Hot Phonon Effects Research Articles

Photocarrier relaxation and saturable absorption in defect-rich, direct chemical vapor deposition-grown graphene glass

Direct growth of large-area uniform graphene films on insulating materials could facilitate the applications of graphene in optoelectronic devices. The ultrafast photocarrier relaxation and saturable absorption of direct chemical vapor deposition-grown graphene glasses, with lots of defects, are studied by using femtosecond time-resolved pump–probe and Z-scan techniques at 800 nm. We find that both the relaxation times associated with hot carrier cooling and the hot phonon effect are greatly suppressed in these defect-rich graphene glasses, which further leads to the increase of both saturation intensity and anisotropy in transient optical response for graphene glasses as compared with defect-free graphene. And, both the suppression effect and saturation intensity increase with the thickness of graphene film. The dominance of defect-assisted carrier-acoustic phonon scattering (i.e., supercollision, the collision of a carrier with both an acoustic phonon and defects) in the cooling process of hot carriers is responsible for the suppression of relaxation time.

Competition Pathways of Energy Relaxation of Hot Electrons through Coupling with Optical, Surface, and Acoustic Phonons

The hot electrons in carbon-based materials exhibit interesting ballistic transport behaviors for designing high-performance single-electron transistors. However, the cooling of such hot electrons back to the equilibrium state may be slowed down by the excessively populated optical phonons, thus limiting their ballistic transport. Therefore, a thorough understanding of the coupling between hot electrons and optical phonons is of critical importance. Here, by varying the thickness of a multilayer graphene film on a supporting substrate, we investigated the competition pathways of the energy relaxation of the photoinduced hot electrons through coupling with the optical, surface, and acoustic phonons. The difference in the τ2 values indicates that thickness plays an important role in the optical phonon population. For the multilayer graphene film thickness less than 3 nm, the super-collision model describes the hot electron cooling dynamics that is strongly affected by the surface phonons from the supporting substrate. As the multilayer graphene film thickness increases from 3 to 20 nm, the accumulation of the optical phonons induces a hot optical phonon effect, resulting in a bottleneck of cooling of the hot electrons. As the multilayer graphene film thickness further increases from 20 to 40 nm, a direct coupling between the hot electrons and acoustic phonons starts to dominate. The surface states of the interfaces at the inner layers of the multilayer graphene film contribute to this direct coupling as an additional cooling channel. The quantitative understanding of the energy relaxation pathways of the hot electrons offers insights into designing high-performance single-electron transistors.

Direct Observation of Ultrafast Lattice Distortions during Exciton-Polaron Formation in Lead Halide Perovskite Nanocrystals.

The microscopic origin of slow hot-carrier cooling in lead halide perovskites remains debated and has direct implications for applications. Slow hot-carrier cooling of several picoseconds has been attributed to either polaron formation or a hot-phonon bottleneck effect at high excited carrier densities (>1018 cm-3). These effects cannot be unambiguously disentangled with optical experiments alone. However, they can be distinguished by direct observations of ultrafast lattice dynamics, as these effects are expected to create qualitatively distinct fingerprints. To this end, we employ femtosecond electron diffraction and directly measure the sub-picosecond lattice dynamics of weakly confined CsPbBr3 nanocrystals following above-gap photoexcitation. While we do not observe signatures of a hot-phonon bottleneck lasting several picoseconds, the data reveal a light-induced structural distortion appearing on a time scale varying between 380 and 1200 fs depending on the excitation fluence. We attribute these dynamics to the effect of exciton-polarons on the lattice and the slower dynamics at high fluences to slower sub-picosecond hot-carrier cooling, which slows down the establishment of the exciton-polaron population. Further analysis and simulations show that the distortion is consistent with motions of the [PbBr3]- octahedral ionic cage, and closest agreement with the data is obtained for Pb-Br bond lengthening. Our work demonstrates how direct studies of lattice dynamics on the sub-picosecond time scale can discriminate between competing scenarios proposed in the literature to explain the origin of slow hot-carrier cooling in lead halide perovskites.

