Generation and detection of very high frequency acoustic phonons in diamond

Generation and detection of very high frequency acoustic phonons in diamond is reported. We generate phonons at a frequency of 28 THz by defect-induced one-phonon absorption of CO₂ laser radiation and observe, after pulsed excitation, phonon decay products in the frequency range from 1 THz to 7 THz. For detection vibronic sideband spectroscopy is used. We find strongly frequency dependent lifetimes for frequencies above 4 THz which we attribute to spontaneous phonon decay.Dedicated to K. Dransfeld on occasion of his 60th birthday     

Generation of coherent terahertz phonons by sharp focusing of a femtosecond laser beam in the bulk of crystalline insulators in a regime of plasma formation

The generation of coherent terahertz phonons in a regime of plasma formation by a femtosecond laser radiation with an intensity of 10¹³ W/cm² in the bulk of crystalline quartz has been detected by the method of probing by a probe pulse of the third harmonic. A smooth increase in the frequency of coherent terahertz phonons from 2.2 to 5.5 THz has been detected, along with its subsequent sharp decrease down to 2.2 THz due to an α-β phase transition in crystalline quartz. The generation of 1-THz coherent phonons has been detected in BaF₂ crystals. A smooth variation of the frequency of coherent phonons from 2 to 2.5 THz has been detected in leucosapphire. The generation of coherent phonons during local laser excitation in CaF₂ and LiF crystals develops at the frequencies of 2.3 and 0.1 THz, respectively.     

Enhanced Third-Order Nonlinearity in Semiconductors Giving Rise to 1 THz Radiation

Third harmonic generation (THG) efficiency is shown to be a greatly enhanced at the onset of inelastic scattering of electrons on optic phonons. Scaling experiments are performed on n-type InP at the pump wave frequency of 9.43 GHz at 80 K. Monte Carlo modeling is employed for scaling the effect to the 3rd harmonic frequency of 1 THz. The THG efficiency in n-type GaAs and InP as well as in the wurtzite phase of n-type InN and GaN compound crystals is compared to that in n-type Si. The efficiency maximum is found to weaken due to the quasi-elastic scattering on acoustic phonons and elastic scattering on ionized impurities. Nevertheless, the THG efficiency at 1 THz in InP crystals cooled down to liquid nitrogen temperatures is predicted to be 2 orders of magnitude higher than the reference value of 0.1% experimentally recorded up to now in n-type Si.     

Resonance effects on coherent phonon generation in lead phthalocyanine crystalline films

We report the first observation of coherent phonons in crystalline lead phthalocyanine (PbPc) films grown on a (0001) sapphire substrate by using a pump–probe technique. Coherent phonon oscillations corresponding to intermolecular (lattice) vibrations in the PbPc film are observed in the frequency region from 1 to 5 THz. It is found that the intensities of coherent phonons are resonantly enhanced at the exciton energies of the Q band observed in the absorption spectrum. PACS 78.47.+p; 78.66.-w; 82.53.Xa; 78.40.Me     

Interface phonons in asymmetric quantum well structures

In semiconductor microstructures with many layers, the phonon modes change from their bulk form and split into ‘confined LO phonons’ (LC) and ‘interface phonons’ (IF), the number and variety of which depends on both the number of layers and the number of different materials in the structure. This affects the electron–phonon scattering rates. Because of the current interest in inter-subband THz emitters, we use these LC and IF modes to evaluate the inter-subband electron–phonon scattering rate in THz emitter prototypes that are based on four-subband stepped quantum wells. These scattering rates in turn affect the population inversion predicted for these devices, so we compare the predicted population inversions for the most promising prototypes against those obtained using bulk phonon scattering rates.     

Terahertz absorption by electrons and confined acoustic phonons in free-standing quantum wells

The acoustic phonon confinement in a free-standing quantum well (FSQW) results in an acoustic phonon energy quantization. Typical quantization energies are in the terahertz frequency range. Free electrons may absorb electromagnetic waves in this frequency range if they emit or absorb acoustic phonons. Therefore, the terahertz absorption reveals the characteristic features of the acoustic phonon spectrum in free-standing structures. We have calculated the absorption coefficient of an electromagnetic wave by free electrons in a FSQW in the terahertz frequency range. We took into account a time dependent electric field, an exact form of the acoustic phonon spectrum and eigenmodes, and electron interactions with confined acoustic phonons through the deformation potential. We demonstrate numerical results for GaAs FSQW of width 100 Å at low lattice temperatures in the frequency range 0.1-1 THz. The absorption coefficient exhibits several structures at frequencies corresponding to the lowest acoustic phonon modes. These features occur due to absorption of photons by electrons, which is accompanied by the emission of corresponding acoustic phonons.     

