Two-phonon bound states in imperfect crystals

The question of the occurrence of two-phonon bound states in imperfect crystals is investigated. It is shown that the anharmonicity mediated two-phonon bound state which is present in perfect crystals gets modified due to the presence of impurities. Moreover, the possibility of the occurrence of a purely impurity mediated two-phonon bound state is demonstrated. The bound state frequencies are calculated using the simple Einstein oscillator model for the host phonons. The two-phonon density of states for the imperfect crystal thus obtained has peaks at the combination and difference frequencies of two host phonons besides the peaks at the bound state frequencies. For a perfect crystal the theory predicts a single peak at the two-phonon bound state frequency in conformity with experimental observations and other theoretical calculations. Experimental data on the two-phonon infrared absorption and Raman scattering from mixed crystals of GA_1−c Al _c P and Ge_1−c Si _c are analysed to provide evidence in support of impurity-mediated two-phonon bound states. The relevance of the zero frequency (difference spectrum) peak to the central peak observed in structural phase transitions, is conjectured; This work is a part of the thesis to be submitted by one of the authors (SS) in partial fulfilment of the degree of Doctor of Philosophy to Utkal University, Bhubaneswar, India.     

Squeezed polarons in one dimension

Starting from a simple one-dimensional model for many-electron and phonon interacting systems we have shown that in order to arrive at a stable minimum of the total energy the ordinary polaronic state must be replaced by the squeezed polaronic state in which the phonon subsystem is in the two-phonon coherent state.     

Resonances of two phonons from different dispersion branches

The study of two-phonon resonances is extended to include resonances of two phonons from different branches of the dispersion curve. The condition for forming a resonance as a sharp peak in the two-phonon spectrum is derived. When the ‘effective masses” of the two phonons are nearly equal in magnitude, but opposite in sign, a resonance can be created by a relatively small value of the anharmonic coupling.     

Resonance Raman scattering of excitonic polaritons by LO and acoustic phonons in ZnTe

We have observed dispersive two-phonon Raman scattering of polaritons by LO and acoustic phonons near the lowest exciton state of ZnTe. From the Stokes shifts of these Raman lines, it has been found that the scattering process switches from an acoustic phonon followed by one LO phonon to the reversed one: a LO phonon followed by an acoustic one.     

Selective resonant enhancement in the two-phonon Raman spectrum of Si and GaP

Resonant enhancement of selective pairs of phonons has been observed by noting the changes in the lineshape of the two-phonon Raman spectrum from Si and GaP as the incident photon energy is made resonant with the indirect energy gap. These selective phonons have the same k as those that are involved in the phonon-assisted optical transition.     

Optical properties of excimers in the field of intense laser radiation

The specific features of the luminescence of excimer molecules are analyzed within the model of a purely repulsive potential for the ground state in the field of intense laser radiation with due regard for the squeezed vibrational states. It is demonstrated that the luminescence band with the inclusion of the equilibrium phonons can be represented by a broad structureless asymmetric bell-shaped curve. The squeezed vibrational states substantially affect the frequency dependence of the luminescence intensity; more specifically, the luminescence band exhibits two maxima in the case of strong electron-phonon coupling. The stabilization of an excited electronic state in the course of luminescence at the fundamental frequency and generation of higher optical harmonics in the field of intense laser radiation is discussed.     

Fermi resonance of optical one-phonon and acoustic two-phonon vibrations in light metals

It is shown that the anharmonicity of crystal lattice vibrations in light metals such as beryllium, can give rise to a Fermi resonance of optical one-phonon and acoustic two-phonon vibrations. New hybridized vibrational states are formed as a result of such a resonance interaction: biphonon and quasibiphonon vibrations and renormalized optical vibrations. Depending on the wave vector, these vibrational states can be both damped and stationary. The corresponding dispersion equation is obtained, whose solution made it possible to determine the spectrum of these vibrations (dispersion curves and the wave vector dependence of the damping for damped vibrations). It is shown that ultrafast damping of optical vibrations, similar to the well-known superradiance effect for Frenkel’ and Wannier-Mott excitons, is possible. Fiz. Tverd. Tela (St. Petersburg) 39, 542–546 (March 1997)     

Remarks on the theory of electron capture into shallow donors in GaAs

A new model for low-temperature recombination of conduction electrons to ionized donors in GaAs is proposed. It assumes that the conduction electron is captured into the ground state of shallow impurity by simultaneous emission of two LA phonons. From a comparison of computed capture rate with recent experimental results the estimated value of the two-phonon deformation potential is d_2LA = 0.02 eV.     

