Fast Carrier Relaxation Research Articles

Exchange-enhanced spin-orbit splitting and its density dependence for electrons in monolayer transition metal dichalcogenides

We show that spin-orbit splitting (SOS) in monolayers of semiconducting transition metal dichalcogenides (TMDs) is substantially enhanced by an electron-electron interaction. This effect, similar to the exchange enhancement of the electron g factor, is most pronounced for conduction band electrons (in particular, in MoS2), and it has a nonmonotonic dependence on the carrier sheet density n. That is, the SOS enhancement is peaked at the onset of filling of the higher-energy spin-split band by electrons, n*, which also separates the regimes of slow (at n<n*) and fast (for n>n*) spin and valley relaxation of charge carriers. Moreover, this density itself is determined by the enhanced SOS value, making the account of exchange renormalization important for the analysis of the spintronic performance of field-effect transistors based on two-dimensional TMDs. Published by the American Physical Society 2024

Scaling Behavior in the Spectral and Power Density Dependent Photovoltaic Response of Hot Polaronic Heterojunctions

AbstractStrongly correlated manganites can be considered as model systems for the study of photovoltaic harvesting of hot polarons that can be excited from the electronically ordered ground state. In order to gain basic understanding of hot polaron harvesting, the deviations of the photovoltaic response of a heterojunction with polaronic absorber from a conventional semiconductor are analyzed. Specifically, the spectral and photon power density dependence of the open circuit voltage Uoc and the short circuit current density Jsc in heterojunctions consisting of orbital ordered Pr1‐xCaxMnO3 (x = 0.1, PCMO) thin films epitaxially grown on single crystalline (100) SrTiO3 (STO) and Nb‐doped (100) SrTiO3 (STNO) substrates are investigated. The observed behavior is fundamentally different from conventional solar cells, in which Uoc is limited by fast carrier relaxation to the band edges. Whereas the spectral and photon power dependence of Uoc of conventional semiconductor junctions is well described by the Shockley‐Queisser (SQ) theory, the hot polaron junctions surprisingly show a scaling law behavior of Uoc. Such scaling laws otherwise apply to equilibrium order parameters in second‐order phase transitions. It is concluded that its physical origin is the unique dependence of the quasi‐Fermi level splitting on temperature, photon energy, and power density in a hot polaron system.

Germanium Nanosheets with Dirac Characteristics as a Saturable Absorber for Ultrafast Pulse Generation.

Bulk germanium as a group-IV photonic material has been widely studied due to its relatively large refractive index and broadband and low propagation loss from near-infrared to mid-infrared. Inspired by the research of graphene, the 2D counterpart of bulk germanium, germanene, has been discovered and the characteristics of Dirac electrons have been observed. However, the optical properties of germanene still remain elusive. In this work, several layers of germanene are prepared with Dirac electronic characteristics and its morphology, band structure, carrier dynamics, and nonlinear optical properties are systematically investigated. It is surprisingly found that germanene has a fast carrier-relaxation time comparable to that of graphene and a relatively large nonlinear absorption coefficient, which is an order of magnitude higher than that of graphene in the near-infrared wavelength range. Based on these findings, germanene is applied as a new saturable absorber to construct an ultrafast mode-locked laser, and sub-picosecond pulse generation in the telecommunication band is realized. The results suggest that germanene can be used as a new type of group-IV material for various nonlinear optics and photonic applications.