Coherent optical phonon generation in Bi3Ge4O12

Time-domain spectroscopy of coherent optical phonons in bismuth germinate (Bi4Ge3O12) is presented. Utilizing both impulsive stimulated Raman scattering and time-domain terahertz spectroscopy, more than 12 unique vibrational states ranging in frequency from 2 to 11 THz are identified, each with coherent lifetimes ranging from 1 to 20 ps. These modes are highly sensitive to crystal orientation and demonstrate frequency shifts on picosecond timescales consistent with an anharmonic lattice potential.     

Superconducting tunnel junctions as quantitative detector of intense thermal phonon radiation

Thermal phonons are emitted from a pulse-heated constantan film into an a-cut sapphire (kept at 1.2 K) and are detected quantitatively by recording the current-voltage characteristic of the tunnel junction during the relatively strong phonon irradiation. These measurements are made with the maximum of the Planck distribution of the emitted phonons varied in the frequency range from 0.3 to 1.5 THz. These momentary diode characteristics coincide within experimental error withd c-characteristics at higher substrate temperatures. Assuming thermal equilibrium between electrons and phonons in the tin film and assuming the validity of the acoustic-mismatch model, a comparison can be made between observed phonon power and theoretically expected phonon power. Good agreement is achieved if the influence of the acoustic cut-off frequencies of the tin detector material is taken into account.Supported by Deutsche Forschungsgemeinschaft     

Balance equations for electron transport in an arbitrary energy band driven by an intense terahertz field. Application to superlattice miniband transport

We suggest a balance-equation approach to hot-electron transport in a single arbitrary energy band subject to an intense radiation field of terahertz (THz) frequency, including all the multiphoton emission and absorption processes and taking account of realistic scatterings due to impurities and phonons. This approach, which allows one to calculate THz-driving, time-averaging transport based on a set of time-independent equations, provides a convenient method to study the effect of an intense THz electric field on carrier transport in a nonparabolic energy band. As an example, these fully three-dimensional, acceleration- and energy-balance equations are applied to the discussion of superlattice miniband transport at lattice temperature T=77 and 300 K driven by the THz radiation field of varying strengths. It is shown that the current through a dc biased miniband superlattice is greatly reduced by the irradiation of an intense THz electric field. Received: 23 January 1998 / Revised: 31 March 1998 / Accepted: 20 April 1998     

Phonon focusing of elastically scattered phonons in GaAs

The propagation of high-frequency phonons through crystals at low temperatures is characterized by both ballistic and diffusive processes. Ballistic propagation of heat pulses is highly anisotropic due to phonon focusing, while diffusive propagation is expected to be nearly isotropic in cubic crystals. By using phonon imaging techniques, we have attempted to identify the heat flux from ballistic and scattered phonons in GaAs. Comparison of this data to Monte Carlo calculations which incorporate elastic scattering shows that the flux from phonons scattered a few times in the bulk retains a significant degree of anisotropy. In particular, a sharp feature discovered by Stock, Ulbrich, and Fieseler and attributed to ballistic propagation of phonons with frequencies up to 1.5 THz is now identified with the scattering of sub-THz phonons. Our analysis provides insights into the evolution of heat propagation from the ballistic to diffusive regimes.     

Dispersive phonon imaging of InAs

The phonon-focusing patterns of ballistic phonons in InAs are measured in the frequency range 0.1 to 1 THz, in an effort to test the global validity of lattice dynamics models for this semiconductor. Phonon caustic patterns depend sensitively on the shapes of constant frequency surfaces. Several tunnel-junction detectors with sensitivity onsets in this frequency range are used to measure dispersive shifts in the phonon caustics. The measured caustic positions are compared to those predicted by rigid-ion and bond-charge models. Similar to the case of InSb studied by Hebboul and Wolfe, a 6-parameter bond-charge model (BCM)-with force constants determined by neutron, X-ray, and Raman scattering-reproduces the phonon-imaging data both qualitatively and quantitatively. Comparisons of the focusing patterns with an 11-parameter rigid-ion model (RIM) do not show good agreement. New structures are predicted in the phononfocusing patterns at frequencies above about 1.2 THz — presently outside our experimental range-which are highly sensitive to the theoretical modeling.     

Characterization of Crystalline Phase‐Transformations in Theophylline by Time‐Domain Terahertz Spectroscopy

Time‐domain terahertz (THz) spectroscopy has been used to characterize polymorphic transformations in polycrystalline theophylline, a widely used pharmaceutical compound. On transformation, different intermolecular bonding arrangements arise owing to changes in the lattice structure of the molecular crystal, leading to distinct THz spectral signatures. Temperature‐dependent THz absorption measurements in anhydrous theophylline confirm that the observed vibrational modes originate from phonons within the crystal structure.     

