Search

We evaluated electrical passivation of crystalline silicon wafers possessing oxidized layers using a laser terahertz (THz) emission microscope, measuring waveforms of laser-excited THz emission from those surfaces with a corona charging setup to tune surface potential without electrical contact. The THz waveform strongly correlated to the surface potential, evaluated by measuring surface photovoltage using a Kelvin probe when the surface was depleted or inverted. The waveform also correlated to the potential of the surface in the accumulation mode and inverted near the flatband condition. The minority carrier lifetime agreed with the theoretically determined dependence on the charge density. These results indicate that the surface potential of a semiconductor covered by an insulator which can be charged by the corona charging setup can be evaluated by assessing the THz emission. Further, such a sample can also be used as a reference to quantitatively relate the waveform of the THz emission and the internal field of surface band bending in semiconductors. [ABSTRACT FROM AUTHOR]

The in-plane dielectric and ferroelectric properties of c-axis oriented epitaxial strontium bismuth tantalate (SBT) thin films were investigated by interdigital surface electrode measurement. The four types of SBT thin films, which have various Sr/Bi atomic ratios, were prepared on MgO substrates by pulsed laser deposition. The dielectric properties at kilohertz and megahertz frequencies were studied from 20 to 870 K. Above room temperature, all the films show the phase transition. Sr0.99Bi1.61Ta2O9, Sr0.97Bi2.10Ta2O9, and Sr0.88Bi1.79Ta2O9 thin films show frequency dispersions near phase transition temperature. At low temperatures, dielectric and ferroelectric properties of Sr0.97Bi2.10Ta2O9 and Sr0.83Bi2.08Ta2O9 thin films were investigated. Both dielectric constant and remanent polarization show a tendency to decrease as temperature decreases, and the rapid change, which may indicate a phase transition, was observed in Sr0.97Bi2.10Ta2O9 near 80 K. [ABSTRACT FROM AUTHOR]

Being an atomically thin material, graphene is known to be extremely susceptible to its environment, including defects and phonons in the substrate on which it is placed as well as gas molecules that surround it. Thus, any device design using graphene has to take into consideration all surrounding components, and device performance needs to be evaluated in terms of environmental influence. However, no methods have been established to date to readily measure the density and distribution of external perturbations in a quantitative and non-destructive manner. Here, we present a rapid and non-contact method for visualizing the distribution of molecular adsorbates on graphene semi-quantitatively using terahertz time-domain spectroscopy and imaging. We found that the waveform of terahertz bursts emitted from graphene-coated InP sensitively changes with the type of atmospheric gas, laser irradiation time, and ultraviolet light illumination. The terahertz waveform change is explained through band structure modifications in the InP surface depletion layer due to the presence of localized electric dipoles induced by adsorbed oxygen. These results demonstrate that terahertz emission serves as a local probe for monitoring adsorption and desorption processes on graphene films and devices, suggesting a novel two-dimensional sensor for detecting local chemical reactions. [ABSTRACT FROM AUTHOR]

We show that a charge-density wave mode submerged in large conductivity of the stripe-type charge-ordered (CO) crystal of Pr0.5Sr0.5MnO3 (PSMO) can be extracted by exciting selective crystallographic planes using polarized terahertz field. Low energy (1-7 meV) dynamics have been explored in the (100), (110), and (111) epitaxial films of PSMO manganite. Of (110) and (111) films representing bulk-like CO, the former exhibits a peak in the conductivity-energy spectrum with attributes of charge-density wave mode along a specific in-plane axis. On the contrary, the CO (111) and the phase-separated (100) films lack this low energy mode but exhibit a Drude-like spectral behavior in the metallic regime. These studies reveal a variety in isothermal charge dynamics originating from the anisotropic nature of the stripe charge-order. [ABSTRACT FROM AUTHOR]

