Long-Lived Charge Separation Following Pump-Energy Dependent Ultrafast Charge Transfer in Graphene/WS$_2$ Heterostructures
Shuai Fu, Indy du Fossé, Xiaoyu Jia, Jingyin Xu, Xiaoqing Yu, Heng Zhang, Wenhao Zheng, Sven Krasel, Zongping Chen, Zhiming M. Wang, Klaas-Jan Tielrooij, Mischa… 展开作者
Shuai Fu, Indy du Fossé, Xiaoyu Jia, Jingyin Xu, Xiaoqing Yu, Heng Zhang, Wenhao Zheng, Sven Krasel, Zongping Chen, Zhiming M. Wang, Klaas-Jan Tielrooij, Mischa Bonn, Arjan J. Houtepen, Hai I. Wang
Van der Waals heterostructures consisting of graphene and transition metal dichalcogenides (TMDCs) have recently shown great promise for high-performance optoelectronic applications. However, an in-depth understanding of the critical processes for device operation, namely interfacial charge transfer (CT) and recombination, has so far remained elusive. Here, we investigate these processes in graphene-WS$_2$ heterostructures, by complementarily probing the ultrafast terahertz photoconductivity in graphene and the transient absorption dynamics in WS$_2$ following photoexcitation. We find that CT across graphene-WS$_2$ interfaces occurs via photo-thermionic emission for sub-A-exciton excitation, and direct hole transfer from WS$_2$ to the valence band of graphene for above-A-exciton excitation. Remarkably, we observe that separated charges in the heterostructure following CT live extremely long: beyond 1 ns, in contrast to ~1 ps charge separation reported in previous studies. This leads to efficient photogating of graphene. These findings provide relevant insights to optimize further the performance of optoelectronic devices, in particular photodetection.
The ultrafast relaxation and recombination dynamics of photogenerated electrons and holes in epitaxial graphene are studied using optical-pump Terahertz-probe spectroscopy. The conductivity in graphene at Terahertz frequencies depends on the carrier concentration as well as the carrier distribution in energy. Time-resolved studies of the conductivity can therefore be used to probe the dynamics associated with carrier intraband relaxation and interband recombination. We report the electron-hole recombination times in epitaxial graphene for the first time. Our results show that carrier cooling o…
Room temperature, wavelength non-degenerate ultrafast pump/probe measurements were performed on GaN and InGaN epilayers and an InGaN multiple quantum well structure. Carrier relaxation dynamics were investigated as a function of excitation wavelength and intensity. Spectrally-resolved sub-picosecond relaxation due to carrier redistribution and QW capture was found to depend sensitively on the wavelength of pump excitation. Moreover, for pump intensities above a threshold of 100 microJ/cm2, all samples demonstrated an additional emission feature arising from stimulated emission (SE). SE is evid…
We present results of wavelength-dependent ultrafast pump-probe experiments on micelle-suspended single-walled carbon nanotubes. The linear absorption and photoluminescence spectra of the samples show a number of chirality-dependent peaks, and consequently, the pump-probe results sensitively depend on the wavelength. In the wavelength range corresponding to the second van Hove singularities (VHSs), we observe sub-picosecond decays, as has been seen in previous pump-probe studies. We ascribe these ultrafast decays to intraband carrier relaxation. On the other hand, in the wavelength range corre…
We study coherent nonlinear dynamics of carriers under ultrafast interband excitation of an intrinsic graphene. The Rabi oscillations of response appear with increasing of pumping intensity. The photoexcited distribution is calculated versus time and energy taking into account the effects of energy relaxation and dephasing. Spectral and temporal dependencies of the response on a probe radiation (transmission and reflection coefficients) are considered for different pumping intensities and the Rabi oscillations versus time and intensity are analyzed.
