Relaxation Dynamics Of Photoexcited Carriers 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 dynamics of Dirac surface and bulk photocarriers in topological-insulator bismuth telluride nanocrystals using terahertz spectroscopy

Unlike conventional semiconductors, Dirac fermions in surface states of topological insulators (TIs) exhibit many fascinating electronic properties relevant for several optoelectronic and spintronic applications. We investigate the relaxation dynamics of photoexcited carriers in bismuth telluride (${\mathrm{Bi}}_{2}{\mathrm{Te}}_{3}$) nanocrystals---a prominent candidate among the three-dimensional (3D) topological insulators, using ultrafast time resolved terahertz (THz) spectroscopy. Upon photoexcitation using an 800 nm pump pulse, we observe a decrease in the THz transmission due to the absorption of THz radiation by the photoexcited carriers. The time evolution of the real part of pump induced conductivity [$\mathrm{\ensuremath{\Delta}}{\ensuremath{\sigma}}_{R}({\ensuremath{\tau}}_{\text{pp}})=\phantom{\rule{4pt}{0ex}}{\ensuremath{\sigma}}_{\text{pump}}{\phantom{\rule{4pt}{0ex}}}_{\text{on}}({\ensuremath{\tau}}_{\text{pp}})\ensuremath{-}{\ensuremath{\sigma}}_{\text{pump}}{\phantom{\rule{4pt}{0ex}}}_{\text{off}}$] with respect to the pump-probe delay time (${\ensuremath{\tau}}_{\text{pp}}$), exhibits a sign change from positive to negative as carriers relax back to their equilibrium distribution, which is also evident from the spectral signatures of $\mathrm{\ensuremath{\Delta}}\ensuremath{\sigma}(\ensuremath{\omega})$, measured at various ${\ensuremath{\tau}}_{\text{pp}}$. While the positive sign of $\mathrm{\ensuremath{\Delta}}{\ensuremath{\sigma}}_{R}({\ensuremath{\tau}}_{\text{pp}})$ is attributed to the contribution from the semiconducting bulk states, the negative sign of $\mathrm{\ensuremath{\Delta}}{\ensuremath{\sigma}}_{R}({\ensuremath{\tau}}_{\text{pp}})$ at longer delay times is shown to arise from the Dirac surface states of TIs due to increased scattering rate of photoexcited charge carriers. We model the differential conductivity spectrum [$\mathrm{\ensuremath{\Delta}}\ensuremath{\sigma}(\ensuremath{\omega})$] and the transient dynamics [$\mathrm{\ensuremath{\Delta}}{\ensuremath{\sigma}}_{R}({\ensuremath{\tau}}_{\text{pp}})$] quantitatively using the Boltzmann transport equation applied to the surface and bulk states. This includes the energy dependence of scattering rates along with the dynamics of hot electron temperature (${T}_{e}$) evaluated in a self-consistent manner. Such an approach enables us to understand various scattering mechanisms associated with the photoexcited carriers both in Dirac surface as well as in bulk electronic states.

Robust hybridization gap in the Kondo insulator YbB12 probed by femtosecond optical spectroscopy

In heavy fermions the relaxation dynamics of photoexcited carriers has been found to be governed by the low energy indirect gap, E$_{g}$, resulting from hybridization between localized moments and conduction band electrons. Here, carrier relaxation dynamics in a prototype Kondo insulator YbB${}_{12}$ is studied over large range of temperatures and over three orders of magnitude. We utilize the intrinsic non-linearity of dynamics to quantitatively determine microscopic parameters, such as electron-hole recombination rate. The extracted value reveals that hybridization is accompanied by a strong charge transfer from localized 4f-levels. The results imply the presence of a hybridization gap up to temperatures of the order of E$_{g}$/k$_{B}\approx200$ K, which is extremely robust against electronic excitation. Finally, below 20 K the data reveal changes in the low energy electronic structure, attributed to short-range antiferromagnetic correlations between the localized levels.