Augmented All‐Optical Active Terahertz Device Using Graphene‐Based Metasurface

AbstractPhoto‐excited graphene has a positive (semiconductor‐like) or negative (metal‐like) response depending on the Fermi level, which is tuned by gate control, doping, and growth. Both negative and positive photoconductive responses have a potential application as an ultrafast optical modulator in the control of light transmission. However, it is challenging to achieve a high on/off ratio in the photo‐excited graphene because of a small absorption of electromagnetic waves and a limitation of photo‐induced conductivity change. Here, the negative‐type high on/off ratio and ultrafast terahertz modulation are experimentally demonstrated using graphene/metal nanoslot antennas. When the graphene covers the nanoslot antennas, the terahertz waves are completely blocked (off‐state). This perfect extinction results from the enhanced intraband absorption in graphene by strong localized fields near the nanogap. However, once the optical pump is applied to the graphene/nanoslot antennas, terahertz transmission becomes recovered resonantly (on‐state) due to the photo‐induced transparency of graphene that leads to a distinctive modulation from off‐ to on‐resonance. Furthermore, the fast carrier relaxation induced by strong terahertz field‐driven carrier redistribution is responsible for the faster modulation of transient terahertz transmission. The results will open up pathways toward negative‐response terahertz modulation applications with high on/off ratio and ultrafast time scale.

Ultrafast Carrier and Lattice Dynamics in Plasmonic Nanocrystalline Copper Sulfide Films.

Excited carrier dynamics in plasmonic nanostructures determines many important optical properties such as nonlinear optical response and photocatalytic activity. Here it is shown that mesoscopic plasmonic covellite nanocrystals with low free‐carrier concentration exhibit a much faster carrier relaxation than in traditional plasmonic materials. A nonequilibrium hot‐carrier population thermalizes within first 20 fs after photoexcitation. A decreased thermalization time in nanocrystals compared to a bulk covellite is consistent with the reduced Coulomb screening in ultrathin films. The subsequent relaxation of thermalized, equilibrium electron gas is faster than in traditional plasmonic metals due to the lower carrier concentration and agrees well with that in a bulk covellite showing no evidence of quantum confinement or hot‐hole trapping at the surface states. The excitation of coherent optical phonon modes in a covellite is also demonstrated, revealing coherent lattice dynamics in plasmonic materials, which until now was mainly limited to dielectrics, semiconductors, and semimetals. These findings show advantages of this new mesoscopic plasmonic material for active control of optical processes.

Direct Visualization and Determination of the Multiple Exciton Generation Rate.

Multiple exciton generation (MEG) takes place in competition to other hot carrier cooling processes. While the determination of carrier cooling rates is well established, direct information on MEG dynamics has been lacking. Here, we present a methodology to obtain the MEG rate directly in the initial ultrafast transient absorption dynamics. This method is most effective to systems with slow carrier cooling rates. Perovskite quantum dots exhibit this property and are used to illustrate this approach. They show a delayed carrier concentration buildup following an excitation pulse above the MEG threshold energy, which is accompanied by a faster carrier relaxation, providing a direct evidence of the MEG process. Numerical modeling within a simple framework of two competing cooling mechanisms allows us to extract the MEG rate and carrier energy cooling rates for this material. The presented methodology could provide new insights in carrier generation physics and valuable information for MEG investigations.

Epitaxial Growth of Topological Insulators on Semiconductors (Bi2Se3/Te@Se) toward High‐Performance Photodetectors

AbstractHeterojunctions, composed of different materials, are widely explored in optoelectronic devices thanks to their unique advantages, such as high carrier mobility and excellent photoelectronic characteristics. In this work, Bi2Se3/Te@Se heterojunctions (Bi2Se3/Te@Se) are synthesized through the epitaxial growth of Bi2Se3 nanosheets (Bi2Se3 NTs) on tellurium@selenium nanotubes (Te@Se NTs) by using a low‐cost and facile solvothermal process. Bi2Se3/Te@Se are further applied in high‐performance photoelectrochemical (PEC)‐type photodetection due to the advantages of broadband optical response and fast carrier relaxation time. The PEC results demonstrate that the as‐prepared photodetectors have pronounced photoresponse behavior from the ultraviolet to visible band with self‐driven ability and excellent long‐term stability. It is anticipated that this work provides a new strategy for epitaxial growth of topological insulators on semiconductors for designing new heterojunctions toward high‐performance optoelectronic devices.

