arXiv subjects

Farhan Rana

Publications and source records attributed to Farhan Rana.

At least 37 records · Page 2Linked to original sources

arXiv2018

Measurement of Ultrafast Dynamics of Photoexcited Carriers in $β$-Ga$_2$O$_3$ by Two-Color Optical Pump-Probe Spectroscopy

We report results from ultrafast two-color optical pump-probe spectroscopy on bulk $β$-Ga$_2$O$_3$. A two-photon absorption scheme is used to photoexcite carriers with the pump pulse and free-carrier absorption of the probe pulse is used to record the subsequent dynamics of the photoexcited carriers. Our results are consistent with carrier recombination via defect-assisted processes. We also observe transient polarization-selective optical absorption of the probe pulse by defect states under nonequilibrium conditions. A rate equation model for electron and hole capture by defects is proposed and used to explain the data. Whereas the rate constants for electron capture by defects are found to be temperature-independent, they are measured to be strongly temperature-dependent for hole capture and point to a lattice deformation/relaxation process accompanying hole capture. Our results shed light on the mechanisms and rates associated with carrier capture by defects in $β$-Ga$_2$O$_3$.

cond-mat.mtrl-sci↗

arXiv2016

Radiative and Non-Radiative Exciton Energy Transfer in Monolayers of Two-Dimensional Transition Metal Dichalcogenides

We present results on the rates of interlayer energy transfer between excitons in two-dimensional transition metal dichalcogenides (TMDs). We consider both radiative (mediated by real photons) and non-radiative (mediated by virtual photons) mechanisms of energy transfer using a unified Green's function approach that takes into account modification of the exciton energy dispersions as a result of interactions. The large optical oscillator strengths associated with excitons in TMDs result in very fast energy transfer rates. The energy transfer times depend on the exciton momentum, exciton linewidth, and the interlayer separation and can range from values less than 100 femtoseconds to more than tens of picoseconds. Whereas inside the light cone the energy transfer rates of longitudinal and transverse excitons are comparable, outside the light cone the energy transfer rates of longitudinal excitons far exceed those of transverse excitons. Average energy transfer times for a thermal ensemble of longitudinal and transverse excitons is temperature dependent and can be smaller than a picosecond at room temperature for interlayer separations smaller than 10 nm. Energy transfer times of localized excitons range from values less than a picosecond to several tens of picoseconds. When the exciton scattering and dephasing rates are small, energy transfer dynamics exhibit coherent oscillations. Our results show that electromagnetic interlayer energy transfer can be an efficient mechanism for energy exchange between TMD monolayers.

cond-mat.mes-hall↗

arXiv2015

Radiative Lifetimes of Excitons and Trions in Monolayers of Metal Dichalcogenide MoS2

We present results on the radiative lifetimes of excitons and trions in a monolayer of metal dichalcogenide MoS2. The small exciton radius and the large exciton optical oscillator strength result in radiative lifetimes in the 0.18-0.30 ps range for excitons that have small in-plane momenta and couple to radiation. Average lifetimes of thermally distributed excitons depend linearly on the exciton temperature and can be in the few picoseconds range at small temperatures and more than a nanosecond near room temperature. Localized excitons exhibit lifetimes in the same range and the lifetime increases as the localization length decreases. The radiative lifetimes of trions are in the hundreds of picosecond range and increase with the increase in the trion momentum. Average lifetimes of thermally distributed trions increase with the trion temperature as the trions acquire thermal energy and larger momenta. We expect our theoretical results to be applicable to most other 2D transition metal dichalcogenides.

cond-mat.mes-hall↗

arXiv2015

Surface Recombination Limited Lifetimes of Photoexcited Carriers in Few-Layer Transition Metal Dichalcogenide MoS2

We present results on photoexcited carrier lifetimes in few-layer transition metal dichalcogenide MoS2 using nondegenerate ultrafast optical pump-probe technique. Our results show a sharp increase of the carrier lifetimes with the number of layers in the sample. Carrier lifetimes increase from few tens of picoseconds in monolayer samples to more than a nanosecond in 10-layer samples. The inverse carrier lifetime was found to scale according to the probability of the carriers being present at the surface layers, as given by the carrier wavefunction in few layer samples, which can be treated as quantum wells. The carrier lifetimes were found to be largely independent of the temperature and the inverse carrier lifetimes scaled linearly with the photoexcited carrier density. These observations are consistent with defect-assisted carrier recombination, in which the capture of electrons and holes by defects occurs via Auger scatterings. Our results suggest that carrier lifetimes in few-layer samples are surface recombination limited due to the much larger defect densities at the surface layers compared to the inner layers.

