Highly intrinsic carrier mobility in tin diselenide crystal accessed with ultrafast terahertz spectroscopy.

Tin diselenide (SnSe2), a layered transition metal dichalcogenide (TMDC), stands out among other TMDCs for its extraordinary photoactive ability and low thermal conductivity. Consequently, it has stimulated many influential researches on photodetectors, ultrafast pulse shaping, thermoelectric devices, etc. However, the carrier mobility in SnSe2, as determined experimentally, remains limited to tens of cm2V-1s-1. This limitation poses a challenge for achieving high-performance SnSe2-based devices. Theoretical calculations, on the other hand, predict that the carrier mobility in SnSe2 can reach hundreds of cm2V-1s-1, approximately one order of magnitude higher than experimental value. Interestingly, the carrier mobility could be underestimated significantly in long-range transportation measurements due to the presence of defects and boundary scattering effects. To address this discrepancy, we employ optic pump terahertz probe spectroscopy to access the photoinduced dynamical THz photoconductivity of SnSe2. Our findings reveal that the intrinsic carrier mobility in conventional SnSe2 single crystal is remarkably high, reaching 353.2 ± 37.7 cm2V-1s-1, consistent with the theoretical prediction. Additionally, dynamical THz photoconductivity measurements reveal that the SnSe2 crystal containing rich defects efficiently capture photoinduced conduction-band electrons and valence-band holes with time constants of ∼20 and ∼200 ps, respectively. Meanwhile, we observe an impulsively stimulated Raman scattering at 0.60 THz. Our study not only demonstrates ultrafast THz spectroscopy as a reliable method for determining intrinsic carrier mobility and detection of low frequency coherent Raman mode in materials but also provides valuable reference for the future application of high-performance SnSe2-based devices.

Terahertz metalens for generating multi-polarized focal points and images with uniform intensity distributions.

Metasurfaces have provided a flexible platform for designing ultracompact metalenses with unusual functionalities. However, traditional multi-foci metalenses are limited to generating circularly polarized (CP) or linearly polarized (LP) focal points, and the intensity distributions are always inhomogeneous/chaotical between the multiple focal points. Here, an inverse design approach is proposed to optimize the in-plane orientation of each meta-atom in a terahertz (THz) multi-foci metalens that can generate multi-polarized focal points with nearly uniform intensity distributions. As a proof-of-principle example, we numerically and experimentally demonstrate an inversely designed metalens for simultaneously generating multiple CP- and LP-based focal points with homogeneous intensity distributions, leading to a multi-polarized image (rather than the holography). Furthermore, the multi-channel and multi-polarized images consisting of multiple focal points with homogeneous intensity distributions are also numerically demonstrated. The unique approach for inversely designing multi-foci metalens that can generate multi-polarized focal points and images with uniform intensity distributions will enable potential applications in imaging and sensing.

Defect-induced helicity dependent terahertz emission in Dirac semimetal PtTe2 thin films.

Nonlinear transport enabled by symmetry breaking in quantum materials has aroused considerable interest in condensed matter physics and interdisciplinary electronics. However, achieving a nonlinear optical response in centrosymmetric Dirac semimetals via defect engineering has remained a challenge. Here, we observe the helicity dependent terahertz emission in Dirac semimetal PtTe2 thin films via the circular photogalvanic effect under normal incidence. This is activated by a controllable out-of-plane Te-vacancy defect gradient, which we unambiguously evidence with electron ptychography. The defect gradient lowers the symmetry, which not only induces the band spin splitting but also generates the giant Berry curvature dipole responsible for the circular photogalvanic effect. We demonstrate that the THz emission can be manipulated by the Te-vacancy defect concentration. Furthermore, the temperature evolution of the THz emission features a minimum in the THz amplitude due to carrier compensation. Our work provides a universal strategy for symmetry breaking in centrosymmetric Dirac materials for efficient nonlinear transport.

Tunable multifunctional polarization conversion in bilayer chiral metamaterials.

A chiral metamaterial composed of bilayer twisted split-ring resonators is proposed and demonstrated to realize tunable, dual-directional, and multifunctional polarization conversion for terahertz waves. Simulations show that the converter can selectively achieve linear-to-linear, linear-to-right-handed circular, or linear-to-left-handed circular polarization conversion by tuning the polarization and propagating direction of the incident waves. Stokes parameters, ellipticity, and a polarization rotation angle are introduced to determine the output polarization. The circular polarization transmission coefficients and surface current distribution are employed to demonstrate the physical mechanisms of the phenomena above. The proposed converter can find potential applications in terahertz imaging and communications.

