THz Emission Research Articles

Revealing Ultrafast Charge-Carrier Thermalization in Tin-Iodide Perovskites through Novel Pump-Push-Probe Terahertz Spectroscopy.

Tin-iodide perovskites are an important group of semiconductors for photovoltaic applications, promising higher intrinsic charge-carrier mobilities and lower toxicity than their lead-based counterparts. Controllable tin vacancy formation and the ensuing hole doping provide interesting opportunities to investigate dynamic intraband transitions of charge carriers in these materials. Here, we present for the first time an experimental implementation of a novel Optical-Pump–IR-Push–THz-Probe spectroscopic technique and demonstrate its suitability to investigate the intraband relaxation dynamics of charge carriers brought into nonequilibrium by an infrared “push” pulse. We observe a push-induced decrease of terahertz conductivity for both chemically- and photodoped FA0.83Cs0.17SnI3 thin films and show that these effects derive from stimulated THz emission. We use this technique to reveal that newly photogenerated charge carriers relax within the bands of FA0.83Cs0.17SnI3 on a subpicosecond time scale when a large, already fully thermalized (cold) population of charge-carriers is present. Such rapid dissipation of the initial charge-carrier energy suggests that the propensity of tin halide perovskites toward unintentional self-doping resulting from tin vacancy formation makes these materials less suited to implementation in hot-carrier solar cells than their lead-based counterparts.

Design and modeling of a planar graphene structure as a terahertz cyclotron radiation source

With incredibly high carrier mobility and saturation velocity, graphene would be an ideal candidate for a miniaturized solid-state cyclotron radiation source. A planar semicircular graphene arc geometry was investigated for emission in the 0.5–1.5 THz range. Analytical studies, confirmed by finite element simulations, show that the emitted THz frequencies are inversely proportional to the arc radius given a fixed charge-carrier velocity. The simulations show that the desired frequency spectrum can be obtained with design radii ranging from 50 to 150 nm. Interestingly, the radiated spectrum is independent of the frequency of the stimulation of the graphene nano-arcs. The simulations also indicate that the total output power correlates well with the Larmor formulation. The device is expected to emit 1 nW/cm2, which confirms the findings of existing research in this field. Such a design could yield a scalable and cost-effective THz source.

Temperature dependence of the picosecond spin Seebeck effect

We performed temperature-dependent optical pump–THz emission measurements in Y3Fe5O12 (YIG)|Pt from 5 K to room temperature in the presence of an externally applied magnetic field. We study the temperature dependence of the spin Seebeck effect and observe a continuous increase as temperature is decreased, opposite to what is observed in electrical measurements, where the spin Seebeck effect is suppressed as 0 K is approached. By quantitatively analyzing the different contributions, we isolate the temperature dependence of the spin-mixing conductance and observe features that are correlated with the bands of magnon spectrum in YIG.

Spintronic terahertz emission from Ni/Pt bilayer grown on MgO

Spintronic THz emission from Ni/Pt bilayer grown on MgO is reported based on the novel THz emitter using metallic structures. The Ni metal was deposited first on a MgO substrate and capped with a thin Pt metal via electron beam deposition. The THz emission data was obtained using a standard terahertz time-domain spectroscopy setup using a Ti: sapphire laser excitation source. Initial measurements were done using 800nm excitation with 7 mW and 185 mW pump powers under upward and downward magnetic field orientations. Polarity reversal of the terahertz signal was observed upon changing the orientation of the magnetic field. Maximum amplitude was found at 0.5 THz with bandwidth up to ~6 THz. A saturation fluence of 85.04 mJ/cm2 was calculated from the pump fluence-dependence plot of the THz peak-to-peak signal. The results are consistent with the spintronic THz emission due to the inverse spin-Hall effect and provide insights for future development and optimizations.

Studying spin–charge conversion using terahertz pulses

Spin–charge conversion is a spin–orbit coupling phenomena where electrical currents can generate transverse spin currents and vice versa. It is one of the central topics in spintronics and widely applied to manipulate the spin and charge degrees of freedom in materials. Previous research on spin–charge conversion was mainly carried out by transport measurements, which lies in the (quasi)equilibrium and DC/low-frequency limit. The recent development of THz emission spectroscopy applied to this field provides additional insights into the dynamics of the spin–charge conversion process, i.e., its ultrafast timescales. Here, the underlying physics and the latest progress of THz studies on spintronics are introduced. The technical details and some features of this technique are summarized, including spin current generation, signal detection, and data analysis. Finally, some possible developments are discussed as well as future research and applications.

