High intensity laser pulses were recently shown to induce a population inverted transient state in graphene [T. Li et al. Phys. Rev. Lett. 108, 167401 (2012)]. Using a combination of hydrodynamic arguments and a kinetic theory we determine the post-transient state relaxation of hot, dense, population inverted electrons towards equilibrium. The cooling rate and charge-imbalance relaxation rate are determined from the Boltzmann-equation including electron-phonon scattering. We show that the relaxation of the population inversion, driven by inter-band scattering processes, is much slower than the relaxation of the electron temperature, which is determined by intra-band scattering processes. This insight may be of relevance for the application of graphene as an optical gain medium.
Observable effects due to trembling motion (Zitterbewegung, ZB) of charge carriers in bilayer graphene, monolayer graphene and carbon nanotubes are calculated. It is shown that, when the charge carriers are prepared in the form of gaussian wave packets, the ZB has a transient character with the decay time of femtoseconds in graphene and picoseconds in nanotubes. Analytical results for bilayer graphene allow us to investigate phenomena which accompany the trembling motion. In particular, it is shown that the transient character of ZB in graphene is due to the fact that wave subpackets related t…
A graphene quantum dot under intense ac field and static low magnetic field is investigated. From a tight-binding perspective, applying a Fourier-Floquet transformation and renormalization process, we observe that graphene -intrinsically anisotropic- reveals field polarization signatures in the quasi-density of states. For the ac field polarized along the armchair direction, the dressed electronic structure shows an emergent property: an ac field induced quantum ring. This is inferred by the orientation-dependent formation of a miniband of energy states periodically modulated with increasing m…
Using transient absorption (TA) microscopy as a hot electron thermometer we show disorder-assisted acoustic-phonon supercollisions (SCs) best describes the rate-limiting relaxation step in graphene over a wide range of lattice temperatures ($T_l=$5-300 K), Fermi energies ($E_F=\pm0.35$ eV), and optical probe energies (~0.3 - 1.1 eV). Comparison with simultaneously collected transient photocurrent, an independent hot electron thermometer, confirms the rate-limiting optical and electrical response in graphene are best described by the SC-heat dissipation rate model, $H=A(T^3_e- T^3_l)$. Our data…
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 pseudospin-dependent density-energy relation (whose differential with respect to energy is density of states) of a monolayer graphene under intense terahertz laser field by exactly solving the time-dependent Schrödinger equation with help of Floquet's theorem. We find that psedospin polarization can be induced by a circular polarized terahertz laser field. The psedospin polarization in K and K$^{\prime}$ valleys can be exactly opposite sign when the electron densities in these two calleys are equivalent. Further more, we find that the psedospin polarization can be manipulate…
Optical responses of graphene in the presence of intense circularly and linearly polarized terahertz fields are investigated based on the Floquet theory. We examine the energy spectrum and density of states. It is found that gaps open in the quasi-energy spectrum due to the single-photon/multi-photon resonances. These quasi-energy gaps are pronounced at small momentum, but decrease dramatically with the increase of momentum and finally tend to be closed when the momentum is large enough. Due to the contribution from the states at large momentum, the gaps in the density of states are effectivel…
We use simulations to examine current saturation in sub-micron graphene transistors on SiO2/Si. We find self-heating is partly responsible for current saturation (lower output conductance), but degrades current densities >1 mA/um by up to 15%. Heating effects are reduced if the supporting insulator is thinned, or in shorter channel devices by partial heat sinking at the contacts. The transient behavior of such devices has thermal time constants of ~30-300 ns, dominated by the thickness of the supporting insulator and that of device capping layers (a behavior also expected in ultrathin body SOI…
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 …
A monolayer of graphene irradiated with circularly polarized light suggests a unique platform for surface electromagnetic wave (plasmon-polariton) manipulation. In fact, the time periodicity of the Hamiltonian leads to a geometric Aharonov-Anandan phase and results in a photovoltaic Hall effect in graphene, creating off-diagonal components of the conductivity tensor. The latter drastically changes the dispersion relation of surface plasmon-polaritons, leading to hybrid wave generation. In this paper we present a systematic and self-contained analysis of the hybrid surface waves obtained from M…
Graphene exhibits extremely strong optical nonlinearity when a strong perpendicular magnetic field is applied, the response current shows strong field dependence even for moderate light intensity, and the perturbation theory fails. We nonperturbatively calculate full optical conductivities induced by a periodic field in an equation-of-motion framework based on the Floquet theorem, with the scattering described phenomenologically. The nonlinear response at high fields is understood in terms of the dressed electronic states, or Floquet states, which is further characterized by the optical conduc…
A transient femtosecond population inversion in graphene was recently reported by Li et al., Phys. Rev. Lett. 108, 167401 (2012). Based on a microscopic theory we clarify the underlying microscopic mechanism: Transient gain and population inversion in graphene occurs due to a complex interplay of strong optical pumping and carrier cooling that fills states close to the Dirac point giving rise to a relaxation bottleneck. The subsequent femtosecond decay of the optical gain is mainly driven by Coulomb-induced Auger recombination.
