THz Phonon Research Articles

Paratellurite Nanowires as a Versatile Material for THz Phonon Polaritons

Paratellurite Nanowires as a Versatile Material for THz Phonon Polaritons

Enhanced Terahertz Phonon Polariton in Lithium Niobate Chip

AbstractTerahertz (THz) phonon polaritons, fundamental quasi‐particles that couple lattice vibrations with electromagnetic fields at THz frequencies, are found in a variety of materials that offer the potential for a wide range of THz optoelectronic devices and on‐chip integrated systems. However, these compact devices and on‐chip systems are hampered by the absence of on‐chip powerful THz phonon polariton sources. In this study, the efficient generation and amplification of THz phonon polaritons are proposed and directly visualized on a lithium niobate (LN) chip via a tilted pulsefront phase matching technique. By combining lateral pumping and phase matching schemes, two orders of magnitude are successfully attained in the interaction distance between the pump light and the LN chip, accompanied by a substantial amplification of generated THz phonon polariton. The results of this study may lead to abundant potential applications in chip scale THz photonic devices and systems based on LN materials and its integrated heterostructures.

THz Pulse Generation and Detection in a Single Crystal Layout

The THz pulse of a few picosecond durations have been generated and detected via optical rectification and electro-optic effect within the same ZnTe crystal. An unbalanced single-shot detection scheme was performed to characterize the signal. As a result, a multicycle signal was obtained, in which two-photon absorption and other associated nonlinear effects were reportedly negligible. The experimental set-up is compact, economical, easy to build and has the added simplicity of facilitating an independent analysis of the horizontal or vertical polarization arm of the THz-modulated chirped probe beam. This work finds a useful application in integrated THz devices, narrow-band THz phonon spectroscopy and spectroscopic investigation of fast-occurring processes.

Ultrafast Coherent THz Lattice Dynamics Coupled to Spins in the van der Waals Antiferromagnet FePS3.

Coherent THz optical lattice and hybridized phonon-magnon modes are triggered by femtosecond laser pulses in the antiferromagnetic van der Waals semiconductor FePS3 . The laser-driven lattice and spin dynamics are investigated in a bulk crystal as well as in a 380nm-thick exfoliated flake as a function of the excitation photon energy, sample temperature and applied magnetic field. The pump-probe magneto-optical measurements reveal that the amplitude of a coherent phonon mode oscillating at 3.2THz decreases as the sample is heated up to the Néel temperature. This signal eventually vanishes as the phase transition to the paramagnetic phase occurs, thus revealing its connection to the long-range magnetic order. In the presence of an external magnetic field, the optically triggered 3.2THz phonon hybridizes with a magnon mode, which is utilized to excite the hybridized phonon-magnon mode optically. These findings open a pathway toward the optical control of coherent THz photo-magnonic dynamics in a van der Waals antiferromagnet, which can be scaled down to the 2D limit.

Revealing the interlayer van der Waals coupling of bi-layer and tri-layer MoS2 using terahertz coherent phonon spectroscopy

In this research, we applied THz coherent phonon spectroscopy to optically probe the vibrational modes of the epitaxially-grown bi-layer and tri-layer MoS2 on sapphire substrate. The layers’ THz vibration is displacively stimulated and temporally retrieved by near-UV femtosecond laser pulses, revealing Raman-active and Raman-inactive modes in one measurement. With the complete breathing modes revealed, here we extend the linear chain model by considering the elastic contact with the substrate and vdWs coupling of the next nearest MoS2 layer to analyze the effective spring constants. We further considered the intralayer stiffness as a correction term to acquire the actual interlayer vdWs coupling. Our THz phonon spectroscopy results indicate the interlayer spring constants of 9.03 × 1019 N/m3 and 9.86 × 1019 N/m3 for bi-layer and tri-layer respectively. The extended model further suggests that a non-negligible substrate mechanical coupling and next nearest neighbor vdWs coupling of 1.48 × 1019 N/m3 and 1.04 × 1019 N/m3 have to be considered.

