Ultrashort THz Pulses Research Articles

Avoided Level Crossing and Entangled States of Interacting Hydrogen Molecules Detected by the Quantum Superposition Microscope.

Pump-probe measurements by ultrashort THz pulses can be used to excite and follow the coherence dynamics in the time domain of single hydrogen molecules (H2) in the junction of a scanning tunneling microscope (STM). By tailoring the resonance frequency through the sample bias, we identified two spectral signatures of the interactions among multiple H2 molecules. First, the avoided level crossing featured by energy gaps ranging from 20 to 80 GHz was observed because of the level repulsion between two H2 molecules. Second, the tip can sense the signal of H2 outside the junction through the projective measurement on the H2 inside the junction, owing to the entangled states created through the interactions. A dipolar-type interaction was integrated into the tunneling two-level system model of H2, enabling accurate reproduction of the observed behaviors. Our results obtained by the quantum superposition microscope reveal the intricate quantum mechanical interplay among H2 molecules and additionally provide a 2D platform to investigate unresolved questions of amorphous materials.

Investigating Coherent Magnetization Control with Ultrashort THz Pulses

Coherent terahertz control of magnetization dynamics is an area of current interest due to its great potential for the realization of magnetization control on ultrafast timescales in commercial devices. Here we report on an experiment realized at the THz beamline of the free electron laser FLASH at DESY which offers a tunable terahertz radiation source and spontaneously synchronized free-electron laser X-ray pulses to resonantly probe the magnetization state of a ferromagnetic film. In this proof-of-principle experiment, we have excited a thin Permalloy film at different THz wavelengths and recorded the induced magnetization dynamics with photons resonantly tuned to the Ni M2,3 absorption edge. For THz pump pulses including higher orders of the undulator source we observed demagnetization dynamics, which precise shape depended on the employed fundamental wavelength of the undulator source. Analyzing the shape in detail, we can reconstruct the temporal profile of the electric field of the THz pump pulse. This offers a new method for the realization of an in-situ terahertz beamline diagnostic which will help researchers to adjust the pulse characteristics as needed, for example, for future studies of THz induced coherent control of magnetization dynamics.

Removal of Spectral Distortion Due to Echo for Ultrashort THz Pulses Propagating Through Multilayer Structures with Thick Substrate

Given the wide range of applications of time-domain spectroscopy, and particularly THz time-domain spectroscopy, the modelling of a probe pulse propagating through a multilayered structure is often required. Due to the fact that the multilayers are usually grown on a substrate much thicker than the other layers, the transmission of a probe pulse includes a series of echo pulses caused by the multiple reflections at the substrate interfaces over a long time. However, experiments often measure only a small time window and construct the transmitted spectrum only from the first transmitted pulse. Due to the fact that typical substrates lead to times of crossing comparable to the spectral bandwidth, the first transmitted pulse’s spectrum and the full transmitted spectrum can importantly differ. It is therefore important to theoretically model the transmission without the echo, to be able to make a direct comparison with experimental results. Here, we propose a method to elegantly and easily theoretically remove the echo from the transmission spectrum. The spectrum of the transmitted pulse without echo will be produced analytically without additional numerical steps.

Population difference gratings created on vibrational transitions by nonoverlapping subcycle THz pulses

We study theoretically a possibility of creation and ultrafast control (erasing, spatial frequency multiplication) of population density gratings in a multi-level resonant medium having a resonance transition frequency in the THz range. These gratings are produced by subcycle THz pulses coherently interacting with a nonlinear medium, without any need for pulses to overlap, thereby utilizing an indirect pulse interaction via an induced coherent polarization grating. High values of dipole moments of the transitions in the THz range facilitate low field strength of the needed THz excitation. Our results clearly show this possibility in multi-level resonant media. Our theoretical approach is based on an approximate analytical solution of time-dependent Schrödinger equation (TDSE) using perturbation theory. Remarkably, as we show here, quasi-unipolar subcycle pulses allow more efficient excitation of higher quantum levels, leading to gratings with a stronger modulation depth. Numerical simulations, performed for THz resonances of the H_20 molecule using Bloch equations for density matrix elements, are in agreement with analytical results in the perturbative regime. In the strong-field non-perturbative regime, the spatial shape of the gratings becomes non-harmonic. A possibility of THz radiation control using such gratings is discussed. The predicted phenomena open novel avenues in THz spectroscopy of molecules with unipolar and quasi-unipolar THz light bursts and allow for better control of ultra-short THz pulses.

