Influence of the optical pulse length on the amplitude and phase of photoinduced coherent phonons

The theoretical dependence of the amplitude and initial phase of photoinduced coherent vibrations of the crystal lattice on the length of a rectangular excitation optical pulse has been derived. Comparison with the experiment for tellurium has been carried out.     

Investigation of coherent phonons in bismuth by femtosecond laser and X-ray pulse probing

Using femtosecond laser pulses, coordinated oscillations (coherent phonons) of Bi single-crystal atoms have been excited and recorded. The comparison with experimental results on the X-ray probing of coherent phonons at the same excitation energy density demonstrates that the observed lifetime and frequency shift of the oscillations are similar in both cases. Moreover, it has been revealed that the relaxation (incoherent) contributions are identical. This coincidence of the photoinduced response parameters indicates that probing in the visible spectrum correctly reflects the coherent dynamics of the Bi crystal lattice.     

Decay of photoinduced oscillations of the optical reflection coefficient of bismuth

A model describing the decay of photoinduced oscillations of the optical reflection coefficient R of bismuth is constructed, taking the crystal lattice anharmonicity into account. The decay time of oscillations of R is calculated as a function of the energy density of a laser pulse. The results of calculations explain the experimental data on the anomalously strong decay of oscillations of the optical reflection coefficient of bismuth (the decay time decreases by more than an order of magnitude with an increase in the laser pulse energy density from 0 to 4 mJ/cm²).     

Investigation of the dependence of the coherent dynamics of a bismuth lattice on the crystal excitation level

Fully symmetric coherent phonons in bismuth have been investigated in a wide range of pumppulse energies by the pump-probe method using femtosecond laser pulses. It has been shown that in the linear regime, which is implemented only for low pump intensities, the coherent amplitude is proportional to the pump intensity, whereas the relaxation rate of the coherent state and its frequency remain unchanged. In the nonlinear regime, which can be divided into superlinear and sublinear regions, the relaxation rate of a photoinduced lattice state can be approximated by a two-component response, where only one component depends strongly on the pump intensity. The nature of the coherence of the phonon subsystem, which is created by an ultrashort laser pulse, is discussed on the basis of the analysis of the data.     

Coherent phonons excited by two optical pulses

Theoretical dependences of the amplitude A and phase φ of photoinduced coherent oscillations of the crystal lattice on the delay time μ between two exciting optical pulses have been derived. It has been shown that φ(μ) is a periodic or decreasing function depending on the experimental conditions. Comparison with the experiment on Bi has been carried out.     

Transient response analysis of photoconductive detector under ultra-short laser pulse radiation

The transient response characteristics of HgCdTe photoconductive detector under the radiation of ultra-short laser pulse have been discussed in detail. Specifically, the transient effect of pulse width to the temperature of electronics and crystal lattice, and corresponding resistance changes of detector are mainly discussed. Based on traditional drift-diffusion model, considering that the temperature of electronics and crystal lattice are different under the ultra-short laser pulse, the double-temperature equation is joined to describe the semiconductor carriers’ dynamics features. Using the numerical method, the transient response characteristics of detector in the case of ultra-short pulse have been worked out. The calculation results show that: When the pulse width is greater than nanosecond pulse, the temperature of electronics will be equal to which of crystal lattice. If the pulse width is less than nanosecond pulse, the temperature of electronics is higher than which of the latter. After the end of a pulse, the rebound resistance of detector will be higher than the dark resistance because of the thermal effect. The heat effect is more obvious when a pulse with narrower width and higher energy density incident to the detector.     

Emission enhancement ratio of the metal irradiated by femtosecond double-pulse laser

A numerical solution of the two-temperature model has been performed up to the double-pulse femtosecond laser heated metal target. The two-temperature model is used to analyze the double-pulse laser with the following major conclusions. We confirm the distinctly different results on the single pulse and double pulse. The double-pulse laser heated lattice temperature is higher than the single pulse. Through the Boltzmann equation, we estimate the variation of the emission enhancement. At the same time, this experimental result is qualitatively similar to the theoretical result.     

On the nature of coherent phonons generated by ultrashort laser pulses in single-crystal antimony

Reflectivity oscillations generated by A_1g coherent phonons in an antimony single crystal have been studied by a method involving pumping and probing by femtosecond laser pulses, which was complemented by spectral filtration of the signal. An analysis of the spectrally resolved signal showed that not only the integrated intensity but also the spectrum of the probe pulse are functions of the delay time between the pumping and probing and oscillate between the Stokes and anti-Stokes components at the optical-phonon frequency. A comparison of the integrated lattice excitation relaxation dynamics with the spectrally resolved lattice excitation relaxation dynamics revealed new facets in the nature and generation mechanism of coherent phonons.     

