Efficient THz Generation Research Articles

Significant Enhancement in THz Emission and Piezoelectricity in Atomically Thin Nb-Doped MoS2.

A significantly enhanced THz radiation generation from femtosecond photoexcited MoS2 layers due to Nb-doping is reported here. Different microscopic mechanisms involved in the THz photocurrent generation vary in their relative contributions in the two cases of photoexcitation, i.e., above and below the electronic bandgap of the layers. For a moderate Nb-doping level of just ∼0.05%, we have observed a multifold enhancement in the THz emission for the case of the above bandgap excitation, which is, though, nearly 1.5 times for the case of the below bandgap excitation of the monolayer MoS2. Alongside the difference in THz generation efficiency, the THz pulse polarity is also reversed at the above bandgap excitation of the Nb-doped layers, consequent to the reversed surface depletion field. Except for a slightly smaller difference in the THz enhancement factor, all the observations are reproducible in the bilayers as well to imply a weaker inversion symmetry and reduced screening of the surface depletion field due to Nb-doping. Furthermore, we employed pristine MoS2 and Nb-doped MoS2 monolayers to fabricate piezoelectric nanogenerator devices. Like enhancement in the ultrafast THz emission, the piezoelectric performance of the nanogenerator, fabricated with the Nb-doped MoS2 monolayer is also increased by a similar factor.

Optimized terahertz generation in BNA organic crystals with chirped Ti:sapphire laser pulses.

We report on the efficient generation of intense terahertz radiation from the organic crystal N-benzyl-2-methyl-4-nitroaniline pumped by chirped Ti:sapphire femtosecond laser pulses. The THz energy and spectrum as a function of the pump fluence and duration of the chirped laser pulses are studied systematically. For the appropriate positively chirped pump pulses, a significant boost in the THz generation efficiency by a factor of around 2.5 is achieved, and the enhancement of high-frequency components (>1 THz) shortens the THz pulse duration. Via complete characterization of THz properties and transmitted laser spectra, this nonlinear behavior is attributed to the extended effective interaction length for phase matching as a result of the self-phase modulation of the intense pump laser pulses. Numerical calculations well reproduce the experimental observation. Our results demonstrate a robust, efficient, strong-field (up to several MV/cm) THz source using the common sub-10 mJ and sub-100 fs Ti:sapphire laser systems without optical parametric amplifiers.

Design and characterization of novel broadband chalcone-based THz optical crystals

By combining extended π-conjugated structures and halogen substituents, two novel chalcone-based optical THz crystals were designed: CBC (C22H17ClO2, Pc) and TFBC (C23H17F3O2, P21). These crystals were synthesized and successfully grown using the solution evaporation method. The effects of different types and quantities of halogen substituents on hydrogen bonding interactions, molecular alignment, and nonlinear strength were analyzed. The second harmonic generation (SHG) efficiency, thermal stability, transmission spectra, dielectric constant, and THz generation of the crystals were characterized. Theoretical calculations were conducted to determine the hyperpolarizability, band gap, density of states, and nonlinear optical coefficients of the crystals. The results showed that the synthesized crystals exhibited higher transparency (≥85%) and SHG efficiencies of 9.5 times and 6.2 times that of standard potassium dihydrogen phosphate (KDP), respectively, compared to previously reported chalcone NLO crystals. For the first time, the THz generation efficiency of the two crystals was confirmed through the optical rectification method, with TFBC demonstrating a wider THz spectrum range compared to CBC.

Temperature dependence of THz generation efficiency, THz refractive index, and THz absorption in lithium-niobate around 275 GHz

In this study, we demonstrate the capabilities of the pulse train excitation approach in determining key material properties of nonlinear crystals, such as refractive index, thermo-optic coefficient, and absorption. The method provides reliable results even at relatively low THz frequencies, where other characterization methods, such as THz time-domain spectroscopy, have difficulties. To illustrate the capabilities of our approach, we used pulse trains with 800-fs long pulses and adjustable time delay to investigate the material properties of periodically poled lithium niobate (PPLN) crystal with a poling period of 400 µm. Via scanning the incident pulse-train frequency, we measured the frequency response of the crystal at different temperatures (78-350 K), which enabled us to determine the temperature dependence of the refractive index and thermo-optic coefficient of the PPLN crystal around 275 GHz with very high precision. We further studied the variation of THz generation efficiency with temperature in detail to understand the temperature dependence of THz absorption in PPLN material. The technique employed is quite general and could be applied to both other frequency ranges and nonlinear crystals.

