Nitride materials, valued for their structural stability and exceptional physical properties, have garnered significant interest in both fundamental research and technological applications. The fabrication of high-quality nitride thin films is essential for advancing their use in microelectronics and spintronics. Yet, achieving single-crystal nitride thin films with excellent structural integrity remains a challenge. Here, we introduce a straightforward yet innovative metallic alloy nitridation technique for the synthesis of stable single-crystal nitride thin films. By subjecting metal alloy thin films to a controlled nitridation process, nitrogen atoms integrate into the lattice, driving structural transformations while preserving high epitaxial quality. Combining nanoscale magnetic imaging with scanning nitrogen-vacancy (NV) magnetometry, X-ray magnetic linear dichroism, and comprehensive transport measurements, we confirm that the nitridated films exhibit a robust antiferromagnetic character with a zero net magnetic moment. This work not only provides a refined and reproducible strategy for the fabrication of nitride thin films but also lays a robust foundation for exploring their burgeoning device applications. Nitride materials, prized for their stability and unique properties, face challenges in achieving high-quality single-crystal thin films for microelectronics and spintronics. Here, the authors present an innovative metallic alloy nitridation technique, producing stable single-crystal nitride films with robust antiferromagnetic properties, paving the way for advanced device applications.
Microring resonators have been widely used in passive optical devices such as wavelength division multiplexers, differentiators, and integrators. Research on terahertz (THz) components has been accelerated by these photonics technologies. Compact and integrated time-domain differentiators that enable low-loss, high-speed THz signal processing are necessary for THz applications. In this study, an on-chip THz temporal differentiator based on all-silicon photonic technology was developed. This device primarily consisted of a microring waveguide resonator and was packaged with standard waveguide compatibility. It performed time-domain differentiation on input signals at a frequency of 405.45 GHz with an insertion loss of 2.5 dB and a working bandwidth of 0.36 GHz. Various periodic waveforms could be handled by this differentiator. This device could work as an edge detector, which detected step-like edges in high-speed input signals through differential effects. This development holds significant promise for future THz data processing technologies and THz communication systems.
CsV3Sb5 is a recently discovered Kagome metal that exhibits a combination of superconductivity with a critical temperature (TC) of 2.5 K and charge density wave (CDW) order at TCDW = 94 K. In this study, we investigate the collective excitations and quasiparticle dynamics in CsV3Sb5 using ultrafast optical pump-probe spectroscopy. According to our results, in addition to the CDW phase related electron and coherent phonon dynamics, we found another electronic symmetry breaking by nematic phase transition at T* ( 20 K), which can mediate the relaxation of carriers. At temperature below T*, a gap about 4 meV related to the nematic order is open, which determines the low-temperature dynamics of carriers in the rst 2 picosecond (ps). Moreover, we also observed the abrupt change of electron dynamics caused by the CDW phase transition at TCDW. Furthermore, we identify the presence of a CDW induced mode at 1.3 THz below TCDW, as well as two collective modes at 3.1 THz and 3.8 THz below 80 K. It is noteworthy that these two collective modes appear to be associated with the breaking of C6 rotational symmetry. These observations suggest the rich phase order below TCDW and emphasize the need for a deeper understanding of CDW and nematicity order in the Kagome metals.
We investigate the quasiparticle dynamics in MnBi2Te4 single crystal using the ultrafast optical spectroscopy. Our results show that there exist anomalous dynamical optical responses below the antiferromagnetic (AFM) ordering temperature TN. In specific, we reveal that both the initial carrier decay and recombination processes can be modulated via introducing the AFM order in sub-picosecond and picosecond timescales, respectively. We also discover a long relaxation process emerging below TN with a timescale approaching to the nanosecond regime, and can be attributed to the T-dependent spin-lattice interaction. There also emerges an unusual phonon energy renormalization below TN , which is found to arise from its coupling the spin degree via the exchange interaction and magnetic anisotropy. Our findings provide key information for understanding the dynamical properties of non-equilibrium carrier, spin and lattice in MnBi2Te4.
We measure the time-resolved terahertz spectroscopy of GeSn thin film and studied the ultrafast dynamics of its photo-generated carriers. The experimental results show that there are photo-generated carriers in GeSn under femtosecond laser excitation at 2500 nm, and its pump-induced photoconductivity can be explained by the Drude-Smith model. The carrier recombination process is mainly dominated by defect-assisted Auger processes and defect capture. The first- and second-order recombination rates are obtained by the rate equation fitting, which are (2.6 +/- 1.1) x 10(-2) ps(-1) and (6.6 +/- 1.8) x 10(-19) cm(3)& sdot;ps(-1), respectively. Meanwhile, we also obtain the diffusion length of photo-generated carriers in GeSn, which is about 0.4 mu m, and it changes with the pump delay time. These results are important for the GeSn-based infrared optoelectronic devices, and demonstrate that GeSn materials can be applied to high-speed optoelectronic detectors and other applications.