We have investigated terahertz (THz) emission from lithium ternary chalcopyrite crystals LiInSe2, LiGaSe2, LiInS2 , and LiGaS2 that were illuminated by 1560nm femtosecond pump laser pulses. Monocyclic THz emission caused by nonlinear optical effects was initially observed in all the illuminated crystals. Narrow-band THz emission from the coherent phonons were observed in LiInSe2 (2.87THz) and LiGaSe2 (2.60 and 3.45 THz). These phonon modes were most likely caused by impulsive stimulated Raman scattering. [ABSTRACT FROM AUTHOR]

Abstract: We have proposed a new type of frequency detection system of sub-terahertz electromagnetic waves using a photomixing technique and a Josephson junction detector. The photomixer illuminated by two lasers with different wavelengths generates coherent electromagnetic waves that include a frequency component corresponding to the frequency difference of the two lasers. The generated electromagnetic waves were radiated from a horn antenna and focused to the Josephson junction detector with Si lens. The high-T c Josephson junction operates as a frequency detector for electromagnetic waves. Using this system, we observed the Shapiro steps of 188μV that correspond to the frequencies of 90.8GHz. [Copyright &y& Elsevier]

We have investigated the initial growth of the SrBi2Ta2O9 (SBT) thin films on MgO, SrTiO3 (STO), (LaAlO3)0.3(Sr2AlTaO6)0.7 (LSAT), LaSrAlO4 (LSAO) and MgAl2O4 (MAO) substrates by atomic force microscopy (AFM). Three types of growth modes corresponding to the degree of lattice mismatch between the thin film and the substrate have been observed. The films prepared on the substrates with a small lattice mismatch such as on STO and LSAT grow in step-flow mode, whereas the films on MgO, which has the larger lattice mismatch of 7.6%, grow three-dimensionally from the initial stage of the growth. In the case of MAO and LSAO, for which lattice mismatches are 3.3% and -1.8%, the islands with flat terraces were formed along the a and b axis of the substrates. [Copyright &y& Elsevier]

We have explored the low energy charge dynamics of charge-ordered Nd0.5Ca0.5MnO3 and Ba-doped Nd0.5Ca0.48Ba0.02MnO3 manganite thin films by recording the complex optical spectra using terahertz time-domain spectroscopy. The extracted frequency- and temperature-dependent optical conductivity (σ) and dielectric constant ([variant_greek_epsilon]1) show distinct features at Néel’s ordering and the charge-ordering temperatures (TN and TCO). We found that the Ba-doping induced cation disorder effects on σ and [variant_greek_epsilon]1 are more pronounced above TCO, but these effects are subtle in a large temperature region below TCO. Both [variant_greek_epsilon]1 and σ increase as a function of temperature and form a scaling relationship [variant_greek_epsilon]1∝σ. [ABSTRACT FROM AUTHOR]

The principle of terahertz radiation emission from multiferroic BiFeO3 thin films was employed to acquire high-resolution images of their photoassisted ferroelectric polarization switching. These images are evidence that poling in “electric-field assisted by illumination of band gap light” enhances the terahertz-emission amplitude by creating additional switchable ferroelectric dipoles. [ABSTRACT FROM AUTHOR]

We have measured the dielectric properties of pulsed-laser-deposited SrTiO3 (STO) thin films by terahertz (THz) time-domain spectroscopy in the frequency range from 80 GHz to 1.5 THz at temperatures from 20 to 290 K. The measured frequency dispersion of the dielectric constant of the STO thin films show a clear Lorentzian oscillator behavior below 180 K and softening of the ferroelectric soft mode of the STO thin films takes place with decreasing temperature. Both eigen frequency and damping of the soft phonon mode show a peak nearly at 110 K that can be attributed to the effect on the Ti–O–Ti bending in STO thin film due to the starting of tilting in oxygen octahedra near the cubic to tetragonal phase transition. Dielectric strength saturates near the temperature 60 K, however, that is a point of further investigation. [ABSTRACT FROM AUTHOR]