Ultrafast state-selective tunneling in two-dimensional semiconductors with a phase- and amplitude-controlled THz-scanning tunneling microscope

THz-pulse driven scanning tunneling microscopy (THz-STM) enables access to the ultrafast quantum dynamics of low-dimensional material systems at simultaneous ultrafast temporal and atomic spatial resolution. State-selective tunneling requires precise amplitude and phase control of the THz pulses combined with quantitative near-field waveform characterization. Here, we employ our state-of-the-art THz-STM with multi-MHz repetition rates, efficient THz generation, and precisely tunable THz waveforms to investigate a single sulfur vacancy in monolayer MoS2. We demonstrate that 2D transition metal dichalcogenides (TMDs) are an ideal platform for near-field waveform sampling by THz cross-correlation. Furthermore, we determine the THz voltage via QEV scans, which measure the THz rectified charge Q as a function of THz field amplitude E and dc bias Vdc. Mapping the complex energy landscape of localized states with a resolution down to 0.01 electrons per pulse facilitates state-selective tunneling to the HOMO and LUMO orbitals of a charged sulfur vacancy.

Intrinsic free carrier absorption limited THz generation from Bi2Te3 and Bi2Se3 topological insulators

We investigate the influence of intrinsic free charge carriers on the ultrashort THz pulse generation efficiency of three-dimensional topological insulators (3dTIs). Wavelength dependence of the optical penetration depth of the femtosecond excitation pulses is exploited to vary the excitation volume within Bi2Te3 and Bi2Se3 crystals and accordingly, the free carrier population, to contribute to THz attenuation. The standard free carrier absorption (FCA) formalism is inadequate to explain wavelength-dependent enhancement in the THz emission as observed in the experiments. Within a modified framework, the THz attenuation by FCA is accounted for accurately, which consistently explains the experimental results for samples having different carrier density and mobility. We conclude that the THz generation efficiency of 3dTIs can be enhanced by engineering samples with high carrier mobility and low intrinsic carrier density and by using excitation wavelengths of minimal penetration depth.

Three-photon and four-photon absorption in lithium niobate measured by the Z-scan technique

Open-aperture Z-scan measurements have been carried out to investigate the three-photon (3 PA) and four-photon absorption (4 PA) coefficients at 800 nm and 1030 nm wavelengths, respectively in congruent and stoichiometric lithium niobate (cLN, sLN) with different concentrations of Mg doping. The laser pulse duration at the two wavelengths were 40 and 190 fs. The peak intensity inside the crystals varied between approximately 110 and 550 GW/cm2. The 3 PA and 4 PA coefficients were evaluated using a theoretical model and the results suggest that their minima are at or around the Mg doping level corresponding to the threshold for suppressing photo-refraction for both cLN and sLN. This result can be attributed to the contribution of crystal defects to the 3 PA and 4 PA processes. Furthermore, the 4 PA at 1030 nm exhibited greater nonlinear absorption than the 3 PA at 800 nm under the same intensity level. Possible reasons for this unexpected behavior are discussed. Overall, comparing the 3 PA and 4 PA values of these crystals will enable for selection of the optimum composition of LN crystal for efficient THz generation and for other nonlinear optical processes requiring high pump intensities.

Efficient THz generation by Hermite-cosh-Gaussian lasers in plasma with slanting density modulation

Efficient THz generation by Hermite-cosh-Gaussian lasers in plasma with slanting density modulation

Compact, low-cost, and broadband terahertz time-domain spectrometer.