First and second order Raman scattering in GaP to 128 kbar

One- and two-phonon room temperature Raman spectra of GaP were measured to 128 kbar using a diamond-anvil pressure cell. Linear and quadratic pressure coefficients were determined for phonons at Γ, L, (X→K), and Σ. The results suggest possible “soft” mode behavior for TA(L) and TA(X→K) phonons.     

Resonant Raman scattering at the indirect exciton in silver bromide

By excitation in the indirect exciton absorption of AgBr at low temperatures selectively enhanced two-phonon Raman scattering is observed. Using different excitation wavelengths the resonance enhancement is found to be associated with the Г-L exciton as intermediate state for the resonant scattering process. The resonant phonons involved are pairs of LA and TA phonons with opposite wave vectors near L. Measurements in the temperature range 2 K ? T ? 40 K show a decrease of the scattering intensity with increasing temperature. The origin of this temperature dependence is due to lifetime broadening of the scattering state. Several features of the indirect exciton absorption of AgBr are discussed.     

Resonant multiphonon Raman scattering in AgBr

Resonant Raman scattering in AgBr single crystals is studied at low temperatures. Excitation in resonance with the indirectΓ — L exciton as intermediate state gives rise to selectively enhanced narrow two-phonon Raman scattering. The phonons involved are pairs ofLA andTO phonons of opposite wavevectors near theL-point. A simple model involving one discrete exciton level is developed to explain the resonance behaviour. The temperature dependence of the scattered intensity, that is studied for 1.8 K <T < 35 K, can consistently be interpreted within this model as being due to the lifetime of the intermediate state. Assuming that the excitons predominantly decay by one-phonon scattering with long wavelength acoustical phonons the predicted temperature dependence of the intensity is found in good agreement with the experimental result. Additional scattering peaks are believed to be due to third-order processes involving an acousticalX-phonon in addition to theL-phonons of the second-order scattering. Using an oriented sample the resonant Raman peaks are found to be polarized.     

一维分子晶体系统的极化子-孤子压缩态、系统基态性质和量子涨落

基于一维分子晶体系统的 Holstein 模型,采用压缩-相干态展开方法,计及电子-声子间量子关联和重整化平移修正,分析和研究电子-双声子相互作用对极化子-孤子系统基态性质和量子涨落的影响.推导了一维极化子-孤子系统的封闭形式非线性方程.应用非线性项展开方法,给出非线性方程的解析解和相关基态特性结果.研究表明,仅当电子-双声子耦合强度 g₁<0时非线性方程才有孤波解,此时声子量子涨落效应随着压缩的增加,极化子-孤子系统基态能量变得更负,孤子局域减少,孤子态更加稳定;另一方面,电子密度涨落〈Δ²n〉和声子坐标-动量的不确定量〈Δ²p〉〈Δ²q〉比无声子压缩效应的大,极化子结合能变得更负.特别是,当g₁<0时,双声子效应的量子涨落〈Δ²n〉与〈Δ²p〉〈Δ²q〉的值比单声子情况有明显增加. 关键词： 压缩-相干态展开 极化子-孤子态与量子涨落 电子-双声子相互作用 非线性薛定谔方程     

Feshbach-Villars perturbation theory for pionic atom problems

It is shown that the commutation relations between the quasiparticles forming phonons can correctly be taken into account within the quasiparticle-phonon nuclear model. The doubly-even deformed nuclei with the isoscalar and isovector multipole-multipole forces are studied. The exact and approximate secular equations are derived. It is shown that the two-phonon poles in the secular equation are shifted due to the Pauli principle. These shifts are large for the two identical collective phonons. In some cases pronounced shifts are found for the poles composed of a low-lying collective phonon and a collective phonon forming the giant resonance. In other cases the shifts are not large, as a rule.     

Correlated squeezed-state approach for the ground state of strongly correlated electrons coupled to local Holstein phonons

Summary In the present work we have applied the correlated squeezed-state approach to investigate the ground state of the extended Hubbard model which is coupled to local Holstein phonons. Our study begins with decoupling the electron and phonon subsystems approximately by introducing a variational correlated squeezed-state ansatz for the phonons. Then assuming the renormalized intersite electron correlation of the effective electronic Hamiltonian to be attractive and the renormalized on-site correlation repulsive, we have applied the generalized Hartree-Fock approximation to obtain the ground state of the system, which is a superconducting state with intersite pairing. With optimal values of the variational parameters the correlated squeezed-state approach will by construction yield a ground-state energy lower than those obtained in previous studies. This means that our variational ansatz is more stable as the ground state of the system. Furthermore, our variational study shows that in the correlated squeezed state the polaronic reduction effect of phonons is much more alleviated, and thus the mass enhancement inherent to the polaron effect is noticeably weakened. This weakening of the reduction effect should, in turn, significantly affect other physical properties of the system.     

