Photoexcited Graphene Research Articles

Optical amplification of surface plasmon polaritons in a graphene single layer integrated with a random grating

In this paper, we design and simulate a terahertz (THz) controllable active plasmonic waveguide structure based on a single graphene layer that is placed on a random SiC grating substrate whose grooves are filled with CaF2. Optical gain in the proposed THz active plasmonic waveguide structure is provided by the stimulated emission process in the photoexcited graphene monolayer that leads to the amplification of surface plasmon polariton (SPP) waves. We use a random grating substrate to introduce Anderson localization of the SPP waves propagating through the graphene monolayer to enhance their optical amplification at resonance frequencies in which more amplification occurs due to multi-scattering and interference effects. It is shown that the input SPP wave can be amplified by 130 times at resonance frequencies of the random system. Significant amplification occurs only for frequencies that are equal to the resonance frequencies corresponding to the passive structure and are located within the gain bandwidth of graphene. The effects of depth and width of filled grooves on the amplification characteristics are also investigated. Furthermore, we show that increasing the ambient temperature by 30 K can reduce the output intensity by a factor of 12. This property of the proposed graphene-based THz plasmonic waveguide structure makes it useful in temperature sensing applications and on/off switchable laser devices.

Tracking photocarrier-enhanced electron-phonon coupling in nonequilibrium

Light-modulated electron-phonon coupling (EPC) is significant in many intriguing phenomena including light-enhanced superconductivity, polaron formation, and hidden charge orders, which provides a powerful strategy to engineer materials’ functionalities on demand. Here we explore EPC in photoexcited graphene during the ultrafast photocarrier dynamics with a phonon bath. Via analysing energy transport between electrons and phonons, light-induced EPC enhancement by more than one order of magnitude is demonstrated, which originates from the dynamic distribution of photoexcited carriers out of equilibrium. Excellent agreements between theory and experiment have been achieved, justifying the validity of the present approach for extracting excited-state dynamic properties. Our result unravels a crucial impact of photoexcitation on EPC by modulating the density and distribution of photocarriers, and provides a useful strategy for tracking ultrafast EPC in real time.

Real-Time GW: Toward an AbInitio Description of the Ultrafast Carrier and Exciton Dynamics in Two-Dimensional Materials.

We demonstrate the feasibility of the time-linear scaling formulation of the GW method [Phys. Rev. Lett. 124, 076601 (2020)PRLTAO0031-900710.1103/PhysRevLett.124.076601] for abinitio simulations of optically driven two-dimensional materials. The time-dependent GW equations are derived and solved numerically in the basis of Bloch states. We address carrier multiplication and relaxation in photoexcited graphene and find deviations from the typical exponential behavior predicted by the Markovian Boltzmann approach. For a resonantly pumped semiconductor we discover a self-sustained screening cascade leading to the Mott transition of coherent excitons. Our results draw attention to the importance of non-Markovian and dynamical screening effects in out-of-equilibrium phenomena.

Hot carrier dynamics and electron-optical phonon coupling in photoexcited graphene via time-resolved ultrabroadband terahertz spectroscopy

Electron-electron (e-e) interaction is known as a source of logarithmic renormalizations for Dirac fermions in quantum field theory. The renormalization of electron-optical phonon coupling (EPC) by e-e interaction, which plays a pivotal role in hot carrier and phonon dynamics, has been discussed since the discovery of graphene. We investigate hot carrier dynamics and EPC strength using time-resolved ultrabroadband terahertz (THz) spectroscopy combined with numerical simulation based on the Boltzmann transport equation and a comprehensive temperature model. The numerical simulation demonstrates that the extrinsic carrier scatterings by the Coulomb potential of the charged impurity and surface polar phonons are significantly suppressed by the carrier screening effect and have negligible contributions to the THz photoconductivity in heavily doped graphene on polyethylene terephthalate (PET) substrate. The large negative photoconductivity and the non-Drude behavior of THz conductivity spectra appear under high pump fluence and can be attributed to the temporal variation of the hot carrier distribution and scattering rate. The transient reflectivity well reflects the EPC strength and temporal evolution of the hot carrier and optical phonon dynamics. We successfully estimate the EPC matrix element of the ${A}_{1}^{\ensuremath{'}}$ optical phonon mode near the $\mathbf{K}$ point as ${\ensuremath{\langle}{D}_{\mathbf{K}}^{2}\ensuremath{\rangle}}_{\mathrm{F}}\ensuremath{\approx}450$ ${(\mathrm{eV}/\AA{})}^{2}$ from the fitting of THz conductivity spectra and temporal evolution of transient THz reflectivity. The corresponding dimensionless EPC constant ${\ensuremath{\lambda}}_{\mathbf{K}}\ensuremath{\approx}0.09$ at Fermi energy ${\ensuremath{\varepsilon}}_{\mathrm{F}}=0.43\phantom{\rule{0.28em}{0ex}}\mathrm{eV}$ is slightly larger than the prediction of the renormalization group approach including the dielectric screening effect of the PET substrate. This leads to a significant difference in hot carrier and phonon dynamics compared with those without the renormalization effect by the e-e interaction. This approach can provide a quantitative understanding of hot carrier and optical phonon dynamics and support the development of future graphene optoelectronic devices.

