The spin photocurrents, direct currents induced by light, hold great promise for introducing new elements to spintronics. However, a general theory for spin photocurrents in real materials which is applicable to systems with spin-orbit coupling or noncollinear magnetism is absent. Here, we develop such a general theory of second-order spin photocurrents. We find that the secondorder spin photocurrents can be classified into Drude, Berry curvature dipole, shift, injection, and rectification currents, which have different physical origins and symmetry properties. Surprisingly, our theory predicts a direct pure spin rectification current in an insulator induced by photons with energies lower than the material band gap. This phenomenon is absent in the case of the charge photocurrent. We find that the pure spin current of BiTeI induced by subgap light is large enough to be observable in experiments. Moreover, the subgap pure spin photocurrent is highly tunable with the polarization of light and the flowing direction of the spin photocurrent. This study lays the groundwork for the study of nonlinear spin photocurrents in real materials and provides a route to engineer light-controlled spin currents.
Rectified electric current induced by irradiating light, so-called photocurrent, is an established phenomenon in optoelectronic physics. In this paper, we present a comprehensive classification of the photocurrent response arising from the parity violation in bulk systems. We clarify the contrasting role of $\mathcal{T}$- and $\mathcal{PT}$-symmetries and consequently find a new type of photocurrent phenomena characteristic of parity-violating magnets, intrinsic Fermi surface effect and gyration current. Especially, the gyration current is induced by the circularly-polarized light and it is th…
Circularly polarized photons are known to generate a directional helicity-dependent photocurrent in three-dimensional topological insulators at room temperature. Surprisingly, the phenomenon is readily observed at photon energies that excite electrons to states far above the spin-momentum locked Dirac cone and the underlying mechanism for the helicity-dependent photocurrent is still not understood. We resolve the puzzle through a comprehensive study of the helicity-dependent photocurrent in (Bi,Sb)_2Te_3 thin films as a function of the incidence angle of the optical excitation, its wavelength,…
We study the second-order nonlinear optical response of a Weyl semimetal (WSM), i.e. a three-dimensional metal with linear band touchings acting as point-like sources of Berry curvature in momentum space, termed "Weyl-Berry monopoles". We first show that the anomalous second-order photocurrent of WSMs can be elegantly parametrized in terms of Weyl-Berry dipole and quadrupole moments. We then calculate the corresponding charge and node conductivities of WSMs with either broken time-reversal invariance or inversion symmetry. In particular, we predict a universal dissipationless second-order anom…
Three-dimensional topological insulators represent a new quantum phase of matter with spin-polarized surface states that are protected from backscattering. The static electronic properties of these surface states have been comprehensively imaged by both photoemission and tunneling spectroscopies. Theorists have proposed that topological surface states can also exhibit novel electronic responses to light, such as topological quantum phase transitions and spin-polarized electrical currents. However, the effects of optically driving a topological insulator out of equilibrium have remained largely…
Photovoltaic conversion efficiency (PCE) of halide perovskite solar cells has risen spectacularly, yet the very crystalline structure of CH3NH3PbI3 remains ambiguous after extensive researches, and its polar nature remains hotly debated. Here we present compelling evidences that CH3NH3PbI3 crystals self-grown on FTO/TiO2 substrate consist of ferroic domains with alternating polar and nonpolar orders, in contrast to previous experimental and theoretical expectations, and polar domains possess reduced photocurrent. It is found that polar and nonpolar orders of CH3NH3PbI3 can be distinguished fro…
Nonlinear photocurrent in time-reversal invariant noncentrosymmetric systems have attracted substantial interest. Here we propose two new types of second-order nonlinear direct photocurrent as the counterpart of normal shift photocurrent (NSC) and normal injection photocurrent (NIC), namely magnetic shift photocurrent (MSC) and magnetic injection photocurrent (MIC) in time-reversal symmetry and inversion symmetry broken system. We show that MSC is mainly governed by shift vector and interband Berry curvature, and MIC is dominated by absorption strength and asymmetry of the group velocity diffe…