Electron energy relaxation in SiGe quantum wells

In this article, we theoretically calculated the hot electron energy relaxation induced by longitudinal acoustic (LA) phonons, longitudinal optical (LO) phonons and importantly two-transverse acoustic (2TA) phonons in two-dimensional SiGe quantum wells, by incorporating dynamic screening effect in LA phonon scattering and hot-phonon effect in LO phonon scattering mechanisms. At the low-temperature regime, the ELR is found to be dominated by LA phonons and at higher temperature ELR is dominated by LO phonons. In the intermediate temperature range, 2TA phonon scattering mechanism is very important and we incorporated in our calculations. The unscreened longitudinal acoustic (LA) phonon due to deformation potential (DP) coupling is dominant over the screened acoustic piezoelectric phonon contribution. At higher temperatures, there is a crossover from ELR due to LA phonons to ELR due to longitudinal optical (LO) phonons with the cross-over temperature being about Te∼40K. The LA phonon screening effect and hot phonon effect is demonstrated to reduce ELR significantly. In the intermediate temperature range (30 K

Determination of hot-electron drift velocity in (Be)ZnMgO/ZnO 2DEG channels

Recent experimental study of electron transport in ZnO/ZnMgO and BeZnMgO/ZnO heterostructures containing two-dimensional electron gas (2DEG) channels of two polarities is reported where electrons are accelerated and become hot by a pulsed electric field. The measurements with electrical pulses ranging from 2 ns to 10 ns in duration ensure the control of self-heating effect. Electron transport in the ZnO 2DEG channels located in ZnO layers at the ZnMgO or BeZnMgO barrier or in ZnO 3DEG channels is treated mainly in terms of drift velocity. The highest values of 1.3 × 107 cm/s at 360 kV/cm, 2.0 × 107 cm/s at 270 kV/cm, and 2.5 × 107 cm/s and 320 kV/cm, respectively, are attained and explained by emphasizing the effect of hot phonons.

Investigation of Two Photon Absorption of Ligand-Modified CsPbBr3 Quantum Dots.

The characteristics and application of nonlinear absorption from CsPbBr3 QDs film with the ligand-modified strategy have been investigated in this work. By means of a near-infrared fs Ti:sapphire laser as a light source, the up-conversion emission of CsPbBr3 QDs film of around 518 nm revealed a quadratic increase with the pump intensity. Through the temperature-dependent up-conversion emission, we obtained the binding energy and longitudinal optical (LO) phonon energy of CsPbBr3 QDs film of around 58.1 and 61.2 meV, respectively. Due to more active thermal coupling between the excited electron or hot phonon effect, the photon decay trace under two-photon excitation was prolonged at higher temperatures. The ligand-modified CsPbBr3 QDs film exhibits a relatively large TPA coefficient of around 28.6 cm/GW by the open aperture Z-scan measurement, and it has been demonstrated as a promising nonlinear medium to obtain the pulsewidth of ultrafast lasers.

Effects of hot phonons and thermal stress in micro-Raman spectra of molybdenum disulfide

Micro-Raman spectroscopy has become an important tool in probing thermophysical properties in functional materials. Localized heating by the focused Raman excitation laser beam can produce both stress and local nonequilibrium phonons in the material. Here, we investigate the effects of hot optical phonons in the Raman spectra of molybdenum disulfide and distinguish them from those caused by thermally induced compressive stress, which causes a Raman frequency blue shift. We use a thermomechanical analysis to correct for this stress effect in the equivalent lattice temperature extracted from the measured Raman peak shift. When the heating Gaussian laser beam is reduced to 0.71 μm, the corrected peak shift temperature rise is 17% and 8%, respectively, higher than those determined from the measured peak shift and linewidth without the stress correction, and 32% smaller than the optical phonon temperature rise obtained from the anti-Stokes to Stokes intensity ratio. This nonequilibrium between the hot optical phonons and the lattice vanishes as the beam width increases to 1.53 μm. Much less pronounced than those reported in prior micro-Raman measurements of suspended graphene, this observed hot phonon behavior agrees with a first-principles based multitemperature model of overpopulated zone-center optical phonons compared to other optical phonons in the Brillouin zone and acoustic phonons of this prototypical transition metal dichalcogenide. The findings provide detailed insight into the energy relaxation processes in this emerging electronic and optoelectronic material and clarify an important question in micro-Raman measurements of thermal transport in this and other two-dimensional materials.

