Stephen McGill

High-performance, hysteresis-free carbon nanotube field-effect transistors via directed assembly

High-performance, single-wall carbon nanotube field-effect transistors (SWCNT-FETs) are fabricated using directed assembly and mass-produced carbon nanotubes (CNTs). These FETs exhibit operating characteristics comparable to state-of-the-art devices, and the process provides a route to large-scale functional CNT circuit assembly that circumvents problems inherent in processes relying on chemical vapor deposition. Furthermore, the integration of hydrophobic self-assembled monolayers in the device structure eliminates the primary source of gating hysteresis in SWCNT-FETs; this leads to hysteresis-free FET operation while exposing unmodified nanotube surfaces to ambient air.

High Photoresponsivity and Short Photoresponse Times in Few-Layered WSe2 Transistors

Here, we report the photoconducting response of field-effect transistors based on three atomic layers of chemical vapor transport grown WSe2 crystals mechanically exfoliated onto SiO2. We find that trilayered WSe2 field-effect transistors, built with the simplest possible architecture, can display high hole mobilities ranging from 350 cm(2)/(V s) at room temperature (saturating at a value of ∼500 cm(2)/(V s) below 50 K) displaying a strong photocurrent response, which leads to exceptionally high photoresponsivities up to 7 A/W under white light illumination of the entire channel for power densities p < 10(2) W/m(2). Under a fixed wavelength of λ = 532 nm and a laser spot size smaller than the conducting channel area, we extract photoresponsitivities approaching 100 mA/W with concomitantly high external quantum efficiencies up to ∼40% at room temperature. These values surpass values recently reported from more complex architectures, such as graphene and transition metal dichalcogenides based heterostructures. Also, trilayered WSe2 phototransistors display photoresponse times on the order of 10 μs. Our results indicate that the addition of a few atomic layers considerably decreases the photoresponse times, probably by minimizing the interaction with the substrates, while maintaining a very high photoresponsivity.

Temperature-dependent photoluminescence of structurally-precise quantum-confined Au25(SC8H9)18 and Au38(SC12H25)24 metal nanoparticles.

Temperature-dependent photoluminescence of structurally precise Au25(SC8H9)18 and Au38(SC12H25)24 monolayer-protected cluster (MPC) nanoparticles were studied using energy-resolved, intensity-integrated, and time-resolved spectroscopy. Measurements were carried out at sample temperatures spanning the range from 4.5 to 200 K following electronic excitation using 3.1 eV pulsed lasers. The integrated PL intensity for Au25(SC8H9)18 increased sharply by 70% as the sample temperature was increased from 4.5 to 45 K. The PL intensity was statistically invariant for temperatures between 45 and 65 K but was quenched when the sample temperature was raised above 65 K. For both MPC samples, the global PL emission included several components. Each PL component exhibited an increase in emission energy when the sample temperature was increased from 4.5 to 40 K. This unexpected behavior may imply that MPCs in the 1 nm domain have negative expansion coefficients. Quantitative analysis of PL emission energies and peak widths obtained at sample temperatures greater than 45 K indicated MPC nonradiative relaxation dynamics are mediated by coupling to low-frequency vibrations associated with the ligand shell that passivated the nanoclusters, which accounted for the low emission yields at high sample temperatures. Contributions from two different vibrational modes were identified: Au(I)-S stretching (200 cm(-1)) and Au(0)-Au(I) stretching (90 cm(-1)). Analysis of each PL component revealed that the magnitude of electronic-vibration coupling was state-specific, and consistently larger for the high-energy portions of the PL spectra. The total integrated PL intensity of the Au25(SC8H9)18 MPC was correlated to the relative branching ratios of the emission components, which confirmed decreased emission for recombination channels associated with strong electron-vibration coupling and high emission yields for low emission energies at low temperature. The efficient low-energy emission was attributed to a charge-transfer PL transition. This conclusion was reached based on the strong correlation between temperature-dependent intensity-integrated and time-resolved emission measurements that revealed an ∼3.5-5.5 meV activation barrier to nonradiative decay. These findings suggest that nanoscale structure and composition can be modified to tailor the optical and mechanical properties and electronic relaxation dynamics of MPC nanostructures.

Giant superfluorescent bursts from a semiconductor magneto-plasma

Superfluorescence—the emission of coherent light from an initially incoherent collection of excited dipoles—is now identified in a semiconductor. Laser-excited electron–hole pairs spontaneously polarize and then abruptly decay to produce intense pulses of light.

EuS nanocrystals: a novel synthesis for the generation of monodisperse nanocrystals with size-dependent optical properties

A novel one-step solvothermal synthesis of stable colloidal EuS nanocrystals (NCs) is reported. The EuS NCs were synthesized in oleylamine directly from europium oleate and diethylammonium diethyldithiocarbamate in the presence of dodecanethiol and phenanthroline. The formation of single crystalline monodisperse EuS NCs, with sizes finely controlled by synthetic conditions, was confirmed by x-ray diffraction and high resolution transmission electron microscopy analysis. The exciton transition of EuS NCs blue-shifts to higher energies with decreasing particle sizes, as revealed by optical absorption and photoluminescence measurements. The feasibility of synthesizing monocrystalline EuS nanorods by solvothermal synthesis was also demonstrated, making them potentially viable materials for device applications.