Terahertz time-domain spectroscopy (THz-TDS) is a powerful technique that enables the characterization of a large range of bulk materials, devices, and products. Although this technique has been increasingly used in research and industry, the standard THz-TDS configuration relying on the use of a near-infrared (NIR) laser source remains experimentally complex and relatively costly, impeding its availability to those without the expertise to build a high-performance setup based on nonlinear optics or without the financial means to acquire a commercial unit. Broadband THz-TDS systems require an even larger financial investment, primarily because the generation and detection of spectral components exceeding 3THz typically need an ultrafast NIR source delivering sub-100-fs pulses. Such an ultrafast source can be bulky and cost upwards of $100,000. Here, we present a broadband, compact, and portable THz-TDS system comprising three modules that allow for the implementation of a single low-cost ultrafast laser, hence significantly decreasing the overall cost of the system. In the first module, the output laser pulses are spectrally broadened through nonlinear propagation in a polarization-maintaining optical fiber and then temporally compressed to achieve a higher peak power. The other two modules utilize thick nonlinear crystals with periodically patterned surfaces that diffract NIR pulses and optimize the efficiency of THz generation and detection processes by enabling a noncollinear beam geometry. Phase-matching conditions in the nonlinear crystals are controlled by the period of the gratings to gain access to a large spectral THz bandwidth. The whole system, combining these three modules, provides access to a THz spectrum peaking at 3.5THz and extending beyond 6THz with a maximum dynamic range of 50dB for time-resolved spectroscopy applications. We demonstrate the functionality of this configuration by performing THz spectroscopy measurements of water vapor contained within a closed cell. Our compact system design paves the way towards a high-performance, yet cost-effective, THz-TDS system that can be readily used in academia and industry.

Prism Couplers with Convex Output Surfaces for Nonlinear Cherenkov Terahertz Generation

Sideways THz generation in Mg:LiNbO3 crystal is studied considering Si-prism-lens couplers with different output surface curvatures. A theoretical approach is developed for modeling the angular distributions of THz radiation power inside the crystal, inside the Si coupler and outside in free space. Our calculations show how the imposition of a plano-convex lens on the standard flat prism can substantially improve the THz generation efficiency. The ratio between the lens curvature radius and the distance from the curvature center to the point of generation on the lens axis is found to be one of the most important parameters. The developed general approach can be used for the further design of the optimal THz extraction elements of a different configuration.

Scalable microstructured semiconductor THz pulse sources.

In recent years several microstructured lithium niobate THz pulse source were suggested for high-energy applications. Two types of those, the reflective and the transmissive nonlinear slab are adopted here for semiconductors. These new sources are scalable both in THz energy and size. Furthermore, they can outperform the already demonstrated contact grating source in diffraction and THz generation efficiency. Compared to the lithium niobate sources, they are more feasible, thanks to the easier manufacturing and the longer pump wavelength. They can produce intense, nearly single-cycle THz pulses at higher frequencies. With 20 mJ pumping at 1.8 µm wavelength, 45 µJ THz energy, and 17 MV/cm focused peak electric field can be expected at 3 THz phase matching frequency from the transmissive nonlinear echelon slab setup consisting of a 4 mm thick structured plan-parallel gallium phosphide crystal.

Femto Seconds Laser Based Efficient THz Generation from Different Temperature Annealed CdTe Thin Films and Effects of Carrier Concentration and Phase Transition on Efficiency of Generation

The paper reports the thermal evaporation based growth process of CdTe thin films on glass substrates. These films were annealed between room temperature to 200, 300 and 400 oC, respectively. The XRD characterization of these films revealed the change in crystalline phase from cubic to triclinic above 200 oC. Finally, these films were subjected to 800 nm wavelength of 35fs pulsed obtained from Ti: sapphire amplifier at 1kHz repetition rate. The incident power of the laser was focused and tuned between 150-350 mW range and generated THz signals were recorded using calibrated Pyroelectric detector at 22.5 Hz frequency. The highest power of the THz signal was 80nW for 200 oC annealed film with respect to incident power of 300mW. The highest efficiency of THz signal was of the order of 3.11E-5%. We have also explained the effect of carrier concentration and phase transition with respect to different annealed temperature for efficient generation of THz signal.