A new degree of freedom, the valley pseudospin, emerges in atomically thin two-dimensional transition metal dichalcogenides (MX2) and has attracted great scientific interest. The capability to manipulate the valley pseudospin, in analogy to the control of spin in spintronics, can open up exciting opportunities in valleytronics. Here we demonstrate that an ultrafast and ultrahigh valley pseudomagnetic field can be generated using circularly polarized femtosecond pulses to selectively control the valley degree of freedom in monolayer MX2. Employing ultrafast pump-probe spectroscopy, we observed …
Femtosecond magneto-optical pump-probe measurements of ultrafast demagnetization show an intriguing difference in the first 100 fs of the magneto-optical Kerr response depending on whether the polarization of the pump and probe beams are in parallel or perpendicular configuration [Bigot et al., Nature Phys. 5, 515 (2009)]. Starting from a most general relativistic Hamiltonian we focus on the ultra-relativistic light-spin interaction and show that this coupling term leads to different light-induced opto-magnetic fields when pump and probe polarization are parallel and perpendicular to each othe…
Pump-probe experiments are used as a controllable way to investigate the properties of photoexcited semiconductors, in particular, the absorption saturation. We present an experiment-theory comparison for ZnSe quantum wells, investigating the energy renormalization and bleaching of the excitonic resonances. Experiments were performed with spin-selective excitation and above-bandgap pumping. The model, based on the semiconductor Bloch equations in the screened Hartree-Fock approximation, takes various scattering processes into account phenomenologically. Comparing numerical results with availab…
We report results from ultrafast two-color optical pump-probe spectroscopy on bulk $β$-Ga$_2$O$_3$. A two-photon absorption scheme is used to photoexcite carriers with the pump pulse and free-carrier absorption of the probe pulse is used to record the subsequent dynamics of the photoexcited carriers. Our results are consistent with carrier recombination via defect-assisted processes. We also observe transient polarization-selective optical absorption of the probe pulse by defect states under nonequilibrium conditions. A rate equation model for electron and hole capture by defects is proposed a…
Atomically-thin molybdenum disulfide is emerging as a new nanomaterial with potential applications in the fields of electronic and photonics. Charge carrier dynamics plays an essential role in determining its electronic and optical properties. We report spatially and temporally resolved pump-probe studies of charge carriers in atomically-thin molybdenum disulfide samples fabricated by mechanical exfoliation. Carriers are injected by interband absorption of a 390-nm pump pulse and detected by measuring differential reflection of a time-delayed and spatially-scanned probe pulse that is tuned to …
We investigate the valley related carrier dynamics in monolayer MoS2 using helicity resolved non-degenerate ultrafast pump-probe spectroscopy at the vicinity of the high-symmetry K point under the temperature down to 78 K. Monolayer MoS2 shows remarkable transient reflection signals, in stark contrast to bilayer and bulk MoS2 due to the enhancement of many-body effect at reduced dimensionality. The helicity resolved ultrafast time-resolved result shows that the valley polarization is preserved for only several ps before scattering process makes it undistinguishable. We suggest that the dynamic…
Controlling Ultrafast Excitations in Germanium:The Role of Pump-Pulse Parameters and Multi-Photon Resonances
Università degli Studi di Salerno（萨莱诺大学）；CNR-SPIN, Unità di Salerno（意大利国家研究委员会自旋物理研究所萨莱诺分部）；CNISM, Unità di Salerno, Università degli Studi di Salerno（意大利凝聚态物质创新科学中心萨莱诺分部，萨莱诺大学）
We explore the influence of the nanoporous structure on the thermal relaxation of electrons and holes excited by ultrashort laser pulses ($\sim 7$ fs) in thin gold films. Plasmon decay into hot electron-hole pairs results in the generation of a Fermi-Dirac distribution thermalized at a temperature $T_{\mathrm{e}}$ higher than the lattice temperature $T_{\mathrm{l}}$. The relaxation times of the energy exchange between electrons and lattice, here measured by pump-probe spectroscopy, is slowed down by the nanoporous structure, resulting in much higher peak $T_{\mathrm{e}}$ than for bulk gold fil…
Spin angular momentum transfer in magnetic bilayers offers the possibility of ultrafast and low-loss operation for next-generation spintronic devices. We report the field- and temperature- dependent measurements on the magnetization precessions in Co$_2$FeAl/(Ga,Mn)As by time-resolved magneto-optical Kerr effect (TRMOKE). Analysis of the effective Gilbert damping and phase shift indicates a clear signature of an enhanced dynamic exchange coupling between the two ferromagnetic (FM) layers due to the reinforced spin pumping at resonance. The temperature dependence of the dynamic exchange-couplin…