Hot and cold phonons in electrically biased graphene

Based on first-principles calculations and semiclassical transport theory, we study the nonequilibrium phonon distribution in graphene in the presence of electrical current. In addition to the hot-phonon effect, we observe a cooling of phonon modes at the same time. Interestingly, the presence of electric current along the direction connecting $K$ and ${K}^{\ensuremath{'}}$ valleys induces an opposite dipolelike temperature distribution in the two valleys and at the $\mathrm{\ensuremath{\Gamma}}$ point. This leads to a ``high-order'' valley polarization of phonon distribution between $K$ and ${K}^{\ensuremath{'}}$. Based on the nonequilibrium phonon distribution, we furthermore study their effect on the lattice parameters and find a negative current-induced expansion coefficient. Similar to graphene's negative thermal expansion, this is rooted in the dominant contribution of out-of-plane acoustic phonons, which do not couple directly to electrons, but gain energy from in-plane phonons through anharmonic scattering.

Hot phonon effects and Auger recombination on 3 μm room temperature lasing in HgTe-based multiple quantum well diodes

We propose an electrically pumped laser diode based on multiple HgTe quantum wells with band structure engineered for Auger recombination suppression. A model for accounting for hot phonons is developed for calculating the nonequilibrium temperature of electrons and holes. Using a comprehensive model accounting for carrier drift and diffusion, Auger recombination, and hot-phonon effects, we predict of lasing at λ∼3 μm at room temperature in the 2.1 nm HgTe/Cd0.85Hg0.15Te quantum well heterostructure. The output power in the pulse can reach up to 600 mW for 100 nanosecond-duration pulses.

Electron heating in GaN/AlGaN quantum well in a longitudinal electric field

The heating of electrons under longitudinal optical phonon scattering in a triangular GaN/AlGaN quantum well was studied theoretically. The energy loss rate of electrons was calculated in consideration of the dynamical screening and the hot phonon effect. The dependence of the electron temperature on the longitudinal electric field was calculated. The integral terahertz emission of hot two-dimensional electrons was simulated. The role of coupled plasmon-phonon mode scattering in the GaN/AlGaN quantum well was discussed.

Ultrafast real-time tracing of surface electric field generated via hot electron transport in polar semiconductors

We trace an ultrafast real-space motion of photo-excited free carriers just near the surface of polar semiconductors GaAs and InAs by using the optical second-harmonic generation (SHG) technique. With a flat distribution of photo-carriers as an initial condition, ultrafast diffusion and drift motion followed by a rapid surface recombination develop a surface electric field which is efficiently probed by the electric-field-induced SHG. From the simulation based on the drift–diffusion equation combined with the ensemble Monte-Carlo approach, we could explain the experimental observation of the temporal evolution of the surface electric field, and extract time constants related to the hot electron cooling. Whereas the hot carrier cooling time is determined to be about 8 ps at room temperature for GaAs, it can be further extended to about 35 ps at 100 K due to the increase of the longitudinal optic phonon life time enhancing the hot phonon effect. Our work can be an important guide in designing optoelectronic nano-devices by providing a clear understanding of the ultrafast electron-hole separation near the surface of polar semiconductors in connection with the hot carrier cooling process.

