals and a tunable single-ring-fiber compressor
University of Ottawa（渥太华大学）；Max Planck Institute for the Science of Light（马克斯·普朗克光科学研究所）；University of Erlangen-Nürnberg（埃尔朗根-纽伦堡大学）；National Research Council Canada（加拿大国家研究委员会）
We demonstrate a data mining approach to discover and develop new organic nonlinear optical crystals that produce intense pulses of terahertz radiation. We mine the Cambridge Structural Database for non-centrosymmetric materials and use this structural data in tandem with density functional theory calculations to predict new materials that efficiently generate terahertz radiation. This enables us to (in a relatively short time) discover, synthesize, and grow large, high-quality crystals of four promising materials and characterize them for intense terahertz generation. In a direct comparison t…
High energy terahertz pulses are produced by optical rectification (OR) in organic crystals DAST and DSTMS by a Ti:sapphire amplifier system centered at 0.8 microns. The simple scheme provides broadband spectra between 1 and 5 THz, when pumped by collimated 60 fs near-infrared pump pulse and it is scalable in energy. Fluence-dependent conversion efficiency and damage threshold are reported as well as optimized OR at visible wavelength.
We report the full characterization of a new organic nonlinear optical (NLO) crystal for intense THz generation: PNPA ((E)-4-((4-nitrobenzylidene)amino)-N-phenylaniline). We discuss crystal growth and structural characteristics. We present the wavelength dependence of THz generation, the thickness dependence of the THz spectrum for PNPA crystals, and measure the efficiency. PNPA enables intense THz generation that surpasses NLO crystals DAST and OH-1, which have been the standard in organic high-field THz generators for several years.
Several years ago, it was shown that strong coupling between an electronic transition in organic molecules and a resonant photonic structure can modify the electronic landscape of the molecules and affect their chemical behavior. Since then, this new concept has evolved into a new field known as polaritonic chemistry, which employs strong coupling as a new tool for controlling material properties and molecular chemistry. An important ingredient in the progress of this field was the recent demonstration of strong coupling of molecular vibrations to mid-infrared resonators, which enabled the mod…
Electromagnetic (EM) wave detection over a large spectrum has recently attracted significant amount of attention. Traditional electronic EM wave sensors use large metallic probes which distort the field to be measured and also have strict limitations on the detectable RF bandwidth. To address these problems, integrated photonic EM wave sensors have been developed to provide high sensitivity and broad bandwidth. Previously we demonstrated a compact, broadband, and sensitive integrated photonic EM wave sensor, consisting of an organic electro-optic (EO) polymer refilled silicon slot photonic cry…
The brightness of a light source defines its applicability to nonlinear phenomena in science. Bright low frequency terahertz (< 5THz) radiation confined to a diffraction-limited spot size is a present hurdle due to the broad bandwidth and long wavelengths associated with single-cycle terahertz pulses as well as due to the lack of terahertz wavefront correctors. Here, using a present-technology system, we employ a new concept of terahertz wavefront manipulation and focusing optimization. We demonstrate a spatio-temporal confinement of terahertz energy at its physical limits to the least possibl…
We demonstrate an efficient procedure for terahertz-wave radiation generation by applying a nonlinear wavelength conversion approach using a mid-infrared pump source. We used a 3.3 μm dual-chirped optical parametric amplification source and a 1.5 μm fiber laser for a comparison of energy conversion efficiencies. Nonlinear inorganic and organic crystals were used, and for the periodically-poled lithium niobate crystal, the efficiencies were 1.3*10^-4 and 5.6*10^-12 for the 3.3 μm source and the 1.5 μm source, respectively. We confirmed that nonlinear crystals could be pumped with tera-watt / cm…
Terahertz (THz) radiation meaning electromagnetic radiation in the range from 0.1 THz (3 mm) to 10 THz (30 mu) has the unique advantage of easily penetrating many obstructions while being non-hazardous to organic tissue since it is non-ionizing. A shortcoming of this domain is the limited availability of high-sensitivity detector arrays respective THz cameras with >1k pixels. To overcome the imaging limitations of the THz domain, compressive imaging in combination with an optically controllable THz spatial light modulator is a promising approach especially when used in a single-pixel imaging m…
The ideal laser source for the emerging research field of nonlinear Terahertz (THz) spectroscopy should offer radiation with a large versatility and deliver both ultra-intense multi-octave spanning single-cycle pulses and user-selectable multi-cycle pulses at narrow linewidth. The absence of such a table-top source has hampered advances in numerous THz disciplines including imaging, nonlinear photonics and spectroscopy, selective out-of-equilibrium excitation of condensed matter and quantum systems. Here we introduce a highly versatile table-top THz laser platform providing single-cycle GV/m t…
In Terahertz (THz) technology, one of the long-standing challenges has been the formation of intense pulses covering the hard-to-access frequency range of 1-15 THz (so-called THz gap). This frequency band, lying between the electronically (<1 THz) and optically (>15 THz) accessible spectrum hosts a series of important collective modes and molecular fingerprints which cannot be fully accessed by present THz sources. While present high-energy THz sources are limited to 0.1-4 THz the accessibility to the entire THz gap with intense THz pulses would substantially broaden THz applications like live…
Visualizing ultrafast dynamics at the atomic scale requires time-resolved pump-probe characterization with femtosecond temporal resolution. For single-shot ultrafast electron diffraction (UED) with fully relativistic electron bunch probes, existing techniques are limited by the achievable electron probe bunch length, charge, and timing jitter. We present the first experimental demonstration of pump-probe UED with THz-driven compression and time-stamping that enable UED probes with unprecedented temporal resolution. This technique utilizes two counter-propagating quasi-single-cycle THz pulses g…
Femtosecond electron bunches with keV energies and eV energy spread are needed by condensed matter physicists to resolve state transitions in carbon nanotubes, molecular structures, organic salts, and charge density wave materials. These semirelativistic electron sources are not only of interest for ultrafast electron diffraction, but also for electron energy-loss spectroscopy and as a seed for x-ray FELs. Thus far, the output energy spread (hence pulse duration) of ultrafast electron guns has been limited by the achievable electric field at the surface of the emitter, which is 10 MV/m for DC …
