Photoexcited Carriers In Graphene Research Articles

Ultrafast Graphene-Plasmonic Hybrid Metasurface Saturable Absorber with Low Saturation Fluence.

Exploring emerging materials with enhanced optical nonlinearities at low power levels with ultrafast response and small footprints is of great interest for information processing, communication, sensing, and quantum systems. Recent progress on nonlinear metamaterials and metasurfaces suggests promising solutions to overcome the limitations of nonlinear materials in nature. Here we present a design concept for highly enhanced saturable absorption effect based on subwavelength-thick (<1/5λ0) hybrid graphene-plasmonic metasurface structures in infrared wavelengths. Our theoretical and experimental results demonstrated that, by exciting nonequilibrium carriers inside nanoscale hotspots, one could not only enhance the saturable absorption in graphene, but also reduce the saturation fluence by over 3 orders of magnitude (from ∼1 mJ/cm2 to ∼100 nJ/cm2). Our pump-probe measurement results suggested an ultrashort saturable absorption recovery time (<60 fs), which is ultimately determined by the relaxation dynamics of photoexcited carriers in graphene. We also observed pulse narrowing effects in our devices based on the autocorrelation measurement results. Such design concepts can be tailored via structure engineering to operate in broader wavelength ranges up to mid- and far- infrared spectral regions. These ultrafast low-saturation fluence saturable absorber designs can enable low-threshold, compact, self-starting mode-locked lasers, laser pulse shaping, and high-speed optical information processing.

Ultrafast Optical Modulation of Harmonic Generation in Two-Dimensional Materials.

The modulation of optical harmonic generation in two-dimensional (2D) materials is of paramount importance in nanophotonic and nano-optoelectronic devices for their applications in optical switching and communication. However, an effective route with ultrafast modulation speed, ultrahigh modulation depth, and broad operation wavelength range is awaiting a full exploration. Here, we report that an optical pump can dynamically modulate the third harmonic generation (THG) of a graphene monolayer with a relative modulation depth above 90% at a time scale of 2.5 ps for a broad frequency ranging from near-infrared to ultraviolet. Our observation, together with the real-time, time-dependent density functional theory (TDDFT) simulations, reveals that this modulation process stems from nonlinear dynamics of the photoexcited carriers in graphene. The superior performance of the nonlinear all-optical modulator based on 2D materials paves the way for its potential applications including nanolasers and optical communication circuits.

Relevance of collinear processes to the ultrafast dynamics of photoexcited carriers in graphene

Abstract The importance of interband transitions on the ultrafast relaxation process in photoexcited pristine graphene is evaluated by means of an ensemble Monte Carlo simulator. Impact ionization and Auger recombination in the collinear limit are considered, together with phonon-induced generation and recombination and intraband scattering mechanisms. The results show that collinear impact ionization is dominant in the first 100 femtoseconds, creating an important excess carrier population that is finally eliminated in the picosecond scale, together with the photoexcited population, by Auger and optical phonon-assisted recombination. The hot phonon effect is also important, stimulating phonon absorption and indirectly reducing the net collinear recombination in the hundreds of femtosecond range. The substrate type is an important factor, appeasing collinear impact ionization via screening and creating additional cooling channels that speed up the relaxation process. The results evidence that interband collinear generation processes are critical to explain the fastest stages of the relaxation process in graphene.

Ultrafast saturable absorption dynamics in hybrid graphene/Si3N4 waveguides

We study the nonlinear optical properties of graphene integrated onto Si3N4 waveguides under picosecond and subpicosecond pulsed excitation at telecom wavelength. Saturable absorption of graphene under guided-mode excitation is measured, and the temporal effects related to the photoexcited carrier dynamics in graphene are highlighted. Thereafter, a model of photoexcited carriers in graphene is implemented into the nonlinear Schrodinger equation in order to simulate the pulse propagation across the hybrid graphene/Si3N4 waveguide. This allows us to extract phenomenological parameters of graphene saturable absorption in chip-based devices, which could provide some guidelines for the design of nonlinear elements in photonic integrated circuits.