In the realm of two-dimensional materials magnetic and transport properties of a unique representative $-$ Fe$_3$GeTe$_2$ $-$ attract ever increasing attention. Here, we use a developed first-principles method for calculating laser-induced response to study the emergence of photo-induced currents of charge and spin in single-layer Fe$_3$GeTe$_2$, which are of second order in the electric field. We provide a symmetry analysis of the emergent photocurrents in the system finding it to be in excellent agreement with ab-initio calculations. We analyse the magnitude and behavior of the charge photoc…
Direct Photocurrent Detection of Optical Vortex Based on the Orbital Photo Galvanic Effect: Progress, Challenge and Perspective
Zhengzhou University（郑州大学）；Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences（中国科学院长春光学精密机械与物理研究所）；University of Chinese Academy of Science（中国科学院大学）；Peking University（北京大学）
Nonlinear optical responses to external electromagnetic field, characterized by second and higher order susceptibilities, play crucial roles in nonlinear optical devices and novel optoelectronics. Herein we present a quantum nonlinear ferroic optical Hall effect (QNFOHE) in multiferroics - a Hall-like direct photocurrent originated from the second order current response to intense electromagnetic field whose direction can be controlled by both internal ferroic orders and external light polarization. QNFOHE consists of two types of nonlinear photocurrent responses - shift current and circular p…
We have studied theoretically the Weyl semimetals the point symmetry group of which has reflection planes and which contain equivalent valleys with opposite chiralities. These include the most frequently studied compounds, namely the transition metals monopnictides TaAs, NbAs, TaP, NbP, and also Bi$_{1-x}$Sb$_x$ alloys. The circular photogalvanic current, which inverts its direction under reversal of the light circular polarization, has been calculated for the light absorption under direct optical transitions near the Weyl points. In the studied materials, the total contribution of all the val…
Bulk photovoltaic (BPV) effect, a second order nonlinear process that generates static current under light irradiation, requires centrosymmetric broken systems as its application platform. In order to realize measurable BPV photocurrent in spatially centrosymmetric materials, various schemes such as chemical doping, structural deformation, or electric bias have been developed. In the current work, we suggest that magnetic proximity effect via van der Waals interfacial interaction, a contact-free strategy, also breaks the centrosymmetry and generate large BPV photocurrents. Using the Bi2Te3 qui…
Antiferromagnetism (AF) in AB'-stacked centrosymmetric bilayer (BL) CrI$_3$ breaks both spatial inversion ($P$) and time-reversal ($T$) symmetries but maintains the combined $PT$ symmetry, thus inducing novel second-order nonlinear optical (NLO) responses such as second-harmonic generation (SHG), linear electric-optic effect (LEO) and bulk photovoltaic effect (BPVE). In this work, we calculate AF-induced NLO responses of the BL CrI$_3$ based on the density functional theory with the generalized gradient approximation (GGA) plus onsite Coulomb correlation (U), i.e., the GGA+U method. Interestin…
In organic bulk heterojunction solar cells, the open circuit voltage ($V_\mathrm{oc}$) suffers from an ultra-high loss at low temperatures. In this work we investigate the origin of the loss through calculating the $V_\mathrm{oc}-T$ plots with the device model method systematically and comparing it with experimentally observed ones. When the energetic disorder is incorporated into the model by considering the disorder-suppressed and temperature-dependent charge carrier mobilities, it is found that for nonselective contacts the $V_\mathrm{oc}$ reduces drastically under the low temperature regim…
The second-order nonlinear optical (NLO) processes, such as the photogalvanic effect and second-order harmonic generation (SHG), play crucial roles in probing and controlling light-matter interactions for energy and device applications. To date, most studies of second-order NLO processes focus on materials with broken spatial inversion symmetry, such as proper ferroelectrics and noncentrosymmetric Weyl semimetals. Nevertheless, inversion symmetry of Shubnikov groups can be broken via spin-ordering in centrosymmetric crystals. Unfortunately, these materials are less common, and their NLO respon…
We present a comprehensive multiphonon Raman and complementary infrared analysis for bulk and monolayer MoS2.For the bulk the analysis consists of symmetry assignment from which we obtain a broad set of allowed second order transitions at the high symmetry M,K and gamma Brillouin zone points. The attribution of about 80 transitions of up to fifth order Raman processes are proposed in the low temperature(95K)resonant Raman spectrum measured with the excitation energy of 1.96 eV,which is slightly shifted from the A exciton. We propose that the main contributions come from four phonons:A1g(M),E12…