Prototype systems of home-made magneto-optical microscopes were fabricated, and preliminary studies were carried out using Bi2Sr2CaCu2O8+δ single crystals and an YBa2Cu3O7-δ superconductor vortex flow transistor. In the study using BSCCO crystals, we succeeded in the observation of magnetic flux penetration into half-peeled thin flake region on the crystal surface, and it was found that the magnetic fluxes penetrate in characteristic one-dimensional alignment almost along the crystal a-axis. On the other hand, in the study using the YBCO device clear changes in the generated magnetic field distribution could be detected corresponding to the current direction. [Copyright &y& Elsevier]

We study macroscopically aligned single-wall carbon nanotube arrays with uniform lengths via polarization-dependent terahertz and infrared transmission spectroscopy. Polarization anisotropy is extreme at frequencies less than ~100 cm-1 with no sign of attenuation when the polarization is perpendicular to the alignment direction. The attenuation for both parallel and perpendicular polarizations increases with increasing frequency, exhibiting a pronounced and broad peak around 450 cm-1 in the parallel case. We model the electromagnetic response of the sample by taking into account both radiative scattering and absorption losses. We show that our sample acts as an effective antenna due to the high degree of alignment, exhibiting much larger radiative scattering than absorption in the mid/far-infrared range. Our calculated attenuation spectrum clearly shows a non-Drude peak at ~450 cm-1 in agreement with the experiment. [ABSTRACT FROM AUTHOR]

The ferroelectric soft mode in a SrTiO3 thin film was impulsively driven to a large amplitude using intense picosecond terahertz pulses. As the terahertz electric field increased, the soft-mode absorption peak exhibited blueshifting and spectral narrowing. A classical anharmonic oscillator model suggests that the induced displacement is comparable to that of the ferroelectric phase transition. The spectral narrowing indicates that the displacement exceeds that induced by any inhomogeneities in the film, demonstrating that the method can be used to explore intrinsic quartic anharmonicity. [ABSTRACT FROM AUTHOR]

The one-dimensional confinement of quasiparticles in individual carbon nanotubes (CNTs) leads to extremely anisotropic electronic and optical properties. In a macroscopic ensemble of randomly oriented CNTs, this anisotropy disappears together with other properties that make them attractive for certain device applications. The question however remains if not only anisotropy but also other types of behaviors are suppressed by disorder. Here, we compare the dynamics of quasiparticles under strong electric fields in aligned and random CNT networks using a combination of terahertz emission and photocurrent experiments and out-of-equilibrium numerical simulations. We find that the degree of alignment strongly influences the excited quasiparticles' dynamics, rerouting the thermalization pathways. This is, in particular, evidenced in the high-energy, high-momentum electronic population (probed through the formation of low energy excitons via exciton impact ionization) and the transport regime evolving from diffusive to superdiffusive.

Polarization control is essential in terahertz (THz) imaging. Liquid crystals (LCs) have the potential to functionalize tunable polarization-control devices. Here, a twisted nematic (TN) cell using a hydrogen-bonded LC is fabricated, and the influence of dichroism in the THz region is discussed. Our results indicate that the polarization state in the Gooch-Tarry minimum condition is affected by the LC dichroism; a nondichroic LC is required for complete linearly polarized output. The output intensity of the dichroic LC-TN cell changed when electrically switched or when the incident THz wave polarization direction was rotated 90°. These intensity variations disappeared when using the nondichroic hydrogen-bonded LC.

Powerful, broadband terahertz (THz) pulses and its application attract an exponential growth of interests. Dual-color laser filamentation in gases is one of the promising THz sources because of the scalability of the THz energy and wavelength with input parameters. But the additional phase induced by the nonlinearities associated with high intensities cannot be neglected because it may result in modulation of the THz waves. We investigate the influences of the infrared pump energy and air dispersion on the terahertz generation in dual-color laser filament. We observe that optimum dual-color laser relative phase of the THz generation undergoes a linear shift with increasing pump energy due to the intensity-induced refractive index change. This phase shift is verified by the spectral broadening of a two-color laser affected by the same mechanism. The result improves our understanding of the theoretical framework for a higher power THz source.

