Over the past three decades a new spectroscopic technique with unique possibilities has emerged. Based on coherent and time-resolved detection of the electric field of ultrashort radiation bursts in the far-infrared, this technique has become known as terahertz time-domain spectroscopy (THz-TDS). In this review article the authors describe the technique in its various implementations for static and time-resolved spectroscopy, and illustrate the performance of the technique with recent examples from solid-state physics and physical chemistry as well as aqueous chemistry. Examples from other fields of research, where THz spectroscopic techniques have proven to be useful research tools, and the potential for industrial applications of THz spectroscopic and imaging techniques are discussed.

Terahertz spectroscopy and imaging – Modern techniques and applications

This review provides a perspective on the recent developments in the transmission of light through subwavelength apertures in metal films. The main focus is on the phenomenon of extraordinary optical transmission in periodic hole arrays, discovered over a decade ago. It is shown that surface electromagnetic modes play a key role in the emergence of the resonant transmission. These modes are also shown to be at the root of both the enhanced transmission and beaming of light found in single apertures surrounded by periodic corrugations. This review describes both the theoretical and experimental aspects of the subject. For clarity, the physical mechanisms operating in the different structures considered are analyzed within a common theoretical framework. Several applications based on the transmission properties of subwavelength apertures are also addressed.

http://digital.csic.es/bitstream/10261/47904/1/Light%20passing.pdf

Light passing through subwavelength apertures

Sources and systems for far-infrared or terahertz (1 THz = 10(12) Hz) radiation have received extensive attention in recent years, with applications in sensing, imaging and spectroscopy. Terahertz radiation bridges the gap between the microwave and optical regimes, and offers significant scientific and technological potential in many fields. However, waveguiding in this intermediate spectral region still remains a challenge. Neither conventional metal waveguides for microwave radiation, nor dielectric fibres for visible and near-infrared radiation can be used to guide terahertz waves over a long distance, owing to the high loss from the finite conductivity of metals or the high absorption coefficient of dielectric materials in this spectral range. Furthermore, the extensive use of broadband pulses in the terahertz regime imposes an additional constraint of low dispersion, which is necessary for compatibility with spectroscopic applications. Here we show how a simple waveguide, namely a bare metal wire, can be used to transport terahertz pulses with virtually no dispersion, low attenuation, and with remarkable structural simplicity. As an example of this new waveguiding structure, we demonstrate an endoscope for terahertz pulses.

Metal wires for terahertz wave guiding

Despite long study, a molecular picture of the mechanism of water reorientation is still lacking Using numerical simulations, we find support for a pathway in which the rotating water molecule breaks a hydrogen bond (H-bond) with an overcoordinated first-shell neighbor to form an H-bond with an undercoordinated second-shell neighbor The H-bond cleavage and the molecular reorientation occur concertedly and not successively as usually considered This water reorientation mechanism involves large-amplitude angular jumps, rather than the commonly accepted sequence of small diffusive steps, and therefore calls for reinterpretation of many experimental data wherein water rotational relaxation is assumed to be diffusive

https://science.sciencemag.org/content/sci/311/5762/832.full.pdf

A molecular jump mechanism of water reorientation.

Within the last several years, the field of terahertz science and technology has changed dramatically. Many new advances in the technology for generation, manipulation, and detection of terahertz radiation have revolutionized the field. Much of this interest has been inspired by the promise of valuable new applications for terahertz imaging and sensing. Among a long list of proposed uses, one finds compelling needs such as security screening and quality control, as well as whimsical notions such as counting the almonds in a bar of chocolate. This list has grown in parallel with the development of new technologies and new paradigms for imaging and sensing. Many of these proposed applications exploit the unique capabilities of terahertz radiation to penetrate common packaging materials and provide spectroscopic information about the materials within. Several of the techniques used for terahertz imaging have been borrowed from other, more well established fields such as x-ray computed tomography and synthetic aperture radar. Others have been developed exclusively for the terahertz field, and have no analogies in other portions of the spectrum. This review provides a comprehensive description of the various techniques which have been employed for terahertz image formation, as well as discussing numerous examples which illustrate the many exciting potential uses for these emerging technologies.

