We present a mechanism by which optically driven chiral phonon modes in rare-earth trihalides generate giant effective magnetic fields acting on the paramagnetic $4f$ spins. With cerium trichloride (CeCl$_3$) as our example system, we calculate the coherent phonon dynamics in response to the excitation by an ultrashort terahertz pulse using a combination of phenomenological modeling and first-principles calculations. We find that effective magnetic fields of over 100 tesla can possibly be generated that polarize the spins for experimentally accessible pulse energies. The direction of induced magnetization can be reversed by changing the handedness of circular polarization of the laser pulse. The underlying process is a phonon analog of the inverse Faraday effect in optics that has been described recently, and which enables novel ways of achieving control over and switching of magnetic order at terahertz frequencies.
Paramagnetic defects in diamond and hexagonal boron nitride possess a unique combination of spin and optical properties that make them prototypical solid-state qubits. Despite the coherence of these spin qubits being critically limited by spin-phonon relaxation, a full understanding of this process is not yet available. Here we apply ab initio spin dynamics simulations to this problem and quantitatively reproduce the experimental temperature dependence of spin relaxation time and spin coherence time. We demonstrate that low-frequency two-phonon modulations of the zero-field splitting are respo…
Reversable phase transitions in ferroic two-dimensional Nb2O2I4 through optically excited coherent phonons
School of Physics, Southeast University（东南大学物理学院）；Key Laboratory of Quantum Materials and Devices of Ministry of Education, Southeast University（东南大学量子材料与器件教育部重点实验室）；Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所北京凝聚态物理国家研究中心）；Songshan Lake Materials Laboratory（松山湖材料实验室）
Electron-phonon interaction during optically induced ultrafast magnetization dynamics of Au/GdFeCo bilayers
光加热后GdFeCo电子的温度演化在GdFeCo的全光开关中起着关键作用，并且主要由电子和声子之间的耦合强度决定。通常，金属中的电子-声子耦合的强度是通过监测光加热后反射率的变化，然后用一个简单的双温度热模型分析瞬态反射率来推导的。在磁性金属中，不能假设反射率的变化仅取决于电子和声子温度，因为金属的反射率也取决于磁化强度。为了推导GdFeCo中的电子-声子耦合常数，我们分析了GdFeCo电子在光加热后Au和GdFeCo双层膜中的热输运。我们利用Au层的反射率来监测Au声子的温度演化。通过用热模型解释双层膜对加热的响应，我们确定GdFeCo中的电子-声子耦合常数为6 x 10^17 W/（m^3-K），对应于GdFeCo中的电子-声子弛豫时间约为150 fs。
Use of optically detected magnetic resonance to correlate germanium electron centers with UV absorption bands in X-ray irradiated germanosilicate glasses
Optically addressable silicon vacancy-related spin centers in rhombic silicon carbide with high breakdown characteristics and ENDOR evidence of their structure
Paramagnetic point defects in solids may exhibit a rich set of interesting and not yet fully resolved physics. In particular, character of wavefunctions and electron-phonon coupling in these defects may highly influence their interaction with external magnetic fields. Complex interplay between the electronic orbitals, phonons and electron spin determines the effective pseudospin of the system that we demonstrate on vanadium and molybdenum defects in hexagonal silicon carbide (SiC) by means of \textit{ab initio} calculations. In this Rapid Communication, we find a giant anisotropy in the $g$-te…
In this study, we use the transient thermal grating optical technique \textemdash a non-contact, laser-based thermal metrology technique with intrinsically high accuracy \textemdash to investigate room-temperature phonon-mediated thermal transport in two nanoporous holey silicon membranes with limiting dimensions of 100 nm and 250 nm respectively. We compare the experimental results to ab initio calculations of phonon-mediated thermal transport according to the phonon Boltzmann transport equation (BTE) using two different computational techniques. We find that the calculations conducted within…
Kagome-net, appearing in areas of fundamental physics, materials, photonic and cold-atom systems, hosts frustrated fermionic and bosonic excitations. However, it is extremely rare to find a system to study both fermionic and bosonic modes to gain insights into their many-body interplay. Here we use state-of-the-art scanning tunneling microscopy and spectroscopy to discover unusual electronic coupling to flat-band phonons in a layered kagome paramagnet. Our results reveal the kagome structure with unprecedented atomic resolution and observe the striking bosonic mode interacting with dispersive …