Gallium nitride (GaN) is a promising wide-bandgap semiconductor, and new characterization tools are needed to study its local crystallinity, carrier dynamics, and doping effects. Terahertz (THz) emission spectroscopy (TES) is an emerging experimental technique that can probe the ultrafast carrier dynamics in optically excited semiconductors. In this work, the carrier dynamics and THz emission mechanisms of GaN were examined in unintentionally doped n-type, Si-doped n-type, and Mg-doped p-type GaN films. The photocarriers excited near the surface travel from the excited-area in an ultrafast manner and generate THz radiation in accordance with the time derivative of the surge drift current. The polarity of the THz amplitude can be used to determine the majority carrier type in GaN films through a non-contact and non-destructive method. Unique THz emission excited by photon energies less than the bandgap was also observed in the p-type GaN film.

Excitons play major roles in optical processes in modern semiconductors, such as single-wall carbon nanotubes (CNTs), transition metal dichalcogenides, and 2D perovskite quantum wells. They possess extremely large binding energies (>100 meV), dominating absorption and emission spectra even at high temperatures. The large binding energies imply that they are stable, that is, hard to ionize, rendering them seemingly unsuited for optoelectronic devices that require mobile charge carriers, especially terahertz emitters and solar cells. Here, we have conducted terahertz emission and photocurrent studies on films of aligned single-chirality semiconducting CNTs and find that excitons autoionize, i.e., spontaneously dissociate into electrons and holes. This process naturally occurs ultrafast (<1 ps) while conserving energy and momentum. The created carriers can then be accelerated to emit a burst of terahertz radiation when a dc bias is applied, with promising efficiency in comparison to standard GaAs-based emitters. Furthermore, at high bias, the accelerated carriers acquire high enough kinetic energy to create secondary excitons through impact exciton generation, again in a fully energy and momentum conserving fashion. This exciton multiplication process leads to a nonlinear photocurrent increase as a function of bias. Our theoretical simulations based on nonequilibrium Boltzmann transport equations, taking into account all possible scattering pathways and a realistic band structure, reproduce all of our experimental data semiquantitatively. These results not only elucidate the momentum-dependent ultrafast dynamics of excitons and carriers in CNTs but also suggest promising routes toward terahertz excitonics despite the orders-of-magnitude mismatch between the exciton binding energies and the terahertz photon energies.

Parallel plate waveguide (PPWG) terahertz (THz) time domain spectroscopy (TDS) is a powerful tool to investigate the properties of thin and low conductive materials. In this Letter, we determine the lower limit of detection of the PPWG-THz-TDS approach. We provide a closed-form expression of the minimal measurable conductivity by the system. The experimental results of amorphous YBa 2 Cu 3 O 7-δ films indicate that the factor limiting the spectroscopic modality is the waveguide device misalignment. On the other hand, the expression of the minimal detectable conductivity provides a clear scheme of optimization by increasing the waveguide length and therefore enhancing the sensitivity of the system.

Adsorption of gas molecules on the surface of atomically layered two-dimensional (2D) materials, including graphene and transition metal dichalcogenides, can significantly affect their electrical and optical properties. Therefore, a microscopic and quantitative understanding of the mechanism and dynamics of molecular adsorption and desorption has to be achieved in order to advance device applications based on these materials. However, recent theoretical calculations have yielded contradictory results, particularly on the magnitude of the adsorption energy. Here, we have experimentally determined the adsorption energy of oxygen molecules on graphene and 2D tungsten disulfide using temperature-programmed terahertz (THz) emission microscopy (TPTEM). The temperature dependence of THz emission from InP surfaces covered with 2D materials reflects the change in oxygen concentration due to thermal desorption, which we used to estimate the adsorption energy of oxygen molecules on graphene (~0.15 eV) and tungsten disulphide (~0.24 eV). Furthermore, we used TPTEM to visualize relative changes in the spatial distribution of oxygen molecules on monolayer graphene during adsorption and desorption. Our results provide much insight into the mechanism of molecular adsorption on the surface of 2D materials, while introducing TPTEM as a novel and powerful tool for molecular surface science.