Recent Progress in Two-Dimensional Nanomaterials for Laser Protection

The Nobel Prize in Physics 2018, “For groundbreaking inventions in the field of laser physics”, went to Arthur Ashkin and Gérard Mourou and Donna Strickland. Their inventions have revolutionized laser physics and greatly promoted the development of laser instruments, which have penetrated into many aspects of people’s daily lives. However, for the purpose of protecting human eyes or optical instruments from being damaged by both pulsed and continuous wave laser radiation, the research on laser protective materials is of particular significance. Due to the intriguing and outstanding physical, chemical, and structural properties, two-dimensional (2D) nanomaterials have been extensively studied as optical limiting (OL) materials owing to their broadband nonlinear optical (NLO) response and fast carrier relaxation dynamics that are important for reducing the laser intensity. This review systematically describes the OL mechanisms and the recent progress in 2D nanomaterials for laser protection.

Spin–Orbit Interactions Greatly Accelerate Nonradiative Dynamics in Lead Halide Perovskites

In this work, we study the role of spin–orbit coupling (SOC) in nonradiative relaxation of hot electrons and holes in methylammonium lead perovskite, MAPbI3. For this purpose, we have developed the nonadiabatic molecular dynamics method with two-component spinor wave functions that are solutions of the relativistic Kohn–Sham (KS) equations. We find that SOC enhances contributions of Pb(px) and Pb(py) orbitals to the conduction and valence bands. As a result, the KS orbitals become more sensitive to nuclear motions, leading to the increased nonadiabatic couplings. Consequently, SOC greatly speeds up the electron and hole relaxation, making the computed relaxation time scales consistent with available experiments. We suggest that the fast hot carrier relaxation facilitated by the SOC allows rapid transition into the long-lived triplet state that extends charge-carrier lifetime and helps achieve high-efficiency perovskite solar cells.

Passive and hybrid mode locking in multi-section terahertz quantum cascade lasers

It is believed that passive mode locking is virtually impossible in quantum cascade lasers (QCLs) because of too fast carrier relaxation time. Here, we revisit this possibility and theoretically show that stable mode locking and pulse durations in the few cycle regime at terahertz (THz) frequencies are possible in suitably engineered bound-to-continuum QCLs. We achieve this by utilizing a multi-section cavity geometry with alternating gain and absorber sections. The critical ingredients are the very strong coupling of the absorber to both field and environment as well as a fast absorber carrier recovery dynamics. Under these conditions, even if the gain relaxation time is several times faster than the cavity round trip time, generation of few-cycle pulses is feasible. We investigate three different approaches for ultrashort pulse generation via THz quantum cascade lasers, namely passive, hybrid and colliding pulse mode locking.

Towards sensitive terahertz detection via thermoelectric manipulation using graphene transistors

Graphene has been highly sought after as a potential candidate for hot-electron terahertz (THz) detection benefiting from its strong photon absorption, fast carrier relaxation, and weak electron-phonon coupling. Nevertheless, to date, graphene-based thermoelectric THz photodetection is hindered by low responsivity owing to relatively low photoelectric efficiency. In this work, we provide a straightforward strategy for enhanced THz detection based on antenna-coupled CVD graphene transistors with the introduction of symmetric paired fingers. This design enables switchable photodetection modes by controlling the interaction between the THz field and free hot carriers in the graphene-channel through different contacting configurations. Hence a novel “bias-field effect” can be activated, which leads to a drastic enhancement in THz detection ability with maximum responsivity of up to 280 V/W at 0.12 THz relative to the antenna area and a Johnson-noise limited minimum noise-equivalent power (NEP) of 100 pW/Hz0.5 at room temperature. The mechanism responsible for the enhancement in the photoelectric gain is attributed to thermophotovoltaic instead of plasma self-mixing effects. Our results offer a promising alternative route toward scalable, wafer-level production of high-performance graphene detectors.