Impact of defects on photoexcited carrier relaxation dynamics in GeSn thin films

We report the results of a study that was conducted to investigate the recombination paths of photoexcited charge carriers in GeSn thin films. The charge carrier lifetime was predicted as a function of temperature from a description of photoconductivity transients, assuming co-influence of Shockley–Read–Hall and radiative carrier recombination paths. We identify that dislocations are the source of a band of electronic states with the highest occupied state at E V + (85÷90) meV that acts as Shockley–Read–Hall centers determining the charge carrier lifetime. The photoluminescence (PL) and photoconductivity spectroscopy have been applied to distinguish between the contribution of both band-to-band and dislocation-related electron transitions. The PL band was found to demonstrate a low-energy shift of about 80 ± 20 meV relative to the edge of the photoconductivity spectra in the indirect bandgap GeSn films with dislocations. The role of a different nature deeper acceptor level at E V + (140 ÷ 160) meV in the recombination processes of the GeSn layers with better structural quality and the Sn content higher than 4% was discussed. This detailed understanding of the recombination processes is of critical importance for developing GeSn/Ge-based optoelectronic devices.

Photo-excited carrier relaxation dynamics in two-dimensional InSe flakes

Carrier relaxation dynamics of InSe flakes is investigated by using time-resolved pump-probe reflectivity measurement. The photocarriers associated with the Pxy orbital band-edge transition at 2.40 eV, which is coupled to the in-plane polarized light, is observed to possess a lifetime of ∼19 ps at room temperature and ∼99 ps at 10 K. The temperature and power dependent carrier lifetime suggests that Shockley–Read–Hall process is the dominant nonradiative recombination mechanism responsible for the carrier relaxation. In addition, the electron scattering with a 14.5 meV optical phonon plays an active role in the carrier relaxation with increasing temperatures. A broad absorption around 1.65–1.90 eV is observed. The photocarriers associated with this broad transition show a long lifetime of ∼200 ps that is nearly independent of temperature and photon energy. This is indicative of bound carriers by defects. Our experimental results provide essential information for the characteristics of carrier dynamics and defects in InSe flakes. The experimental findings are fundamentally important for further development of microelectronics and optoelectronics based on InSe.

Time-resolved, nonequilibrium carrier and coherent acoustic phonon dynamics in (Cd, Mg)Te single crystals for radiation detectors

We present time-resolved nonequilibrium carrier and coherent acoustic phonon dynamics in (Cd, Mg)Te single crystals intended for detection of high-energy x-ray photons. Our (Cd, Mg)Te crystals were grown using a vertical Bridgman method and during the process were doped either with In (a shallow dopant) or Ge (a deep impurity). Next they were cut into platelets and, subsequently, tested as as-grown specimens, or, before testing, long-term annealed in a temperature range of 750 °C–800 °C to improve their crystalline properties. All samples exhibited high resistivities of 109–1010 Ω cm, as required for x-ray detection applications. We have performed femtosecond optical spectroscopy, pump-probe measurements on all samples in both one-color (high-intensity 800 nm pump and low-intensity 800 nm probe) and two-color (high-intensity 400 nm pump and low-intensity 800 nm probe) configurations, and analyzed the results using our carrier dynamics rate-equation model. The model allowed us to perform a comprehensive, time-resolved analysis of relaxation dynamics of photoexcited carriers and investigate the role of carrier traps present in all tested samples. Two-color measurements also allowed us to observe and analyze the propagation of acoustic coherent phonons excited by the high-energy pump pulse. We observed that the dependence of phonon mode frequency, after including a correction of the experimentally measured crystal index of refraction dependence on the probe wavelength, was dispersionless and led to the value for the sound velocity of 3367 m s−1, which is in excellent agreement with the literature data. The intrinsic lifetime of coherent phonons in (Cd, Mg)Te was estimated to be of the order of 10 ns. Finally, we conclude that among our tested samples, the In-doped, annealed (Cd, Mg)Te crystal exhibits the best characteristics for radiation detection applications.

