Photoinduced Spin Dynamics Research Articles

Photoexcitation induced magnetic phase transition and spin dynamics in antiferromagnetic MnPS3 monolayer

Antiferromagnetic spin dynamics is the key issue to develop spintronic devices. We adopt ab initio nonadiabatic molecular dynamics with spin–orbit-coupling (SOC) to investigate photoinduced spin dynamics in an antiferromagnetic semiconductor MnPS3 monolayer. Optical doping triggers MnPS3 from Néel antiferromagnetic to ferromagnetic phase at an experimentally achievable electron–hole pair density of 1.11 × 1014 cm−2. This phase transition can be ascribed to the light-induced mid-gap states of S-p orbitals, which lower the electron excitation energy and strengthen the SOC effect between S-p and Mn-d orbitals. The excited S-p electrons first decay to the mid-gap states due to p–p electron–phonon-coupling and then relax to the spin-down Mn-d orbitals via SOC. Such a dramatic relaxation process prolongs the photogenerated carrier lifetime up to 648 fs, providing an explanation for the unusual optoelectronic performance of MnPS3. The reversible switching of magnetic order via optical means gives an important clue for information storage and highly efficient photocatalysts utilizing antiferromagnetic semiconductors.

Nonlinear subswitching regime of magnetization dynamics in photomagnetic garnets

We analyze, both experimentally and numerically, the nonlinear regime of the photo-induced coherent magnetization dynamics in cobalt-doped yttrium iron garnet films. Photo-magnetic excitation with femtosecond laser pulses reveals a strongly nonlinear response of the spin subsystem with a significant increase of the effective Gilbert damping. By varying both laser fluence and the external magnetic field, we show that this nonlinearity originates in the anharmonicity of the magnetic energy landscape. We numerically map the parameter workspace for the nonlinear photo-induced spin dynamics below the photo-magnetic switching threshold. Corroborated by numerical simulations of the Landau-Lifshitz-Gilbert equation, our results highlight the key role of the cubic symmetry of the magnetic subsystem in reaching the nonlinear spin precession regime. These findings expand the fundamental understanding of laser-induced nonlinear spin dynamics as well as facilitate the development of applied photo-magnetism.

Photoinduced transient states of antiferromagnetic orderings in La1/3Sr2/3FeO3 and SrFeO3−δ thin films observed through time-resolved resonant soft x-ray scattering

The relationship between the magnetic interaction and photoinduced dynamics in antiferromagnetic perovskites is investigated in this study. In La1/3Sr2/3FeO3 thin films, commensurate spin ordering is accompanied by charge disproportionation, whereas SrFeO3−δ thin films show incommensurate helical antiferromagnetic spin ordering due to increased ferromagnetic coupling compared to La1/3Sr2/3FeO3. To understand the photoinduced spin dynamics in these materials, we investigate the spin ordering through time-resolved resonant soft x-ray scattering. In La1/3Sr2/3FeO3, ultrafast quenching of the magnetic ordering within 130 fs through a nonthermal process is observed, triggered by charge transfer between the Fe atoms. We compare this to the photoinduced dynamics of the helical magnetic ordering of SrFeO3−δ . We find that the change in the magnetic coupling through optically induced charge transfer can offer an even more efficient channel for spin-order manipulation.

Photoinduced Kerr rotation spectroscopy for microscopic spin systems using heterodyne detection.

We develop a transient photoinduced Kerr rotation spectroscopy technique using a heterodyne detection scheme to study spin dynamics of microscopic quantum states in solids, such as single quantum dots and spin helixes. The use of the heterodyne beat note signal generated by the interference of the frequency-shifted probe and reference pulses realizes the Kerr rotation measurements in combination with micro-spectroscopy, even when the probe pulse propagates collinearly with the strong pump pulse, which resonantly excites the probing state. In addition, the interference gives an optical amplification of the Kerr signal, which provides a clear observation of the photoinduced spin dynamics by the weak probe intensity. Here, we present results of Kerr rotation measurements for a single quantum dot exciton, which shows a maximum rotation angle of few µrad.

