Ultrafast optical pump-probe spectroscopy measurement on monolayer graphene observes significant optical nonlinearities. We show that strongly photoexcited graphene monolayers with 35 fs pulses quasi-instantaneously build up a broadband, inverted Dirac fermion population. Optical gain emerges and directly manifests itself via a negative conductivity at the near-infrared region for the first 200fs, where stimulated emission completely compensates absorption loss in the graphene layer. To quantitatively investigate this transient, extremely dense photoexcited Dirac-fermion state, we construct a two-chemical-potential model, in addition to a time-dependent transient carrier temperature above lattice temperature, to describe the population inverted electronic state metastable on the time scale of tens of femtoseconds generated by a strong exciting pulse. The calculated transient optical conductivity reveals a complete bleaching of absorption, which sets the saturation density during the pulse propagation. Particularly, the model calculation reproduces the negative optical conductivity at lower frequencies in the states close to saturation, corroborating the observed femtosecond stimulated emission and optical gain in the wide near-infrared window.
Black phosphorus has recently emerged as a promising material for high performance electronic and optoelectronic device for its high mobility, tunable mid-infrared bandgap and anisotropic electronic properties. Dynamical evolution of photo excited carriers and its induced change of transient electronic properties are critical for materials' high field performance, but remains to be explored for black phosphorus. In this work, we perform angle resolved transient reflection spectroscopy to study the dynamical evolution of anisotropic properties of black phosphorus under photo excitation. We find…
Terahertz (THz) Faraday rotation measurements were performed to investigate carrier dynamics in p-type CVD graphene. We used static and time-resolved polarization-sensitive THz transmission measurements in a magnetic field to probe free carriers in GaAs, InP and Graphene. Static measurements probe the equilibrium carrier density and momentum scattering rate. Time-resolved (optical pump/THz probe) measurements probe the change in these quantities following photoexcitation. In a typical CVD graphene sample we found that 0.5ps following photoexcitation with 1*10^13 photons/cm2 pulses at 800nm the…
The saga of the primary photoexcitations in $π$-conjugated polymers has been a source of extraordinary scientific curiosity that has lasted for more than three decades. From soliton excitations in trans-polyacetylene, to singlet and triplet excitons and polarons in other polymers, to charge transfer excitons in blends of polymers and fullerenes, the field has been rich with a variety of different photoexcitation species. Here we show the photogeneration of a novel primary intrachain photoexcitation species, namely the composite multi-exciton (CME) in $π$-conjugated donor-acceptor (DA)-copolyme…
We present a detailed investigation of ultrafast (subpicosecond) exciton dynamics in the lattice model of a donor/acceptor heterojunction. Exciton generation by means of a photoexcitation, exciton dissociation, and further charge separation are treated on equal footing. The experimentally observed presence of space-separated charges at $\lesssim 100$ fs after the photoexcitation is usually attributed to ultrafast transitions from excitons in the donor to charge transfer and charge separated states. Here, we show, however, that the space-separated charges appearing on $\lesssim 100$-fs time sca…
We study the generation of THz radiation from the acceleration of ultrafast photoexcited charge carriers in graphene in the presence of a DC electric field. Our model is based on calculating the transient current density from the time-dependent distribution function which is determined using the Boltzmann transport equation within a relaxation time approximation. We include the time-dependent generation of carriers by the pump pulse by solving for the carrier generation rate using the Bloch equations in the rotating wave approximation (RWA). The linearly polarized pump pulse generates an aniso…
Through the integration of semiconductors or complex oxides into metal resonators, tunable metamaterials have been achieved by a change of environment using an external stimulus. Metals provide high conductivity to realize a strong resonant response in metamaterials; however, they contribute very little to the tunability. The complex conductivity in high-temperature superconducting films is highly sensitive to external perturbations, which provides new opportunities in achieving tunable metamaterials resulting directly from the resonant elements. Here we demonstrate ultrafast dynamical tuning …
The transient evolution of carriers in an intrinsic graphene under ultrafast excitation, which is caused by the collisionless interband transitions, is studied theoretically. The energy relaxation due to the quasielastic acoustic phonon scattering and the interband generation-recombination transitions due to thermal radiation are analyzed. The distributions of carriers are obtained for the limiting cases when carrier-carrier scattering is negligible and when the intercarrier scattering imposes the quasiequilibrium distribution. The transient optical response (differential reflectivity and tran…