Ultrafast carrier dynamics in Ge by ultra-broadband mid-infrared probe spectroscopy

In this study, we carried out 800-nm pump and ultra-broadband mid-infrared (MIR) probe spectroscopy with high time-resolution (70 fs) in bulk Ge. By fitting the time-resolved difference reflection spectra [ΔR(ω)/R(ω)] with the Drude model in the 200–5000 cm−1 region, the time-dependent plasma frequency and scattering rate have been obtained. Through the calculation, we can further get the time-dependent photoexcited carrier concentration and carrier mobility. The Auger recombination essentially dominates the fast relaxation of photoexcited carriers within 100 ps followed by slow relaxation due to diffusion. Additionally, a novel oscillation feature is clearly found in time-resolved difference reflection spectra around 2000 cm−1 especially for high pump fluence, which is the Lorentz oscillation lasting for about 20 ps due to the Coulomb force exerted just after the excitation.

Fast Relaxation of Photo-Excited Carriers in 2-D Transition Metal Dichalcogenides

We predict a fast relaxation of photo-excited carriers in monolayer transition metal dichalcogenides (TMDCs), which is mediated by the emission of longitudinal optical (LO) phonons. By evaluating Born effective charges for ${\rm MoS_2, MoSe_2,WS_2}$, and ${\rm WSe_2}$, we find that, due to the polar coupling of electrons with LO phonons, the relaxation times for hot electrons and holes are of the order of a few ps.

Localized Surface Plasmon Resonance Assisted Photothermal Catalysis of CO and Toluene Oxidation over Pd–CeO2 Catalyst under Visible Light Irradiation

The extinction peak of Pd particles generally locates at the ultraviolet light region, suggesting that only 4% of solar light can be absorbed. Furthermore, the efficiency of LSPR hot electrons converted to chemical energy of reaction is very low due to the fast relaxation of carriers. It is extremely valuable to design Pd-based catalysts which have strong response to the visible light irradiation and high efficiency in photon to chemical energy. The Pd–CeO2 catalyst was synthesized via the hexadecyltrimethylammonium bromide (CTAB) assisted liquid-phase reduction method to generate more active interfaces. The significant extinction of Pd–CeO2 in the visible to near-infrared region indicates the strong electron interaction between Pd and CeO2. LSPR hot electrons, transferring from the Pd metal particles to the conduction band of ceria, promote the dissociation of adsorbed oxygen. Therefore, the reaction temperature of CO and toluene oxidation can be significantly lowered by visible light irradiation. The ma...

Carrier relaxation in (In,Ga)As quantum dots with magnetic field-induced anharmonic level structure

Sophisticated models have been worked out to explain the fast relaxation of carriers into quantum dot ground states after non-resonant excitation, overcoming the originally proposed phonon bottleneck. We apply a magnetic field along the quantum dot heterostructure growth direction to transform the confined level structure, which can be approximated by a Fock–Darwin spectrum, from a nearly equidistant level spacing at zero field to strong anharmonicity in finite fields. This changeover leaves the ground state carrier population rise time unchanged suggesting that fast relaxation is maintained upon considerable changes of the level spacing. This corroborates recent models explaining the relaxation by polaron formation in combination with quantum kinetic effects.

Ultrafast Nonlinear Excitation Dynamics of Black Phosphorus Nanosheets from Visible to Mid-Infrared.

The recent progress on black phosphorus makes it a promising candidate material for broadband nanophotonic devices, especially operating in the mid-infrared spectral region. Here, the excited carrier dynamics and nonlinear optical response of unoxidized black phosphorus nanosheets and their wavelength dependence were systematically studied from 800 nm to 2.1 μm. The wavelength-dependent relaxation times of black phosphorus nanosheets are determined to be 360 fs to 1.36 ps with photon energies from 1.55 to 0.61 eV. In a comparative study with graphene, we found that black phosphorus has a faster carrier relaxation in near- and mid-infrared region. With regard to nonlinear optical absorption, the response of black phosphorus significantly increases from near- to mid-infrared, and black phosphorus is also confirmed to be better as saturable absorber to MoS2 in infrared region.