We investigate the dynamics of photoexcited carriers and nonequilibrium phonons in graphene by solving the microscopic kinetic Bloch equations. The pump and drift effects from the laser field as well as the relevant scatterings (including the Coulomb scattering with dynamic screening) are explicitly included. When the pump-photon energy is high enough, the influence of the drift term is shown to be negligible and the isotropic hot-electron Fermi distribution is established under the scattering during the linearly polarized laser pulse investigated here. However, in the case with low pump-phono…
The transport of optically excited, hot electrons in heterostructures is analyzed by femtosecond, time-resolved two-photon photoelectron emission spectroscopy (2PPE) for epitaxial Au/Fe/MgO(001). We compare the temporal evolution of the 2PPE intensity upon optically pumping Fe or Au, while the probing occurs on the Au surface. In the case of Fe-side pumping, assuming independent relaxation in the Fe and Au layers, we determine the hot electron relaxation times in these individual layers by an analysis of the Au layer thickness dependence of the observed, effective electron lifetimes in the het…
High-resolution angle-resolved photoemission spectroscopy and ultrafast optical pump-probe spectroscopy were used to study semimetallic 1T - TiTe2 quasiparticle dispersion and dynamics. A kink and a flat band, having the same energy scale and temperature-dependent behaviors along the G-M direction, were detected. Both manifested at low temperatures but blurred as temperature increased. The kink was formed by an electron-phonon coupling. And the localized flat band might be closely related to an electron-phonon coupling. Ultrafast optical spectroscopy identified multiple distinct time scales in…
The role of photon angular momentum in laser-induced demagnetization of Nickel thin films is investigated by means of pump-probe time-resolved magneto-optical Kerr effect in the polar geometry. The recorded data display a strong dependency on pump helicity during pump-probe temporal overlap, which is shown to be of non-magnetic origin. By accurately fitting the demagnetization curves we also show that demagnetization time and electron-phonon equilibration time are not affected by pump-helicity. Thereby our results do not support direct transfer of angular momentum between photons and spins to …
Tunnel-Barrier-Engineered Ultrafast Demagnetization and Spin Transport in Graphene-Based Heterostructures
S. N. Bose National Center for Basic Sciences（S.N. 玻色基础科学国家中心）；Indian Institute of Science Education and Research Kolkata（加尔各答印度科学与教育研究所）；Uppsala University（乌普萨拉大学）
Quantum materials represent one of the most promising frontiers in the quest for faster, lightweight, energy efficient technologies. However, their inherent complexity and rich phase landscape make them challenging to understand or manipulate in useful ways. Here we present a new ultrafast electron calorimetry technique that can systematically uncover new phases of quantum matter. Using time- and angle-resolved photoemission spectroscopy, we measure the dynamic electron temperature, band structure and heat capacity. We then show that this is a very sensitive probe of phase changes in materials…
Point defects in crystalline materials often occur in multiple charge states. Although many experimental methods to study and explore point defects are available, techniques to explore the non-equilibrium dynamics of the charge states of these defects at ultrafast (sub-nanosecond) time scales have not been discussed before. We present results from ultrafast optical-pump supercontinuum-probe spectroscopy measurements on $β$-Ga$_2$O$_3$. The study of point defects in $β$-Ga$_2$O$_3$ is essential for its establishment as a material platform for high-power electronics and deep-UV optoelectronics. …
We study the optical-pump induced ultrafast transient change of the X-ray absorption at the $L_3$ absorption resonances of the transition metals Ni and Fe in Fe$_{0.5}$Ni$_{0.5}$ alloy. We find the effect for both elements to occur simultaneously on a femtosecond timescale. This effect may hence be used as a handy cross-correlation scheme providing a time-zero reference for ultrafast optical-pump soft X-ray-probe measurement. The method benefits from a relatively simple experimental setup as the sample itself acts as time-reference tool. In particular, this technique works with low flux ultraf…
Ultrafast imaging is essential in physics and chemistry to investigate the femtosecond dynamics of nonuniform samples or of phenomena with strong spatial variations. It relies on observing the phenomena induced by an ultrashort laser pump pulse using an ultrashort probe pulse at a later time. Recent years have seen the emergence of very successful ultrafast imaging techniques of single non-reproducible events with extremely high frame rate, based on wavelength or spatial frequency encoding. However, further progress in ultrafast imaging towards high spatial resolution is hampered by the lack o…
Transition metal nitrides have recently gained attention in the fields of plasmonics, plasmon-enhanced photocatalysis, photothermal applications, and nonlinear optics because of their suitable optical properties, refractory nature, and large laser damage thresholds. This work reports comparative studies of the transient response of films of titanium nitride, zirconium nitride, and Au under femtosecond excitation. Broadband transient optical characterization helps to adjudicate earlier, somewhat inconsistent reports regarding hot electron lifetimes based upon single wavelength measurements. The…