https://iopscience.iop.org/article/10.1088/0034-4885/70/8/R02/pdf

Imaging with terahertz radiation

Particle accelerators driven by the interaction of ultraintense and ultrashort laser pulses with a plasma(1) can generate accelerating electric fields of several hundred gigavolts per metre and deliver high-quality electron beams with low energy spread(2-5), low emittance(6) and up to 1 GeV peak energy(7,8). Moreover, it is expected they may soon be able to produce bursts of electrons shorter than those produced by conventional particle accelerators, down to femtosecond durations and less. Here we present wide-band spectral measurements of coherent transition radiation which we use for temporal characterization. Our analysis shows that the electron beam, produced using controlled optical injection(9), contains a temporal feature that can be identified as a 15 pC, 1.4-1.8 fs electron bunch (root mean square) leading to a peak current of 3-4 kA depending on the bunch shape. We anticipate that these results will have a strong impact on emerging applications such as short-pulse and short-wavelength radiation sources(10,11), and will benefit the realization of laboratory-scale free-electron lasers(12-14).

/pdf/few-femtosecond-few-kiloampere-electron-bunch-produced-by-a-3iffbgptpb.pdf

Few femtosecond, few kiloampere electron bunch produced by a laser-plasma accelerator

We present a complete frequency-domain description of electro-optic (EO) detection of terahertz (THz) electromagnetic radiation, including a description of the ellipsometry technique employed. These frequency-domain results show the effect of EO detection of a pulse of THz radiation as the product of three spectral filters acting on the complex amplitude spectrum of the THz pulse that is entering the EO crystal. For the usual experimental situation in which the optical bandwidth of the interrogating light pulse is small compared with the optical carrier frequency, we obtain an important simplification of our general result for the detected EO signal. When this simplified result is rewritten in the time domain, a more general description of the previous time-domain picture of EO detection is obtained.

Electro-optic detection of terahertz radiation

A pump-probe experiment is described to study femtosecond dynamics of hydrogen bonds in liquid water. The key element of the experimental setup is a laser source emitting 150 fs pulses in the 2.5– 4.4 mm spectral region, at a 10 mJ power level. The OH-stretching band is recorded for different excitation frequencies and different pump-probe delay times. Time-dependent solvatochromic shifts are observed and are interpreted with the help of statistical mechanics of nonlinear optical processes. Using these spectral data, the OH · · · O motions are “photographed” in real time. [S0031-9007(98)08298-2]

Femtosecond dynamics of hydrogen bonds in liquid water : a real time study

Phase retarders usually present a strong frequency dependence. We discuss the design and characterization of a terahertz achromatic quarter-wave plate. This wave plate is made from six birefringent quartz plates precisely designed and stacked together. Phase retardation has been measured over the whole terahertz range by terahertz polarimetry. This achromatic wave plate demonstrates a huge frequency bandwidth (upsilonmax/upsilonmin approximately 7), and therefore can be applied to terahertz time domain spectroscopy and polarimetry.

/pdf/terahertz-achromatic-quarter-wave-plate-4frx5f81nc.pdf

Terahertz achromatic quarter-wave plate

Via THz time-domain spectroscopy, we have measured the absorption and index of refraction of single-crystal 〈110〉 ZnTe from 0.3 to 4.5 THz. We find that the absorption is dominated by two lower-frequency phonon lines at 1.6 and 3.7 THz and not by the transverse-optical (TO) -phonon line at 5.3 THz as previously assumed. However, the index of refraction is determined mainly by the TO-phonon line. Using these data, we discuss a frequency-domain picture of electro-optic detection of THz radiation below the TO-phonon resonance and compare with the photoconductive THz receiver over the same frequency range.

/pdf/measurements-of-the-thz-absorption-and-dispersion-of-znte-rmvop9abvo.pdf

Guilhem Gallot

Papers

Few femtosecond, few kiloampere electron bunch produced by a laser-plasma accelerator

Electro-optic detection of terahertz radiation

Femtosecond dynamics of hydrogen bonds in liquid water : a real time study

Terahertz achromatic quarter-wave plate

Measurements of the thz absorption and dispersion of znte and their relevance to the electro-optic detection of thz radiation