Pulse shaping in the terahertz frequency range for the control of photo-excited carriers in graphene

The shape of a few-cycle terahertz (THz) laser pulse can be optimized to provide control over conduction band populations in graphene. To demonstrate this control in a theoretical way, a spectral parametrization of the driving pulse using $B$-splines is used in order to obtain experimentally realistic pulses of bandwidth $\sim$ 30 THz. Optimization of the spectral shape is performed via differential evolution, using the $B$-splines expansion coefficients as decision variables. Numerical results show the possibility of changing the carrier density in graphene by a factor of 4 for a fixed pulse energy. In addition, we show that it is possible to selectively suppress or enhance multi-photon absorption features by optimizing over narrow windows in reciprocal space. The application of pulse shaping to the control of scattering mechanisms in graphene is also discussed.

Non-destructive measurement of photoexcited carrier transport in graphene with ultrafast grating imaging technique

Graphene has great potential for fabrication of ultrafast opto-electronics, in which relaxation and transport of photoexcited carriers determine device performance. Even though ultrafast carrier relaxation in graphene has been studied vigorously, transport properties of photoexcited carriers in graphene are largely unknown. In this work, we utilize an ultrafast grating imaging technique to measure lifetime (τr), diffusion coefficient (D), diffusion length (L) and mobility (μ) of photoexcited carriers in mono- and multi-layer graphene non-invasively. In monolayer graphene, D∼10,000 cm2/s and μ∼120,000 cm2/V have been observed, both of which decrease drastically in multilayer graphene, indicating that the remarkable transport properties in monolayer graphene originate from its unique Dirac-Cone energy structure. Mobilities of photoexcited carriers measured here are several times larger than the Hall and Field-Effect mobilities reported in literature (<15,000 cm2/V), due to the high energy of photoexcited carriers. Our results indicate the importance of obtaining monolayer graphene to realize high-performance graphene devices, as well as the necessity to use transport properties of photoexcited carriers for predicting the performance of graphene-based opto-electronics.

Defect-induced supercollision cooling of photoexcited carriers in graphene.

Defects play a fundamental role in the energy relaxation of hot photoexcited carriers in graphene, thus a complete understanding of these processes are vital for improving the development of graphene devices. Recently, it has been theoretically predicted and experimentally demonstrated that defect-assisted acoustic phonon supercollision, the collision between a carrier and both an acoustic phonon and a defect, is an important energy relaxation process for carriers with excess energy below the optical phonon emission. Here, we studied samples with defects optically generated in a controlled manner to experimentally probe the supercollision model as a function of the defect density. We present pump and probe transient absorption measurements showing that the decay time decreases as the density of defect increases as predicted by the supercollision model.

Non-equilibrium Dirac carrier dynamics in graphene investigated with time- and angle-resolved photoemission spectroscopy.

We have used time- and angle-resolved photoemission spectroscopy (tr-ARPES) to assess the influence of many-body interactions on the Dirac carrier dynamics in graphene. From the energy-dependence of the measured scattering rates we directly determine the imaginary part of the self-energy, visualizing the existence of a relaxation bottleneck associated with electron-phonon coupling. A comparison with static line widths obtained by high-resolution ARPES indicates that the dynamics of photo-excited carriers in graphene are solely determined by the equilibrium self-energy. Furthermore, the subtle interplay of different many-body interactions in graphene may allow for carrier multiplication, where the absorption of a single photon generates more than one electron-hole pair via impact ionization. We find that, after photo-excitation, the number of carriers in the conduction band along the ΓK-direction keeps increasing for about 40 fs after the pump pulse is gone. A definite proof of carrier multiplication in graphene, however, requires a more systematic study, carefully taking into account the contribution of momentum relaxation on the measured rise time.

Diffusion of photoexcited carriers in graphene

The diffusion of electron-hole pairs, which are excited in an intrinsic graphene by the ultrashort focused laser pulse in mid-IR or visible spectral region, is described for the cases of peak-like or spread over the passive region distributions of carriers. The spatio-temporal transient optical response on a high-frequency probe beam appears to be strongly dependent on the regime of diffusion and can be used for verification of the elasic relaxation mechanism. Sign flip of the differential transmission coefficient takes place due to interplay of the carrier-induced contribution and weak dynamic conductivity of undoped graphene.