Orthogonal Molecular Assembly: Eliminating Intrinsic Phonon Modes in Organic THz Generators

AbstractThis work reports a series of new organic electro‐optic salt crystals possessing unusual orthogonal dipole‐coupling assembly that act as dimple‐free THz generators. In the new crystals, optically anisotropic aromatic anions introducing highly electronegative fluorinated substituents are orthogonally assembled with optically anisotropic nonlinear optical benzothiazolium cations. These orthogonal cation–anion assembled crystals exhibit strong suppression of intrinsic THz phonon modes along the polar axis, which results in a wide THz absorption‐free range from 1.5 to 4.0 THz without substantial absorption peaks. This is sharply in contrast to previous benchmark crystals with parallel cation–anion assembly; for example, in analogous crystals, several strong absorption peaks appear in this frequency range. This absence of strong absorption peaks is attributed to the orthogonal cation–anion dipole coupling assembly, the formation of fluorinate‐induced strong interionic interactions, and a high packing ability of uniaxial anions. With top‐level macroscopic optical nonlinearity, new orthogonal‐dipole assembled crystals make dimple‐free THz wave generation possible in the range of about 1.5–4.0 THz, which is very beneficial for characterizing signature peaks related to molecular phonon motions of analytes in THz spectroscopy. Therefore, orthogonal molecular assembly of optically highly anisotropic molecules provides an efficient way to substantially reduce and control intrinsic THz phonon modes.

Laser-induced THz piezomagnetism and lattice dynamics of antiferromagnets [formula omitted] and [formula omitted

The piezomagnetic effect manifests itself in emergence of a net magnetic moment in a mechanically-stressed magnetically ordered material. Up to now, this effect was theoretically analyzed and experimentally studied for the case of static or low frequency deformations of antiferromagnets, and in our brief overview we present the recent progress in exploring the piezomagnetic effect at the THz frequencies. We discuss particular lattice distortions in the model piezomagnetic antiferromagnets MnF2 and CoF2 that are associated with the Raman-active phonons. We show that the phonons of the Eg and B2g symmetry should support emergence of a dynamic magnetic moment oscillating at the corresponding THz phonon frequencies. We further analyze conditions for coherent excitations of these modes by using ultrashort laser pulses via the mechanism of impulsive stimulated Raman scattering. We show that observation of transverse piezomagnetic effect is, in principle, feasible for the Eg phonon. We also discuss experimental results demonstrating laser-induced excitation of coherent Eg phonon in MnF2 and CoF2, as well as speculate about possibilities to detect piezomagnetic effect at the THz frequencies.

An achromatic pump-probe setup for broadband, few-cycle ultrafast spectroscopy in quantum materials.

In this work, we present an achromatic pump-probe setup covering the visible (VIS) to near-infrared (NIR) wavelength regions (500-3000nm) for few-cycle pulses. Both the pump and probe arms can work either in the VIS or the NIR wavelength regions, making our setup suitable for multi-color, broadband pump-probe measurements. In particular, our setup minimizes time-smearing due to the phase front curvature, an aspect of ultrafast spectroscopy that has been missing from previous works and allowing us to achieve sub-20-fs temporal resolution. We demonstrate the capabilities of our setup by performing measurements on Pr0.5Ca1.5MnO4. We pump and probe in both wavelength regions with a range of pump fluences and demonstrate how the observed dynamics depend strongly on the probe wavelength. Furthermore, the observation of a 16.5THz phonon demonstrates the high temporal resolution of the setup.

Detecting electron-phonon coupling during photoinduced phase transition

Photo-induced phase transitions have been intensively studied owing to the ability to control a material of interest in the ultrafast manner, which can induce exotic phases unable to be attained at equilibrium. However, the key mechanisms are still under debate, and it has currently been a central issue how the couplings between the electron, lattice, and spin degrees of freedom are evolving during photo-induced phase transitions. Here, we develop a new analysis method, frequency-domain angle-resolved photoemission spectroscopy, to gain precise insight into electron-phonon couplings during photo-induced insulator-to-metal transitions for Ta$_2$NiSe$_5$. We demonstrate that multiple coherent phonons generated by displacive excitations show band-selective coupling to the electrons. Furthermore, we find that the lattice modulation corresponding to the 2 THz phonon mode, where Ta lattice is sheared along the a-axis, is the most relevant for the photo-induced semimetallic state.

Vibrational analysis and physical property studies of 6-Methoxy-2-[(E)-phenyliminomethyl]-phenol in the THz, IR and UV-visible spectral regions.

Bulk single crystals of 6-Methoxy-2-[(E)-phenyliminomethyl]phenol were grown after preparing the material by Schiff base condensation of ortho-vanillin alternatively called 2-hydroxy-3-methoxybenzaldehyde and aniline. The three dimensional molecular and crystal structure of the title compound is confirmed by X-ray diffraction. Molecules crystallized in the orthorhombic crystal system and noncentrosymmetric space group P212121. Geometry optimization, vibrational analysis, Calculation of HOMO-LUMO band gap and molecular hyperpolarizability of the proposed material have been carried out. Terahertz time domain spectroscopic studies have been performed and the refractive index and absorption coefficient of material is calculated in the THz regime. Molecular vibrations responsible for different THz phonon modes are identified with the help of density functional theory based calculations.