Terahertz probe of photoexcited carrier dynamics in the Dirac semimetal Cd3As2

The relaxation dynamics of photoexcited quasiparticles of three-dimensional (3D) Dirac semimetals are vital towards their application in high performance electronic and optoelectronic devices. In this work, the relaxation dynamics of photoexcited carriers of 3D Dirac semimetal Cd3As2 are investigated by transient terahertz spectroscopy. The visible pump-THz probe spectroscopy measurement shows clear biexponential decays with two characteristic time constants. According to the pump-power and temperature dependence, these two characteristic time constants are attributed to the electron phonon coupling (1-4 ps) and anharmonic decay of hot coupled phonons to electronic uncoupled phonons (2-9 ps), respectively. An anomalous electron-optical phonon coupling reduction and a bottleneck slowing of hot optical phonons relaxation are observed with higher excitation intensities similar to that in graphene. On the other hand, the electron-optical phonon coupling can be enhanced due to the phonon frequency broadening and softening at elevated lattice temperature. Furthermore, the transient THz spectrum response is strongly modified by the phonon assisted intraband absorption of hot carriers from a pure electronic Drude model, which is evidenced by a characteristic THz absorption dip in the transient THz absorption spectrum. This absorption dip is pinned by the discrete optical phonon energy that assists the intraband transition enabled by photoexcitation of hot carriers.

Ultrafast relaxation dynamics of photoexcited Dirac fermions in the three-dimensional Dirac semimetalCd3As2

Three dimensional (3D) Dirac semimetals which can be seen as 3D analogues of graphene have attracted enormous interests in research recently. In order to apply these ultrahigh-mobility materials in future electronic/optoelectronic devices, it is crucial to understand the relaxation dynamics of photoexcited carriers and their coupling with lattice. In this work, we report ultrafast transient reflection measurements of the photoexcited carrier dynamics in cadmium arsenide (Cd3As2), which is one of the most stable Dirac semimetals that have been confirmed experimentally. By using low energy probe photon of 0.3 eV, we probed the dynamics of the photoexcited carriers that are Dirac-Fermi-like approaching the Dirac point. We systematically studied the transient reflection on bulk and nanoplate samples that have different doping intensities by tuning the probe wavelength, pump power and lattice temperature, and find that the dynamical evolution of carrier distributions can be retrieved qualitatively by using a two-temperature model. This result is very similar to that of graphene, but the carrier cooling through the optical phonon couplings is slower and lasts over larger electron temperature range because the optical phonon energies in Cd3As2 are much lower than those in graphene.

Ultraviolet saturable absorption and ultrafast carrier dynamics in ultrasmall black phosphorus quantum dots.

Understanding the photoexcited carrier-relaxation actions in ultrasmall black phosphorus quantum dots (BPQDs) will play a crucial role in the fields of electronics and optoelectronics. Herein, we report the ultraviolet (UV) saturable absorption and ultrafast photoexcited carrier-relaxation dynamics of BPQDs. The ultrasmall BPQDs are synthesized using a facile liquid-exfoliation method and possess a diameter of 3.8 ± 0.6 nm and a thickness of 1.5 ± 0.4 nm. Femtosecond open-aperture (OA) Z-scan measurements showed typical saturable absorption properties in the UV band. A negative nonlinear optical (NLO) absorption coefficient of -(1.4 ± 0.3) × 10-3 cm GW-1 and a saturable intensity of 6.6 ± 1.3 GW cm-2 were determined. Using a degenerate pump-probe technique, an ultrafast photoexcited carrier-recombination time was observed in the range of 216-305 fs, which was 3 orders of magnitude faster than that of BP nanosheets. Such an ultrafast relaxation component may be attributable to the edge- and step-mediated recombination and was confirmed by our density functional theory (DFT) calculations. This work provides fundamental insight into the underlying mechanism of the photoexcited carrier relaxation dynamic action in BPQDs which can enable UV photonic devices.