Terahertz emission spectroscopy of GaN-based heterostructures

This study investigates the band bending profile of gallium-nitride-based heterostructures with respect to the change in the direction of the induced current in the out-of-plane plane direction, which gives the phase of the terahertz emission peak and can be detected by laser THz emission microscopy. We use a wavelength-tunable laser THz emission spectroscope to observe the transport of charges within the band bending regions, excitation of nearby photocarriers, and carrier scattering. We observe flip-flop peak-to-peak THz emission waveforms for a GaN heterostructure field-effect transistor (FET) compared to a strong THz emission radiated from an Al0.3Ga0.7N/GaN high-electron-mobility-transistor (HEMT). The flip-flop THz emission indicates the emission from various interfaces inside the FET structure, and intense THz emission from the HEMT structure indicates band-edge excitation. Our results provide a valuable perspective for characterizing complex heterostructures that provide insight into possible defects, carrier mobilities, and band bending of multilayer interface electronic devices.

Frequency-angular distribution for terahertz emission of single-color laser filament plasma under an electrostatic field

Frequency-angular distributions for THz emission in the range of 0.1–3 THz generated in a single-color laser filament plasma both under an electrostatic field and without one are experimentally studied for what we believe is the first time. The angular distribution for various spectral components of this THz emission is demonstrated to differ significantly. The maximal propagation angles for these components increase under the electric field. The angular distribution for the low-frequency THz emission depends significantly on the laser pulse energy in contrast to the case of no electric field. An increase in the laser pulse energy leads to a decrease of the propagation angles for low-frequency THz emission and to disappearance of the local minimum in the angular distribution on the propagation axis.

Impact of sulfur doping on broadband terahertz emission in gallium selenide single crystals via optical rectification

The impact of sulfur doping on broadband terahertz emission in GaSe single crystals was investigated by optical rectification with oo-o phase matching. The maximum peak value of THz radiation generated from S-doped 2.5 mass% GaSe is 28.3% larger than that of intrinsic GaSe with pump fluence of 637 mW cm−2 and azimuthal angle of 0o. The saturation of THz emission in S-doped 2.5 mass% GaSe is increased compared with that of intrinsic and S-doped 7 mass% GaSe. The results demonstrate that GaSe with appropriate S-doping concentration can effectively improve the broadband THz radiation and saturation.

Spin Injection Efficiency at Metallic Interfaces Probed by THz Emission Spectroscopy

AbstractTerahertz (THz) spin‐to‐charge conversion has become an increasingly important process for THz pulse generation and as a tool to probe ultrafast spin interactions at magnetic interfaces. However, its relation to traditional, steady state, ferromagnetic resonance techniques is poorly understood. Here, nanometric trilayers of Co/X/Pt (X = Ti, Au or an Au:W alloy) are investigated as a function of the “X” layer thickness, where THz emission generated by the inverse spin Hall effect is compared to the Gilbert damping of the ferromagnetic resonance. Through the insertion of the “X” layer it is shown that the ultrafast spin current injected in the non‐magnetic layer defines a direct‐spin‐conductance, whereas the Gilbert damping leads to an effective spin‐mixing‐conductance of the trilayer. Importantly, it is shown that these two parameters are connected to each other and that spin‐memory‐losses can be modeled via an effective Hamiltonian with Rashba fields. This work highlights that magneto‐circuit concepts can be successfully extended to ultrafast spintronic devices, as well as enhancing the understanding of spin‐to‐charge conversion processes through the complementarity between ultrafast THz spectroscopy and steady state techniques.

Surface plasmon enhanced THz emission with nanoporous gold supported CdTe.