We investigated ultrafast carrier dynamics in graphene with near-infrared transient absorption measurement after intense half-cycle terahertz pulse excitation. The terahertz electric field efficiently drives the carriers, inducing large transparency in the near-infrared region. Theoretical calculations using the Boltzmann transport equation quantitatively reproduce the experimental findings. This good agreement suggests that the intense terahertz field should promote remarkable impact ioniza- tion process, which leads to suppression of optical phonon emission and results in efficient carrier t…
We theoretically study the electronic and transport properties of two graphene layers vertically coupled by an insulating layer under the influence of a time-periodic external light field. The non-adiabatic driving induces excitations of electrons and a redistribution of the occupied states which is manifested in the opening of gaps in the quasienergy spectrum of graphene. When a voltage is applied between the top and bottom graphene layers, the photo-induced nonequilibrium occupation modifies the transport properties of the contact. We investigate the electronic and transport properties of th…
Mechanism of transient population inversion in graphene with multi-splitted (interdigitated) top-gate and grounded back gate is suggested and examined for the mid-infrared (mid-IR) spectral region. Efficient stimulated emission after fast lateral spreading of carriers due to drift-diffusion processes is found for the case of a slow electron-hole recombination in the passive region. We show that with the large gate-to-graphene distance the drift process always precedes the diffusion process, due to the ineffective screening of the inplane electric field by the gates. Conditions for lasing with …
We present a microscopic explanation of the controversially discussed transient negative differential transmission observed in degenerate optical pump-probe measurements in graphene. Our approach is based on the density matrix formalism allowing a time- and momentum-resolved study of carrier-light, carrier-carrier, and carrier-phonon interaction on microscopic footing. We show that phonon-assisted optical intraband transitions give rise to transient absorption in the optically excited hot carrier system counteracting pure absorption bleaching of interband transitions. While interband transitio…
We review our recent time- and angle-resolved photoemission spectroscopy experiments, which measure the transient electronic structure of optically driven graphene. For pump photon energies in the near infrared ($\hbarω_{\text{pump}}=950$meV) we have discovered the formation of a population-inverted state near the Dirac point, which may be of interest for the design of THz lasing devices and optical amplifiers. At lower pump photon energies ($\hbarω_{\text{pump}}<400$meV), for which interband absorption is not possible in doped samples, we find evidence for free carrier absorption. In addition…
It is a fact that the minimal conductivity $σ_0$ of most graphene samples is larger than the well-established universal value for ideal graphene $4e^2/πh$; in particular, larger by a factor $\gtrsimπ$. Despite intense theoretical activity, this fundamental issue has eluded an explanation so far. Here we present fully atomistic quantum mechanical estimates of the graphene minimal conductivity where electron-electron interactions are considered in the framework of density functional theory. We show the first conclusive evidence of the dominant role on the minimal conductivity of charged impuriti…
Thermal management is an important challenge in modern electronics, avionics, automotive, and energy storage systems. While passive thermal solutions (like heat sinks or heat spreaders) are often used, actively modulating heat flow (e.g. via thermal switches or diodes) would offer additional degrees of control over the management of thermal transients and system reliability. Here we report the first thermal switch based on a flexible, collapsible graphene membrane, with low operating voltage, < 2 V. We also employ active-mode scanning thermal microscopy (SThM) to measure the device behavior an…
In this work we develop a time-dependent extension of the Landauer-Büttiker approach to study transient dynamics in time-dependent quantum transport through molecular junctions. A key feature of the approach is that it provides a closed integral expression for the time-dependence of the density matrix of the molecular junction after switch-on of a bias or gate potential which can be evaluated without the necessity of propagating individual single-particle orbitals. This allows for the study of time-dependent transport in large molecular systems coupled to wide band leads. As an application of …
Response of electronic systems in intense lights (AC electric fields) to DC source-drain fields is formulated with the Floquet method. We have then applied the formalism to graphene, for which we show that a non-linear effect of a circularly polarized light can open a gap in the Dirac cone, which leads to a photo-induced dc Hall current. This is numerically confirmed for a graphene ribbon attached to electrodes with the Keldysh Green's function.