Anomalous Nernst Effect Induced Terahertz Emission in a Single Ferromagnetic Film.

Despite its important role in understanding ultrafast spin dynamics and revealing novel spin/orbit effects, the mechanism of the terahertz (THz) emission from a single ferromagnetic nanofilm upon a femtosecond laser pump still remains elusive. Recent experiments have shown exotic symmetry, which is not expected from the routinely adopted mechanism of ultrafast demagnetization. Here, by developing a bidirectional pump-THz emission spectroscopy and associated symmetry analysis method, we set a benchmark for the experimental distinction of the THz emission induced by various mechanisms. Our results unambiguously unveil a new mechanism─anomalous Nernst effect (ANE) induced THz emission due to the ultrafast temperature gradient created by a femtosecond laser. Quantitative analysis shows that the THz emission exhibits interesting thickness dependence where different mechanisms dominate at different thickness ranges. Our work not only clarifies the origin of the ferromagnetic-based THz emission but also offers a fertile platform for investigating the ultrafast optomagnetism and THz spintronics.

Ultrafast light-driven magneto-optical nonlinearity in ferromagnetic heterostructures.

The dynamic control of magnetization by short laser pulses has recently attracted interest. The transient magnetization at the metallic magnetic interface has been investigated through second-harmonic generation and the time-resolved magneto-optical effect. However, the ultrafast light-driven magneto-optical nonlinearity in ferromagnetic heterostructures for terahertz (THz) radiation remains unclear. Here, we present THz generation from a metallic heterostructure, Pt/CoFeB/Ta, which is ascribed to an ∼6-8% contribution from the magnetization-induced optical rectification and an ∼94-92% contribution from both spin-to-charge current conversion and ultrafast demagnetization. Our results show that THz-emission spectroscopy is a powerful tool to study the picosecond-time-scale nonlinear magneto-optical effect in ferromagnetic heterostructures.

Correction to "Terahertz Magnon-Polaritons in TmFeO3".

[This corrects the article DOI: 10.1021/acsphotonics.7b01402.].

Terahertz Emission Spectroscopy of Ultrafast Coupled Spin and Charge Dynamics in Nanometer Ferromagnetic Heterostructures.

Due to its high sensitivity and because it does not rely on the magneto-optical response, terahertz (THz) emission spectroscopy has been used as a powerful time-resolved tool for investigating ultrafast demagnetization and spin current dynamics in nanometer-thick ferromagnetic (FM)/heavy metal (HM) heterostructures. Here, by changing the order of the conductive HM coating on the FM nanometer film, the dominant electric dipole contribution to the laser-induced THz radiation can be unraveled from the ultrafast magnetic dipole. Furthermore, to take charge equilibration into account, we separate the femtosecond laser-induced spin-to-charge converted current and the instantaneous discharging current within the illuminated area. The THz emission spectroscopy gives us direct information into the coupled spin and charge dynamics during the first moments of the light-matter interaction. Our results also open up new perspectives to manipulate and optimize the ultrafast charge current for promising high-performance and broadband THz radiation.

Photoinduced large polaron transport and dynamics in organic-inorganic hybrid lead halide perovskite with terahertz probes.

Organic-inorganic hybrid metal halide perovskites (MHPs) have attracted tremendous attention for optoelectronic applications. The long photocarrier lifetime and moderate carrier mobility have been proposed as results of the large polaron formation in MHPs. However, it is challenging to measure the effective mass and carrier scattering parameters of the photogenerated large polarons in the ultrafast carrier recombination dynamics. Here, we show, in a one-step spectroscopic method, that the optical-pump and terahertz-electromagnetic probe (OPTP) technique allows us to access the nature of interplay of photoexcited unbound charge carriers and optical phonons in polycrystalline CH3NH3PbI3 (MAPbI3) of about 10 µm grain size. Firstly, we demonstrate a direct spectral evidence of the large polarons in polycrystalline MAPbI3. Using the Drude-Smith-Lorentz model along with the FrÓ§hlich-type electron-phonon (e-ph) coupling, we determine the effective mass and scattering parameters of photogenerated polaronic carriers. We discover that the resulting moderate polaronic carrier mobility is mainly influenced by the enhanced carrier scattering, rather than the polaron mass enhancement. While, the formation of large polarons in MAPbI3 polycrystalline grains results in a long charge carrier lifetime at room temperature. Our results provide crucial information about the photo-physics of MAPbI3 and are indispensable for optoelectronic device development with better performance.