Direct observation of mode-specific phonon-band gap coupling in methylammonium lead halide perovskites

Methylammonium lead iodide perovskite is an outstanding semiconductor for photovoltaics. One of its intriguing peculiarities is that the band gap of this perovskite increases with increasing lattice temperature. Despite the presence of various thermally accessible phonon modes in this soft material, the understanding of how precisely these phonons affect macroscopic material properties and lead to the peculiar temperature dependence of the band gap has remained elusive. Here, we report a strong coupling of a single phonon mode at the frequency of ~ 1 THz to the optical band gap by monitoring the transient band edge absorption after ultrafast resonant THz phonon excitation. Excitation of the 1 THz phonon causes a blue shift of the band gap over the temperature range of 185 ~ 300 K. Our results uncover the mode-specific coupling between one phonon and the optical properties, which contributes to the temperature dependence of the gap in the tetragonal phase.

THz Acoustic Spectroscopy by using Double Quantum Wells and Ultrafast Optical Spectroscopy.

GaN is a pivotal material for acoustic transducers and acoustic spectroscopy in the THz regime, but its THz phonon properties have not been experimentally and comprehensively studied. In this report, we demonstrate how to use double quantum wells as a THz acoustic transducer for measuring generated acoustic phonons and deriving a broadband acoustic spectrum with continuous frequencies. We experimentally investigated the sub-THz frequency dependence of acoustic attenuation (i.e., phonon mean-free paths) in GaN, in addition to its physical origins such as anharmonic scattering, defect scattering, and boundary scattering. A new upper limit of attenuation caused by anharmonic scattering, which is lower than previously reported values, was obtained. Our results should be noteworthy for THz acoustic spectroscopy and for gaining a fundamental understanding of heat conduction.

Nonlinear and time-resolved optical study of the 112-type iron-based superconductor parentCa1−xLaxFeAs2across its structural phase transition

The newly discovered 112-type ferropnictide superconductors contain chains of As atoms that break the tetragonal symmetry between the $a$ and $b$ axes. This feature eliminates the need for uniaxial strain that is usually required to stabilize large single domains in the electronic nematic state that exists in the vicinity of magnetic order in the iron-based superconductors. We report detailed structural symmetry measurements of 112-type Ca$_{0.73}$La$_{0.27}$FeAs$_{2}$ using rotational anisotropy optical second harmonic generation. This technique is complementary to diffraction experiments and enables a precise determination of the point group symmetry of a crystal. By combining our measurements with density functional theory calculations, we uncover a strong optical second harmonic response of bulk electric dipole origin from the Fe and Ca $3d$-derived states that enables us to assign $C_2$ as the crystallographic point group. This makes the 112-type materials high-temperature superconductors without a center of inversion, allowing for the possible mixing of singlet and triplet Cooper pairs in the superconducting state. We also perform pump-probe transient reflectivity experiments that reveal a 4.6 THz phonon mode associated with the out-of-plane motion of As atoms in the FeAs layers. We do not observe any suppression of the optical second harmonic response or shift in the phonon frequency upon cooling through the reported monoclinic-to-triclinic transition at 58 K. This allows us to identify $C_1$ as the low-temperature crystallographic point group but suggests that structural changes induced by long-range magnetic order are subtle and do not significantly affect electronic states near the Fermi level.

First-Principles Calculation of Terahertz Absorption with Dispersion Correction of 2,2′-Bithiophene as Model Compound

Terahertz absorption of organic materials is closely linked to molecular arrangements and their intermolecular interactions and is important for material identification as well as THz generation. Theoretical calculations of solid-state vibrations known as phonons help to understand intermolecular interactions responsible for THz absorption but frequently are of limited use without considering dispersion interaction. In this study, we have calculated the THz phonon modes of an organic model crystal 2,2′-bithiophene, considering dispersion intermolecular interactions assuming the fixed cell dimensions. Both energies and intensities of phonon modes at low frequencies were interpreted concentrating on the intermolecular level in conjunction with hydrogen bonds and showed an excellent agreement with the experimental results. This approach to identify the phonon modes responsible for strong THz absorptions and to interpret those modes in terms of intermolecular vibrations is also expected to be applicable to the field of THz generation using nonlinear optical organic crystals.