Terahertz emission by ultrafast excitation of semiconductor/metal interfaces was found strongly enhanced by plasmon resonance. Here, a three-dimensional nanoporous gold (NPG) was used to form semiconductor/metal compound with cadmium telluride (CdTe). We investigated the specific impact of surface plasmon from randomly nanoporous structure in the ultrafast optoelectronic response for THz generation, and observed a THz amplitude enhancement around an order of magnitude from CdTe on NPG compared to that from CdTe on silicon. Moreover, the plasmon enhancement for THz emission from NPG is stronger than that from gold film, indicating that randomly nanoporous structure is also effective for plasmonic enhancement in THz band.

Simultaneous elliptically and radially polarized THz from one-color laser-induced plasma filament

THz-based technologies and research applications have seen a rapid increment in recent period together with the development of novel radiation sources based both on relativistic electrons and laser techniques. In this framework, laser-induced plasma filament plays an important role in generating intense and broadband THz radiation. Although many attentions have been paid to THz emission from two-color plasma filaments, one-color plasma emission has been scarcely investigated. In particular, the polarization state of one-color THz emission is still controversial due to the limitations of the existing THz detection techniques, which are incapable of simultaneously detecting elliptically and radially polarized THz radiation. In this manuscript, we develop a novel detection method and unambiguously demonstrate for the first time that one-color laser-induced plasma filament simultaneously emits elliptically and radially polarized THz radiation. These polarization states suggest that the generation mechanism results from electric quadrupole, showing a new route for producing more complex polarization states and THz vortex beams.

Antenna-Coupled Titanium Microbolometers: Application for Precise Control of Radiation Patterns in Terahertz Time-Domain Systems.

An ability of lensless titanium-based antenna coupled microbolometers (Ti-bolometers) operating at room temperature to monitor precisely radiation patterns in terahertz time-domain spectroscopy (THz-TDS) systems are demonstrated. To provide comprehensive picture, two different THz-TDS systems and Ti-bolometers coupled with three different antennas—narrowband dipole antennas for 0.3 THz, 0.7 THz and a log-periodic antenna for wideband detection—were selected for experiments. Radiation patterns, spatial beam profiles and explicit beam evolution along the propagation axis are investigated; polarization-sensitive properties under various THz emitter power ranges are revealed. It was found that the studied Ti-bolometers are convenient lensless sensors suitable to discriminate and control THz radiation pattern features in various wideband THz-TDS systems.

Ultrafast Terahertz Nanoseismology of GaInN/GaN Multiple Quantum Wells

AbstractTerahertz (THz) emission spectroscopy and microscopy are applied to investigate the electron and lattice dynamics of Ga0.8In0.2N/GaN multiple quantum wells (MQWs). The THz emission consists of three distinct, differently timed signals, whose physical mechanisms are attributed to i) laser‐induced ultrafast dynamical screening of built‐in bias electric field in MQWs followed by ii) capacitive charge oscillation of the excited carriers and iii) the coherent acoustic phonon (CAP)‐driven polarization surge at the discontinuity between the GaN capping layer and air. These multifunctional optical responses show strong dependence on the quantum well width and photon energies. The temporal separation between the first and third THz pulses corresponds to the propagation of the CAP across the GaN capping layer of the MQW structure, whose thickness can thus be determined with 10 nm precision.

Two-color two-dimensional terahertz spectroscopy: A new approach for exploring even-order nonlinearities in the nonperturbative regime.

Nonlinear two-dimensional terahertz (2D-THz) spectroscopy at frequencies of the emitted THz signal different from the driving frequencies allows for exploring the regime of (off-)resonant even-order nonlinearities in condensed matter. To demonstrate the potential of this method, we study two phenomena in the nonlinear THz response of bulk GaAs: (i) The nonlinear THz response to a pair of femtosecond near-infrared pulses unravels novel fourth- and sixth-order contributions involving interband shift currents, Raman-like excitations of transverse-optical phonon and intervalence-band coherences. (ii) Transient interband tunneling of electrons driven by ultrashort mid-infrared pulses can be effectively controlled by a low-frequency THz field with amplitudes below 50 kV/cm. The THz field controls the electron-hole separation modifying decoherence and the irreversibility of carrier generation.