As novel classes of two-dimensional (2D) materials and heterostructures continue to emerge at an increasing pace, methods are being sought for elucidating their electronic properties rapidly, non-destructively, and sensitively. Terahertz (THz) time-domain spectroscopy is a well-established method for characterizing charge carriers in a contactless fashion, but its sensitivity is limited, making it a challenge to study atomically thin materials, which often have low conductivities. Here, we employ THz parallel-plate waveguides to study monolayer graphene with low carrier densities. We demonstrate that a carrier density of ~2 × 10(11) cm(-2), which induces less than 1% absorption in conventional THz transmission spectroscopy, exhibits ~30% absorption in our waveguide geometry. The amount of absorption exponentially increases with both the sheet conductivity and the waveguide length. Therefore, the minimum detectable conductivity of this method sensitively increases by simply increasing the length of the waveguide along which the THz wave propagates. In turn, enabling the detection of low-conductivity carriers in a straightforward, macroscopic configuration that is compatible with any standard time-domain THz spectroscopy setup. These results are promising for further studies of charge carriers in a diverse range of emerging 2D materials.

Wide-gap semiconductors have received significant attention for their advantages over existing semiconductors in energy-efficient power devices. To realize stable and reliable wide-gap semiconductor devices, the basic physical properties, such as the electric properties on the surface and at the interface, should be revealed. Here, we report visualization of terahertz (THz) emission from the surface of GaN, which is excited by ultraviolet femtosecond laser pulses. We found that the THz emission is enhanced by defects related to yellow luminescence, and this phenomenon is explained through the modification of band structures in the surface depletion layer owing to trapped electrons at defect sites. Our results demonstrate that the surface potential in a GaN surface could be detected by laser-induced THz emission. Moreover, this method enables feasible evaluation of the distribution of non-radiative defects, which are undetectable with photoluminescence, and it contributes to the realization normally-off GaN devices.

We present a simple scheme of narrowband terahertz (THz) generation by optical rectification in the lithium niobate crystal covered by a binary phase mask. It is shown that a single-domain crystal illumination by spatiotemporal shaped fs-laser pulses is equivalent to the formation of a transversally patterned, quasi-phase-matching structure. Decrease of the optical beam size on the mask leads to an increase of the THz-wave linewidth from 17 GHz to a few THz. The frequency of the generation was tuned in the range of 0.4-1.0 THz by building images of the mask in the crystal with various magnifications. Application results of the presented THz source for measuring transmittance of the superconducting NbN thin film in the 4.2-15 K temperature range are also presented.

A simple approach to generate high energy, frequency and bandwidth tunable multicycle THz pulses by optical rectification (OR) of spatially shaped femtosecond laser pulses in the lithium niobate (LN) crystal is proposed and demonstrated. A one dimensional binary shadow mask is used as a laser beam shaper. By building the mask's image in the bulk LN crystal with various demagnifications, the frequency of THz generation was tuned in the range of 0.3 - 1.2 THz. There exist also an opportunity to tune the bandwidth of THz generation from 20 GHz to approximately 1 THz by changing the optical beam size on the crystal. The energy spectral density of narrowband THz generation is almost independent of the bandwidth and is typically 0.18 μJ/THz for ~1 W pump power at 1 kHz repetition rate.

We have fabricated a centimeter-size single-layer graphene device with a gate electrode, which can modulate the transmission of terahertz and infrared waves. Using time-domain terahertz spectroscopy and Fourier-transform infrared spectroscopy in a wide frequency range (10-10 000 cm(-1)), we measured the dynamic conductivity change induced by electrical gating and thermal annealing. Both methods were able to effectively tune the Fermi energy, E(F), which in turn modified the Drude-like intraband absorption in the terahertz as well as the "2E(F) onset" for interband absorption in the mid-infrared. These results not only provide fundamental insight into the electromagnetic response of Dirac fermions in graphene but also demonstrate the key functionalities of large-area graphene devices that are desired for components in terahertz and infrared optoelectronics.