Theory of the effective Seebeck coefficient for photoexcited two-dimensional materials: Graphene

Thermoelectric phenomena in photoexcited graphene have been the topic of several theoretical and experimental studies because of their potential usefulness in optoelectronic applications. However, available theoretical descriptions of the thermoelectric effect in terms of the Seebeck coefficient do not take into account the role of the photoexcited electron density. In this work, we adopt the concept of effective Seebeck coefficient [G. D. Mahan, J. Appl. Phys. 87, 7326 (2000)] and extend it to the case of a photoexcited two-dimensional (2D) electron gas. We calculate the effective Seebeck coefficient for photoexcited graphene, we compare it to the commonly used ``phenomenological'' Seebeck coefficient, and we show how it depends on the photoexcited electron density and temperature. Our results are necessary inputs for any quantitative microscopic theory of thermoelectric effects in graphene and related 2D materials.

Exceptional Points in Flat Optics: A Non-Hermitian Line-Wave Scenario

Line waves are recently discovered wave entities that are localized along two directions, and therefore can be viewed as the one-dimensional counterpart of surface waves. These waves can be supported at discontinuities of the surface reactance and/or resistance of low-dimensional materials such as metasurfaces or graphene. Here, a broader class of non-Hermitian surface-impedance junctions is studied that can support coupled line waves, and allows investigating different one-dimensional waveguiding mechanisms in a unified framework. It is theoretically demonstrated that, under parity-time-symmetry conditions, exceptional points can occur in a truly flat-optics scenario, hence endowing these waveguiding systems with the attractive features of both line-wave and exceptional-point physics, and shedding further light on the phase transitions existing in these systems. It is also shown that the required surface-impedance parameters are compatible with those attainable with typical models of photoexcited graphene metasurfaces at terahertz frequencies. Besides providing additional understanding in the physics of line waves, which is still in its infancy, these results pave the way to intriguing developments in the largely unexplored field of non-Hermitian flat optics, with possible applications ranging from sensing to lasing and on-chip optical signal processing.

Ultrafast Interfacial Electron Transfer from Graphene Quantum Dot to 2,4-Dinitrotoluene

Ultrafast photoinduced electron transfer (PET) from a photoexcited graphene quantum dot (GQD*) to an electron-deficient molecule 2,4-dinitrotoluene (DNT) is studied in a water–methanol mixture (1:1 by volume) at different temperatures (5 °C–60 °C). The temperature-dependent study reveals that quenching of GQD emission by DNT is a complex process, where use of collisional or static quenching alone in the fitting model cannot fit the entire time regime of the kinetics. Irrespective of temperature, the collisional quenching rate obtained from the TCSPC lifetime quenching study appears at the upper limit of the bimolecular diffusion-controlled rate of the medium. The weak solubility of DNT in the polar solvents leads to GQD–DNT complex formation through hydrophobic interactions, allowing one to obtain a diffusion-free ultrafast PET timescale of the complex using a femtosecond upconversion setup. GQD–DNT complex formation is manifested by the heat change in the isothermal titration calorimetry (ITC) study upon mixing of DNT with GQD. Findings of our work would reinforce the understanding of the interfacial charge transfer process of GQD and thereby expand the promises to its real applications, especially in sensing and photovoltaics where materials with ultrafast PET are highly desirable.