Intense light-matter interactions and unique structural and electrical properties make Van der Waals heterostructures composed by Graphene (Gr) and monolayer transition metal dichalcogenides (TMD) promising building blocks for tunnelling transistors, flexible electronics, as well as optoelectronic devices, including photodetectors, photovoltaics and quantum light emitting devices (QLEDs), bright and narrow-line emitters using minimal amounts of active absorber material. The performance of such devices is critically ruled by interlayer interactions which are still poorly understood in many resp…
We show that strongly photoexcited graphene monolayers with 35fs pulses quasi-instantaneously build up a broadband, inverted Dirac fermion population. Optical gain emerges and directly manifests itself via a negative optical conductivity for the first 200fs, where stimulated emission completely compensates absorption loss in the graphene layer. Our experiment-theory comparison with two distinct electron and hole chemical potentials reproduce absorption saturation and gain at 40fs, revealing, particularly, the evolution of the transient state from a hot classical gas to a dense quantum fluid wi…
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 dynami…
Higher harmonic generation in plane graphene quantum dots initiated by intense coherent radiation is investigated, using dynamical Hartree-Fock mean-field theory. A microscopic theory describing the extreme nonlinear optical response of plane graphene quantum dots is developed. The closed set of differential equations for the single-particle density matrix at the graphene quantum dots-strong laser field multiphoton interaction is solved numerically. The obtained solutions indicate the significance of the type of edge and lateral size, and bandgap and laser field strength in the high harmonic g…
Using ultrafast optical pump-probe spectroscopy, we have measured carrier relaxation times in epitaxial graphene layers grown on SiC wafers. We find two distinct time scales associated with the relaxation of nonequilibrium photogenerated carriers. An initial fast relaxation transient in the 70-120 fs range is followed by a slower relaxation process in the 0.4-1.7 ps range. The slower relaxation time is found to be inversely proportional to the degree of crystalline disorder in the graphene layers as measured by Raman spectroscopy. We relate the measured fast and slow time constants to carrier-…
We identify and describe how intense short light pulses couple to massless Dirac fermions in two-dimensional systems. The ensuing excitation dynamics exhibits unusual scaling with the wavelength of the light due the linear dispersion of the band structure and the fact that light coupling is efficient only close to the Dirac points. We exploit these features to achieve valley polarization of more than 70 % with simple pulse shapes. Quantitative results are given for pristine graphene.
The possibility of transporting spin information over long distances in graphene, owing to its small intrinsic spin-orbit coupling (SOC) and the absence of hyperfine interaction, has led to intense research into spintronic applications. However, measured spin relaxation times are orders of magnitude smaller than initially predicted, while the main physical process for spin dephasing and its charge-density and disorder dependences remain unconvincingly described by conventional mechanisms. Here, we unravel a spin relaxation mechanism for nonmagnetic samples that follows from an entanglement bet…
In this paper, optical and electronic properties of diamond shaped graphene quantum dots (DQDs) have been studied by employing large-scale electron-correlated calculations. The computations have been performed using the π-electron Pariser-Parr-Pople model Hamiltonian, which incorporates long-range Coulomb interactions. The influence of electron-correlation effects on the ground and excited states has been included by means of the configuration-interaction approach, used at various levels. Our calculations have revealed that the absorption spectra are red-shifted with the increasing sizes of qu…
When two sheets of graphene stack in a twisted bilayer graphene (tBLG) configuration, the resulting constrained overlap between interplanar 2p orbitals produce angle-tunable electronic absorption resonances. Using a novel combination of multiphoton transient absorption (TA) microscopy and TEM, we resolve the resonant electronic structure, and ensuing electronic relaxation inside single tBLG domains. Strikingly, we find that the transient electronic population in resonantly excited tBLG domains is enhanced many fold, forming a major electronic relaxation bottleneck. 2-photon TA microscopy shows…
The transient response of an intrinsic graphene, which is caused by the ultrafast interband transitions, is studied theoretically for the range of pumping correspondent to the saturated absorption regime. Spectral and temporal dependencies of the photoexcited concentration as well as the transmission and relitive absotption coefficients are considered for mid-IR and visible (or near-IR) spectral regions at different durations of pulse and broadening energies. The characteristic intencities of saturation are calculated and the results are compared with the experimental data measured for the nea…