The coupling between phonon and magnon is ubiquitous in magnetic materials and plays a crucial role in many aspects of magnetic properties, most notably in spintronics. Yet, this academically and technologically interesting problem still poses a severe challenge to a general understanding of the issue in certain materials. We report that Ni3TeO6 exhibits clear evidence of significant magnon-phonon coupling in both longitudinal thermal conductivity ($κ_{xx}$) and thermal Hall coefficient ($κ_{xy}$). The Debye-Callaway model, a phenomenological description for phonon heat conduction, can explain…
Using femtosecond time-resolved X-ray diffraction, we investigated optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches our simulations. We observed an asymmetry in the spectral lineshape of the longitudinal mode that is notably absent from the shear mode, suggesting a time-dependent frequency chirp that is likely driven by photoinduced carrier diffusion. We argue on the basis of symmetry that these acou…
Lattice vibration in solids may carry angular momentum. But unlike the intrinsic spin of electrons, the lattice vibration is rarely rotational. To induce angular momentum, one needs to find a material that can accommodate a twisted normal mode, two orthogonal modes or excitation of magnons. If excitation is too strong, one may exceed the Lindemann limit, so the material melts. Therefore these methods are not ideal. Here, we theoretically propose a new route to phonon angular momentum in a molecular crystal $\rm C_{60}$. We find that a single laser pulse is able to inject a significant amount o…
We provide a microscopic approach to describe the onset of radial oscillation of a silver nanoparticle. Using the Heisenberg equation of motion framework, we find that the coupled ultrafast dynamics of coherently excited electron occupation and the coherent phonon amplitude initiate periodic size oscillations of the nanoparticle. Compared to the established interpretation of experiments, our results show a more direct coupling mechanism between the field intensity and coherent phonons. This interaction triggers a size oscillation via an optically induced electron density gradient occurring dir…
Triplet excited states in organic semiconductor materials and devices are notoriously difficult to detect and study with established spectroscopic methods. Yet, they are a crucial intermediate step in next-generation organic light emitting diodes (OLED) that employ thermally activated delayed fluorescence (TADF) to upconvert non-emissive triplets to emissive singlet states. In organic photovoltaic (OPV) devices, however, triplets are an efficiency-limiting exciton loss channel and are also involved in device degradation. Here, we introduce an innovative spin-sensitive method to study triplet s…
We investigate the effect of local electron-phonon coupling on nonlinear optical conductivity in an interacting ferroelectric system. Using real-time simulations, we show an enhancement in nonlinear conductivity under linearly-polarized light due to generation of the phonon-assisted ballistic-current in addition to the injection-current generated by electron-hole pairs. The optically excited phonon modes generate an asymmetric carrier distribution that causes a strong directional ballistic-current. The ballistic-current enhances the photocurrent several times at above band-gap excitation frequ…
Magnetic circular dichroism of THz modes and selection rules of Raman-active optical phonons in the polar altermagnet candidate \ce{Mn2Mo3O8}
University of Augsburg（奥格斯堡大学）；Kazan (Volga region) Federal University（喀山（伏尔加沿岸）联邦大学）；Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）；Budapest University of Technology and Economics（布达佩斯技术与经济大学）；HUN-REN Wigner Research Centre for Physics（匈牙利研究与教育网络维格纳物理研究中心）
High-frequency pulse electron paramagnetic resonance (EPR) and electron nuclear double resonance (ENDOR) were used to clarify the electronic structure of the color centers with an optically induced high-temperature spin-3/2 alignment in hexagonal 4H-, 6H- and rhombic 15R- silicon carbide (SiC) polytypes. The identification is based on resolved ligand hyperfine interactions with carbon and silicon nearest, next nearest and the more distant neighbors and on the determination of the spin state. The ground state and the excited state were demonstrated to have spin S = 3/2. The microscopic model su…