Ultrafast semiconductor-metal phase transition in vanadium dioxide induced by a femtosecond laser pulse

A model is proposed for a photoinduced Peierls-type semiconductor-metal phase transition that makes it possible to determine the time dependence of the bandgap width in the electronic spectrum of vanadium dioxide subjected to a light field and the dependence of the time at which a photoinduced semiconductor-metal phase transition occurs on the laser pulse duration. The theoretical results obtained are consistent with experimental data on the illumination of a VO₂ film with an intense laser pulse.     

Damage threshold of lithium niobate crystal under single and multiple femtosecond laser pulses: theoretical and experimental study

The damage threshold of lithium niobate crystal under single and multiple femtosecond laser pulses has been studied theoretically and experimentally. Firstly, the model for the damage threshold prediction of crystal materials based on the improved rate equation has been proposed. Then, the experimental measure method of the damage threshold of crystal materials has been given in detail. On the basis, the variation of the damage threshold of lithium niobate crystal with the pulse duration has also been analyzed quantitatively. Finally, the damage threshold of lithium niobate crystal under multiple laser pulses has been measured and compared to the theoretical results. The results show that the transmittance of lithium niobate crystal is almost a constant when the laser pulse fluence is relative low, whereas it decreases linearly with the increase in the laser pulse fluence below the damage threshold. The damage threshold of lithium niobate crystal increases with the increase in the duration of the femtosecond laser pulse. And the damage threshold of lithium niobate crystal under multiple laser pulses is obviously lower than that irradiated by a single laser pulse. The theoretical data fall in good agreement with the experimental results.     

具有几个光振荡周期长度的飞秒激光脉冲在线性色散介质中的传输

给出了描写具有几个光振荡周期长度的飞秒激光脉冲在线性色散介质中传输方程的解。对脉冲的传输特性进行了数值摸拟 ,分别考察了来源于电子和晶格的正常和反常群速色散对脉冲展宽和脉冲形状畸变的影响。     

Effect of phonon spectrum heating on the formation of laser-induced electron plasma in wide-gap insulators

The effect of lattice heating by laser pulses on the dynamics of electron plasma generation in transparent solids has been theoretically studied. Several ways of taking into account the contribution of the phonon spectrum heating to the electron avalanche dynamics, depending on the type of the effective (with respect to the field energy transfer to electrons) phonons and laser pulse duration, have been proposed. A comparative analysis of the results of Monte Carlo computation of electron gas heating in the laser pulse field, which were obtained for cold and heated lattices, has been performed. It is shown that the consideration of the effect of lattice heating on the probabilities of electron-phonon and electron-phonon-photon scattering leads to an increase in the avalanche rate, which is more pronounced at longer wavelengths of the incident radiation and under longer laser pulses. Some qualitative features of the redistribution of the energy, absorbed during a pulse, between the electron plasma and lattice are revealed, which suggest initiation of irreversible microscopic changes in the insulator. In particular, the ratio R of the energy accumulated in the electron subsystem to the excess (with respect to the initial equilibrium state) energy in the phonon subsystem has been calculated for different initial lattice temperatures. It is shown that this ratio increases with a decrease in the laser wavelength in the computation scheme with lattice heating disregarded and decreases at all pulse durations when the lattice heating is taken into account.     

Capturing one-dimensional precursors of a photoinduced transformation in a material

Achieving control of photoinduced phase transitions requires understanding how materials work during transformation induced by a laser pulse. Here we investigate the precursors of a photoinduced phase transition in the highly cooperative charge-transfer molecular crystal tetrathiafulvalene-p-chloranil and provide key insights. The photogeneration of one-dimensional nanoscale clusters was detected by time-resolved diffuse x-ray scattering with 50-ps time resolution. Such clustering of structurally relaxed electronic excitations is expected to be a common process in many materials presenting photoinduced transformations.     

Second-harmonic generation from a KBe(2) BO(3)F(2) crystal in the deep ultraviolet

By use of KBe(2)BO(3)F(2) (KBBF) crystal with a size of 10 mmx10 mm x1.2 mm and a special prism-coupling technique (PCT), fourth-harmonic generation of Ti:sapphire laser systems from 200 to 179.4 nm has been achieved. Moreover, with a Ti:sapphire laser with a 50-fs pulse duration and a 1-kHz repetition rate, conversion efficiency as high as 13% from 400 to 200 nm without any surface-loss correction has also been obtained. The data show that with the PCT a KBBF crystal can produce deep-UV coherent light with measurable power output.     