Pump- and Probe-polarization Analyses of Ultrafast Carrier Dynamics in Organic Superconductors

We investigated photo-excited carrier relaxation dynamics in the strongly correlated organic superconductors κ-(BEDT-TTF)2Cu(NCS)2 and κ-(BEDT-TTF)2Cu[N(CN)2]Br, using different polarizations of pump and probe pulses. Below the glasslike transition temperature (T g) anisotropic responses for probe polarization were observed in both compounds. Decomposing the data into anisotropic and isotropic components, we found the anisotropic component shows no pump polarization dependence, meaning that dissipative excitation process was dominant for the anisotropic carrier relaxation. This behavior indicates that the appearance of anisotropic responses can be associated with spatial symmetry breaking due to structural change of BEDT-TTF molecules.

Carrier-carrier and carrier-phonon interactions in the dynamics of photoexcited electrons in graphene

In this work we use the Monte Carlo method to simulate the photoexcited carrier relaxation dynamics in suspended monolayer graphene to unveil the role of the different scattering mechanisms involved. The results show a strong activity of carrier-carrier and carrier-optical phonon interactions in the very early stages of the relaxation process driving the thermalization and cooling dynamics. The consideration of the coupling between the electron and phonon population reveals an intense damping in the cooling rates that is dependent on the pumped carrier concentration.

Measurement of sub-10 fs Auger processes in monolayer graphene.

Despite the concerted efforts to directly probe the electron-electron (e-e) scattering mediated relaxation process in graphene using transient absorption spectroscopy, the initial sub-10 fs photoexcited carrier relaxation dynamics has remained elusive. Herein, we utilize a simple z-scan approach to elucidate this process and discern its mechanisms in CVD grown single layer graphene using femtosecond laser pulses with temporal pulse widths far longer than the relaxation time. We report the first experimental observation of e-e scattering lifetime shortening with increasing fluence, which had been theoretically predicted. Analysis from two-body Coulombic scattering suggests that Auger processes are essential relaxation channels in single layer graphene. Importantly, our straightforward approach on the graphene model system is applicable to the family of emergent layered materials.

Ultrafast dynamics of hot electrons and phonons in chemical vapor deposited graphene

The relaxation dynamics of photoexcited carriers in a chemical vapor deposited graphene transferred on quartz substrate has been investigated by using ultrafast optical-pump terahertz (THz)-probe spectroscopy. Terahertz transmission through graphene sample is reduced by optical pumping. The change of transmission decays exponentially after the optical pulse. We find the relaxation time is insensitive to the substrate temperature from 10 K to 300 K but increases sublinearly with pump fluence. We model the relaxation process involving electron-phonon coupling together with a set of rate equations to describe the transient responses of quasi-particles and optical phonons. The increases of the extracted carrier temperature and the measured relaxation time with pump fluence are associated with the fact that high pump fluence significantly increases the carrier temperature and broadens the carrier distribution. As a result, it leads to the reduction of optical phonon emission efficiency and the decrease of cooling rate as well.

Picosecond to Millisecond Transient Absorption Spectroscopy of Broad-Band Emitting Chiral CdSe Quantum Dots

The relaxation dynamics of photoexcited carriers in water-soluble, penicillamine-capped, optically active and luminescent chiral CdSe quantum dots (QDs) were investigated. Three pump–probe techniques, namely broad-band UV–visible transient absorption (TA), picosecond time-resolved infrared (ps-TRIR) transient absorption, and nanosecond laser flash photolysis spectroscopy, were used to record transient decays from the picosecond up to the millisecond time scale. Picosecond experiments were carried out at a range of energies per unit area down to ca. 30 μJ cm–2, where only single photon excitation is expected. Whereas ps-UV–visible TA spectra show both bleach and transient features which are associated with depopulation of the lowest lying electron quantized state, the infrared transient bands are broad and structureless. The mid-IR transient absorption and excitonic bleach recovery is only partial, and its decay kinetics were found to be multiexponential in nature. The initial picosecond decay component is...

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.

