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arXiv:1712.07337 · Scientific Reports

Coherent control theory and experiment of optical phonons in diamond

Hiroya Sasaki, Riho Tanaka, Yasuaki Okano, Fujio Minami, Yosuke Kayanuma, Yutaka Shikano, Kazutaka G. Nakamura

Published Jun 19, 2018• 28 citations
arXivHTMLPDF

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.

DOI
10.1038/s41598-018-27734-1

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Quantum Electronics and Laser Science Conference•Jan 20, 2003•0 citations
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.
A theory of the coherent control of optical phonons by double-pulse excitation was modified for the calculation of a large detuning case such as diamond; we calculated the amplitude of the optical phonons without using a rotating-wave approximation. Additionally, we took the frequency chirping and non-Gaussian pulse shape into consideration. The coherent control of the amplitude of 40 THz optical phonons in diamond was demonstrated by using a pair of infrared pulses at a pump-pump delay between $\ensuremath{-}10$ and 120 fs, and analyzed by using the modified theory.
The nitrogen-vacancy (NV) center in diamond has emerged as a versatile atom-like system, finding diverse applications at both ambient and cryogenic temperatures. At room temperature, the NV center's spin-triplet electronic ground state has a long coherence time and can be read out and initialized using nonresonant optical excitation, which has enabled a wide range of metrology and quantum information applications. At cryogenic temperatures, the NV center exhibits a variety of narrow, atom-like optical transitions, which has made the NV center a promising platform for quantum optics applications. We use coherent optical manipulation of the NV center at cryogenic temperatures to probe its internal dynamics and aspects of its interactions with its environment.\nFirst, we investigate the intersystem crossing (ISC) process, which is a spin-dependent nonradiative decay mechanism that enables the electronic spin state to be optically initialized and read out at room temperature. We measure the ISC rates from different excited states as well as the rate at which interactions with phonons redistribute population between these states. Based on these measurements, we develop a theoretical model that unifies the phonon-induced mixing and ISC mechanisms. We find that our model is in excellent agreement with experiment and that it can be used to predict unknown elements of the NV center's electronic structure.\nSecond, we investigate a novel method of using coherent optical manipulation of the NV center's electronic spin to control a nearby nuclear spin. Coherent interactions between the NV center and nearby nuclear spins have enabled the development of NV center-based, multi-qubit quantum registers, but these techniques have generally required the application of microwave or radio-frequency radiation. We demonstrate control of the nuclear spin using an all-optical Raman technique and theoretically evaluate the extent to which the intrinsic physics of the NV center limits the coherence of this Raman-based manipulation technique.
Detecting coherent phonons pose different challenges compared to coherent photons due to the much stronger interaction between phonons and matter.This is especially true for high frequency heat carrying phonons, which are intrinsic lattice vibrations experiencing many decoherence events with the environment, and are thus generally assumed to be incoherent.Two photon interference techniques, especially coherent population trapping (CPT) and electromagnetically induced transparency (EIT), have led to extremely sensitive detection, spectroscopy and metrology.Here, we propose the use of two photon interference in a three-level system to sense coherent phonons.Unlike prior works which have treated phonon coupling as damping, we account for coherent phonon coupling using a full quantum-mechanical treatment.We observe strong asymmetry in absorption spectrum in CPT and negative dispersion in EIT susceptibility in the presence of coherent phonon coupling which cannot be accounted for if only pure phonon damping is considered.Our proposal has application in sensing heat carrying coherent phonons effects and understanding coherent bosonic multi-pathway interference effects in three coupled oscillator systems.Phonons are packets of vibrational energy that shares many similarities with its bosonic cousin photons.Advances in nanofabrication has enabled many parallels between the development of photon and phonon control.Parallel developments in passive control techniques include photonic [1] versus phonoic crystals [2], optical [3] versus acoustic metamaterials [4] etc. Development in active manipulation of electromagnetic waves through light-matter interaction have led to creation of nanoscale optical emitters [5] and gates [6] and similar progress have been made in controlling phonons using their interaction with matter especially in the realms of optomechanics [7] and phononic devices [8,9].Phonons span a vast frequency range and while techniques to control and sense lower frequency coherent phonons have been well-developed [10-19], heat carrying coherent terahertz acoustic phonons have been harder to measure directly due to the small wavelength and numerous scattering mechanism at these small wavelengths [20].In the past, THz crystal phonons have been generated and detected in low temperature experiments with defect doped crystals [21-24], with experimental evidence of coherent phonon generation [25][26][27].At the same time, interpretation of non-equilibrium phonon transport, with the advancement of nanoscale electrical heating and ultrafast optical pump-probe techniques, have allowed us to infer phonon coherence from broadband thermal conductivity measurements [28][29][30][31][32].There have been also interest of using defect-based techniques as a thermal probe using perturbation to energy levels due to changes in temperature [33].Furthermore, surface deflection techniques with ultrafast optics have also been used to generate phonons close to THz frequencies in materials [34][35][36][37].Defect-based techniques are attractive compared to both thermal conductivity measurement and deflection techniques due to its ability to directly access atomic length scales where THz phonon wavelength resides.Also, the energy levels in the excited state [21,38,39] and ground state [25,40] electron manifold of these defects can match the phonon energy precisely, resulting in a narrow band phonon detector.In light of the success of defect-based optical absorption techniques in coupling directly to high frequency phonons, we propose the use of two photon interference to measure the coherence properties of these phonons.
Summary form only given. The coherence decay of optically excited electronic systems provides one of the most powerful tools to investigate interaction processes of excited states. In semiconductors, the optical coherence phenomena are usually investigated by nonlinear techniques such as four wave mixing (FWM), photon echo, or reflectivity experiments. Exciton-phonon, exciton-exciton, or exciton-free carriers scattering processes have been explored in recent years with these techniques. As demonstrated recently, a direct measurement of the optical dephasing time can be obtained through the temporal coherent control of electronic excitations. In these experiments, the emission following the excitation by an ultrashort optical pulse sequence, is detected in a non-specular direction (secondary emission). This provides an alternative approach to FWM techniques, which allows us to analyse the scattering processes either with phonons or due to mutual collisions. Using the coherent control technique monitored through the secondary emission (SE), we report on the coherent dynamics of excitons in bare quantum wells (QW) and compare it to that of exciton-polaritons in microcavity (MC) embedded quantum wells.