Chaotic light at mid-infrared wavelength.

The onset of nonlinear dynamics and chaos is evidenced in a mid-infrared distributed feedback quantum cascade laser both in the temporal and frequency domains. As opposed to the commonly observed route to chaos in semiconductor lasers, which involves undamping of the laser relaxation oscillations, quantum cascade lasers first exhibit regular self-pulsation at the external cavity frequency before entering into a chaotic low-frequency fluctuation regime. The bifurcation sequence, similar to that already observed in class A gas lasers under optical feedback, results from the fast carrier relaxation dynamics occurring in quantum cascade lasers, as confirmed by numerical simulations. Such chaotic behavior can impact various practical applications including spectroscopy, which requires stable single-mode operation. It also allows the development of novel mid-infrared high-power chaotic light sources, thus enabling secure free-space high bit-rate optical communications based on chaos synchronization.

Spike processing with a graphene excitable laser.

Novel materials and devices in photonics have the potential to revolutionize optical information processing, beyond conventional binary-logic approaches. Laser systems offer a rich repertoire of useful dynamical behaviors, including the excitable dynamics also found in the time-resolved “spiking” of neurons. Spiking reconciles the expressiveness and efficiency of analog processing with the robustness and scalability of digital processing. We demonstrate a unified platform for spike processing with a graphene-coupled laser system. We show that this platform can simultaneously exhibit logic-level restoration, cascadability and input-output isolation—fundamental challenges in optical information processing. We also implement low-level spike-processing tasks that are critical for higher level processing: temporal pattern detection and stable recurrent memory. We study these properties in the context of a fiber laser system and also propose and simulate an analogous integrated device. The addition of graphene leads to a number of advantages which stem from its unique properties, including high absorption and fast carrier relaxation. These could lead to significant speed and efficiency improvements in unconventional laser processing devices, and ongoing research on graphene microfabrication promises compatibility with integrated laser platforms.

Multilayer-WS2:ferroelectric composite for ultrafast tunable metamaterial-induced transparency applications

An ultrafast and low-power all-optical tunable metamaterial-induced transparency is realized, using polycrystalline barium titanate doped gold nanoparticles and multilayer tungsten disulfide microsheets as nonlinear optical materials. Large nonlinearity enhancement is obtained associated with quantum confinement effect, local-field effect, and reinforced interaction between light and multilayer tungsten disulfide. Low threshold pump intensity of 20 MW/cm2 is achieved. An ultrafast response time of 85 ps is maintained because of fast carrier relaxation dynamics in nanoscale crystal grains of polycrystalline barium titanate. This may be useful for the study of integrated photonic devices based on two-dimensional materials.

Strong charge-carrier localization in InAs/GaAs submonolayer stacks prepared by Sb-assisted metalorganic vapor-phase epitaxy

Stacks of InAs/GaAs submonolayer depositions forming small In-rich islands are interesting for efficient optoelectronic applications due to the high areal density of localization centers and their fast carrier relaxation. The electronic confinement of charge carriers in InAs/GaAs submonolayers can be influenced by adding Sb during growth. Eight-band $k\ifmmode\cdot\else\textperiodcentered\fi{}p$ simulations show that electrons and holes experience a different localization depending on where the Sb is incorporated into the submonolayer stacks. Samples grown with metalorganic vapor-phase epitaxy show sharp interfaces between InAs(Sb)/GaAs submonolayers and the surrounding matrix material in transmission electron microscopy and x-ray diffraction measurements. Cross-sectional scanning tunneling microscopy shows the formation of In-rich agglomerations as well as a slight clustering of Sb atoms. Temperature-dependent photoluminescence and spatially resolved cathodoluminescence show evidence for strong electronic confinement whose depth is controlled by the Sb amount.