We investigate the attosecond transient absorption spectroscopy (ATAS) of graphene by numerically solving four-band density-matrix equations, which demonstrates apparent fish bone resonance structures. To gain insight into these interesting structures, we exploit a simplified model that only considers the electrons of $Γ$ and M points in the Brillouin zone. With the help of this model, we can analytically express the ATAS spectrum as the sum of zeroth- and first-order Bessel functions in the variables of the strength and frequency of the infrared pump field as well as the effective mass of ele…
We study nonlinear optical response of graphene in the quantum Hall regime to an intense laser pulse. In particular, we consider harmonic generation process. We demonstrate that the generalized magneto-optical conductivity of graphene on the harmonics of a strong pump laser radiation has a characteristic Hall plateaus feature. The plateaus heights depend on the laser intensity and broadening of Landau levels, so that are not quantized exactly. This nonlinear effect remains robust against the significant broadening of Landau levels. We predict realization of an experiment through the observatio…
When electrons are confined in two dimensions and subjected to strong magnetic fields, the Coulomb interactions between them become dominant and can lead to novel states of matter such as fractional quantum Hall liquids. In these liquids electrons linked to magnetic flux quanta form complex composite quasipartices, which are manifested in the quantization of the Hall conductivity as rational fractions of the conductance quantum. The recent experimental discovery of an anomalous integer quantum Hall effect in graphene has opened up a new avenue in the study of correlated 2D electronic systems, …
We obtain a class of adiabatic solutions of Dirac equation for the charged massless relativistic quasi-particles that arise from the low-energy excitations \cite{foot-1} in a 2D graphene sheet, interacting with an electromagnetic field. The analytic solutions obtained are useful for {\it non-perturbative} investigation of processes in intense laser fields. As a first example we employ them to predict copious emissions of high order harmonics by THz lasers interacting with the occupied states of graphinos in the vicinity of the degenerate Dirac points. The relative intensity of the emitted harm…
Using the partition-free time-dependent Landauer-B{ü}ttiker formalism for transient current correlations, we study the traversal times taken for electrons to cross graphene nanoribbon (GNR) molecular junctions. We demonstrate electron traversal signatures that vary with disorder and orientation of the GNR. These findings can be related to operational frequencies of GNR-based devices and their consequent rational design.
The Dirac point and linear band structure in Graphene bestow it with remarkable electronic and optical properties, a subject of intense ongoing research. Explanations of high electronic mobility in graphene, often invoke the masslessness of electrons based on the effective relativistic Dirac-equation behavior, which are inaccessible to most undergraduate students and are not intuitive for non-physics researchers unfamiliar with relativity. Here, we show how to use only basic concepts from semiconductor theory and the linear band structure of graphene to explain its unusual effective mass and m…
A new theory is proposed for explaining the experimental results with intense short optical pulses. The theory is characterized by conjugate momentum interaction and especially large quantum enhancement factor and will unify the generation processes of coherent phonon formerly assigned as ISRS and DECP. It is applied to the instantaneous generation of lattice strain and the quantitative relation between the incident fluence and the resultant strain is shown.
Using optical-pump terahertz-probe spectroscopy, we study the relaxation dynamics of photoexcited carriers in graphene at different temperatures. We find that at lower temperatures the tail of the relaxation transients as measured by the differential probe transmission becomes slower, extending beyond several hundred picoseconds at temperatures below 50K. 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 ho…
Irradiating solids with ultrashort laser pulses is known to initiate femtosecond timescale magnetization dynamics. However, sub-femtosecond spin dynamics have not yet been observed or predicted. Here, we explore ultrafast light-driven spin dynamics in a highly non-resonant strong-field regime. Through state-of-the-art ab-initio calculations, we predict that a non-magnetic material can be transiently transformed into a magnetic one via dynamical extremely nonlinear spin-flipping processes, which occur on attosecond timescales and are mediated by a combination of multi-photon and spin-orbit inte…
Generating, controlling, and sensing strong magnetic fields at ever shorter time and length scales is important for both fundamental solid-state physics and technological applications such as magnetic data recording. Here, we propose a scheme for producing strong ultrashort magnetic pulses localized at the nanoscale. We show that a bimetallic nanoring illuminated by femtosecond laser pulses responds with transient thermoelectric currents of picosecond duration, which in turn induce Tesla-scale magnetic fields in the ring cavity. Our method provides a practical way of generating intense nanosca…
Graphene quantum dots are attractive candidates for solid-state quantum bits. In fact, the predicted weak spin-orbit and hyperfine interaction promise spin qubits with long coherence times. Graphene quantum dot devices have been extensively investigated with respect to their excitation spectrum, spin-filling sequence, and electron-hole crossover. However their relaxation dynamics remain largely unexplored. This is mainly due to challenges in device fabrication, in particular regarding the control of carrier confinement and the tunability of the tunnelling barriers, both crucial to experimental…