Observation of extremely efficient terahertz generation from mid-infrared two-color laser filaments

Extreme nonlinear interactions of THz electromagnetic fields with matter are the next frontier in nonlinear optics. However, reaching this frontier in free space is limited by the existing lack of appropriate powerful THz sources. Here, we experimentally demonstrate that two-color filamentation of femtosecond mid-infrared laser pulses at 3.9 μm allows one to generate ultrashort sub-cycle THz pulses with sub-milijoule energy and THz conversion efficiency of 2.36%, resulting in THz field amplitudes above 100 MV cm−1. Our numerical simulations predict that the observed THz yield can be significantly upscaled by further optimizing the experimental setup. Finally, in order to demonstrate the strength of our THz source, we show that the generated THz pulses are powerful enough to induce nonlinear cross-phase modulation in electro-optic crystals. Our work paves the way toward free space extreme nonlinear THz optics using affordable table-top laser systems.

Response of nonequilibrium nonstationary plasma created by intense femtosecond UV laser pulse in rare gases: emission in the THz frequency band

SynopsisWe analyse the response of the current in plasma created in the process of gas ionization by an intense UV laser pulse in the terahertz frequency band. Our consideration allows us to take into account both temporal retardation of the EVDF evolution with respect to the external electric field and the effect of the relaxation of the strongly nonequilibrium EVDF due to elastic electron - atomic collisions The suggested theory enables to properly describe propagation of short and ultra-short THz pulses in laser plasma waveguides.

Impact of Antenna Design on the Electric-Field Direction Sensitivity of Zero-Biased Y–Ba–Cu–O Detectors to Ultra-Short THz Pulses

Detectors made from sub-micron-sized bridges of the high-T <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">c</sub> superconductor Y-Ba-Cu-O have unique properties useful for the detection of THz radiation, namely evidence of a detector response with an additional sensitivity to the direction of the electric field of short THz pulses when used without a transport current in the so-called “zero-bias” regime. In order to examine the influence of the antenna design on the detector response, we have conducted electromagnetic simulations and performed experiments at a synchrotron light source and with a photomixing setup as sources for short THz pulses. In this paper, we evaluate a narrow-band double-slot antenna as well as a broadband log-spiral antenna design.

Attenuation of THz Beams: A \u201cHow to\u201d Tutorial

Attenuation of ultrashort THz pulses poses a significant technological challenge due to the broadband nature of such light pulses. Several methods exist for this purpose, including crossed wire grid polarizers, high refractive index, high resistivity silicon wafers, and ultrathin metal films. In this review, we discuss the operational principles of these methods, and highlight some of the advantages and potential pitfalls of the methods. We describe the limits of high-frequency operation of wire grid polarizers, relevant for contemporary ultra-broadband THz sources in air photonics. We discuss the effects of multiple reflections and interference in sequences of silicon wafers for attenuation, and finally discuss the potential of using ultrathin metallic films for broadband attenuation.

Ti, Ni, and TiNi Alloys in the Generation of THz Pulses and Their Use in Bolometers

A study is performed of the generation of ultrashort THz pulses in Ti, Ni, and TiNi plates, compared to Au, Ag, Cu plates. The possibility of using them as photosensitive materials in bolometers is considered. Such sources can be used in atmosphere monitoring systems.

Terahertz Nanofocusing with Cantilevered Terahertz-Resonant Antenna Tips

We developed THz-resonant scanning probe tips, yielding strongly enhanced and nanoscale confined THz near fields at their tip apex. The tips with length in the order of the THz wavelength (λ = 96.5 μm) were fabricated by focused ion beam (FIB) machining and attached to standard atomic force microscopy (AFM) cantilevers. Measurements of the near-field intensity at the very tip apex (25 nm radius) as a function of tip length, via graphene-based (thermoelectric) near-field detection, indicate their first and second order geometrical antenna resonances for tip length of 33 and 78 μm, respectively. On resonance, we find that the near-field intensity is enhanced by one order of magnitude compared to tips of 17 μm length (standard AFM tip length), which is corroborated by numerical simulations that further predict remarkable intensity enhancements of about 107 relative to the incident field. Because of the strong field enhancement and standard AFM operation of our tips, we envision manifold and straightforward future application in scattering-type THz near-field nanoscopy and THz photocurrent nanoimaging, nanoscale nonlinear THz imaging, or nanoscale control and manipulation of matter employing ultrastrong and ultrashort THz pulses.