CuTe is a two-dimensional (2D) layered material, yet forming a quasi-one-dimensional (quasi-1D) charge-density-wave (CDW) along the a-axis in the ab-plane at high transition temperature $T_{CDW}=335$ K. However, the anisotropic properties of CuTe remain to be explored. Here we performed combined transport, polarized infrared reflectivity, and ultrafast pump-probe spectroscopy to investigate the underlying CDW physics of CuTe. Polarized optical measurement clearly revealed that an energy gap gradually forms along the a-axis upon cooling, while optical evidence of gap signature is absent along t…
By using constrained density functional theory modeling, we demonstrate that ultrafast optical pumping unveils hidden charge orders in group VI monolayer transition metal ditellurides. We show that irradiation of the insulating 2H phases stabilizes multiple transient charge density wave orders with light-tunable distortion, periodicity, electronic structure and bandgap. Moreover, optical pumping of the semimetallic 1T' phases generates a transient charge ordered metallic phase composed of 2D diamond clusters. For each transient phase we identify the critical fluence at which it is observed and…
Optical pump-probe spectroscopy is a powerful tool to directly probe the carrier dynamics in materials down to sub-femtosecond resolution. To perform such measurement, while keeping the pump induced perturbation to the sample as small as possible, it is essential to have a detection scheme with high signal to noise ratio. Achieving such high signal to noise ratio is easy with phase sensitive detection based on lock-in-amplifier when a high repetition rate laser is used as the optical pulse source. However such a lock-in-amplifier based method does not work well when a low repetition rate laser…
Inorganic van der Waals bonded semiconductors like transition metal dichalcogenides are subject of intense research due to their electronic and optical properties which are promising for next-generation optoelectronic devices. In this context, understanding the ultrafast carrier dynamics, as well as charge and energy transfer at the interface between metals and semiconductors is crucial and yet quite unexplored. Here, we present an experimental study on how thermally induced ultrafast charge carrier injection affects the exciton formation dynamics in bulk WS2 by employing a pump-push-probe sch…
We have performed a two-color time-resolved magneto-optical Kerr effect (MOKE) study of a ferromagnetic InMnAs/GaSb heterostructure. We observed ultrafast photo-induced changes in the MOKE signal induced by a large density of spin-polarized transient carriers created only within the InMnAs layer using intense 140 fs mid-infrared pulses. Our data clearly demonstrates that magnetic properties, e.g., remanence and coercivity, can be strongly modified. The dependence of these changes on the time delay, pump polarization, pump intensity, and sample temperature is discussed.
Copper (Cu), gold (Au) (111) crystals were illuminated with 120 fs pulses and probed by 600 fs X-ray pulses. Rocking curves were measured versus 267 nm (UV) pump- 0.154 nm probe delay time. Curve width broadening, peak diffracted intensity and angular shift were recorded for the range of UV excitation intensities of 2-8 mJ/cm2 . Observed oscillations in time delay dependences of shift, width and of peak intensity of rocking curves are correlated, as described by acoustic pulse bouncing between crystal surfaces. In (111) Au, acoustic pulse originates from pump absorption layer, and peak intensi…
In recent years, ultrafast pump-probe spectroscopy has provided insightful information about nonequilibrium dynamics of excitations in materials. In a typical experiment of time-resolved x-ray absorption spectroscopy, the systems are excited by a femtosecond laser pulse (pump pulse) followed by an x-ray (probe pulse) after a time delay to measure the absorption spectra of the photoexcited systems. We present a theory for nonequilibrium x-ray absorption spectroscopy in one-dimensional strongly correlated systems. The core hole created by x-ray is modeled as an additional effective potential of …
In high-temperature superconductivity, the process that leads to the formation of Cooper pairs, the fundamental charge carriers in any superconductor, remains mysterious. We use a femtosecond laser pump pulse to perturb superconducting Bi2Sr2CaCu2O8+δ, and study subsequent dynamics using time- and angle-resolved photoemission and infrared reflectivity probes. Gap and quasiparticle population dynamics reveal marked dependencies on both excitation density and crystal momentum. Close to the d-wave nodes, the superconducting gap is sensitive to the pump intensity and Cooper pairs recombine slowly.…
Femtosecond, 8.04 KeV x-ray pulses are used to probe the lattice dynamics of 150 nm Cu (111) single crystal on mica substrate irradiated with 400 nm, 100 fs laser pulses. For pump fluencies below the damage and melting threshold, we observed lattice contraction due to the formation of a blast force, and coherent acoustic phonons with a period of ~69 ps. At larger pump fluence, solid to liquid phase transition, annealing, and recrystallization were measured in real time by monitoring the intensity evolution of the probing fs x-ray rocking curves and agreed with theoretical simulation results. T…