Probing subcycle spectral structures and dynamics of high-order harmonic generation in crystals

Subcycle spectral structures and dynamics of high-order harmonic generation (HHG) processes of atoms and molecules driven by intense laser fields on the attosecond time scale have been originally studied theoretically and experimentally. However, the time scale of HHG dynamics in crystals is in the order of sub-femtosecond, and the carrier dynamics of HHG in crystals driven by subcycle laser pulses are largely unexplored. Here we perform a theoretical study of subcycle structures, spectra, and dynamics of HHG of crystals in mid-infrared laser fields subject to excitation by a subcycle laser pulse with a time delay. The HHG spectra as a function of time delay between two laser fields are calculated by using a single-band model for the intra-band carrier dynamics in crystal momentum space and by solving the time-dependent Schrödinger equation in velocity gauge for the treatment of multi-band crystal systems. The results exhibit a complex time-delay-dependent oscillatory pattern, and the enhancement and suppression of the HHG related to subcycle pulse are observed at the given time delay in either single-band or multi-band crystal systems. To understand oscillation structures with respect to the dependence for the subcycle laser fields, the time-frequency characteristics of the HHG as well as the probability density distribution of the radiation are analyzed in detail.     

Photoinduced spin-Peierls phase transition

An equation is obtained for the order parameter ξ of the spin-Peierls phase transition in a light field. This equation is used to derive the expressions for the frequency ν of the photogenerated longitudinal optical phonon mode and the time τ of the photoinduced phase transition. Numerical values of the quantities ν and τ calculated in terms of the proposed model agree well with the experimental data for the quasi-one-dimensional compound potassium tetracyanoquinodimethane (K TCNQ) irradiated by a laser pulse. Original Russian Text ? A.L. Semenov, 2009, published in Fizika Tverdogo Tela, 2009, Vol. 51, No. 1, pp. 164–167.     

Investigation of ultrafast processes in photoexcited bismuth by broadband probing in the wavelength range 0.4–0.9 μm

The decay of the photoexcited state of a bismuth single crystal is investigated in the wavelength range from 400 to 900 nm by means of femtosecond laser reflection spectroscopy. Oscillations produced by coherent fully symmetric A _1g phonons have been detected in the photoinduced response, along with a relaxation component. The dynamics of the electronic subsystem of the crystal is shown to be characterized by three values of the decay time: 1 ps, 7 ps, and ∼1 ns. The spectral dependence of the reflectivity oscillation amplitude has been measured; the possible cause of the shape of the derived curve is described.     

Molecular-dynamics calculation of the thermal conductivity coefficient of the germanium single crystal

The thermal conductivity coefficient of the germanium crystal lattice has been calculated by molecular dynamics simulation. Calculations have been performed for both the perfect crystal lattice and the crystal lattice with defects such as monovacancies. For the perfect germanium single crystal, the dependence of the thermal conductivity coefficient on the lattice temperature has been obtained in the temperature range of 150–1000 K. The thermal conductivity coefficient of the germanium lattice has been calculated as a function of the monovacancy concentration.     

Structural preablation dynamics of graphite observed by ultrafast electron crystallography

By means of time-resolved electron crystallography, we report direct observation of the structural dynamics of graphite, providing new insights into the processes involving coherent lattice motions and ultrafast graphene ablation. When graphite is excited by an ultrashort laser pulse, the excited carriers reach their equilibrium in less then one picosecond by transferring heat to a subset of strongly coupled optical phonons. The time-resolved diffraction data show that on such a time scale the crystal undergoes a contraction whose velocity depends on the excitation fluence. The contraction is followed by a large expansion which, at sufficiently high fluence, leads to the ablation of entire graphene layers, as recently predicted theoretically.     

短脉冲激光加工双温方程的优化运算

为研究双温方程中电子热传导项和电子与晶格耦合项对激光辐照物体表面温度场求解的影响,对这两项施加了约束条件。由于飞秒和亚皮秒激光与物质相互作用时间短,电子与晶格来不及耦合,所以对耦合项施加时间约束;根据相分离条件(CPPS),对热传导项施加空间约束。利用有限元方法建立了激光烧蚀金属铜膜表面的有限元模型。通过分析双温方程中热传导项和耦合项对计算结果的影响,发现短脉冲激光与铜金属相互作用过程中电子与晶格耦合项可以忽略,而传导项不可忽略。求解适当激光功率下的双温方程,得到了激光作用中心电子与晶格在不同脉冲宽度激光辐照下的温度变化关系。根据100 fs激光作用后晶格温度场的空间分布情况,研究了激光作用的相分离区域、相爆炸区域以及熔融区域的分布情况。