Role of non-thermal electrons in ultrafast spin dynamics of ferromagnetic multilayer

Understanding of ultrafast spin dynamics is crucial for future spintronic applications. In particular, the role of non-thermal electrons needs further investigation in order to gain a fundamental understanding of photoinduced demagnetization and remagnetization on a femtosecond time scale. We experimentally demonstrate that non-thermal electrons existing in the very early phase of the photoinduced demagnetization process play a key role in governing the overall ultrafast spin dynamics behavior. We simultaneously measured the time-resolved reflectivity (TR-R) and the magneto-optical Kerr effect (TR-MOKE) for a Co/Pt multilayer film. By using an extended three-temperature model (E3TM), the quantitative analysis, including non-thermal electron energy transfer into the subsystem (thermal electron, lattice, and spin), reveals that energy flow from non-thermal electrons plays a decisive role in determining the type I and II photoinduced spin dynamics behavior. Our finding proposes a new mechanism for understanding ultrafast remagnetization dynamics.

Laser-driven quantum magnonics and terahertz dynamics of the order parameter in antiferromagnets

The impulsive generation of two-magnon modes in antiferromagnets by femtosecond optical pulses, so-called femto-nanomagnons, leads to coherent longitudinal oscillations of the antiferromagnetic order parameter that cannot be described by a thermodynamic Landau-Lifshitz approach. We argue that this dynamics is triggered as a result of a laser-induced modification of the exchange interaction. In order to describe the oscillations we have formulated a quantum mechanical description in terms of magnon pair operators and coherent states. Such an approach allowed us to} derive an effective macroscopic equation of motion for the temporal evolution of the antiferromagnetic order parameter. An implication of the latter is that the photo-induced spin dynamics represents a macroscopic entanglement of pairs of magnons with femtosecond period and nanometer wavelength. By performing magneto-optical pump-probe experiments with 10 femtosecond resolution in the cubic KNiF$_3$ and the uniaxial K$_2$NiF$_4$ collinear Heisenberg antiferromagnets, we observed coherent oscillations at the frequency of 22 THz and 16 THz, respectively. The detected frequencies as a function of the temperature ideally fit the two-magnon excitation up to the N\'eel point. The experimental signals are described as dynamics of magnetic linear dichroism due to longitudinal oscillations of the antiferromagnetic vector.

Light-Induced Spin State Switching in Copper(II)-Nitroxide-Based Molecular Magnet at Room Temperature.

Molecular magnets Cu(hfac)2LR exhibit an unusual type of photoinduced magnetostructural switching in exchange-coupled copper(II)-nitroxide clusters. Such photoswitching from strongly coupled to weakly coupled spin state (SS → WS) was recently found to be ultrafast, thus enhancing the interest in these systems and the scope of their potential applications. However, to date such SS → WS photoswitching was demonstrated only at cryogenic temperatures, being limited by the absence of suitable SS states and short relaxation times at T > 100 K. In this work we selected model compound Cu(hfac)2Liso-Pr residing in the mixed SS/WS state at room temperature and investigated it using femtosecond optical spectroscopy. Photoinduced spin dynamics was detected, and an ultrafast SS → WS photoswitching was for the first time demonstrated at room temperature, constituting an important milestone in the development of copper(II)-nitroxide molecular magnets for practical purposes.

Anticrossing Spin Dynamics of Diamond Nitrogen-Vacancy Centers and All-Optical Low-Frequency Magnetometry

