Terahertz time-domain spectroscopy

Constructing a THz-TDS experiment using low temperature grown GaAs (LT-GaAs) based antennas requires a laser whose photon energy exceeds the band gap of the material. Ti:sapphire lasers tuned to around 800 nm, matching the energy gap in LT-GaAs, are ideal as they can generate optical pulses as short as 10 fs. These lasers are available as commercial, turnkey systems.

Silver-coated mirrors are optimum for use as steering mirrors for infrared pulses around 800 nm. Their reflectivity is higher than gold and much higher than aluminum at that wavelength.

A beamsplitter is used to divide a single ultrashort optical pulse into two separate beams. A 50/50 beamsplitter is often used, supplying equal optical power to the terahertz generator and detector, though it is common to provide the terahertz generation path with more power given the inefficiency of the terahertz generation process compared to the detection efficiency of infrared (typically 800 nm wavelength) light.

An optical delay-line is implemented using a movable stage to vary the path length of one of the two beam paths. A delay stage uses a moving retroreflector to redirect the beam along a well-defined output path but following a delay. Movement of the stage holding the retroreflector corresponds to an adjustment of path length and consequently the time at which the terahertz detector is gated relative to the source terahertz pulse.

A purge box is typically used so that absorption of THz radiation by gaseous water molecules is minimized. A dry air source is often used for this purpose, however, a nitrogen gas source may also be used.

Water is known to have many discrete absorptions in the THz region that are rotational modes of water molecules. Alternatively, nitrogen, as a diatomic molecule, has no electric dipole moment, and does not (for the purposes of typical THz-TDS) absorb THz radiation. Thus, a purge box may be filled with nitrogen gas so no unintended discrete absorptions in the THz frequency range occur.

A parabolic mirror is shown with important focal lengths and several exemplary rays.

Off-axis parabolic mirrors are commonly used to collimate and focus THz radiation. Radiation from an effective point source, such as from a low-temperature gallium arsenide (LT-GaAs) antenna (active region ~5 μm) incident on an off-axis parabolic mirror becomes collimated, while collimated radiation incident on a parabolic mirror is focused to a point (see diagram). Terahertz radiation can thus be manipulated spatially using optical components such as metal-coated mirrors as well as lenses made from materials that are transparent at THz wavelengths. Samples for spectroscopy are commonly placed at a focus where the terahertz beam is most concentrated.

When an ultra-short (100 femtoseconds or shorter) optical pulse illuminates a semiconductor and its wavelength (energy) is above the energy band-gap of the material, it photogenerates mobile carriers. Most carriers are generated near the surface of the material (typically within 1 micrometre) because pulses are absorbed exponentially with respect to depth. This has two main effects. Firstly, it generates a band bending that has the effect of accelerating carriers of different signs in opposite directions (normal to the surface), creating a dipole. This effect is known as surface field emission. Secondly, the presence of a surface creates a break of symmetry that causes carriers to move (on average) only into the bulk of the semiconductor. This phenomenon, combined with the difference of mobilities of electrons and holes, also produces a dipole. This is known as the photo-Dember effect and is particularly strong in high-mobility semiconductors such as indium arsenide.

When generating THz radiation via a photoconductive emitter, an ultrafast pulse (typically 100 femtoseconds or shorter) creates charge carriers (electron-hole pairs) in a semiconductor material. This incident laser pulse abruptly changes the antenna from an insulating state into a conducting state. Due to an electric bias applied across the antenna, a sudden electric current transmits across the antenna. This changing current lasts for about a picosecond, and thus emits terahertz radiation since the Fourier transform of a picosecond length signal will contain THz components.

Typically the two antenna electrodes are patterned on a low temperature gallium arsenide (LT-GaAs), semi-insulating gallium arsenide (SI-GaAs), or other semiconductor (such as InP) substrate. In a commonly used scheme, the electrodes are formed into the shape of a simple dipole antenna with a gap of a few micrometers and have a bias voltage up to 40 V between them. The ultrafast laser pulse must have a wavelength that is short enough to excite electrons across the bandgap of the semiconductor substrate. This scheme is suitable for illumination with a Ti:sapphire oscillator laser with photon energies of 1.55 eV and pulse energies of about 10 nJ. For use with amplified Ti:sapphire lasers with pulse energies of about 1 mJ, the electrode gap can be increased to several centimeters with a bias voltage of up to 200 kV.