Ultrafast Photocarrier Dynamics in Vertically Aligned SnS2 Nanoflakes Probing with Transient Terahertz Spectroscopy.

By employing optical pump Terahertz (THz) probe spectroscopy, ultrafast photocarrier dynamics of a two-dimensional (2D) semiconductor, SnS2 nanoflake film, has been investigated systematically at room temperature. The dynamics of photoexcitation is strongly related to the density of edge sites and defects in the SnS2 nanoflakes, which is controllable by adjusting the height of vertically aligned SnS2 during chemical vapor deposition growth. After photoexcitation at 400 nm, the transient THz photoconductivity response of the films can be well fitted with bi-exponential decay function. The fast and slow processes are shorter in the thinner film than in the thicker sample, and both components are independent on the pump fluence. Hereby, we propose that edge-site trapping as well as defect-assisted electron-hole recombination are responsible for the fast and slow decay progress, respectively. Our experimental results demonstrate that the edge sites and defects in SnS2 nanoflakes play a dominant role in photocarrier relaxation, which is crucial in understanding the photoelectrochemical performance of SnS2 nanoflakes.

Third-order harmonic generation in a bi-chromatic elliptical laser field.

The low-order harmonic generation induced by a strong laser field produces a bright, ultrashort, supercontinuum radiation ranging from the terahertz to ultraviolet band. By controlling the phase-delay and ellipticity of the bi-chromatic laser fields, the third harmonic generation is experimentally and theoretically investigated for elucidating the mechanism of the low-order harmonics. The third harmonic generation is found to be strongly suppressed in the counter-rotating bi-chromatic laser field due to the selection rule for harmonic emissions. The continuum-continuum transition in the strong field approximation is extended to explain the third harmonic generation as a function of the phase delay and ellipticity of the bi-chromatic laser fields. Compared with the semi-classical photocurrent model, the continuum-continuum transition on the basis of quantum-mechanical treatment achieves better agreement with the experimental observations. Our work indicates that the overlapping in continuum states via different quantum paths of a single electron plays a role in low-order harmonics generation under elliptical bi-chromatic laser fields.

Observation of Negative Terahertz Photoconductivity in Large Area Type-II Dirac Semimetal PtTe_{2}.

As a newly emergent type-II Dirac semimetal, platinum telluride (PtTe_{2}) stands out from other two dimensional noble-transition-metal dichalcogenides for the unique band structure and novel physical properties, and has been studied extensively. However, the ultrafast response of low energy quasiparticle excitation in terahertz frequency remains nearly unexplored yet. Herein, we employ optical pump-terahertz probe (OPTP) spectroscopy to systematically study the photocarrier dynamics of PtTe_{2} thin films with varying pump fluence, temperature, and film thickness. Upon photoexcitation the terahertz photoconductivity (PC) of PtTe_{2} films shows abrupt increase initially, while the terahertz PC changes into negative value in a subpicosecond timescale, followed by a prolonged recovery process that lasted a few nanoseconds. The magnitude of both positive and negative terahertz PC response shows strongly pump fluence dependence. We assign the unusual negative terahertz PC to the formation of small polaron due to the strong electron-phonon (e-ph) coupling, which is further substantiated by temperature and film thickness dependent measurements. Moreover, our investigations give a subpicosecond timescale of simultaneous carrier cooling and polaron formation. The present study provides deep insights into the underlying dynamics evolution mechanisms of photocarrier in type-II Dirac semimetal upon photoexcitation, which is of crucial importance for designing PtTe_{2}-based optoelectronic devices.

Ultrastrong magnon-magnon coupling dominated by antiresonant interactions.