Uniformly scalable lithium niobate THz pulse source in transmission geometry.

A novel THz source, based on optical rectification in LiNbO3 using the tilted-pulse-front technique, is proposed and experimentally demonstrated. The pulse-front tilt is introduced by a volume phase holographic grating, efficiently used at perpendicular incidence in transmission, and the THz pulses are produced in a LiNbO3 plane-parallel nonlinear echelon slab, arranged parallel to the grating. As a unique feature, the entire setup has a plane-parallel, transmission-type configuration, which straightforwardly enables distortion-free scaling to large sizes, high pulse energies and high THz field strengths. The possibility of operating the setup at cryogenic temperature for increased THz generation efficiency is also investigated. Calculations predict efficiencies of 95% for diffraction and 2% for THz generation at room temperature with a refractive-index-matching liquid between the grating and the echelon slab.

Anti-Correlated Plasma and THz Pulse Generation during Two-Color Laser Filamentation in Air

The THz generation efficiency and the plasma density generated by a filament in air have been found anti-correlated when pumped by 800 nm + 1600 nm two-color laser field. The plasma density near zero delay of two laser pulses has a minimum value, which is opposite to the trend of THz generation efficiency and contradicts common sense. The lower plasma density cannot be explained by the static tunneling model according to the conventional photocurrent model, but it might be attributed to the electron trapping by the excited states of nitrogen molecule. The present work also clarifies the dominant role of the drifting velocity accelerated by the two-color laser field during the THz pulse generation process. The results promote our understanding on the optimization of the THz generation efficiency by the two-color laser filamentation.

Optical damage limit of efficient spintronic THz emitters

SummaryTHz pulses are generated from femtosecond pulse-excited ferromagnetic/nonmagnetic spintronic heterostructures via inverse spin Hall effect. The highest possible THz signal strength from spintronic THz emitters is limited by the optical damage threshold of the corresponding heterostructures at the excitation wavelength. For the thickness-optimized spintronic heterostructure, the THz generation efficiency does not saturate with the excitation fluence even up till the damage threshold. Bilayer (Fe, CoFeB)/(Pt, Ta)-based ferromagnetic/nonmagnetic (FM/NM) spintronic heterostructures have been studied for an optimized performance for THz generation when pumped by sub-50 fs amplified laser pulses at 800 nm. Among them, CoFeB/Pt is the best combination for an efficient THz source. The optimized FM/NM spintronic heterostructure having α-phase Ta as the nonmagnetic layer shows the highest damage threshold as compared to those with Pt, irrespective of their generation efficiency. The damage threshold of the Fe/Ta heterostructure on a quartz substrate is ∼85 GW/cm2.

Highly efficient THz generation by optical rectification of mid-IR pulses in DAST

We report on efficient THz generation in DAST by optical rectification of intense mid-IR pulses centered at (i) 3.9 μm and (ii) its second harmonic at 1.95 μm. Suppression of multi-photon absorption shifts the onset of saturation of the THz conversion efficiency to pump energy densities, which are almost an order of magnitude higher as compared to conventional pump schemes at 1.5 μm. Despite strong linear absorption at 3.9 μm, DAST exhibits a high optical-to-THz conversion efficiency, which we attribute to resonantly enhanced nonlinearity and advantageous phase matching of the THz phase velocity and group velocity of the driving pulse. At 1.95 μm, we find that low linear and multi-photon absorption in combination with cascaded optical rectification lead to record optical-to-THz conversion efficiencies approaching 6%. The observed high sensitivity of the THz generation to the parameters of the mid-IR driving pulses motivates an in-depth study of the underlying interplay of nonlinear wavelength- and intensity-dependent effects.