Cooling of photoexcited carriers in graphene by internal and substrate phonons

We investigate the energy relaxation of hot carriers produced by photoexcitation of graphene through coupling to both intrinsic and remote (substrate) surface polar phonons using the Boltzmann equation approach. We find that the energy relaxation of hot photocarriers in graphene on commonly used polar substrates, under most conditions, is dominated by remote surface polar phonons. We also calculate key characteristics of the energy relaxation process, such as the transient cooling time and steady state carrier temperatures and photocarriers densities, which determine the thermoelectric and photovoltaic photoresponse, respectively. Substrate engineering can be a promising route to efficient optoelectronic devices driven by hot carrier dynamics.

Dynamics of photoexcited carriers in graphene

The nonequilibrium dynamics of carriers and phonons in graphene is investigated by solving the microscopic kinetic equations with the carrier-phonon and carrier-carrier Coulomb scatterings explicitly included. The Fermi distribution of hot carriers are found to be established within 100 fs and the temperatures of electrons in the conduction and valence bands are very close to each other, even when the excitation density and the equilibrium density are comparable, thanks to the strong inter-band Coulomb scattering. Moreover, the temporal evolutions of the differential transmission obtained from our calculations agree with the experiments by Wang et al. [Appl. Phys. Lett. 96, 081917 (2010)] and Hale et al. [Phys. Rev. B 83, 121404 (2011)] very well, with two distinct differential transmission relaxations presented. We show that the fast relaxation is due to the rapid carrier-phonon thermalization and the slow one is mainly because of the slow decay of hot phonons. In addition, it is found that the temperatures of the hot phonons in different branches are different and the temperature of hot carriers can be even lower than that of the hottest phonons. Finally, we show that the slow relaxation rate exhibits a mild valley in the excitation density dependence and is linearly dependent on the probe-photon energy.

Very Slow Cooling Dynamics of Photoexcited Carriers in Graphene Observed by Optical-Pump Terahertz-Probe Spectroscopy

Using optical-pump terahertz-probe spectroscopy, we study the relaxation dynamics of photoexcited carriers in graphene at different substrate temperatures. We find that at lower temperatures the tail of the relaxation transients measured by the differential probe transmission become slower, extending beyond several hundred picoseconds below 50 K. We interpret the observed relaxation transients as resulting from the cooling of the photoexcited carriers via phonon emission. The slow cooling of the photoexcited carriers at low temperatures is attributed to the bulk of the electron and hole energy distributions moving close enough to the Dirac point that both intraband and interband scattering of carriers via optical phonon emission become inefficient for removing heat from the carriers. Our model, which includes intraband carrier scattering and interband carrier recombination and generation, agrees very well with the experimental observations.

Broadband Light-Induced Absorbance Change in Multilayer Graphene

We report the ultrafast light-induced absorbance change in CVD-grown multilayer graphene. Using femtosecond pump-probe measurements in 1100-1800 nm spectral range, we revealed broadband absorbance change when the probe photon energy was higher than that of the pump photon. The observed phenomenon is interpreted in terms of the Auger recombination and impact ionization playing a significant role in the dynamics of photoexcited carriers in graphene.

Carrier recombination and generation rates for intravalley and intervalley phonon scattering in graphene

Electron-hole generation and recombination rates for intravalley and intervalley phonon scattering in graphene are presented. The transverse and the longitudinal optical phonon modes E2g modes near the zone center point contribute to intravalley interband carrier scattering. At the zone edge KK point, only the transverse optical phonon mode A 1 mode contributes significantly to intervalley interband scattering with recombination rates faster than those due to zone-center phonons. The calculated recombination times range from less than a picosecond to more than hundreds of picoseconds and are strong functions of temperature and electron and hole densities. The theoretical calculations agree well with experimental measurements of the recombination rates of photoexcited carriers in graphene.