双能态自旋-晶格声子耦合量子隧道系统的非经典能态和量子相干耗散

采用关联表象变分波函数方案, 介入三个非经典关联效应, 求解有限温度双能态自旋-晶格声子耦合量子隧道系统的非经典态, 着重研究化解由于粒子自旋-单声子相互作用引起的量子涨落导致双能态系统的退相干性量子耗散. 这三个非经典关联效应是: 1) 声子位移-粒子自旋 (σ_z)间强非绝热关联; 2) 声子压缩态效应及其伴随发生的单声子相干态-声子压缩态两过程相干效应; 3) 由关联表象导致的声子位移(U_D)与声子压缩(U_S)的表象关联非绝热修正. 结果表明: 由于引入粒子自旋-双声子相互作用, 大幅度地增强了声子场压缩态, 特别是更进一步极大幅度地增强了非经典压缩-相干态效应. 因此, 由粒子自旋-单声子相互作用产生的Debye-Walle相干弹性散射效应导致量子隧道项(-Δ₀σ_x)的强烈指数衰减及其伴随严重的量子相干损失的极大幅度的抑制, 并且自旋-晶格声子耦合量子隧道系统的非经典态能量大幅度降低. 关键词： 非经典能态 量子隧穿相干损失 自旋-双声子相互作用 压缩相干态效应     

Coherent longitudinal-optical ground-state phonon in CdSe quantum dots triggered by ultrafast charge migration

We observe the CdSe longitudinal-optical ground-state phonon in the electron transfer system composed of CdSe quantum dots and methylviologen directly by femtosecond absorption spectroscopy. A significant phase shift indicates that the coherent oscillations are triggered by an ultrafast charge migration, which is the consequence of an electron transfer from the photoexcited quantum dot to the molecular acceptor methylviologen. In contrast, the observed coherent phonons in isolated quantum dots stem from the frequency modulation of the quantum dot excited-state spectrum. From the probe wavelength dependence of the longitudinal-optical phonons in the electronic ground state and excited state it is possible to determine a biexciton binding energy of 35?meV.     

Dispersive phonon linewidths: the E2 phonons of ZnO

Phonon linewidths can exhibit a large variation when either pressure or isotopic masses are changed. These effects yield detailed information about the mechanisms responsible for linewidths and lifetimes, e.g., anharmonicity or isotopic disorder. We report Raman measurements of the linewidth of the upper E2 phonons of ZnO crystals with several isotopic compositions and their dependence on pressure. Changes by a factor of 12 are observed at a given temperature. Comparison with calculated densities of one-phonon states, responsible for isotope scattering, and of two-phonon states, responsible for anharmonic decay, yields a consistent picture of these phenomena. Isotopic disorder broadening by 7 cm(-1) is found in samples with mixed 16O-18O content, whereas the anharmonic processes involve decay into sums and differences of two phonons.     

Two-phonon absorption in InP and GaP

Far-infrared absorption in crystals of GaP and InP was investigated using a high-resolution Fourier-transform spectrometer. The two-phonon absorption was found to be very similar in these two materials. Van Hove singularities on the GaP spectrum were identified with the aid of calculated two-phonon sum and overtone density-of-states curves. The analysis of the InP spectrum was based on its homology to GaP. Many of the prominent features of the absorption spectra are assigned to pairs of phonons on the hexagonal face of the Brillouin zone while phonon pairs at Γ, X and L generally contribute only minor features to the spectra.     

Ultrafast acoustics in the middle UV range: coherent phonons at higher frequencies and in smaller objects

We show that the propagation of coherent acoustic phonons generated by femtosecond optical excitation can be clearly resolved using a probe laser in the middle UV (MUV) range. The MUV probe is easily produced from a high-repetition-rate femtosecond laser and a homemade frequency tripler. We present various experimental results that demonstrate efficient and high frequency detection of acoustic phonons. Thus, we show that the MUV range offers a unique way to reach higher frequencies and probe smaller objects in ultrafast acoustics.     

Picosecond spectroscopy of polaritons in anthracene crystals II. Luminescence

The low-temperature luminescence spectrum of anthracene crystals is investigated by applying simultaneous time and frequency resolution. The complicated kinetics of the emission in the polariton bottleneck region reflects directly the evolution and relaxation of the polariton distribution in the crystal. Three distinct relaxation stages are distinguished: (1) the ultrafast decay of initial vibronic excitations, mediated by optical phonons and resulting in a broad distribution of polaritons near the band bottom; (2) the formation of a narrow distribution of polaritons with a characteristic time of 30 ps, which is caused by scattering on acoustic phonons; (3) relaxation through the bottleneck region on a subnanosecond time scale. It is suggested that the polaritons immediately below the resonance frequency are responsible for the observed excitonic energy transfer in anthracene crystals.