Photoconductive Semiconductor-Based Optoelectronic Devices for Generation of Terahertz Radiation

We report on the development and fabrication of a superlattice-based InAlAs/InGaAs heterostructure featuring an ultrashort photocarrier lifetime which has been used as a material base for a photoconductive antenna (PCA)-emitter with a frequency bandwidth of 10 GHz — 3.0 THz and dynamic range above 60 dB. We show an efficiency of plasmonic electrodes embedded into the 10 μm PCA’s gap demonstrating the enhancement of the emitted THz power up to 10 μW (at bias voltage 20—30 V and average pump power 10 mW). The results could open a pathway towards the development of the Russian THz spectroscopic and imaging systems.

Switchable generation of azimuthally- and radially-polarized terahertz beams from a spintronic terahertz emitter.

We propose and demonstrate a method of generating two fundamental terahertz cylindrical vector beams (THz-CVBs), namely the azimuthally- and radially-polarized THz pulses, from a spintronic THz emitter. We begin by presenting that the spintronic emitter generates the HE21 mode, a quadrupole like polarization distribution, when placed between two magnets with opposing polarity. By providing an appropriate mode conversion using a triangular Si prism, we show both from experiment and numerical calculation that we obtain azimuthal and radial THz vector beams. The proposed method facilitates the access of CVBs and paves the way toward sophisticated polarization control in the THz regime.

Terahertz Emission and Ultrafast Carrier Dynamics of Ar-Ion Implanted Cu(In,Ga)Se2 Thin Films

We investigated THz emission from Ar-ion-implanted Cu(In,Ga)Se2 (CIGS) films. THz radiation from the CIGS films increases as the density of implanted Ar ions increases. This is because Ar ions contribute to an increase in the surface surge current density. The effect of Ar-ion implantation on the carrier dynamics of CIGS films was also investigated using optical pump THz probe spectroscopy. The fitted results imply that implanted Ar ions increase the charge transition of intra-and carrier–carrier scattering lifetimes and decrease the bandgap transition lifetime.

Semi-insulating GaAs surface modifications and their influence in the response of THz devices

In this work, we use the Metal-Assisted Chemical Etching (MACE) technique together with an NH3 plasma treatment using a Remote Plasma-Enhanced Chemical Vapor Deposition (RPECVD) equipment to modify the surface of semi-insulating GaAs (SI-GaAs) substrates. Using our modified SI-GaAs, we fabricate photoconductive antennas for THz emission to study the modification's influence on the optical and electrical antenna response. We found substantial gaps in the frequency-domain spectra of the devices, whose origin could reside in a change of the substrate's optical absorption due to: (a) a surficial chemical change or (b) a substrate topographic modification or a combination of both. We showed experimentally that slight and reproducible substrate surface modifications could lead to significant variations in the electrical behavior and THz response of SI-GaAs devices.

Simulation study of phase-matched THz emission from an axially modulated magnetized plasma

We studied and demonstrated the emission of THz waves by the beating of two CW-laser beams in an axially modulated plasma in the presence of a static magnetic field (applied transversely to the direction of propagation of lasers) from two-dimensional particle-in-cell simulation. The ponderomotive-force-induced nonlinear current drives THz radiation with frequency close to the beat frequency (Δω = ω1 − ω2) that propagates in the forward direction. Inside the plasma, THz radiation consists of a mixture of linear and radial polarization, while outside the plasma, only linear polarization dominates; however, radial polarization is stronger in the case of unmagnetized plasma. When the ripple is used, several modes are excited and the mode excited at Δk = (k1 − k2) − kq that meets the phase matching condition is resonantly enhanced. The THz field amplitude grows resonantly with time and it becomes saturated due to the excited higher-order mode coupling. The saturation level is reached about five times higher than the nonrippled plasma case in the vacuum side.

THz emission from a Bi2Sr2CaCu2O8+δ cross-whisker junction

Cuprate superconductor Bi2Sr2CaCu2O8+δ (BSCCO) has been a promising candidate of a coherent, continuous, and compact THz light source owing to its intrinsic Josephson junction (IJJ) inside the crystal structure. In this paper, we utilized BSCCO cross-whisker (CW) junctions to produce THz emitter device using the whisker crystals which can be easily obtained compared with single crystals. As a result, we have successfully observed the emission from the CW IJJ at the frequency of ∼0.7 THz, which is the first observation of a THz emission from whiskers to our knowledge. Our findings would enlarge the applicability of BSCCO superconductors for compact THz emission sources.