cond-mat.mes-hall↗

arXiv2015

Ultrafast Response of Monolayer Molybdenum Disulfide (MoS2) Photodetectors

The strong light emission and absorption exhibited by single atomic layer transitional metal dichalcogenides in the visible to near-infrared wavelength range makes them attractive for optoelectronic applications. In this work, using two-pulse photovoltage correlation technique, we show that monolayer molybdenum disulfide photodetector can have intrinsic response times as short as 3 ps implying photodetection bandwidths as wide as 300 GHz. The fast photodetector response is a result of the short electron-hole and exciton lifetimes in this material. Recombination of photoexcited carriers in most two-dimensional metal dichalcogenides is dominated by non-radiative processes, most notable among which is Auger scattering. The fast response time, and the ease of fabrication of these devices, make them interesting for low-cost ultrafast optical communication links.

cond-mat.mes-hall↗

arXiv2014

Fast Exciton Annihilation by Capture of Electrons or Holes by Defects via Auger Scattering in Monolayer Metal Dichalcogenides

The strong Coulomb interactions and the small exciton radii in two-dimensional metal dichalcogenides can result in very fast capture of electrons and holes of excitons by mid-gap defects from Auger processes. In the Auger processes considered here, an exciton is annihilated at a defect site with the capture of the electron (or the hole) by the defect and the hole (or the electron) is scattered to a high energy. In the case of excitons, the probability of finding an electron and a hole near each other is enhanced many folds compared to the case of free uncorrelated electrons and holes. Consequently, the rate of carrier capture by defects from Auger scattering for excitons in metal dichalcogenides can be 100-1000 times larger than for uncorrelated electrons and holes for carrier densities in the $10^{11}$-$10^{12}$ cm$^{-2}$ range. We calculate the capture times of electrons and holes by defects and show that the capture times can be in the sub-picosecond to a few picoseconds range. The capture rates exhibit linear as well as quadratic dependence on the exciton density. These fast time scales agree well with the recent experimental observations, and point to the importance of controlling defects in metal dichalcogenides for optoelectronic applications.

cond-mat.mes-hall↗

arXiv2014

Ultrafast Dynamics of Defect-Assisted Electron-Hole Recombination in Monolayer MoS2

In this letter, we present non-degenerate ultrafast optical pump-probe studies of the carrier recombination dynamics in MoS$_{2}$ monolayers. By tuning the probe to wavelengths much longer than the exciton line, we make the probe transmission sensitive to the total population of photoexcited electrons and holes. Our measurement reveals two distinct time scales over which the photoexcited electrons and holes recombine; a fast time scale that lasts $\sim$2 ps and a slow time scale that lasts longer than $\sim$100 ps. The temperature and the pump fluence dependence of the observed carrier dynamics are consistent with defect-assisted recombination as being the dominant mechanism for electron-hole recombination in which the electrons and holes are captured by defects via Auger processes. Strong Coulomb interactions in two dimensional atomic materials, together with strong electron and hole correlations in two dimensional metal dichalcogenides, make Auger processes particularly effective for carrier capture by defects. We present a model for carrier recombination dynamics that quantitatively explains all features of our data for different temperatures and pump fluences. The theoretical estimates for the rate constants for Auger carrier capture are in good agreement with the experimentally determined values. Our results underscore the important role played by Auger processes in two dimensional atomic materials.

cond-mat.mes-hall↗

arXiv2014

High Intrinsic Mobility and Ultrafast Carrier Dynamics in Multilayer Metal Dichalcogenide MoS2

The ultimate limitations on carrier mobilities in metal dichalcogenides, and the dynamics associated with carrier relaxation, are unclear. We present measurements of the frequency-dependent conductivity of multilayer dichalcogenide MoS2 by optical-pump terahertz-probe spectroscopy. We find mobilities in this material approaching 4200 cm2/Vs at low temperatures. The temperature dependence of scattering indicates that the mobility, an order of magnitude larger than previously reported for MoS2, is intrinsically limited by acoustic phonon scattering at THz frequencies. Our measurements of carrier relaxation reveal picosecond cooling times followed by recombination lasting tens of nanoseconds and dominated by Auger scattering into defects. Our results provide a useful context in which to understand and evaluate the performance of MoS2-based electronic and optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2014

