Keshav M. Dani

Subpicosecond Optical Switching with a Negative Index Metamaterial

We demonstrate a nanoscale, subpicosecond (ps) metamaterial device capable of terabit/second all-optical communication in the near-IR. The 600 fs response, 2 orders of magnitude faster than previously reported, is achieved by accessing a previously unused regime of high-injection level, subpicosecond carrier dynamics in the alpha-Si dielectric layer of the metamaterial. Further, we utilize a previously unrecognized, higher-order, shorter-wavelength negative-index resonance in the fishnet structure, thereby extending device functionality (via structural tuning of device dimensions) over 1.0-2.0 microm. The pump energy required to modulate a single bit is only 3 nJ over our current 700 microm(2) area device and can be easily scaled into the picoJoule regime with smaller cross sectional areas.

Ultrafast Enhancement of Ferromagnetism via Photoexcited Holes in GaMnAs

We report on the observation of ultrafast photoenhanced ferromagnetism in GaMnAs. It is manifested as a transient magnetization increase on a 100 ps time scale, after an initial subpicosecond demagnetization. The dynamic magnetization enhancement exhibits a maximum below the Curie temperature T(c) and dominates the demagnetization component when approaching T(c). We attribute the observed ultrafast collective ordering to the p-d exchange interaction between photoexcited holes and Mn spins, leading to a correlation-induced peak around 20 K and a transient increase in T(c).

Chemical Vapor Deposition Synthesized Atomically Thin Molybdenum Disulfide with Optoelectronic-Grade Crystalline Quality

The ability to synthesize high-quality samples over large areas and at low cost is one of the biggest challenges during the developmental stage of any novel material. While chemical vapor deposition (CVD) methods provide a promising low-cost route for CMOS compatible, large-scale growth of materials, it often falls short of the high-quality demands in nanoelectronics and optoelectronics. We present large-scale CVD synthesis of single- and few-layered MoS2 using direct vapor-phase sulfurization of MoO2, which enables us to obtain extremely high-quality single-crystal monolayer MoS2 samples with field-effect mobility exceeding 30 cm(2)/(V s) in monolayers. These samples can be readily synthesized on a variety of substrates, and demonstrate a high-degree of optoelectronic uniformity in Raman and photoluminescence mapping over entire crystals with areas exceeding hundreds of square micrometers. Because of their high crystalline quality, Raman spectroscopy on these samples reveal a range of multiphonon processes through peaks with equal or better clarity compared to past reports on mechanically exfoliated samples. This enables us to investigate the layer thickness and substrate dependence of the extremely weak phonon processes at 285 and 487 cm(-1) in 2D-MoS2. The ultrahigh, optoelectronic-grade crystalline quality of these samples could be further established through photocurrent spectroscopy, which clearly reveal excitonic states at room temperature, a feat that has been previously demonstrated only on samples which were fabricated by micro-mechanical exfoliation and then artificially suspended across trenches. Our method reflects a big step in the development of atomically thin, 2D-MoS2 for scalable, high-quality optoelectronics.

Imaging the motion of electrons across semiconductor heterojunctions

Technological progress since the late twentieth century has centred on semiconductor devices, such as transistors, diodes and solar cells. At the heart of these devices is the internal motion of electrons through semiconductor materials due to applied electric fields or by the excitation of photocarriers. Imaging the motion of these electrons would provide unprecedented insight into this important phenomenon, but requires high spatial and temporal resolution. Current studies of electron dynamics in semiconductors are generally limited by the spatial resolution of optical probes, or by the temporal resolution of electronic probes. Here, by combining femtosecond pump-probe techniques with spectroscopic photoemission electron microscopy, we imaged the motion of photoexcited electrons from high-energy to low-energy states in a type-II 2D InSe/GaAs heterostructure. At the instant of photoexcitation, energy-resolved photoelectron images revealed a highly non-equilibrium distribution of photocarriers in space and energy. Thereafter, in response to the out-of-equilibrium photocarriers, we observed the spatial redistribution of charges, thus forming internal electric fields, bending the semiconductor bands, and finally impeding further charge transfer. By assembling images taken at different time-delays, we produced a movie lasting a few trillionths of a second of the electron-transfer process in the photoexcited type-II heterostructure-a fundamental phenomenon in semiconductor devices such as solar cells. Quantitative analysis and theoretical modelling of spatial variations in the movie provide insight into future solar cells, 2D materials and other semiconductor devices.