Nonlinear optical properties are investigated using the static and time-resolved second harmonic generation in the topological material molybdenum phosphide(Mo P) with three-component fermions. Giant second harmonic generation signals are detected and the derived χ (2) value is larger than that of the typical electro–optic material.Upon optical excitation, no photoinduced change of the symmetry is detected in MoP, which is quite different from previous observations in several other topological materials.
Strong second-order optical nonlinearities often require broken material centrosymmetry, thereby limiting the type and quality of materials used for nonlinear optical devices. Here, we report a giant and highly tunable terahertz (THz) emission from thin polycrystalline films of the centrosymmetric Dirac semimetal PtSe 2 . Our PtSe 2 THz emission is turned on at oblique incidence and locked to the photon momentum of the incident pump beam. Notably, we find an emitted THz efficiency that is giant: It is two orders of magnitude larger than the standard THz-generating nonlinear crystal ZnTe and has values approaching that of the noncentrosymmetric topological material TaAs. Further, PtSe 2 THz emission displays THz sign and amplitude that is controlled by the incident pump polarization and helicity state even as optical absorption is only weakly polarization dependent and helicity independent. Our work demonstrates how photon drag can activate pronounced optical nonlinearities that are available even in centrosymmetric Dirac materials.
The study of the interaction between terahertz (THz) radiation and quantum materials has been an active area of research due to its potential for understanding fundamental physics and the development of novel technologies. In this review, we focus on the time-dependent photocurrents, behind which are the up-to-date understanding of the physical processes. We provide the recent advancements in revealing the unique properties of quantum materials via the THz emission spectroscopy. Because the theoretical interpretation of some new experimental results is still evolving, this review is intended to inspire further research in this exciting and rapidly growing field.
Singlet fission (SF) materials have been applied in varioustypesof solar cells to pursue higher power conversion efficiency (PCE)beyond the Shockley-Queisser (SQ) limit. SF implementationin perovskite solar cells has not been successfully realized yet dueto the insufficient understanding of the SF/perovskite heterojunctions.In this work, we attempt to elucidate the charge dynamics of an SF/perovskitesystem by incorporating a well-known SF molecule, TIPS-pentacene,and a triple-cation perovskite Cs-0.05(FA(0.85)MA(0.15))(0.95)PbI2.55Br0.45, owing to their well-matched energy structures. The transient absorptionspectra and kinetic fitting plots suggest an electron-transfer processfrom the triplet state of TIPS-pentacene to perovskite in the picosecondregime, which increases the carrier density by 20% in the perovskitelayer. This work confirms the existence of an electron-transfer processbetween the SF material and perovskite, providing a pathway to SF-enhancedperovskite solar cells.
In this work, we measured the time-resolved terahertz spectroscopy of GeSn thin film and studied the ultrafast dynamics of its photo-generated carriers. The experimental results show that there are photo-generated carriers in GeSn under femtosecond laser excitation at 2500 nm, and its pump-induced photoconductivity can be explained by the Drude-Smith model. The carrier recombination process is mainly dominated by defect-assisted Auger processes and defect capture. The first- and second-order recombination rates are obtained by the rate equation fitting, which are (2.6 ± 1.1) × 10−2 ps−1 and (6.6 ± 1.8) × 10−19 cm3 ps−1, respectively. Meanwhile, we also obtain the diffusion length of photo-generated carriers in GeSn, which is about 0.4 μm, and it changes with the pump delay time. These results are important for the GeSn-based infrared optoelectronic devices, and demonstrate that GeSn materials can be applied to high-speed optoelectronic detectors and other applications.
Here, using the ultrafast optical pump-probe spectroscopy, we have studied the quasiparticle dynamics in the type-II Dirac semimetal NiTe2. Anomalous dynamic optical responses are detected around a critical temperature T* (-60 K), which is also evidenced by the transport experiment. In specific, our results reveal a phonon -assisted electron-hole recombination process showing an anomaly at T* <^>' 60 K. We discover an unusual phonon renormalization behavior, manifested by the T-dependent phonon energy and lifetime exhibiting anomalies at T*. We unveil that the observed anomalous T-dependencies can be attributed to the sudden shift of the phonon mode involved in the recombination, which originates from the abrupt change of electronic structure near the Fermi surface. These findings can provide deeper insight into the nonequilibrium carrier and lattice properties in the topological materials.
Spintronic terahertz emitters are broadband and efficient sources of terahertz radiation, which emerged at the intersection of ultrafast spintronics and terahertz photonics. They are based on efficient spin-current generation, spin-to-charge-current conversion, and current-to-field conversion at terahertz rates. In this Editorial, we review the recent developments and applications, the current understanding of the physical processes, and the future challenges and perspectives of broadband spintronic terahertz emitters.