Direct band gaps in multiferroic h-LuFeO3

We measured the optical properties of epitaxial thin films of the metastable hexagonal polymorph of LuFeO3 by absorption spectroscopy, magnetic circular dichroism, and photoconductivity. Comparison with complementary electronic structure calculations reveals a 1.1 eV direct gap involving hybridized Fe 3dz2+O 2pz→Fe d excitations at the Γ and A points, with a higher energy direct gap at 2.0 eV. Both charge gaps nicely overlap the solar spectrum.

Fermi-edge superfluorescence from a quantum-degenerate electron-hole gas

Nonequilibrium can be a source of order. This rather counterintuitive statement has been proven to be true through a variety of fluctuation-driven, self-organization behaviors exhibited by out-of-equilibrium, many-body systems in nature (physical, chemical, and biological), resulting in the spontaneous appearance of macroscopic coherence. Here, we report on the observation of spontaneous bursts of coherent radiation from a quantum-degenerate gas of nonequilibrium electron-hole pairs in semiconductor quantum wells. Unlike typical spontaneous emission from semiconductors, which occurs at the band edge, the observed emission occurs at the quasi-Fermi edge of the carrier distribution. As the carriers are consumed by recombination, the quasi-Fermi energy goes down toward the band edge, and we observe a continuously red-shifting streak. We interpret this emission as cooperative spontaneous recombination of electron-hole pairs, or superfluorescence (SF), which is enhanced by Coulomb interactions near the Fermi edge. This novel many-body enhancement allows the magnitude of the spontaneously developed macroscopic polarization to exceed the maximum value for ordinary SF, making electron-hole SF even more “super” than atomic SF.

Dynamics of photoexcited carriers and spins in InAsP ternary alloys

The recent rapid progress in the field of spintronics involves extensive measurements of carrier and spin relaxation dynamics in III-V semiconductors. In addition, as the switching rates in devices are pushed to higher frequencies, it is important to understand carrier dynamic phenomena in semiconductors on femtosecond time-scales. In this work, we employed time and spin resolved differential transmission measurements; to probe carrier and spin relaxation times in several InAsP ternary alloys. Our results demonstrate the sensitivity of the spin and carrier dynamics in this material system to the excitation wavelengths, the As concentrations, and temperature.

Photoconductivity of few-layered p-WSe2 phototransistors via multi-terminal measurements

Recently, two-dimensional materials and in particular transition metal dichalcogenides (TMDs) were extensively studied because of their strong light-matter interaction and the remarkable optoelectronic response of their field-effect transistors (FETs). Here, we report a photoconductivity study from FETs built from few-layers of p-WSe2 measured in a multi-terminal configuration under illumination by a 532 nm laser source. The photogenerated current was measured as a function of the incident optical power, of the drain-to-source bias and of the gate voltage. We observe a considerably larger photoconductivity when the phototransistors were measured via a four-terminal configuration when compared to a two-terminal one. For an incident laser power of 248 nW, we extract 18 A/W and ~4000% for the two-terminal responsivity (R) and the concomitant external quantum efficiency (EQE) respectively, when a bias voltage Vds = 1 V and a gate voltage Vbg = 10 V are applied to the sample. R and EQE are observed to increase by 370% to ~85 A/W and ~20000% respectively, when using a four-terminal configuration. Thus, we conclude that previous reports have severely underestimated the optoelectronic response of transition metal dichalcogenides, which in fact reveals a remarkable potential for photosensing applications.

Generation of superfluorescent bursts from a fully tunable semiconductor magneto-plasma

Quantum particles sometimes cooperate to develop a macroscopically ordered state with extraordinary properties. Superconductivity and Bose-Einstein condensation are examples of such cooperative phenomena where macroscopic order appears spontaneously. Here, we demonstrate that such an ordered state can also be obtained in an optically excited semiconductor quantum well in a high magnetic field. When we create a dense electron-hole plasma with an intense laser pulse, after a certain delay, an ultrashort burst of coherent radiation emerges. We interpret this striking phenomenon as a manifestation of superfluorescence (SF), in which a macroscopic polarization spontaneously builds up from an initially incoherent ensemble of excited quantum oscillators and then decays abruptly producing giant pulses of coherent radiation. SF has been observed in atomic gases, but the present work represents the first observation of SF in a solid-state setting. While there is an analogy between the recombination of electron-hole pairs and radiative transitions in atoms, there is no a priori reason for SF in semiconductors to be similar to atomic SF. This is a complex many-body system with a variety of ultrafast interactions, where the decoherence rates are at least 1,000 times faster than the radiative decay rate, an unusual situation totally unexplored in previous atomic SF studies. We show, nonetheless, that collective many-body coupling via a common radiation field does develop under certain conditions and leads to SF bursts. The solid-state realization of SF resulted in an unprecedented degree of controllability in the generation of SF, opening up opportunities for both fundamental many-body studies and device applications. We demonstrate that the intensity and delay time of SF bursts are fully tunable through an external magnetic field, temperature, and pump laser power.