Intrinsic and extrinsic effects on intraband optical conductivity of hot carriers in photoexcited graphene

We present a numerical study on the intraband optical conductivity of hot carriers at quasi-equilibria in photoexcited graphene based on the semiclassical Boltzmann transport equations (BTE) with the aim of understanding the effects of intrinsic optical phonon and extrinsic coulomb scattering caused by charged impurities at the graphene--substrate interface. Instead of using full-BTE solutions, we employ iterative solutions of the BTE and the comprehensive model for the temporal evolutions of hot-carrier temperature and hot-optical-phonon occupations to reduce computational costs. Undoped graphene exhibits large positive photoconductivity owing to the increase in thermally excited carriers and the reduction in charged impurity scattering. The frequency dependencies of the photoconductivity in undoped graphene having high concentrations of charged impurities significantly deviate from those observed in the simple Drude model, which can be attributed to temporally varying charged impurity scattering during terahertz (THz) probing in the hot-carrier cooling process. Heavily doped graphene exhibits small negative photoconductivity similar to that of the Drude model. In this case, charged impurity scattering is substantially suppressed by the carrier-screening effect, and the temperature dependencies of the Drude weight and optical phonon scattering governs the negative photoconductivity. In lightly doped graphene, the appearance of negative and positive photoconductivity depends on the frequency and the crossover from negative photoconductivity to positive emerges from increasing the charged impurity concentration. This indicates the change of the dominant scattering mechanism from optical phonons to charged impurities. Our approach provides a quantitative understanding of non-Drude behaviors and the temporal evolution of photoconductivity in graphene.

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.

On-chip terahertz modulation and emission with integrated graphene junctions

The efficient modulation and control of ultrafast signals on-chip is of central importance in terahertz (THz) communications and a promising route toward sub-diffraction limit THz spectroscopy. Two-dimensional (2D) materials may provide a platform for these endeavors. We explore this potential, integrating high-quality graphene p–n junctions within two types of planar transmission line circuits to modulate and emit picosecond pulses. In a coplanar strip line geometry, we demonstrate the electrical modulation of THz signal transmission by 95%. In a Goubau waveguide geometry, we achieve complete gate-tunable control over THz emission from a photoexcited graphene junction. These studies inform the development of on-chip signal manipulation and highlight prospects for 2D materials in THz applications.

Tunable terahertz structure based on graphene hyperbolic metamaterials

Photoexcited graphene can behave as the gain medium aiming to come up with the coherent radiation at low THz spectral region. However, its response is very weak because of its atomic dimensions. Herein, a different design aiming to obtain effective tunable THz amplifiers, having small dimensions and lasers with broadband operation based on active THz hyperbolic metamaterials (HMM) is demonstrated. HMMs are considered by employing multiple stacked photoexcited graphene sheets divided by dielectric spacers. Herein, we study and characterize the hyperbolic THz regime of the studied atomic active HMM. A broadband slow-wave propagation regime takes place if the graphene-based HMM system is periodically patterned. This occurs due to the hyperbolic dispersion. Doing so, reconfigurable amplification of THz waves in a broad-spectrum region is attained. This might be engineered by tuning the quasi-Fermi level of graphene. Moreover, the mechanisms leading to the increase of the frequency region of bound surface wave have been proposed in the frame of the current study.

Tunable terahertz amplification based on photoexcited active graphene hyperbolic metamaterials [Invited