Based on a structure consisting of a single graphene layer situated on a periodic dielectric grating, we show theoretically that intense terahertz (THz) radiations can be generated by an electron bunch moving atop the graphene layer. The underlying physics lies in the fact that a moving electron bunch with rather low electron energy ($\sim$1 keV) can efficiently excite graphene plasmons (GPs) of THz frequencies with a strong confinement of near-fields. GPs can be further scattered into free space by the grating for those satisfying the phase matching condition. The radiation patterns can be co…
We discover an unusual phenomenon that occurs when a graphene monolayer is illuminated by a short and intense pulse at normal incidence. Due to the pulse-induced oscillations of the Dirac cones, a dynamical breaking of the layer's centrosymmetry takes place, leading to the generation of second harmonic waves. We prove that this result can only be found by using the full Dirac equation and show that the widely used semiconductor Bloch equations fail to reproduce this and some other important physics of graphene. Our results open new windows in the understanding of nonlinear light-matter interac…
The issue of whether local magnetic moments can be formed by introducing adatoms into graphene is of intense research interest because it opens the window to fundamental studies of magnetism in graphene, as well as of its potential spintronics applications. To investigate this question we measure, by exploiting the well-established weak localization physics, the phase coherence length L_phi in dilute fluorinated graphene. L_phi reveals an unusual saturation below ~ 10 K, which cannot be explained by non-magnetic origins. The corresponding phase breaking rate increases with decreasing carrier d…
Spontaneous optical emission of graphene irradiated by intense single-cycle terahertz pulses was investigated experimentally and explained theoretically. We found that emitted photons are polarized predominantly perpendicular to the electric field of the terahertz pulse, which proves that the terahertz field not only heats the electrons, but also creates a strongly nonequilibrium momentum distribution. Comparison of the measured optical spectrum and polarization anisotropy with the results of numerical modeling allowed us to estimate a momentum isotropization time for electrons in graphene to …
For gapped graphene, we predict that an intense ultrashort (single-oscillation) circularly-polarized optical pulse can induce a large population of the conduction band and a large valley polarization. With an increase in the bandgap, the magnitude of the valley polarization gradually increases from zero (for the native gapless graphene) to a value on the order of unity. The energy bandwidth of the electrons excited into the conduction band can be very large ($\gtrsim 10$ eV for a reasonable pulse amplitude of $\sim 0.5$ $\mathrm{V/Å}$). These phenomena are due to the effect of topological reso…
An intense laser field in the high-frequency regime drives carriers in graphene nanoribbons (GNRs) out of equilibrium and creates topologically-protected edge states. Using Floquet theory on driven GNRs, we calculate the time evolution of local excitations of these edge states and show that they exhibit a robust dynamics also in the presence of very localized lattice defects (atomic vacancies), which is characteristic of topologically non-trivial behavior. We show how it is possible to control them by a modulated electrostatic potential: They can be fully transmitted on the same edge, reflecte…
Multiphoton excitation of a solid by a few-cycle, intense laser pulse forms a very non-equilibrium distribution of charge carriers, where occupation probabilities do not necessarily decrease with energy. We show that, under certain conditions, significant population inversion can emerge between pairs of valence- or conduction-band states, where transitions between the Bloch states are dipole-allowed. This population inversion leads to stimulated emission in a laser-excited solid at frequencies where the unperturbed solid is transparent. We establish the optimal conditions for observing the str…
We explore the relaxation of photo-excited graphene by solving a transient Boltzmann transport equation with electron-phonon (e-ph) and electron-electron (e-e) scattering. Simulations show that when the excited carriers are relaxed by e-ph scattering only, a population inversion can be achieved at energies determined by the photon energy. However, e-e scattering quickly thermalizes the carrier energy distributions washing out the negative optical conductivity peaks. The relaxation rates and carrier multiplication effects are presented as a function of photon energy and dielectric constant.
The experimental Raman spectra of graphene exhibit a few intense two-phonon bands, which are enhanced through double-resonant scattering processes. Though there are many theoretical papers on this topic, none of them predicts the spectra within a single model. Here, we present results for the two-phonon Raman spectra of graphene calculated by means of the quantum perturbation theory. The electron and phonon dispersions, electronic lifetime, electron-photon and electron-phonon matrix elements, are all obtained within a density-functional-theory-based non-orthogonal tight-binding model. We study…