Exotic quantum vacuum phenomena are predicted in cavity quantum electrodynamics systems with ultrastrong light-matter interactions. Their ground states are predicted to be vacuum squeezed states with suppressed quantum fluctuations owing to antiresonant terms in the Hamiltonian. However, such predictions have not been realized because antiresonant interactions are typically negligible compared to resonant interactions in light-matter systems. Here we report an unusual, ultrastrongly coupled matter-matter system of magnons that is analytically described by a unique Hamiltonian in which the relative importance of resonant and antiresonant interactions can be easily tuned and the latter can be made vastly dominant. We found a regime where vacuum Bloch-Siegert shifts, the hallmark of antiresonant interactions, greatly exceed analogous frequency shifts from resonant interactions. Further, we theoretically explored the system's ground state and calculated up to 5.9 dB of quantum fluctuation suppression. These observations demonstrate that magnonic systems provide an ideal platform for exploring exotic quantum vacuum phenomena predicted in ultrastrongly coupled light-matter systems.

Ultrafast terahertz magnetometry.

A material's magnetic state and its dynamics are of great fundamental research interest and are also at the core of a wide plethora of modern technologies. However, reliable access to magnetization dynamics in materials and devices on the technologically relevant ultrafast timescale, and under realistic device-operation conditions, remains a challenge. Here, we demonstrate a method of ultrafast terahertz (THz) magnetometry, which gives direct access to the (sub-)picosecond magnetization dynamics even in encapsulated materials or devices in a contact-free fashion, in a fully calibrated manner, and under ambient conditions. As a showcase for this powerful method, we measure the ultrafast magnetization dynamics in a laser-excited encapsulated iron film. Our measurements reveal and disentangle distinct contributions originating from (i) incoherent hot-magnon-driven magnetization quenching and (ii) coherent acoustically-driven modulation of the exchange interaction in iron, paving the way to technologies utilizing ultrafast heat-free control of magnetism. High sensitivity and relative ease of experimental arrangement highlight the promise of ultrafast THz magnetometry for both fundamental studies and the technological applications of magnetism.

Magnetic field tuning of spin resonance in TmFeO3 single crystal probed with THz transient.

TmFeO3, a canted antiferromagnet, has two intrinsic spin resonance modes in the terahertz (THz) frequency regime: quasi-ferromagnetic (q-FM) mode and quasi-antiferromagnetic (q-AFM) mode. Both the q-FM and q-AFM modes show strong magnetic field and temperature dependence. Hereby, by employing THz time-domain spectroscopy combined with external magnetic field and low temperature system, we systematically investigated the magnetic field induced frequency shift of q-FM and q-AFM modes as well as the temperature driven spin reorientation phase transition in TmFeO3 single crystal. In contrast to the isotropic temperature dependent two-mode, the magnetic field dependence of two-mode is strongly anisotropic: the magnetic field applied along c-axis (a-axis) can harden (soften) the spin resonance frequency of q-FM mode for Γ4 phase of TmFeO3, and the field applied along b-axis shows negligible frequency shift for the q-FM mode, with the q-AFM mode relatively stable. The present study provides solid evidence that the magnetic anisotropy in rare earth orthoferrite plays a dominant role in the q-FM mode and the occurrence of spin reorientation phase transition. With the magnetic anisotropic energy obtained from the temperature dependent q-FM and q-AFM mode frequencies, we can predict both magnetic field and temperature dependence of spin resonance in TmFeO3 single crystal via phenomenological analysis.

Design of an online spectrometer for the diagnosis of free-electron lasers.

A self-amplified spontaneous emission free-electron laser (FEL) is under construction at the Shanghai Soft X-ray Free-Electron Facility. Therefore, it is necessary to develop a suitable diagnostic tool capable of resolving the natural emission band of each FEL pulse. Thus, an online spectrometer with a plane mirror and plane variable-line-spacing grating at grazing incidence to monitor each single FEL pulse during the propagation of FEL radiation has been designed and is presented in this work. The method of ray tracing is used for monitoring incident radiation in order to understand spectral characteristics, and SHADOW, an X-ray optics simulation tool, and SRW, an X-ray optics wavefront tool, are applied to study the resolving power and focusing properties of the grating. The designed resolving power is ∼3 × 104 at 620 eV. Meanwhile, the effect of the actual slope error of mirrors on the ray-tracing results is also discussed. In order to provide further optimization for the choice of grating, a comparison of resolving powers between 2000 lines mm-1 and 3000 lines mm-1 gratings at different energies is analyzed in detail and radiation damage of mirrors as well as parameters such as the first-order diffraction angle ß, the exit-arm length r2, and the tilt angle θ between the focal plane and the diffraction arm are studied and optimized. This work has provided comprehensive designing methods and detailed data for the design of diagnostic spectrometers in soft X-ray FELs and will be favorable to the design of other similar instruments.