The efficient amplification and lasing of electromagnetic radiation at terahertz (THz) frequencies is a non-trivial task achieved mainly by quantum cascade laser configurations with limited tunability and narrowband functionality. There is a strong need of compact and efficient THz electromagnetic sources with reconfigurable operation in a broad frequency range. Photoexcited graphene can act as the gain medium to produce coherent radiation at low THz frequencies but its response is very weak due to its ultrathin thickness. In this work, we demonstrate an alternative design to achieve efficient tunable and compact THz amplifiers and lasers with broadband operation based on active THz hyperbolic metamaterials (HMM) designed by multiple stacked photoexcited graphene layers separated by thin dielectric sheets. The hyperbolic THz response of the proposed ultrathin active HMM is analytically and numerically studied and characterized. When the graphene-based HMM structure is periodically patterned, a broadband slow-wave propagation regime is identified, thanks to the hyperbolic dispersion. In this scenario, reconfigurable amplification of THz waves in a broad frequency range is obtained, which can be made tunable by varying the quasi-Fermi level of graphene. We demonstrate that the THz response of the presented tunable THz amplifiers or lasers is controlled by the incident optical pumping (photodoping) and the loaded dielectric materials in the HMM waveguide array, an interesting property that can have great potential for THz amplification, emission, and sensing applications.

Reconfigurable topological phases in photoexcited graphene nanoribbon arrays

We introduced here a reconfigurable topological phase using optically pumped graphene nanoribbon arrays with homogeneous spacing at terahertz frequencies. By adjusting the profile of imaginary potential, various topologically non-trivial dimer chains composed of graphene nanoribbons can be selectively produced. These dimer chains support different kinds of midgap states. Moreover, we numerically demonstrated that these midgap states are robust against some perturbations, such as non-Hermitian and lattice disorders, and can be further adjusted by varying the pumping strength on the specific graphene nanoribbon. Consequently, the reconfigurable topological phase can be obtained by only tuning the profile of imaginary potential without altering the geometry of the system. These tunable topological phases may provide a convenient method to tune the spatial profile of graphene-based topological lasers and have potential applications in topologically protected waveguiding in terahertz frequency range.

Ultrafast photocarrier dynamics in single-layer graphene driven by strong terahertz pulses

Time-resolved high-field terahertz (THz) spectroscopy of photoexcited graphene demonstrates extraordinary photocarrier dynamics in single-layer graphene. Strong THz fields and photoexcitation simultaneously enhance the THz transmission of graphene mainly due to the increase of carrier scattering rates. A theoretical analysis confirms that the graphene conductivity undergoes transient decreases to the large extent under the THz and optical excitations, indicating that both the strong THz fields and photoexcitation effectively elevate the carrier scattering rates. The relaxation of photocarriers, on the other hand, shows opposite effects of the THz fields and photoexcitation. Photoexcitation increases the relaxation time via the reabsorption of optical phonons by photocarriers, while strong THz fields reduce the relaxation time because the field-induced redistribution of electrons opens up unoccupied states in the conduction band and consequently enhances the relaxation and the phonon emission.

The ultrafast dynamics and conductivity of photoexcited graphene at different Fermi energies.

For many of the envisioned optoelectronic applications of graphene, it is crucial to understand the subpicosecond carrier dynamics immediately following photoexcitation and the effect of photoexcitation on the electrical conductivity-the photoconductivity. Whereas these topics have been studied using various ultrafast experiments and theoretical approaches, controversial and incomplete explanations concerning the sign of the photoconductivity, the occurrence and significance of the creation of additional electron-hole pairs, and, in particular, how the relevant processes depend on Fermi energy have been put forward. We present a unified and intuitive physical picture of the ultrafast carrier dynamics and the photoconductivity, combining optical pump-terahertz probe measurements on a gate-tunable graphene device, with numerical calculations using the Boltzmann equation. We distinguish two types of ultrafast photo-induced carrier heating processes: At low (equilibrium) Fermi energy (EF ≲ 0.1 eV for our experiments), broadening of the carrier distribution involves interband transitions (interband heating). At higher Fermi energy (EF ≳ 0.15 eV), broadening of the carrier distribution involves intraband transitions (intraband heating). Under certain conditions, additional electron-hole pairs can be created [carrier multiplication (CM)] for low EF, and hot carriers (hot-CM) for higher EF. The resultant photoconductivity is positive (negative) for low (high) EF, which in our physical picture, is explained using solely electronic effects: It follows from the effect of the heated carrier distributions on the screening of impurities, consistent with the DC conductivity being mostly due to impurity scattering. The importance of these insights is highlighted by a discussion of the implications for graphene photodetector applications.