We investigate the non-linear response and energy absorption in bulk silicon irradiated by intense 12-fs near-infrared laser pulses. Depending on the laser intensity, we distinguish two regimes of non-linear absorption of the laser energy: for low intensities, energy deposition and photoionization involve perturbative three-photon transition through the direct bandgap of silicon. For laser intensities near and above 10$^{14}$ W/cm$^2$, corresponding to photocarrier density of order 10$^{22}$ cm$^{-3}$, we find that absorption at near-infrared wavelengths is greatly enhanced due to excitation o…
Using ultrafast optical pump-probe spectroscopy, we study the relaxation dynamics of hot optical phonons in few-layer and multi-layer graphene films grown by epitaxy on silicon carbide substrates and by chemical vapor deposition on nickel substrates. In the first few hundred femtoseconds after photoexcitation, the hot carriers lose most of their energy to the generation of hot optical phonons which then present the main bottleneck to subsequent carrier cooling. Optical phonon cooling on short time scales is found to be independent of the graphene growth technique, the number of layers, and the…
Direct observation of ultrafast defect-bound and free exciton dynamics in defect-engineered WS$_2$ monolayers
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory（橡树岭国家实验室纳米材料科学中心）；Center for Integrated Nanotechnologies, Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室集成纳米技术中心）；Honda Research Institute USA Inc.（本田美国研究院）；Department of Materials Science and Engineering, University of Tennessee, Knoxville（田纳西大学诺克斯维尔分校材料科学与工程系）
The use of femtosecond laser pulses to impulsively excite thermal and mechanical transients in matter has led, in the last years, to the development of picosecond acoustics. Recently, the pump-probe approach has been applied to nano-engineered materials to optically generate and detect acoustic waves in the GHz-THz frequency range. In this paper, we review the latest advances on ultrafast generation and detection of thermal gradients and pseudo-surface acoustic waves in two-dimensional lattices of metallic nanostructures. Comparing the experimental findings to the numeric analysis of the full …
In order to determine the role of non-thermal transport of hot carriers which is decisive for the dissipation of energy in condensed matter we performed time-resolved broadband femtosecond transient reflectivity measurements on $7-197 \mathrm{nm}$ thick Bi(111) films epitaxially grown on Si(111). We monitored the behavior of the Fourier amplitude and the central frequency of the coherent $A_\mathrm{1g}$ phonon mode as function of the incident fluence, film thickness, and probe wavelength in the range of $580 -700 \mathrm{nm}$. The frequency redshift that follows photoexcitation was used as a r…
We use time- and angle-resolved photoemission spectroscopy (tr-ARPES) to investigate ultrafast charge transfer in an epitaxial heterostructure made of monolayer WS$_2$ and graphene. This heterostructure combines the benefits of a direct gap semiconductor with strong spin-orbit coupling and strong light-matter interaction with those of a semimetal hosting massless carriers with extremely high mobility and long spin lifetimes. We find that, after photoexcitation at resonance to the A-exciton in WS$_2$, the photoexcited holes rapidly transfer into the graphene layer while the photoexcited electro…
We investigate the hot carrier dynamics of ZrTe$_5$ by ultrafast time-resolved optical reflectivity. Our results reveal a phonon-mediated across-gap recombination, consistent with its temperature-dependent gap nature as observed previously by photoemission. In addition, two distinct relaxations with a kink feature right after initial photoexcitation are well resolved, suggesting the complexity of electron thermalization process. Our findings indicate that correlated many-body effects play important role for the transient dynamics of ZrTe$_5$.
We investigate theoretically the dynamic multiferroic response of coupled ferroelectric/ferromagnetic composites upon excitation by a photo-induced acoustic strain pulse. Two magnetoelectric mechanisms are considered: interface strain- and charge-mediated magnetoelectric couplings. The former results in demagnetization, depolarization and repolarization within tens of picoseconds via respectively magnetostriction and piezoelectricity. Charge magnetoelectric interaction affects the ferroelectric/ferromagnetic feedback response leading to magnetization recovery. Experimental realization based on…
Time-resolved pump-probe measurements were made at variable heat accumulation in Co/Pd superlattices. Heat accumulation increases the baseline temperature and decreases the equilibrium magnetization. Transient ultrafast demagnetization first develops with higher fluence in parallel with strong equilibrium thermal spin fluctuations. The ultrafast demagnetization is then gradually removed as the equilibrium temperature approaches the Curie temperature. The transient magnetization time-dependence is fit well with the spin-flip scattering model.