Phonon Modes of Organic Electro-Optic Molecular Crystals for Terahertz Photonics

We investigate theoretically and experimentally the phonon modes of organic electro-optic crystals for THz-wave photonics. THz phonon modes significantly influence the characteristics of THz-wave generation and detection through the THz absorption and refractive-index dispersion. For a model as THz generation material, electro-optic PNP (2-(N-prolinol)-5-nitropyridine) molecular crystal containing a relatively small numbers of atoms in the unit cell is chosen for phonon-mode calculation. THz phonon modes with their frequencies and intensities are calculated by periodic density functional theory, and the resulting spectrum exhibits a good agreement with the experimental absorption spectrum measured by THz time-domain spectroscopy. THz-wave generation experiment is performed with PNP as THz generator and the organic electro-optic OH1 (2-(3-(4-hydroxystyryl)-5,5-dimethylcyclohex-2-enylidene)malononitrile) crystal as THz detector. Considering the phase matching condition and THz absorption, which are both influenced by the THz phonon modes of THz generation and detection materials, the calculated THz generation spectrum also matches well with the experimental THz spectrum obtained by optical rectification at the pump wavelength of 1300 nm. Therefore, the phonon mode identification is very important for optimizing and designing new THz source and detection materials as well as for THz spectroscopy.

Ultrafast Phase Transition via Catastrophic Phonon Collapse Driven by Plasmonic Hot-Electron Injection

Ultrafast photoinduced phase transitions could revolutionize data-storage and telecommunications technologies by modulating signals in integrated nanocircuits at terahertz speeds. In quantum phase-changing materials (PCMs), microscopic charge, lattice, and orbital degrees of freedom interact cooperatively to modify macroscopic electrical and optical properties. Although these interactions are well documented for bulk single crystals and thin films, little is known about the ultrafast dynamics of nanostructured PCMs when interfaced to another class of materials as in this case to active plasmonic elements. Here, we demonstrate how a mesh of gold nanoparticles, acting as a plasmonic photocathode, induces an ultrafast phase transition in nanostructured vanadium dioxide (VO2) when illuminated by a spectrally resonant femtosecond laser pulse. Hot electrons created by optical excitation of the surface-plasmon resonance in the gold nanomesh are injected ballistically across the Au/VO2 interface to induce a subpicosecond phase transformation in VO2. Density functional calculations show that a critical density of injected electrons leads to a catastrophic collapse of the 6 THz phonon mode, which has been linked in different experiments to VO2 phase transition. The demonstration of subpicosecond phase transformations that are triggered by optically induced electron injection opens the possibility of designing hybrid nanostructures with unique nonequilibrium properties as a critical step for all-optical nanophotonic devices with optimizable switching thresholds.

Terahertz phonon polariton imaging

In this article, we primarily review the time-resolved imaging of THz phonon polariton, which is generated by femtosecond laser in ferroelectric crystal. We pay more attention to the imaging in thin crystal, which can be used as an integration platform for terahertz-optics or terahertz-electrics. The imaging techniques, which can get quantitatively in-focus time-resolved images, are introduced in more detail. They have made enormous progress in recent years, and are powerful tools for the research of phonon polariton, optics, and THz wave. We also briefly introduce the generation principle and general propagation properties of THz phonon polariton.

Phonon-mediated coupling between quantum dots through an off-resonant microcavity

We present experimental results showing phonon-mediated coupling between two quantum dots embedded inside a photonic crystal microcavity. With only one of the dots being spectrally close to the cavity, we observe both frequency up-conversion and down-conversion of the pump light via a $\sim1.2$ THz phonon. We demonstrate this process for both weak and strong regimes of dot-cavity coupling, and provide a simple theoretical model explaining our observations.

THZ Phonon Spectroscopy of Bi-2223 and Bi-2212: Evidence for Phonon Pairing

Abstract Facts are presented evidencing the strong electron–phonon interaction and the scaling of a superconducting gap and a critical temperature in doped Bi-2212 single crystals. A sharp extra structure in the current-voltage characteristics (CVC's) of Bi-2212 contacts is attributed to the presence of the extended van Hove singularity (EVHS) close to the Fermi level in slightly overdoped and slightly underdoped samples. THZ phonon spectroscopy studies of Bi-2223 and Bi-2212 are overviewed. An observed giant instability in I(V) – characteristics of Bi-2223 nanosteps is probably caused by a resonant emission of 2Δ – optical phonons in a process of recombination of nonequilibrium quasiparticles (Krasnov model).

Effects of breathing and oblong mode phonons on transport properties in a single-electrontransistor

We investigate theoretically the transport characteristics of a single-electron transistoraffected by the dynamic deformation of the device configuration due to phonons. Byconsidering changes in capacitances and tunnel resistances caused by the breathing andoblong vibrations of the island that forms part of the transistor, we formulate theelectron–phonon interaction peculiar to the device and derive its transport properties bymeans of the master equation. For a single electron transistor with a gold nanoparticleisland of radius 1 nm, we demonstrate the contribution to the transport properties thatoriginates from tunneling channels associated with THz phonon emission andabsorption.