Photoexcited carrier dynamics of thin film Cd3As2 grown on a GaAs(111)B substrate by molecular beam epitaxy

The topological Dirac semimetal ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ has drawn great attention for its novel physics and technical applications in optoelectronic devices operating in the infrared and THz regimes. Exploring the photoexcited carrier dynamics in ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ is helpful to understand the transient carrier occupation and cooling processes that are closely associated with its unconventional band characteristic. Here, the photoexcited carrier dynamics in the ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ thin film epitaxially grown on the $\mathrm{GaAs}(111)B$ substrate was investigated by employing the time-resolved midinfrared transient reflectance measurements, along with a theoretical modeling concerning the electron-polar optical ($e$-PO) phonon interaction. The measured photoexcited electron relaxation time of ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ increases with the probe wavelength, and increases with temperature at temperatures higher than 30 K. Theoretical modeling under the framework of the two-temperature model can give qualitatively good description on both the temperature and probe wavelength dependence of the carrier relaxation time. Additionally, theoretical modeling shows that charge screening of the interaction of electrons with polar optical phonons can greatly reduce the hot carrier relaxation rate. The measured transient reflectance analyses indicate that the hot phonon effect plays a negligible role on the carrier relaxation in ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$. Our findings provide further insight into the photoexcited carrier dynamics in ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ and valuable reference for developing its high-performance infrared optoelectronic devices.

Oscillations of the electron energy loss rate in two-dimensional transition-metal dichalcogenides in the presence of a quantizing magnetic field

We study the hot electron energy-loss rate (ELR) induced by acoustic ${P}^{\mathrm{ac}}$ and optical ${P}^{\mathrm{op}}$ phonons, in two-dimensional transition-metal dichalcogenides (TMDCs), in presence of quantizing magnetic field $B$, including the hot-phonon effect. At the low-temperature regime, the ELR is found to display a quantum oscillations with their amplitude being found to increase with the increase of the magnetic field. The unscreened TA phonon due to deformation potential (DP) coupling is dominant over the other screened acoustic phonon contributions. In the extreme Bloch-Gr\"uneisen (BG) region, the ELR displays a pronounced ${P}^{\mathrm{ac}}\ensuremath{\propto}{T}^{4}\phantom{\rule{0.16em}{0ex}}({T}^{6})$ temperature dependence for unscreened TA-DP phonons (other screened mechanisms). When the temperature increases, ${T}_{e}>{T}_{\mathrm{BG}}$, the ELR shows a linear ${P}^{\mathrm{ac}}\ensuremath{\propto}T$ behavior in the equipartition region. At higher temperatures, there is a crossover from ${P}^{\mathrm{ac}}$ dominated ELR to ${P}^{\mathrm{op}}$ by zeroth-order DP coupling dominated ELR with the cross-over temperature being about ${T}_{e}\ensuremath{\sim}50\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. The hot phonon effect is demonstrated to reduce ELR significantly. The effect of the magnetic field is found to enhance the ELR significantly, making $B$ as its another tuning knob. Among the four TMDC materials, ${\mathrm{MoS}}_{2}$ (${\mathrm{MoSe}}_{2}$) displays the biggest ELR due to acoustic (optical) phonon scattering while ${\mathrm{WSe}}_{2}$ (${\mathrm{WS}}_{2}$) shows the smallest ELR. Our results for the ${\mathrm{MoS}}_{2}$ material are compared with those of the zero-field ELR.

Hot-phonon effects in photo-excited wide-bandgap semiconductors

Carrier and lattice relaxation after optical excitation is simulated for the prototypical wide-bandgap semiconductors CuI and ZnO. Transient temperature dynamics of electrons, holes as well as longitudinal-optic (LO), transverse-optic (TO) and acoustic phonons are distinguished. Carrier-LO-phonon interaction constitutes the dominant energy-loss channel as expected for polar semiconductors and hot-phonon effects are observed for strong optical excitation. Our results support the findings of recent time-resolved optical spectroscopy experiments.