Coupling of Plasmon Modes in Graphene Microstructures

A variety of different graphene plasmonic structures and devices have been proposed and demonstrated experimentally. Plasmon modes in graphene microstructures interact strongly via the depolarization fields. An accurate quantitative description of the coupling between plasmon modes is required for designing and understanding complex plasmonic devices. Drawing inspiration from microphotonics, we present a coupled-mode theory for graphene plasmonics in which the plasmon eigenmodes of a coupled system are expressed in terms of the plasmon eigenmodes of its uncoupled sub-systems. The coupled-mode theory enables accurate computation of the coupling between the plasmon modes and of the resulting dynamics. We compare theory with experiments performed on the plasmon modes in coupled arrays of graphene strips. In experiments, we tune the coupling by changing the spacing between the graphene strips in the array. Our results show that the coupling parameters obtained from the coupled-mode theory and the plasmon frequency changes resulting from this coupling agree very well with experiments. The work presented here provides a framework for designing and understanding coupled graphene plasmonic structures.

cond-mat.mes-hall↗

arXiv2014

Absorption of Light by Excitons and Trions in Monolayers of Metal Dichalcogenide MoS$_{2}$: Experiments and Theory

We measure the optical absorption spectra and optical conductivities of excitons and trions in monolayers of metal dichalcogenide MoS$_{2}$ and compare the results with theoretical models. Our results show that the Wannier-Mott model for excitons, with modifications to account for small exciton radii and large exciton relative wavefunction spread in momentum space, phase space blocking due to Pauli exclusion in doped materials, and wavevector dependent dielectric constant, gives results that agree well with experiments. The measured exciton optical absorption spectra are used to obtain experimental estimates for the exciton radii that fall in the $7-10Å$ range and agree well with theory. The measured trion optical absorption spectra are used to obtain values for the trion radii that also agree well with theory. The measured values of the exciton and trion radii correspond to binding energies that are in good agreement with values obtained from first principles calculations.

cond-mat.mes-hall↗

arXiv2014

Temperature Renormalization of Optical Spectra of Monolayer MoS2

Newly measured optical absorption and photoluminescence spectra reveal substantial frequency shifts of both exciton and trion peaks as monolayer MoS2 is cooled from 363 K to 4 K. First-principles simulations using the GW-Bethe-Salpeter Equation approach satisfactorily reproduce these frequency shifts by incorporating many-electron interactions and the thermal expansion of the in-plane lattice constant. Studying these temperature effects in monolayer MoS2 is crucial for rectifying the results of room-temperature experiments with the previous predictions of zero-temperature-limit simulations. Moreover, we estimate that the thermal expansion coefficient of monolayer MoS2 is around 25% less than that of bulk counterpart by tracking the frequency shifts of the exciton or trion peaks in optical spectra. This may serve as a convenient way to estimate thermal expansion coefficients of general two-dimensional chalcogenides.

cond-mat.mes-hall↗

arXiv2013

Confined Plasmons in Graphene Microstructures: Experiments and Theory

Graphene, a two-dimensional material with a high mobility and a tunable conductivity, is uniquely suited for plasmonics. The frequency dispersion of plasmons in bulk graphene has been studied both theoretically and experimentally, whereas no theoretical models have been reported and tested against experiments for confined plasmon modes in graphene microstructures. In this paper, we present experimental measurements as well as analytical and computational models for such confined modes. We compare experimental measurements with theory for plasmon modes in interacting arrays of graphene strips and demonstrate a good agreement. The comparison between experimental and theoretical results reveals the important role played by interaction among the plasmon modes of neighboring graphene structures.

cond-mat.mes-hall↗

arXiv2011

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 temperatures. We find that at lower temperatures the tail of the relaxation transients as measured by the differential probe transmission becomes slower, extending beyond several hundred picoseconds at temperatures below 50K. We interpret the observed relaxation transients as resulting from the cooling of the photoexcited carriers via phonon emission. The slow cooling of the photoexcited carriers at low temperatures is attributed to the bulk of the electron and hole energy distributions moving close enough to the Dirac point such that both intraband and interband scattering of carriers via optical phonon emission becomes 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.