Optically controlled ultrafast terahertz switching in a CdTe nanostructure thin film.

The speed of optical modulation on a terahertz (THz) pulse is mainly dominated by the optical response of the photocarrier. In order to achieve ultrafast THz modulation, the effective method is to reduce the lifetime of the photocarrier by introducing defects that can trap the photocarriers efficiently. In this paper, we reported the ultrafast optical modulation of THz switching in a 10 nm CdTe nanostructure film. After photoexcitation at 800/400 nm, the THz response of the film is extremely fast with a lifetime of ${\sim}{1.3}\;{\rm ps}$∼1.3ps. Further, the ultrafast transient THz transmission shows almost temperature independence down to 100 K. On the other hand, the transient absorption spectroscopy reveals that the lifetime of photocarriers in CdTe nanostructure film lasts as long as several ns. The 1.3 ps THz photoconductivity response is due to the substantial decrease of photocarrier mobility in a CdTe nanostructure, which comes from the increase of the photocarrier scattering between the photocarrier and the surface states of CdTe nanostructural film. Our experimental results provide a new method to design optically driven ultrafast THz response devices, such as THz switch and THz modulator.

The modulation of terahertz photoconductivity in CVD grown n-doped monolayer MoS2 with gas adsorption.

The as-grown atomically thin transition metal dichalcogenides (TMDs) usually have extremely large surface-to-volume ratios. Hence, the electrical and optical properties are always affected by the adsorption of atmospheric gases. By using optical pump terahertz (THz) probe spectroscopy, THz photoconductivity dynamics of chemical vapor deposition grown monolayer MoS2 has been investigated in nitrogen, air and oxygen atmospheric environments. Our study reveals that the photoconductivity of MoS2 at THz frequencies is dramatically altered by the adsorption of oxygen. The relaxation dynamics of photoconductivity strongly depends on atmospheres, which is attributed to photo-excited different quasi-particles, such as free charge carriers, excitons and trions. This study highlights the role of oxygen passivation of the photoconductivity in monolayer MoS2, which may have important applications for the design of future MoS2-based electronic devices.

Ultrafast formation and dynamics of interlayer exciton in a large-area CVD-grown WS2/WSe2 heterostructure.

A WS2/WSe2 heterostructure is constructed by stacking a WS2 monolayer on the top of WSe2 monolayer fabricated with chemical vapor deposition (CVD) method. Ultrafast transient spectroscopy is used to demonstrate the ultrafast charge transfer and interlayer exciton dynamics in the heterostructure. When the WS2/WSe2 heterostructure was photoexcitated at 617 nm (2.01 eV) to excite the A-exciton transition of WS2, an ultrafast photobleaching was observed around the WSe2 A-exciton transition at 749 nm. The bleaching signal lasts several nanoseconds, which is much longer than the A-exciton lifetime in both the WS2 and WSe2 monolayer film. Moreover, by selectively photoexciting the A-exciton of WSe2 at 749 nm in the heterostructure, an ultrafast photobleaching occurs around the WS2 A-exciton transition, the recovery of the bleaching shows a single exponential relaxation with typical time constant of ~1.8 ps. The very fast relaxation in the heterostructure probing around 620 nm is indicative that rich defect states exist below the conduction band in WS2, which can efficiently trap these electrons transferred from the WSe2 upon photoexcitation. Our spectroscopic results reveal that our CVD-grown WS2/WSe2 bilayer film has a type II heterostructure in nature at room temperature. With photoexcitation, electrons and holes can be separately confined in the WS2 and WSe2 layer, respectively; as a result, interlayer excitons are formed.

Observation of Dicke cooperativity in magnetic interactions.

The interaction of N two-level atoms with a single-mode light field is an extensively studied many-body problem in quantum optics, first analyzed by Dicke in the context of superradiance. A characteristic of such systems is the cooperative enhancement of the coupling strength by a factor of N. In this study, we extended this cooperatively enhanced coupling to a solid-state system, demonstrating that it also occurs in a magnetic solid in the form of matter-matter interaction. Specifically, the exchange interaction of N paramagnetic erbium(III) (Er3+) spins with an iron(III) (Fe3+) magnon field in erbium orthoferrite (ErFeO3) exhibits a vacuum Rabi splitting whose magnitude is proportional to N. Our results provide a route for understanding, controlling, and predicting novel phases of condensed matter using concepts and tools available in quantum optics.