An official website of the United States government
Abstract Next-generation terahertz (THz) sources demand lightweight, low-cost, defect-tolerant, and robust components with synergistic, tunable capabilities. However, a paucity of materials systems simultaneously possessing these desirable attributes and functionalities has made device realization difficult. Here we report the observation of asymmetric spintronic-THz radiation in Two-Dimensional Hybrid Metal Halides (2D-HMH) interfaced with a ferromagnetic metal, produced by ultrafast spin current under femtosecond laser excitation. The generated THz radiation exhibits an asymmetric intensity toward forward and backward emission direction whose directionality can be mutually controlled by the direction of applied magnetic field and linear polarization of the laser pulse. Our work demonstrates the capability for the coherent control of THz emission from 2D-HMHs, enabling their promising applications on the ultrafast timescale as solution-processed material candidates for future THz emitters.
more »
« less
Colossal Terahertz Emission with Ultrafast Tunability Based on Van der Waals Ferroelectric NbOI 2
Abstract Terahertz (THz) technology is critical for quantum material physics, biomedical imaging, ultrafast electronics, and next‐generation wireless communications. However, standing in the way of widespread applications is the scarcity of efficient ultrafast THz sources with on‐demand fast modulation and easy on‐chip integration capability. Here the discovery of colossal THz emission is reported from a van der Waals (vdW) ferroelectric semiconductor NbOI2. Using THz emission spectroscopy, a THz generation efficiency an order of magnitude higher than that of ZnTe, a standard nonlinear crystal for ultrafast THz generation is observed. The underlying generation mechanisms associated are further uncovered with its large ferroelectric polarization by studying the THz emission dependence on excitation wavelength, incident polarization, and fluence. Moreover, the ultrafast coherent amplification and annihilation of the THz emission and associated coherent phonon oscillations by employing a double‐pump scheme are demonstrated. These findings combined with first‐principles calculations, inform a new understanding of the THz light–matter interaction in emergent vdW ferroelectrics and pave the way to develop high‐performance THz devices on them for quantum materials sensing and ultrafast electronics.
more »
« less
- Award ID(s):
- 2309000
- PAR ID:
- 10576174
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Optical Materials
- Volume:
- 13
- Issue:
- 15
- ISSN:
- 2195-1071
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Coherent phonons in the Terahertz (THz) regime have gained attention as potential candidates for next-generation high-speed, low-energy information carriers in atomically thin phononic or phonon-integrated on-chip devices. Nevertheless, achieving efficient control of the phonon generation dynamics over THz coherent phonons continues to pose a considerable challenge. In this work, we explore THz coherent phonon generation in exfoliated van der Waals (vdW) flakes of WSe2 on Au (WSe2/Au) and Si (WSe2/Si) by using time-resolved pump–probe spectroscopy. The generation of THz coherent phonons was studied as a function of the WSe2 layer thickness and laser wavelength. Notably, a significant enhancement in THz coherent phonon generation was observed in the WSe2/Au structure, but only within a specific range of WSe2 thicknesses and laser wavelengths. The results from numerical simulations, which consider a self-hybridized optical cavity depending on WSe2 thickness and optical reflectance and Raman spectroscopy measurements, all align well with the time-domain observations of THz coherent phonon generation. We propose that the observed enhancement in THz coherent phonon generation is strongly influenced by light–matter interactions in the WSe2 cavity, a mechanism that may be applicable to a broader range of vdW materials. These findings offer promising insights for the development of THz phononic or phonon-integrated devices.more » « less
-
Abstract Resonant tunneling is a quantum‐mechanical effect in which electron transport is controlled by the discrete energy levels within a quantum‐well (QW) structure. A ferroelectric resonant tunneling diode (RTD) exploits the switchable electric polarization state of the QW barrier to tune the device resistance. Here, the discovery of robust room‐temperature ferroelectric‐modulated resonant tunneling and negative differential resistance (NDR) behaviors in all‐perovskite‐oxide BaTiO3/SrRuO3/BaTiO3QW structures is reported. The resonant current amplitude and voltage are tunable by the switchable polarization of the BaTiO3ferroelectric with the NDR ratio modulated by ≈3 orders of magnitude and an OFF/ON resistance ratio exceeding a factor of 2 × 104. The observed NDR effect is explained an energy bandgap between Ru‐t2gand Ru‐egorbitals driven by electron–electron correlations, as follows from density functional theory calculations. This study paves the way for ferroelectric‐based quantum‐tunneling devices in future oxide electronics.more » « less
-
Abstract Excitation of coherent high-frequency magnons (quanta of spin waves) is critical to the development of high-speed magnonic devices. Here we computationally demonstrate the excitation of coherent sub-terahertz (THz) magnons in ferromagnetic (FM) and antiferromagnetic (AFM) thin films by a photoinduced picosecond acoustic pulse. Analytical calculations are also performed to reveal the magnon excitation mechanism. Through spin pumping and spin-charge conversion, these magnons can inject sub-THz charge current into an adjacent heavy-metal film which in turn emits electromagnetic (EM) waves. Using a dynamical phase-field model that considers the coupled dynamics of acoustic waves, spin waves, and EM waves, we show that the emitted EM wave retains the spectral information of all the sub-THz magnon modes and has a sufficiently large amplitude for near-field detection. These predictions indicate that the excitation and detection of sub-THz magnons can be realized in rationally designed FM or AFM thin-film heterostructures via ultrafast optical-pump THz-emission-probe spectroscopy.more » « less
-
Van der Waals (vdW) materials have recently attracted significant interest in the context of orientation-dependent linear and nonlinear optical properties. Recently, arsenic trisulfide (As2S3) or orpiment is identified as a new vdW layered material having anisotropic vibrational and optomechanical responses due to the reduced in-plane crystal symmetry, but its nonlinear optical response is still not well understood yet. Herein, the anisotropic third-harmonic generation (THG) response of mechanically exfoliated As2S3thin flakes is reported. The polarization-dependent evolution of THG emission from butterfly-shaped pattern to four-lobe pattern is comprehensively explored. Moreover, the third-order nonlinear susceptibility of As2S3crystal is extracted by analyzing the thickness-dependent THG emission. We anticipate that the discussed results will not only update the existing understanding on the nonlinear light-matter interaction in anisotropic vdW materials, but also promote future applications in integrated photonic circuits, on-chip nonlinear signal processing, and polarization-sensitive optical devices.more » « less