Generation of ultra-short THz pulses in new optical nonlinear materials based on organic polymers

Using the method of optical rectification of femtosecond laser pulses, we report the generation of short (a few field cycles) terahertz pulses in the samples of films based on polyimides with covalently bound chromophore molecules of DR type. The spectral width of the produced pulses is limited by the pump pulse duration. The quadratic nonlinear optical properties are imparted to the films in the process of their fabrication by orienting the chromophore molecules in the external electric field of the applied electrodes having an original configuration. The samples are compared with the ZnTe crystal. Using the methods of coherent spectroscopy, their transmission and refractive index dispersion spectra are investigated in the frequency range . The studied polymer composition is promising for the application in coherent spectrometers both for increasing the working spectral range without dips and for improving the spatial resolution in the near-field terahertz spectroscopy.

THz Electron Paramagnetic Resonance / THz Spectroscopy at BESSY II

The THz beamline at BESSY II employs high power broadband femto- to picosecond long THz pulses for magneto-optical THz and FIR studies. A newly designed set-up exploits the unique properties of ultrashort THz pulses generated by laser-energy modulation of electron bunches in the storage ring or alternatively from compressed electron bunches. Experiments from 0.15 to 5 THz (~ 5 – 150 cm-1) may be conducted at a user station equipped with a fully evacuated high resolution FTIR spectrometer (0.0063 cm-1), lHe cooled bolometer detectors, a THz TDS set-up and different sample environments, including a superconducting high field magnet (+11 T - 11T) with variable temperature insert (1.5 K – 300 K), a sample cryostat and a THz attenuated total reflection chamber. Main applications are Frequency Domain Fourier transform THz-Electron Paramagnetic Resonance (FD-FT THz-EPR), THz-FTIR spectroscopy and optical pump - THz probe time domain spectroscopy (TDS), with sub-ps time resolution.

Heating of Nanosized Liquid Water in High-Intensity Terahertz Pulses**Supported by the National Natural Science Foundation of China under Grant Nos 10975033, 11404070 and 11275048, the Science Foundation for Youths of Guangxi Province under Grant No 2014GXNSFBA118022, and the Scientific Research Foundation of Guangxi Education Department under Grant No 2013ZD039.

Non-equilibrium molecular dynamics simulations of liquid water in picosecond high-power terahertz pulses are performed by using a non-polarizable potential model. Numerical results show that the energy absorption of water molecules exhibits a pronounced resonance with THz pulses in the frequency range of 14-17 THz. With the THz pulse at resonant frequencies, the maximum temperature is about 562K by heating the water at room temperature. Further investigation indicates that the results are independent of the size of the nanoscale water box. The efficiency of energy transfer by resonant absorption is more than seven times of microwave heating. These studies show promising applications of ultrashort THz pulses.

Ultrafast Energy Transfer to Liquid Water by Sub‐Picosecond High‐Intensity Terahertz Pulses: An Ab Initio Molecular Dynamics Study

Sub-picosecond heating of bulk water is accomplished by ultrashort and intense THz pulses which are able to transfer a large amount of energy to the liquid. The energy transferred corresponds to a temperature jump of about 600 K. Liquid water becomes a structureless and hot gas-like system still at the density of the liquid, in which the hydrogen-bonding structure has been washed out.

FLUTE: A versatile linac-based THz source

A new compact versatile linear accelerator named FLUTE is currently being designed at the Karlsruhe Institute of Technology. This paper presents the status of this 42 MeV machine. It will be used to generate strong (several 100 MV/m) ultra-short (~1 ps) THz pulses (up to ~4-25 THz) for photon science experiments, as well as to conduct a variety of accelerator studies. The latter range from comparing different coherent THz radiation generation schemes to compressing electron bunches and studying the electron beam stability. The bunch charge will cover a wide range (~100 pC-3 nC). Later we plan to also produce ultra-short x-ray pulses from the electron bunches, which, for example, could then be combined for THz pump-x-ray probe experiments.