We investigate the photo-induced spin dynamics of single nitrogen-vacancy (NV) centres in diamond near the electronic ground state level anti-crossing (GSLAC), which occurs at an axial magnetic field around 1024 G. Using optically detected magnetic resonance spectroscopy, we first find that the electron spin transition frequency can be tuned down to 100 kHz for the \NV{14} centre, while for the \NV{15} centre the transition strength vanishes for frequencies below about 2 MHz owing to the GSLAC level structure. Using optical pulses to prepare and readout the spin state, we observe coherent spin oscillations at 1024 G for the \NV{14}, which originate from spin mixing induced by residual transverse magnetic fields. This effect is responsible for limiting the smallest observable transition frequency, which can span two orders of magnitude from 100 kHz to tens of MHz depending on the local magnetic noise. A similar feature is observed for the \NV{15} centre at 1024 G. As an application of these findings, we demonstrate all-optical detection and spectroscopy of externally-generated fluctuating magnetic fields at frequencies from 8 MHz down to 500 kHz, using a \NV{14} centre. Since the Larmor frequency of most nuclear spin species lies within this frequency range near the GSLAC, these results pave the way towards all-optical, nanoscale nuclear magnetic resonance spectroscopy, using longitudinal spin cross-relaxation.

Influence of C2-Methylation of Imidazolium Based Ionic Liquids on Photoinduced Spin Dynamics of the Dissolved ZnTPP Studied by Time-Resolved EPR

Abstract Unusual physical properties of ionic liquids (ILs) can be implemented in many different applications and are very sensitive to the structure of IL. In this work we investigate the spin dynamics of probe molecule Zn tetraphenylporphyrin (ZnTPP) dissolved in a series of ILs using time-resolved electron paramagnetic resonance (TR EPR). We compare the TR EPR characteristics in C2-methylated imidazolium-based ILs [bmmim]BF4 and [bmmim]PF6 and in their C2-protonated analogs [bmim]BF4 and [bmim]PF6 to assess the influence of C2-methylation. The corresponding TR EPR signatures are drastically different in the two types of ILs. The analysis of experimental data allows assumptions that the ZnTPP molecule is distorted in C2-methylated ILs, contrary to other organic media and C2-protonated analogs. The mobility of ZnTPP in C2-methylated ILs is smaller compared to that in C2-protonated analogs, implying different microenvironment formed around dissolved ZnTPP.

Photo-Induced Spin Dynamics in Nanoelectronic Devices

The present research is devoted to the investigation of electron spin transmission through a nanoelectronic device. This device is modeled as nonmagnetic semiconductor quantum dot coupled to two diluted magnetic semiconductor leads. The spin transport characteristics through such a device are investigated under the effect of an ac-field of a wide range of frequencies. The present result shows a periodic oscillation of the conductance for both the cases of parallel and antiparallel spin alignment. These oscillations are due to Fano-resonance. Results for spin polarization and giant magneto-resistance show the coherency property. The present research might be useful for developing single spin-based quantum bits (qubits) required for quantum information processing and quantum spin-telecommunication.

Photo-Induced Spin Dynamics in Semiconductor Quantum Wells.

We experimentally investigate the dynamics of spins in GaAs quantum wells under applied electric bias by photoluminescence (PL) measurements excited with circularly polarized light. The bias-dependent circular polarization of PL (PPL) with and without magnetic field is studied. ThePPLwithout magnetic field is found to be decayed with an enhancement of increasing the strength of the negative bias. However,PPLin a transverse magnetic field shows oscillations under an electric bias, indicating that the precession of electron spin occurs in quantum wells. The results are discussed based on the electron–hole exchange interaction in the electric field.

General Features of Photoinduced Spin Dynamics in Ferromagnetic and Ferrimagnetic Compounds

Ultrafast photoinduced spin dynamics has been investigated by time-resolved magneto-optical Kerr spectroscopy for various ferromagnetic and ferrimagnetic compounds: FeCr2S4, CoCr2S4, CuCr2Se4, CdCr2Se4, La0.6Sr0.4MnO3, and SrRuO3. The temporal demagnetization process, which is observed commonly for all the compounds, essentially consists of two components: One is an instantaneous change which originates perhaps from multiple emissions of magnetic excitations during nonradiative decay of photoexcited carriers, and the other is a delayed response due to thermalization of the spin system. The time constant of the delayed change depends strongly on materials and is scaled with the magnetocrystalline anisotropy, indicating that spin-orbit coupling is a dominant interaction for this process.