Coherent control theory and experiment of optical phonons in diamond

Abstract

The coherent control of optical phonons has been experimentally demonstrated in various physical systems. While the transient dynamics for optical phonons can be explained by phenomenological models, the coherent control experiment cannot be explained due to the quantum interference. Here, we theoretically propose the generation and detection processes of the optical phonons and experimentally confirm our theoretical model using the diamond optical phonon by the doublepump-probe type experiment.

Coherent control of 40-THz optical phonons in diamond using femtosecond optical pulses

“…Figure 3 is a two-dimensional map of the transient transmittance change ∆T /T 0 as a function of the pump1probe delay (t: horizontal axis) and pump1-pump2 delay (τ : vertical axis). At the fixed pump1-pump2 delay (τ ), ∆T /T 0 shows the sharp peak at delay zero between pump and probe and the successive oscillation with a frequency of 39.9±0.05 THz, which have been reported in a previous paper 20 . The oscillation is assigned to the opti- cal phonons in diamond.…”

“…Recently, a theory of the coherent control of optical phonons by double-pulse excitation had been developed base on the simple quantum mechanical model with two-electronic bands and shifted harmonic oscillators 18,19 . We demonstrated the coherent control experiment on the optical phonons in a single crystal of diamond and analyzed the data by using the developed theory 20 .…”

“…The coherent optical phonons in diamond have been studied using femtosecond optical pulses and its generation mechanism has also been discussed with quantum mechanical calculations. 19,20,[25][26][27][28] We have demonstrated the coherent control of amplitude and phase of the coherent optical-phonon oscillation in diamond using a pair of sub-10-fs infrared pulses at delays between 230 and 270 fs, in which two pump pulses were well separated 20 . The observed behavior of the amplitude and phase were well reproduced by the developed theory.…”

Time-resolved multimode heterodyne detection for dissecting coherent states of matter

“…The measurement of the Raman response in P&P experiments relies on the fact that impulsive photo-excitation (i.e. the interaction with light pulses on a timescale shorter than the period of the excitation in the material) triggers coherent nonequilibrium states of low energy excitations, such as phonons [1,2], magnons [3], or electronic excitations [4,5,6], whose time evolution can be subsequently characterized by the ultrashort probe pulse. ISRS has been historically introduced and discussed treating both the coherent vibrational state in matter, which is often dubbed coherent phonon, and the interacting electric field with a classical formalism [7,8,9].…”

Multiscale time-dependent density functional theory for a unified description of ultrafast dynamics: Pulsed light, electron, and lattice motions in crystalline solids

“…Nowadays, measurements are carried out quite often in time domain using pump-probe technique as a typical method and the time resolution reaches a few tens of attosecond [6,7]. Extremely nonlinear phenomena has attracted interests such as high harmonic generation in solids [8,9], ultrafast control of electrons motion in dielectrics that aims for future signal processing using pulsed light [10][11][12], and ultrafast coherent optical phonon control [13][14][15][16][17][18][19][20][21][22] and photoinduced structural phase transition of materials [23][24][25][26].In this paper, we report a progress to develop firstprinciples computational method to describe nonlinear optical processes in solids that arise from coupled dynamics of light electromagnetic fields, electrons, and atoms in crystalline solids. In condensed matter physics and materials sciences, first-principles computational approaches represented by density functional theory have been widely used and recognized as an indispensable tool [27].…”