20 THz broadband generation using semi-insulating GaAs interdigitated photoconductive antennas

We demonstrate broadband (20 THz), high electric field, terahertz generation using large area interdigitated antennas fabricated on semi-insulating GaAs. The bandwidth is characterized as a function of incident pulse duration (15-35 fs) and pump energy (2-30 nJ). Broadband spectroscopy of PTFE is shown. Numerical Drude-Lorentz simulations of the generated THz pulses are performed as a function of the excitation pulse duration, showing good agreement with the experimental data.

Protecting the properties of monolayer MoS2 on silicon based substrates with an atomically thin buffer

Semiconducting 2D materials, like transition metal dichalcogenides (TMDs), have gained much attention for their potential in opto-electronic devices, valleytronic schemes, and semi-conducting to metallic phase engineering. However, like graphene and other atomically thin materials, they lose key properties when placed on a substrate like silicon, including quenching of photoluminescence, distorted crystalline structure, and rough surface morphology. The ability to protect these properties of monolayer TMDs, such as molybdenum disulfide (MoS2), on standard Si-based substrates, will enable their use in opto-electronic devices and scientific investigations. Here we show that an atomically thin buffer layer of hexagonal-boron nitride (hBN) protects the range of key opto-electronic, structural, and morphological properties of monolayer MoS2 on Si-based substrates. The hBN buffer restores sharp diffraction patterns, improves monolayer flatness by nearly two-orders of magnitude, and causes over an order of magnitude enhancement in photoluminescence, compared to bare Si and SiO2 substrates. Our demonstration provides a way of integrating MoS2 and other 2D monolayers onto standard Si-substrates, thus furthering their technological applications and scientific investigations.

Ultrafast Intrinsic Photoresponse and Direct Evidence of Sub-gap States in Liquid Phase Exfoliated MoS2Thin Films

2-Dimensional structures with swift optical response have several technological advantages, for example they could be used as components of ultrafast light modulators, photo-detectors, and optical switches. Here we report on the fast photo switching behavior of thin films of liquid phase exfoliated MoS2, when excited with a continuous laser of λ = 658 nm (E = 1.88 eV), over a broad range of laser power. Transient photo-conductivity measurements, using an optical pump and THz probe (OPTP), reveal that photo carrier decay follows a bi-exponential time dependence, with decay times of the order of picoseconds, indicating that the photo carrier recombination occurs via trap states. The nature of variation of photocurrent with temperature confirms that the trap states are continuously distributed within the mobility gap in these thin film of MoS2, and play a vital role in influencing the overall photo response. Our findings provide a fundamental understanding of the photo-physics associated with optically active 2D materials and are crucial for developing advanced optoelectronic devices.

Ultrafast nonlinear optical spectroscopy of a dual-band negative index metamaterial all-optical switching device.

We study the nonlinear optical response of a fishnet structure-metamaterial all-optical switching device that exhibits two near-infrared negative-index resonances. We study and compare the nonlinear optical response at both resonances and identify transient spectral features associated with the negative index resonance. We see a significantly stronger response at the longer wavelength resonance, but identical temporal dynamics at both resonances, providing insight into separately engineering the switching time and switching ratio of such a fishnet structure metamaterial all-optical switch. We also numerically reproduce the nonlinear behavior of our device using the Drude conductivity model and a finite integration technique over wide spectral and pump fluence ranges. Thereby, we show that beyond the linear properties of the device, the magnitude of the pump-probe response is completely described by only two material parameters. These results provide insight into engineering various aspects of the nonlinear response of fishnet structure metamaterials.

Intraband conductivity response in graphene observed using ultrafast infrared-pump visible-probe spectroscopy

Graphene, a monolayer of carbon atoms arranged in a hexagonal pattern, provides a unique two-dimensional (2D) system exhibiting exotic phenomena such as quantum Hall effects, massless Dirac quasiparticle excitations and universal absorption&conductivity. The linear energy-momentum dispersion relation in graphene also offers the opportunity to mimic the physics of far-away relativistic particles like neutron stars and white dwarfs. In this letter, we perform a counterintuitive ultrafast pump-probe experiment with high photon energies to isolate the Drude-like intraband dynamics of photoexcited carriers. We directly demonstrate the relativistic nature of the photoexcited Dirac quasiparticles by observing a nonlinear scaling of the response with the density of photoexcited carriers. This is in striking contrast to the linear scaling that is usually observed in conventional materials. Our results also indicate strong electron-phonon coupling in graphene, leading to a sub-100 femtosecond thermalization between high energy photoexcited carriers and optical phonons.

Observing the interplay between surface and bulk optical nonlinearities in thin van der Waals crystals.

Thickness dependence of second harmonic generation in atomically thin InSe is studied. A strong resonance is observed, attributed to interference between distinct surface and bulk nonlinear contributions.