Influence of long lifetime absorption process on the measurement of ultrafast carrier dynamics

The wavelength dependence of ultrafast relaxation dynamics of photoexcited carriers in bulk GaAs is studied using femtosecond time-resolved pump-probe transmission spectroscopy under the same photoexcited carrier concentration and the ratio of pump to probe in intensity. Negative and oscillating time-delayed signals are observed at central wavelengths of 760 nm and 780 nm and judged to be incorrect physically by comparson with a simulated computation result. It is found by waveform analysis that they are caused by the phase reversal of the output waveforms from a photodetector, while the phase reversal originates from a long lifetime absorption process existing in GaAs sample. It is pointed out that the phase reversal of the waveform can be corrected by raising the ratio of pump to probe in intensity at the photodetector, so that right transient traces can be obtained. However, raising the ratio is incompatible with the viewpoint that the scattered contribution to the photodetector from pump light should be filtered as much as possible. This result has an important reference value for the acquisition of correct ultrafast dynamics using time-resolved pump-probe spectroscopy.

Photoexcited carrier relaxation dynamics and terahertz response of photoconductive antennas made on proton bombarded GaAs materials

We present a model reproducing the instrumental response of a time-domain spectrometer that integrates photoconductive transmitter and receiver antennas made on identical proton-bombarded GaAs substrates. This model is used to determine the ultrafast capture time of the photoexcited carriers by the ion-bombardment-induced traps. A 0.5 ps capture time can be extracted for a low laser pump fluence of 0.66 μJ/cm2 per pulse. This carrier trapping time gets longer as the pump fluence increases. This behavior is explained by a gradual filling of the traps that are distributed over a 1 μm depth from the GaAs surface. This interpretation is supported by time-resolved measurements obtained on the same photoconductive material using both an 820 nm pump/terahertz-probe transmission experiment and a degenerate 760 nm pump/probe reflectivity experiment. The differential transmission and reflectivity dynamics are reproduced using a biexponential function which correctly describes the photoexcited carrier relaxation and transport dynamics in this material. The strong agreement observed between these different measurements reinforces the validity of the theoretical model used to reproduce the instrumental response of the terahertz setup.

(Cd,Mn)Te detectors for characterization of X-ray emissions generated during laser-driven fusion experiments

We present our measurements of (Cd,Mn)Te photoconductive detectors (PCDs), intending to characterize both the temporal and spectral dependence of X-ray emissions from laser-illuminated targets during inertial confinement fusion experiments. Our Cd1−xMnxTe (x=0.05) single crystals, doped with V, were grown using a vertical Bridgman method and annealed in Cd vapor for the highest resistivity of ∼1010Ωcm. The 1-mm-long and 2.3-mm-long detectors were placed in the same housing as two 1-mm-long diamond PCDs. Each device was preceded by a Be X-ray filter with 37% X-ray transmission at the 1keV cutoff energy. Energy of the incident OMEGA laser pulses varied from 2.3 to 28kJ. Using targets of empty plastic shells, we observed two X-ray emission events separated by 1.24ns: the first event was caused by heating of the shell that created a hot corona, while the second event was an X-ray emission from the fully compressed target. Experiments with targets with steel cores enabled us to analyze the time-resolved relaxation dynamics of photo-excited carriers in the (Cd,Mn)Te crystals. According to our calculations, the (Cd,Mn)Te material can very effectively absorb X-rays with energies of up to above 100keV and the (Cd,Mn)Te PCDs are likely to complement the diamond detectors currently used in laser-confinement fusion experiments.

Photo-excited carrier relaxation dynamics in InN films

Photo-excited carrier relaxation dynamics in InN films were investigated using femtosecond transient measurements. We measured two samples with different background carrier densities, and discussed the influence of the carrier densities on the relaxation dynamics. We also found that the slow decay component disappears under the optimized condition because of the effects of equilibrium band filling and bandgap renormalization.

Photoexcited carrier relaxation dynamics in pentacene probed by ultrafast optical spectroscopy: Influence of morphology on relaxation processes

We present a comparative study of ultrafast photoexcited state relaxation in pentacene single crystals and in pure and C60-doped pentacene films using optical pump-probe spectroscopy. The photoinduced absorption spectra in pentacene crystals is consistent with a dominant singlet–triplet fission decay channel for above-gap excitation. This decay channel is suppressed in thin films and even further suppressed by electron trapping in C60-doped films. Thus we show that suppression of triplet state production, which is necessary for free carrier formation and thus photovoltaic and photodiode performance, is controllable via sample morphology.