It is known that ultrafast laser pulses can be used to deterministically switch magnetisation and create skyrmions, however the deterministic creation of a single Néel skyrmion after ultrafast demagnetisation remains an open question. Here we show domain wall skyrmions also emerge in systems with broken inversion symmetry after exposure to an ultrafast laser pulse, carrying an integer topological charge. Whilst domain wall skyrmions do not appear in the relaxed state due to quick thermal decay following an Arrhenius law, they play a key role in controlling the final skyrmion population through…
We demonstrate an ultrafast reversible modulation of resonant terahertz (THz) response in strongly photoexcited metamaterials. The transient spectral-temporal response of the dipole transition ~1.6 THz exhibits a distinct non-monotonic variation as a function of pump fluence. The transition energy shift, strength, spectral width and density-dependent ultrafast relaxation manifest a remarkable re-emergence of the resonances after initial quenching. Our simulation, incorporating the first-order diffraction from the photoinduced transient grating, reproduces the salient features, providing a new …
In this article, we study non-radiative and radiative relaxation processes in a hybrid formed by combining Ag nanoparticle (NP) and CdTe quantum dots (QD) using transient transmission spectroscopy. The ultrafast transient transmission of hybrid, when excited at 400 nm, shows a faster recovery of hot electrons at a shorter time scale (few picoseconds) while it shows a slower recovery at a longer time scale (few tens of picoseconds). Further, it is found that the contribution of CdTe QD to the transient transmission is increased in the presence of Ag NP. However, the radiative relaxation in CdTe…
Ultrafast carrier dynamics in the topological insulator Bi2Se3 have recently been intensively studied using a variety of techniques. However, we are not aware of any successful experiments exploiting transient absorption (TA) spectroscopy for these purposes. Here we demonstrate that if the ~730 nm wavelength pumping (~1.7 eV photon energy) is applied to ultrathin Bi2Se3 films, TA spectra cover the entire visible region, thus unambiguously pointing to two-photon excitation (~3.4 eV). The carrier relaxation dynamics is found to be governed by the polar optical phonon cascade emission occurring i…
Ultrafast carrier relaxation in the 2D topological insulator (TI) Bi2Se3 [gapped Dirac surface states (SS)] and how it inherits ultrafast relaxation in the 3D TI Bi2Se3 (gapless Dirac SS) remains a challenge for developing new optoelectronic devices based on these materials. Here ultrashort (100 fs) pumping pulses of ~340 nm wavelength (~3.65 eV photon energy) were applied to study ultrafast electron relaxation in the 2D TI Bi2Se3 films with a thickness of 2 and 5 quintuple layers (~2 and ~5 nm, respectively) using transient absorption (TA) spectroscopy in the ultraviolet-visible spectral regi…
In spin-based electronics, information is encoded by the spin state of electron bunches. Processing this information requires the controlled transport of spin angular momentum through a solid, preferably at frequencies reaching the so far unexplored terahertz (THz) regime. Here, we demonstrate, by experiment and theory, that the temporal shape of femtosecond spin-current bursts can be manipulated by using specifically designed magnetic heterostructures. A laser pulse is employed to drive spins from a ferromagnetic Fe thin film into a nonmagnetic cap layer that has either low (Ru) or high (Au) …
Experimental investigations of ultrafast magnetization dynamics increasingly employ resonant magnetic spectroscopy in the ultraviolet spectral range. Besides allowing to disentangle the element-specific transient response of functional magnetic systems, these techniques also promise to access attosecond to few-femtosecond dynamics of spin excitations. Here, we report on a systematic study of transient magnetic circular dichroism (MCD) on the transition metals Fe, Co and Ni as well as on a FeNi and GdFe alloy and reveal a delayed onset between the electronic and magnetic response. Supported by …