Effect of spin–orbit coupling on the hot-electron energy relaxation in nanowires

The energy relaxation of hot electrons is proposed based on the spin–orbit (SO) interaction of both Rashba and Dresselhaus types with the effect of hot phonons. A continuum theory of optical phonons in nanowires taking into account the influence of confinement is used to study the hot-electron energy relaxation. The energy relaxation due to both confined (CO) and interface (IO) optical phonon emission on nanowire radius, electrical field strength, parameters of SO couplings and electron temperature is calculated. For considered values of the nanowire radius as well as other system parameters, scattering by IO phonons prevails over scattering by CO phonons. The presence of an electric field leads to the decrease of power loss in transitions between states with the same spin quantum numbers. With the increase of the electric field strength, the influence of the Dresselhaus SO interaction on the energy relaxation rate decreases. The effect of SO interaction does not change the previously obtained increasing dependence of power loss on electron temperature. The sensitivity of energy relaxation to the electric field also through the Rashba parameter allows controlling the rate of energy by electric field.

Giant isotope effect on phonon dispersion and thermal conductivity in methylammonium lead iodide.

Lead halide perovskites are strong candidates for high-performance low-cost photovoltaics, light emission, and detection applications. A hot-phonon bottleneck effect significantly extends the cooling time of hot charge carriers, which thermalize through carrier-optic phonon scattering, followed by optic phonon decay to acoustic phonons and finally thermal conduction. To understand these processes, we adjust the lattice dynamics independently of electronics by changing isotopes. We show that doubling the mass of hydrogen in methylammonium lead iodide by replacing protons with deuterons causes a large 20 to 50% softening of the longitudinal acoustic phonons near zone boundaries, reduces thermal conductivity by ~50%, and slows carrier relaxation kinetics. Phonon softening is attributed to anticrossing with the slowed libration modes of the deuterated molecules and the reduced thermal conductivity to lowered phonon velocities. Our results reveal how tuning the organic molecule dynamics enables control of phonons important to thermal conductivity and the hot-phonon bottleneck.

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.

Drift velocity saturation and large current density in intrinsic three-dimensional Dirac semimetal cadmium arsenide

Transport of electrons at high electric fields is investigated in intrinsic three-dimensional Dirac semimetal cadmium arsenide, considering the scattering of electrons from acoustic and optical phonons. Screening and hot phonon effect are taken in to account. Expressions for the hot electron mobility μ and power loss P are obtained as a function of electron temperature Te. The dependence of drift velocity vd on electric field E and electron density ne has been studied. Hot phonon effect is found to set in the saturation of vd at relatively low E and to significantly degrade its magnitude. The drift velocity is found to saturate at a value vds ∼ 107 cm s−1 and it is weakly dependent on ne. A large saturation current density ∼ 106 A cm−2 is predicted.

Observation of the hot-phonon effect in monolayer MoS2

Femtosecond transient absorption measurements have been performed to study the pump wavelength- and fluence-dependent hot carrier relaxation dynamics in monolayer MoS2. The relaxation process of the photoinduced carriers monitored within hundreds of femtoseconds after photoexcitation is demonstrated to be achieved through the carrier–phonon scattering mechanism. It is observed that an efficient hot-phonon effect can slow down the relaxation rate by around three times with the injected carrier density changing from 1 × 1012 to 3 × 1013 cm−2. A pronounced increase in the hot carrier relaxation time with decreasing temperature is further detected, which is attributed to the decreased phonon occupancy at lower temperature.

AlGaN/GaN High-Electron-Mobility Transistors on a Silicon Substrate Under Uniaxial Tensile Strain

This paper reports pulsed DC and RF characteristics of GaN high-electron-mobility transistors (HEMTs) on a silicon substrate under external mechanical tensile strain. Tensile strain enhanced two-dimensional electron gas (2DEG) density resulted in increasing ID, fT and fmax at CW measurement. Eliminating self-heating by pulse measurement, DC and RF characteristics between flat and bend devices were slightly increased for small-width devices, and decreased for wide-width devices. This was because maximum electron drift velocity was reduced by a hot phonon effect while 2DEG density increased by tensile strain for wide-width devices. Results indicated that the tensile strain on thinner substrates decreased the DC and RF performances of wide-width GaN-based RF power devices. This phenomenon should be considered while using GaN-based RF power devices for compact packages, especially in high-power applications.