There is still no general consensus on how one can describe the out-of-equilibrium phenomena in matter induced by an ultrashort light pulse. We investigate the pulse-induced dynamics in a layered Dirac semimetal SrMnBi2 by pump-and-probe photoemission spectroscopy. At ~<1 ps, the electronic recovery slowed upon increasing the pump power. Such a bottleneck-type slowing is expected in a two-temperature model (TTM) scheme, although opposite trends have been observed to date in graphite and in cuprates. Subsequently, an unconventional power-law cooling took place at ~100 ps, indicating that spatia…
We demonstrate that the dispersion of surface plasmon polaritons in a periodically perforated gold film can be efficiently manipulated by femtosecond laser pulses with the wavelengths far from the intrinsic resonances of gold. Using a time- and frequency- resolved pump-probe technique we observe shifting of the plasmon polariton resonances with response times from 200 to 800 fs depending on the probe photon energy, through which we obtain comprehensive insight into the electron dynamics in gold. We show that Wood anomalies in the optical spectra provide pronounced resonances in differential tr…
We present a laboratory system for single-shot magneto-optical (MO) imaging of ultrafast magnetization dynamics with high-sensitivity of MO rotation. We create a stack of MO images repeatedly employing a single pair of a pump and defocused probe pulses to induce and visualize MO changes in the sample. Both laser beams are independently wavelength-tunable allowing for a flexible, resonant adjustable two-color pump and probe scheme. To increase the MO contrast the probe beam is spatially filtered. We performed the all-optical switching experiment in Co-doped yttrium iron garnet films (YIG:Co) to…
Revealing Rotational Symmetry Breaking Charge-density Wave Order in Kagome Superconductor (Rb, K)V$_3$Sb$_5$ by Ultrafast Pump-probe Experiments
University of Pennsylvania（宾夕法尼亚大学）；Weizmann Institute of Science（魏茨曼科学研究所）；University of California Santa Barbara（加州大学圣巴巴拉分校）；Oak Ridge National Laboratory（橡树岭国家实验室）
We report femtosecond time-resolved reflectivity measurements of coherent phonons in tellurium performed over a wide range of temperatures (3K to 296K) and pump laser intensities. A totally symmetric A$_{1}$ coherent phonon at 3.6 THz responsible for the oscillations in the reflectivity data is observed to be strongly positively chirped (i.e, phonon time period decreases at longer pump-probe delay times) with increasing photoexcited carrier density, more so at lower temperatures. We show for the first time that the temperature dependence of the coherent phonon frequency is anomalous (i.e, incr…
Optical pump-probe experiments carried out in the time domain reveal both the intrinsic low energy dynamics and its connections to higher energy excitations in correlated electron systems. In this work, we propose two microscopic mechanisms for the optical generation of coherent magnetic modes in van der Waals magnets, and derive the corresponding effective light-spin interactions: either through pumping atomic orbital excitations resonantly or via a light-induced Floquet spin Hamiltonian, the ground state of the system is driven out of equilibrium. The subsequent long-time relaxational dynami…
Recently, the switching between the different charge-ordered phases of 1T-TaS2 has been probed by ultrafast techniques, revealing unexpected phenomena such as "hidden" metastable states and peculiar photoexcited charge patterns. Here, we apply broadband pump-probe spectroscopy with varying excitation energy to study the ultrafast optical properties of 1T-TaS2 in the visible regime. By scanning the excitation energy in the near-IR region we unravel the coupling between different charge excitations and the low-lying charge-density wave state. We find that the amplitude mode of the charge-density…
We have developed a novel multiscale computational scheme to describe coupled dynamics of light electromagnetic field with electrons and atoms in crystalline solids, where first-principles molecular dynamics based on time-dependent density functional theory is used to describe the microscopic dynamics. The method is applicable to wide phenomena in nonlinear and ultrafast optics. To show usefulness of the method, we apply it to a pump-probe measurement of coherent phonon in diamond where a Raman amplification takes place during the propagation of the probe pulse.
We calculate the time evolution of the transient reflection signal in an MoS$_2$ monolayer on a SiO$_2$/Si substrate using first-principles out-of-equilibrium real-time methods. Our simulations provide a simple and intuitive physical picture for the delayed, yet ultrafast, evolution of the signal whose rise time depends on the excess energy of the pump laser: at laser energies above the A- and B-exciton, the pump pulse excites electrons and holes far away from the K valleys in the first Brillouin zone. Electron-phonon and hole-phonon scattering lead to a gradual relaxation of the carriers towa…