Photoexcited Graphene Metasurfaces: Significantly Enhanced and Tunable Magnetic Resonances

Artificially constructed metamaterials or metasurfaces with tailored resonant elements provide a revolutionary platform for controlling light at the subwavelength scale. Switchable or frequency-agile meta-devices are highly desirable in achieving more flexible functionalities and have been explored extensively by incorporating various materials, which respond to external stimuli. Graphene, a two-dimensional material showing extraordinary physical properties, has been found very promising for tunable meta-devices. However, the high intrinsic loss of graphene severely obstructs us from achieving high-quality resonance in various graphene metamaterials and metasurfaces, and the loss compensation can be considered as a straightforward strategy to take further advantages of enhanced light–graphene interactions. Here, we demonstrate that the photoexcited graphene, in which the quasi-Fermi energy of graphene changes corresponding to optical pumping, can boost the originally extremely weak magnetic resonance in a...

Polarization and plasmons in hot photoexcited graphene

We present a robust and exact method for calculating the polarization function and plasmon dispersion of graphene, for an arbitrary (isotropic) non-equilibrium carrier distribution, within random phase approximation (RPA). This is demonstrated for a range of carrier distributions, including hot carrier distributions which occur within the femtoseconds following photoexcitation. We show that qualitatively different behaviour from the equilibrium case can occur. As the polarization function determines dynamic screening, its calculation shall be essential to quantifying carrier-carrier scattering channels for graphene far from equilibrium.

Tailoring Eigenmodes at Spectral Singularities in Graphene-based PT Systems

The spectral singularity existing in PT-synthetic plasmonic system has been widely investigated. Only lasing-mode can be excited resulting from the passive characteristic of metallic materials. Here, we investigated the spectral singularity in the hybrid structure composed of the photoexcited graphene and one-dimensional PT-diffractive grating. In this system, both lasing- and absorption-modes can be excited with the surface conductivity of photoexcited graphene being loss and gain, respectively. Remarkably, the spectral singularity will disappear with the optically pumped graphene to be lossless. In particular, we find that spectral singularities can exhibit symmetry-modes, when the loss and gain of the grating is unbalanced. Meanwhile, by tuning the loss (gain) of graphene and non-PT diffraction grating, lasing- and absorption-modes can also be excited. We hope that tunable optical modes at spectral singularities can have some applications in designing novel surface-enhanced spectroscopies and plasmon lasers.

Ultrafast momentum imaging of pseudospin-flip excitations in graphene

The pseudospin of Dirac electrons in graphene manifests itself in a peculiar momentum anisotropy for photo-excited electron-hole pairs. These interband excitations are in fact forbidden along the direction of the light polarization, and are maximum perpendicular to it. Here, we use time- and angle-resolved photoemission spectroscopy to investigate the resulting unconventional hot carrier dynamics, sampling carrier distributions as a function of energy and in-plane momentum. We first show that the rapidly-established quasi-thermal electron distribution initially exhibits an azimuth-dependent temperature, consistent with relaxation through collinear electron-electron scattering. Azimuthal thermalization is found to occur only at longer time delays, at a rate that depends on the substrate and the static doping level. Further, we observe pronounced differences in the electron and hole dynamics in n-doped samples. By simulating the Coulomb- and phonon-mediated carrier dynamics we are able to disentangle the influence of excitation fluence, screening, and doping, and develop a microscopic picture of the carrier dynamics in photo-excited graphene. Our results clarify new aspects of hot carrier dynamics that are unique to Dirac materials, with relevance for photo-control experiments and optoelectronic device applications.

Photoexcited terahertz conductivity dynamics of graphene tuned by oxygen-adsorption

By using optical pump-terahertz (THz) probe spectroscopy, the photoexcited terahertz conductivity dynamics of chemical vapor deposition grown graphene is investigated in different atmospheric environments. It is shown that the Fermi energy of doped graphene is engineered by oxygen adsorption and desorption, which is probed by transient THz conductivity measurement. We show that the ultrafast energy relaxation processes depend on Fermi energy (changed by environmental gas) and the density of excited carriers (changed by photo-excitation fluence). The rise process of the negative conductivity dynamics becomes less efficient upon decreasing the Fermi energy and/or increasing the pump fluence. All findings show that the Fermi energy of graphene engineered by environmental gas allows us to tune the ultrafast energy relaxation pathways in photoexcited graphene.