cond-mat.mes-hall↗

arXiv2011

Ultrafast Carrier Recombination and Generation Rates for Plasmon Emission and Absorption in Graphene

Electron-hole generation and recombination rates for plasmon emission and absorption in Graphene are presented. The recombination times of carriers due to plasmon emission have been found to be in the tens of femtoseconds to hundreds of picoseconds range. The recombination times depend sensitively on the carrier energy, carrier density, temperature, and the plasmon dispersion. Carriers near the Dirac point are found to have much longer lifetimes compared to carriers at higher energies. Plasmons in a Graphene layer on a polar substrate hybridize with the surface optical phonons and this hybridization modifies the plasmon dispersion. We also present generation and recombination rates of carriers due to plasmon emission and absorption in Graphene layers on polar substrates.

cond-mat.mes-hall↗

arXiv2009

Ultrafast Relaxation Dynamics of Hot Optical Phonons in Graphene

Using ultrafast optical pump-probe spectroscopy, we study the relaxation dynamics of hot optical phonons in few-layer and multi-layer graphene films grown by epitaxy on silicon carbide substrates and by chemical vapor deposition on nickel substrates. In the first few hundred femtoseconds after photoexcitation, the hot carriers lose most of their energy to the generation of hot optical phonons which then present the main bottleneck to subsequent carrier cooling. Optical phonon cooling on short time scales is found to be independent of the graphene growth technique, the number of layers, and the type of the substrate. We find average phonon lifetimes in the 2.5-2.55 ps range. We model the relaxation dynamics of the coupled carrier-phonon system with rate equations and find a good agreement between the experimental data and the theory. The extracted optical phonon lifetimes agree very well with the theory based on anharmonic phonon interactions.

cond-mat.mes-hall↗

arXiv2009

Emission of Terahertz Radiation from SiC

We report the emission of strong coherent broadband terahertz radiation from 6H-Silicon-Carbide (SiC) excited with optical pulses. The measured terahertz spectral signal-to-noise ratio is better than one thousand. We determine that the terahertz radiation is generated via second order optical nonlinearity (optical rectification). We present a measurement of the ratio of nonlinear susceptibility tensor elements $χ_{zzz}^{(2)}/χ_{zxx}^{(2)}$ and the complex index of refraction of silicon carbide at THz frequencies.

cond-mat.mtrl-sci↗

arXiv2009

Measurements of the Carrier Dynamics and Terahertz Response of Oriented Germanium Nanowires using Optical-Pump Terahertz-Probe Spectroscopy

We have measured the terahertz response of oriented germanium nanowires using ultrafast optical-pump terahertz-probe spectroscopy. We present results on the time, frequency, and polarization dependence of the terahertz response. Our results indicate intraband energy relaxation times of photoexcited carriers in the 1.5-2.0 ps range, carrier density dependent interband electron-hole recombination times in the 75-125 ps range, and carrier momentum scattering rates in the 60-90 fs range. Additionally, the terahertz response of the nanowires is strongly polarization dependent despite the subwavelength dimensions of the nanowires. The differential terahertz transmission is found to be large when the field is polarized parallel to the nanowires and very small when the field is polarized perpendicular to the nanowires. This polarization dependence of the terahertz response can be explained in terms of the induced depolarization fields and the resulting magnitudes of the surface plasmon frequencies.

cond-mat.mes-hall↗

arXiv2009

Carrier Recombination and Generation Rates for Intravalley and Intervalley Phonon Scattering in Graphene

Electron-hole generation and recombination rates for intravalley and intervalley phonon scattering in Graphene are presented. The transverse and the longitudinal optical phonon modes ($E_{2g}$-modes) near the zone center ($Γ$-point) contribute to intravalley interband carrier scattering. At the zone edge ($K(K')$-point), only the transverse optical phonon mode ($A'_{1}$-mode) contributes significantly to intervalley interband scattering with recombination rates faster than those due to zone center phonons. The calculated recombination times range from less than a picosecond to more than hundreds of picoseconds and are strong functions of temperature and electron and hole densities. The theoretical calculations agree well with experimental measurements of the recombination rates of photoexcited carriers in graphene.

cond-mat.mes-hall↗