In this work, broadband terahertz (THz) wave emissions have been detected from the trigonal layered PtBi2 on the excitation of the femtosecond laser pulses. Such THz generation is found to arise from the dominated linear photogalvanic effect, which is further discovered to strongly depend on the unique electronic structures of PtBi2. Furthermore, an effective nonlinear susceptibility of PtBi2 is also obtained and is nearly two orders of magnitude larger than that of the traditional nonlinear crystal for THz generation.
We have investigated the quasiparticle dynamics and collective excitations in the quasi-one-dimensional material ZrTe5 using ultrafast optical pump-probe spectroscopy. Our time-domain results reveal two coherent oscillations having extremely low energies of ħω1 ∼0.33 meV (0.08 THz) and ħω2 ∼1.9 meV (0.45 THz), which are softened as the temperature approaches two different critical temperatures (∼54 K and ∼135 K). We attribute these two collective excitations to the amplitude mode of photoinduced dynamic charge density waves in ZrTe5 with tremendously small nesting wave vectors. Furthermore, a peculiar quasiparticle decay process associated with the ħω2 mode with a timescale of ∼1–2 ps is found below the transition temperature T* (∼135 K). Our findings provide pivotal information for studying the fluctuating order parameters and their associated quasiparticle dynamics in various low-dimensional topological systems and other materials.
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.
The generation and detection of ultrafast spin current, preferably reaching a frequency up to terahertz, is the core of spintronics. Studies have shown that the Weyl semimetal WTe2 is of great potential in generating spin currents. However, the prior studies have been limited to the static measurements with the in-plane spin orientation. In this work, we demonstrate a picosecond spin-photocurrent in a Td-WTe2 thin film via a terahertz time domain spectroscopy with a circularly polarized laser excitation. The anisotropic dependence of the circular photogalvanic effect (CPGE) in the terahertz emission reveals that the picosecond spin-photocurrent is generated along the rotational asymmetry a-axis. Notably, the generated spins are aligned along the out-of-plane direction under the light normally incident to the film surface, which provides an efficient means to manipulate magnetic devices with perpendicular magnetic anisotropy. A spin-splitting band induced by intrinsic inversion symmetry breaking enables the manipulation of a spin current by modulating the helicity of the laser excitation. Moreover, CPGE nearly vanishes at a transition temperature of ∼175 K due to the carrier compensation. Our work provides an insight into the dynamic behavior of the anisotropic spin-photocurrent of Td-WTe2 in terahertz frequencies and shows a great potential for the future development of terahertz-spintronic devices with Weyl semimetals.
Transparent conductive oxides (TCOs)—materials that have the twin desirable features of high optical transmission and electrical conductivity—play an increasingly significant role in the fields of photovoltaics and information technology. As an excellent TCO, Ta-doped anatase TiO2 shows great promise for a wide range of applications. Here, terahertz time-domain spectroscopy is used to study the complex optical conductivity σ̃ω of the TCO—heavily Ta-doped TiO2 thin films with different Ta-doping concentrations, in the frequency range of 0.3–2.7 THz and the temperature range of 10–300 K. Fitting the complex optical conductivity to a Drude-like behavior allows us to extract the temperature dependence of the effective mass, which suggests the existence of many-body large polarons. Moreover, the carrier scattering rate of Ta-doped TiO2 with different carrier concentrations agrees with the interacting polaron gas theory. Our results suggest that with increasing electron density in TiO2, the interaction between polarons is larger and electron–phonon coupling is smaller, which is beneficial for achieving high mobility and conductivity in TiO2.
Terahertz technology shows great potential applications in imaging, sensing and security. As is well known, the conventional solid-state broadband terahertz sources rely primarily on the nonlinear optical crystals and photoconductive antennas. Therefore, one major challenge for the next generation of terahertz technology is to develop the high-efficient, ultra-broadband and low-cost terahertz sources. In recent years, much attention has been paid to the spintronic terahertz emitters made of the metallic magnetic heterostructures on a nanometer scale. In this paper, the underlying physical mechanisms associated with this type of terahertz emitter is discussed. They mainly include the ultrafast demagnetization and the spin-charge interconversion processes. In order to further improve the terahertz emission efficiency, three main aspects are considered: appropriate choice of the materials (including conditions of the sample growing), film thickness, and new structure design. In the end, a short conclusion and future perspective for this research direction are given briefly.
Since tantalum arsenide (TaAs) has been experimentally verified as a Weyl semimetal, intensive research has been devoted to study of the unique properties of the material. Despite this, the ultrafast dynamics of TaAs is still not very well understood. In this work, we study the relaxation dynamics in TaAs using transient reflection spectroscopy. From the transient reflection measurement, we observe either a single (fast) or a dual (fast and slow) relaxation, depending on the probing wavelength. The additional relaxation channel is attributed to an asymmetric population of photoexcited electrons and holes.