More recent advances towards cost-efficient and compact THz-TDS systems are based on mode-locked fiber laser sources emitting at a center wavelength of 1550 nm. Therefore, the photoconductive emitters must be based on semiconductor materials with smaller band gaps of approximately 0.74 eV such as Fe-doped indium gallium arsenide[4] or indium gallium arsenide/indium aluminum arsenide heterostructures.[5]

The short duration of THz pulses generated (typically ~2 ps) are primarily due to the rapid rise of the photo-induced current in the semiconductor and short carrier lifetime semiconductor materials (e.g., LT-GaAs). This current may persist for only a few hundred femtoseconds to several nanoseconds depending on the substrate material. This is not the only means of generation but is currently (as of 2008) the most common.

Pulses produced by this method have average power levels on the order of several tens of microwatts.[5] The peak power during pulses can be many orders of magnitude higher due to the low duty cycle of mostly >1%, which is dependent on the repetition rate of the laser source. The maximum bandwidth of the resulting THz pulse is primarily limited by the duration of the laser pulse, while the frequency position of the maximum of the Fourier spectrum is determined by the carrier lifetime of the semiconductor.[6]

In optical rectification, a high-intensity ultrashort laser pulse passes through a transparent crystal material that emits a terahertz pulse without any applied voltages. It is a nonlinear-optical process, where an appropriate crystal material is quickly electrically polarized at high optical intensities. This changing electrical polarization emits terahertz radiation.

Because of the high laser intensities that are necessary, this technique is mostly used with amplified Ti:sapphire lasers. Typical crystal materials are zinc telluride, gallium phosphide, and gallium selenide.

The bandwidth of pulses generated by optical rectification is limited by the laser pulse duration, terahertz absorption in the crystal material, the thickness of the crystal, and a mismatch between the propagation speed of the laser pulse and the terahertz pulse inside the crystal. Typically, a thicker crystal will generate higher intensities, but lower THz frequencies. With this technique, it is possible to boost the generated frequencies to 40 THz (7.5 µm) or higher, although 2 THz (150 µm) is more commonly used since it requires less complex optical setups.

The original problem responsible for the “Terahertz gap” (the colloquial term for the lack of techniques in the THz frequency range) was that electronics routinely have limited operation at frequencies at and above 10¹² Hz. Two experimental parameters make such measurement possible in THz-TDS with LT-GaAs antennas: the femtosecond “gating” pulses and the < 1 ps lifetimes of the charge carriers in the antenna (effectively determining the antenna's “on” time). When all optical path lengths have fixed length, an effective dc current results at the detection electronics due to their low time resolution. Picosecond time resolution does not come from fast electronic or optical techniques, but from the ability to adjust optical path lengths on the micrometer (μm) scale. To measure a particular segment of a THz pulse, the optical path lengths are fixed and the (effective dc) current at the detector due to the a particular segment of electric field of the THz pulse.

THz-TDS measurements are typically not single-shot measurements.

Photoconductive detection is similar to photoconductive generation. Here, the voltage bias across the antenna leads is generated by the electric field of the THz pulse focused onto the antenna, rather than some external generation. The THz electric field drives current across the antenna leads, which is usually amplified with a low-bandwidth amplifier. This amplified current is the measured parameter that corresponds to the THz field strength. Again, the carriers in the semiconductor substrate have an extremely short lifetime. Thus, the THz electric field strength is only sampled for an extremely narrow slice (femtoseconds) of the entire electric field waveform.

The materials used for generation of terahertz radiation by optical rectification can also be used for its detection by using the Pockels effect, where particular crystalline materials become birefringent in the presence of an electric field. The birefringence caused by the electric field of a terahertz pulse leads to a change in the optical polarization of the detection pulse, proportional to the terahertz electric-field strength. With the help of polarizers and photodiodes, this polarization change is measured.

As with the generation, the bandwidth of the detection is dependent on the laser pulse duration, material properties, and crystal thickness.