THz detection of small molecule vapors in the atmospheric transmission windows

Using a low power beam of ultrashort THz pulses that propagate in the ambient laboratory environment we have measured the rotational signatures of small molecule vapors at frequencies within the atmospheric transmission windows. We investigate two types of apparatus. In the first type the THz beam propagates along a 6.7 meter round trip path that is external to the spectrometer, and which contains a long sample tube (5.4 meter round trip path) that holds the analyte vapor. The environment of the tube is controlled to simulate dry or humid conditions. In the second apparatus the THz beam propagates over a much longer 170 meter round trip path with analyte vapor contained in a relatively short 1.2 meter round trip path sample chamber. We describe the rotational signatures for each apparatus in the presence of the strong interference from water vapor absorption. For the shorter path long-tube apparatus we find that the peak detection sensitivity is sufficient to resolve a 1% absorption feature. For the more challenging 170 meter path apparatus we find that the peak detection sensitivity is sufficient to resolve a 3-5% absorption feature. The experiments presented here represent a first step towards using ultrashort THz pulses for coherent broad band detection of small molecule gases and vapors under ambient conditions.

Broadband terahertz spectroscopy (Invited Paper)

An overview of the major techniques to generate and detect THz radiation so far, especially the major approaches to generate and detect coherent ultra-short THz pulses using ultra-short pulsed laser, has been presented. And also, this paper, in particularly, focuses on broadband THz spectroscopy and addresses on a number of issues relevant to generation and detection of broadband pulsed THz radiation as well as broadband time-domain THz spectroscopy (THz-TDS) with the help of ultra-short pulsed laser. The time-domain waveforms of coherent ultra-short THz pulses from photoconductive antenna excited by femtosecond laser with different pulse durations and their corresponding Fourier-transformed spectra have been obtained via the numerical simulation of ultrafast dynamics between femtosecond laser pulse and photoconductive material. The origins of fringes modulated on the top of broadband amplitude spectrum, which is measured by electric-optic detector based on thin nonlinear crystal and extracted by fast Fourier transformation, have been analyzed and the major solutions to get rid of these fringes are discussed.

Single-shot spatiotemporal measurements of ultrashort THz waveforms using temporal electric-field cross correlation

A new single-shot technique based on linear spectral interferometry between a temporally short reader pulse and a temporally long probe pulse is demonstrated for measuring the spatiotemporal phase and amplitude of an optical probe for use as an ultrafast diagnostic. The probe spatiotemporal field information is recovered, with a resolution set by the duration of the reader pulse, by applying a single Fourier transform operation to the interferogram image, without need of any reference data. The technique was used in conjunction with electro-optic sampling to measure waveforms of coherent, ultrashort THz pulses emitted by electron bunches from a laser-plasma accelerator with sub-50fs resolution. The presence of strong spatiotemporal coupling in the THz waveforms and of complex temporal electron-bunch structure was determined.

Design of high-energy terahertz sources based on optical rectification

Detailed analysis of the tilted-pulse-front pumping scheme used for ultrashort THz pulse generation by optical rectification of femtosecond laser pulses is presented. It is shown that imaging errors in a pulse-front-tilting setup consisting of a grating and a lens can lead to a THz beam with strongly asymmetric intensity profile and strong divergence, thereby limiting applications. Optimized setup parameters are given to reduce such distortions. We also show that semiconductors can offer a promising alternative to LiNbO(3) in high-energy THz pulse generation when pumped at longer wavelengths. This requires tilted-pulse-front pumping, however the small tilt angles allow semiconductors to be easily used in such schemes. Semiconductors can be advantageous for generating THz pulses with high spectral intensity at higher THz frequencies, while LiNbO(3) is better suited to generate THz pulses with very large relative spectral width. By using optimized schemes the upscaling of the energy of ultrashort THz pulses is foreseen.

Volumetric spectral analysis of materials using terahertz-tomography techniques

We present for the first time a system and new algorithms for spectral THz-tomography. The electric field of single cycle ultra short THz-pulses can be measured time resolved in amplitude and phase. By focusing ultra short THz-pulses to a sample and analyzing the transmitted or reflected beams the inner structure of the sample can be investigated with a resolution up to 0.4 mm by evaluating the time resolved data. Thus a spectrum of every scanned THz-pulse can be calculated with the usage of the fast Fourier transform. In contrast to classical computed tomography (CT) with X-rays a higher amount of information can be obtained. Based on the characteristic absorption spectra of varying materials it is now possible to identify different substances inside a sample by terahertz-tomography with probabilities that are higher than 80%.