We have proposed and developed a scanning laser terahertz (THz) near-field imaging system using a 1.56 μm femtosecond fiber laser for high spatial resolution and high-speed measurement. To obtain the two-dimensional (2D) THz images of samples, the laser pulses are scanned over a 2D THz emitter plate [DASC: 4'-dimenthylamino-N-methyl-4- stilbazolium p-chlorobenzenesulfonate] by a galvano meter. In this system, THz wave pulses locally generated at the laser irradiation spots transmit through the sample set on the emitter, and the amplitude of the transmitted THz wave pulse is detected by using a typical THz time-domain spectroscopy (THz-TDS) technique. Using this system, we have succeeded in obtaining THz transmission images of a triangle shaped metal sheet of millimeter-size and a human hair sample with a spatial resolution of sub-wavelength order up to ~27 μm (~λTHz/28) at an imaging speed of about 47 seconds/image for 512 x 512 pixels.

A new scheme of optical rectification (OR) of femtosecond laser pulses in a periodically poled lithium niobate (PPLN) crystal, which generates high energy and bandwidth tunable multicycle THz pulses, is proposed and demonstrated. We show that the number of the oscillation cycles of the THz electric field and therefore bandwidth of generated THz spectrum can easily and smoothly be tuned from a few tens of GHz to a few THz by changing the pump optical spot size on PPLN crystal. The minimal bandwidth is 17 GHz that is smallest ever of reported in scheme of THz generation by OR at room temperature. Similar to the case of Cherenkov-type OR in single-domain LiNbO₃, the spectrum of THz generation extends from 0.1 THz to 3 THz when laser beam is focused to a size close to half-period of PPLN structure. The energy spectral density of narrowband THz generation is almost independent of the bandwidth and is typically 220 nJ/THz for ~1 W pump power at 1 kHz repetition rate.

The ferroelectric soft mode in a SrTiO(3) thin film was impulsively driven to a large amplitude using intense picosecond terahertz pulses. As the terahertz electric field increased, the soft-mode absorption peak exhibited blueshifting and spectral narrowing. A classical anharmonic oscillator model suggests that the induced displacement is comparable to that of the ferroelectric phase transition. The spectral narrowing indicates that the displacement exceeds that induced by any inhomogeneities in the film, demonstrating that the method can be used to explore intrinsic quartic anharmonicity.

We demonstrate a terahertz polarizer built with stacks of aligned single-walled carbon nanotubes (SWCNTs) exhibiting ideal broadband terahertz properties: 99.9% degree of polarization and extinction ratios of 10(-3) (or 30 dB) from ~0.4 to 2.2 THz. Compared to structurally tuned and fragile wire-grid systems, the performance in these polarizers is driven by the inherent anistropic absorption of SWCNTs that enables a physically robust structure. Supported by a scalable dry contact-transfer approach, these SWCNT-based polarizers are ideal for emerging terahertz applications., (© 2012 American Chemical Society)

We describe a film of highly aligned single-walled carbon nanotubes that acts as an excellent terahertz linear polarizer. There is virtually no attenuation (strong absorption) when the terahertz polarization is perpendicular (parallel) to the nanotube axis. From the data, the reduced linear dichrosim was calculated to be 3, corresponding to a nematic order parameter of 1, which demonstrates nearly perfect alignment as well as intrinsically anisotropic terahertz response of single-walled carbon nanotubes in the film.

A new type of laser-terahertz emission system for noncontact investigations of chemical solutions has been developed. The system monitors terahertz emission from a sensing plate, which consists of silicon oxide and silicon thin film layers on a sapphire substrate. Sensing of chemical solutions with pH values between 1.68 and 10.01 was demonstrated. The amplitude of the terahertz emission from the sensing plate increased with increasing pH value. This change in the amplitude was caused by a change in the depletion layers of the silicon thin film when protons were adsorbed on the surface of the sensing plate. This study demonstrates that full noncontact monitoring of chemical solutions is possible using the laser-terahertz emission system.