Study of THz-wave-induced photoluminescence quenching in GaAs and CdTe

A novel model of ultrafast interaction between THz pulse and carriers is built to study the THz-wave-induced quenching of femtosecond-laser-excited photoluminescence in CdTe and GaAs. Photoluminescence quenching is due to the nonequilibrium intervalley phonons induced by the THz field and subsequent decrease of the recombination efficiency of the electron?Chole pairs. And the PLQ versus laser intensity experimental result agrees with the analysis.     

Coherent phonons, nanoseismology and THz radiation in InGaN/GaN heterostructures

The ultrafast optical photoexcitation of hot electrons and holes in semiconductors by femtosecond laser pulses can trigger coherent phonon oscillations. We discuss the huge coherent acoustic phonons which have been generated in InGaN/GaN heterostructures and epilayers and how they might be used in imaging of surfaces and interfaces in nanostructures. We also discuss the THz radiation emitted from these phonons.     

Low frequency lattice vibrations of LaF3 by neutron scattering

The phonon modes having frequencies less than 3 THz in the high symmetry directions of LaF₃ are reported. These are compared to the results of previous optical studies. A previously unobserved branch of low group velocity is found near 1.2 THz polarized both parallel and perpendicular to the basal plane. Its significance for the lifetimes of zone boundary acoustic phonons is discussed.     

Optical conductivity spectral anomalies in the off-center rattling system β-Ba8Ga16Sn30

We present optical conductivity studies of the type-I clathrate Ba8Ga16Sn30, using a terahertz time-domain spectrometer (0.3-3.0?THz). The lowest-lying spectral peak at 0.72?THz due to the Ba(2) ion's off-center vibration in the oversized cage shows a drastic and anomalous temperature dependence. Below about 100?K, the single broad peak splits into two subpeaks, and with further lowering of the temperature, the spectral shape of this so-called rattling phonon shows non-Boltzmann broadening to the point that the linewidth becomes comparable to the peak frequency. Whereas the initial splitting can be understood by assuming a multiwell anharmonic potential, the strong linewidth broadening toward low temperature cannot, since the Boltzmann factor generally sharpens the low-temperature spectra. The observed behavior suggests strong interaction between the local anharmonic phonons and other excitations.     

Phonon mediated photodetector

Quantum-wells and quantum dots and related semiconductor nanostructures have been widely investigated for infrared devices. Here we propose a new general approach to make use of polar optical phonons in quantum-wells for infrared (IR) and terahertz (THz) detection. As the first example, we show the coupling of phonon and intersubband transition leading to Fano resonance in photocurrent spectra. We investigate the phenomenon experimentally in specially designed GaAs/AlGaAs quantum-well infrared photodetectors. Finally, we discuss the future research and potentials.     

Terahertz-wave generation with periodically inverted gallium arsenide

We overview methods of THz-wave generation using frequency down-conversion in GaAs with periodically-inverted crystalline orientation. First, we compare different nonlinear-optical materials suitable for THz generation, analyze THz generation process in quasi-phase-matched crystals and consider theoretical limits of optical-to-THz conversion. Then, we review single-pass optical rectification experiments with femtosecond pump pulses, performed in periodically-inverted GaAs, where monochromatic THz output tunable in the range 0.9–3.0 THz was produced. Finally, we describe a novel approach to create a compact highly efficient tunable (0.5–3.5 THz) room temperature monochromatic THz source, based on the concept of intracavity THz generation via resonantly-enhanced difference frequency mixing. This approach allowed generating of 1 mW of average THz power, potentially scalable to 10–100 mW.     

Narrow-band terahertz wave generation and detection in one periodically poled lithium niobate crystal

In this article, we present studies on therahertz (THz) wave generation and frequency up-conversion in a periodically poled lithium niobate (PPLN) crystal. A frequency at 1.37 THz was generated as femtosecond pump pulses passed through a PPLN crystal with grating periods of 30 μm. The pump-induced THz wave interacts with the probe wave in the crystal by frequency mixing. The frequency up-converted THz wave is easily detected by a normal photodiode. A new scheme for generation and detection of THz wave in one non-linear crystal was proposed.     

PbB_4O_7晶体的太赫兹光谱和软光学声子

对实验测量的PbB4O7晶体样品的太赫兹(1012Hz)光谱、拉曼光谱以及红外—可见—紫外光谱进行了分析.在0.25—2.5THz波段介电函数随频率变化曲线ε(ν)出现共振型尖峰.四方面的分析表明PbB4O7晶体中存在软光学声子:1)介电函数随频率的变化曲线ε(ν)满足LST(Lyddane-Sachs-Teller)关系;2)在共振峰的频率附近(3.10THz)有很强的拉曼散射峰;3)吸收系数随频率的变化曲线α(ν)满足极化激元的特征;4)透过晶体的光子的色散关系ν(k)发生断开的畸变.PbB4O7晶体中存在软光学声子的意义在于,在满足产生极化激元的条件下,透过晶体的光子的频率会发生劈裂,分为升高和降低的两支,有可能利用这种原理来改变光子的频率.