Ultra-short pulse for plasma induced THz generation using carbon nano tubes

In the present investigation, a high intense ultra-short pulse configuration has been proposed for plasma induced THz generation in carbon nano tubes. When a high intense ultra-short electromagnetic wave interacts with the periodically structured carbon nano tubes possessing second order susceptibility, the electromagnetic wave imparts oscillatory velocities to electrons that produce the heat. The generation of excess heat may deform the structure of the carbon nano tubes which lead to the reduction in the efficiency of THz generation. Therefore, the pulse parameters evolution such as normalized energy of the pulse, pulse width, position of the pulse center and reflectivity coefficient of the medium is investigated theoretically on plasma generation. The outcome of the theoretically investigated reveals that the increment in the heating rate can be caused by decrease in the pulse width, increment in reflectivity coefficient and the pulse peak power. Finally, an array of ultra-short pulse configurations has been proposed for efficient THz generation. The present work is helpful to regulate the heating of nanostructure during ultra-short pulse interaction.

Optical Damage Threshold and THz Generation Efficiency of (Fe,CoFeB)/(Ta,Pt) Spintronic Emitters

THz pulses are generated from femtosecond pulse-excited ferromagnetic/nonmagnetic spintronic heterostructures via inverse spin Hall effect. The highest possible THz signal strength from spintronic THz emitters is limited by the optical damage threshold of the corresponding heterostructures at the excitation wavelength. For the thickness-optimized spintronic heterostructure, the THz generation efficiency does not saturate with the excitation fluence even up till the damage threshold. Bilayer (Fe, CoFeB)/(Pt, Ta) based FM/NM spintronic heterostructures have been studied for an optimized performance for THz generation when pumped by sub-50 fs amplified laser pulses at 800 nm. Among them, CoFeB/Pt is the best combination for an efficient THz source. The optimized FM/NM spintronic heterostructure on a quartz substrate, having α-phase Ta as the nonmagnetic layer, shows the highest damage threshold as compared to those with Pt, irrespective of their generation efficiency. The damage threshold of the Fe/Ta heterostructure on a quartz substrate is ~85 GW/cm2.

Organic Broadband THz Generators Optimized for Efficient Near-Infrared Optical Pumping.

New organic THz generators are designed herein by molecular engineering of the refractive index, phonon mode, and spatial asymmetry. These benzothiazolium crystals simultaneously satisfy the crucial requirements for efficient THz wave generation, including having nonlinear optical chromophores with parallel alignment that provide large optical nonlinearity; good phase matching for enhancing the THz generation efficiency in the near‐infrared region; strong intermolecular interactions that provide restraining THz self‐absorption; high solubility that promotes good crystal growth ability; and a plate‐like crystal morphology with excellent optical quality. Consequently, the as‐grown benzothiazolium crystals exhibit excellent characteristics for THz wave generation, particularly at near‐infrared pump wavelengths around 1100 nm, which is very promising given the availability of femtosecond laser sources at this wavelength, where current conventional THz generators deliver relatively low optical‐to‐THz conversion efficiencies. Compared to a 1.0‐mm‐thick ZnTe crystal as an inorganic benchmark, the 0.28‐mm‐thick benzothiazolium crystal yields a 19 times higher peak‐to‐peak THz electric field with a broader spectral bandwidth (>6.5 THz) when pumped at 1140 nm. The present work provides a valuable approach toward realizing organic crystals that can be pumped by near‐infrared sources for efficient THz wave generation.

Enhanced ultrabroadband antireflection properties of ZnTe crystal with sub-wavelength surface structures by maskless reactive ion etching method

Abstract ZnTe as the electro-optic (EO) crystal has been widely used in the THz spectroscopy and imaging system, however, the maximum generation and detection efficiency have yet to be achieved due to surface reflection. In this work, antireflective sub-wavelength structures (SWSs) on ZnTe crystals were fabricated by reactive ion etching (RIE) method. The surface morphology was investigated by tailoring etching time and radio-frequency power. The SWSs with dimensions less than 20 nm spontaneously formed without artificial mask, bringing roughness of 2.07 nm. The infrared and visible-near-infrared transmission spectra demonstrated that the mean transmittance of ZnTe crystals with prepared SWSs was increased 4.4% and 5.8% than as-grown ZnTe crystals, respectively. Simultaneously, the average transmittance in the range of 0.3–2.5 THz was improved ~15.4%. These findings inform an effective way to achieve ultrabroadband (from visible to terahertz) antireflection properties, which is favorable for further enhancing the THz generation and detection efficiency.