Yuri N. Gartstein

Giant-Stroke, Superelastic Carbon Nanotube Aerogel Muscles

Improved electrically powered artificial muscles are needed for generating force, moving objects, and accomplishing work. Carbon nanotube aerogel sheets are the sole component of new artificial muscles that provide giant elongations and elongation rates of 220% and (3.7 × 104)% per second, respectively, at operating temperatures from 80 to 1900 kelvin. These solid-state–fabricated sheets are enthalpic rubbers having gaslike density and specific strength in one direction higher than those of steel plate. Actuation decreases nanotube aerogel density and can be permanently frozen for such device applications as transparent electrodes. Poissons ratios reach 15, a factor of 30 higher than for conventional rubbers. These giant Poissons ratios explain the observed opposite sign of width and length actuation and result in rare properties: negative linear compressibility and stretch densification.

Coherent emission from a disordered organic semiconductor induced by strong coupling with surface plasmons.

In this Letter, we show that the strong coupling between a disordered set of molecular emitters and surface plasmons leads to the formation of spatially coherent hybrid states extended on macroscopic distances. Young-type interferometric experiments performed on a system of J-aggregated dyes spread on a silver layer evidence the coherent emission from different molecular emitters separated by several microns. The coherence is absent in systems in the weak-coupling regime demonstrating the key role of the hybridization of the molecules with the plasmon.

Efficient radiative and nonradiative energy transfer from proximal CdSe/ZnS nanocrystals into silicon nanomembranes

We demonstrate efficient excitonic sensitization of crystalline Si nanomembranes via combined effects of radiative (RET) and nonradiative (NRET) energy transfer from a proximal monolayer of colloidal semiconductor nanocrystals. Ultrathin, 25-300 nm Si films are prepared on top of insulating SiO(2) substrates and grafted with a monolayer of CdSe/ZnS nanocrystals via carboxy-alkyl chain linkers. The wet chemical preparation ensures that Si surfaces are fully passivated with a negligible number of nonradiative surface state defects and that the separation between nanocrystals and Si is tightly controlled. Time-resolved photoluminescence measurements combined with theoretical modeling allow us to quantify individual contributions from RET and NRET. Overall efficiency of ET into Si is estimated to exceed 85% for a short distance of about 4 nm from nanocrystals to the Si surface. Effective and longer-range radiative coupling of nanocrystals emission to waveguiding modes of Si films is clearly revealed. This demonstration supports the feasibility of an advanced thin-film hybrid solar cell concept that relies on energy transfer between strong light absorbers and adjacent high-mobility Si layers.

Visible to near-infrared sensitization of silicon substrates via energy transfer from proximal nanocrystals: further insights for hybrid photovoltaics.

We provide a unified spectroscopic evidence of efficient energy transfer (ET) from optically excited colloidal nanocrystal quantum dots (NQDs) into Si substrates in a broad range of wavelengths: from visible (545 nm) to near-infrared (800 nm). Chemical grafting of nanocrystals on hydrogenated Si surfaces is achieved via amine-modified carboxy-alkyl chain linkers, thus ensuring complete surface passivation and accurate NQD positioning. Time-resolved photoluminescence (PL) has been measured for a set of CdSe/ZnS and CdSeTe/ZnS NQDs of various sizes and compositions grafted on Si and SiO2 substrates. The measured acceleration of the PL decays on Si substrates is in good agreement with theoretical expectations based on the frequency-dependent dielectric properties of Si and NQD-Si separation distances. A comparative analysis reveals separate contributions to ET coming from the nonradiative (NRET) and radiative (RET) channels: NRET is a dominant mechanism for proximal NQDs in the middle of the visible range and becomes comparable with RET toward near-infrared wavelengths. The broad range over which the ET efficiency is estimated to be at the level of ∼90% further supports the concept that hybrid nanocrystal/silicon thin-film photovoltaic devices could efficiently harvest solar energy across the entire spectrum of wavelengths.

Increasing the efficiency of thermoacoustic carbon nanotube sound projectors

Carbon nanotubes (CNTs) can generate smooth-spectra sound emission over a wide frequency range (1-10(5) Hz) by means of thermoacoustics (TA). However, in the low frequencies f, where the need for large area sound projectors is high, the sound generation efficiency η of open CNT sheets is low, since η [proportionality] f(2). Together with this problem, the nanoscale thickness of CNT sheets, their high sensitivity to the environment and the high surface temperatures useful for TA sound generation are other drawbacks, which we address here by protective encapsulation of free-standing CNT sheets in inert gases. We provide an extensive experimental study of such closed systems for different thermodynamic regimes and rationalize our observations within a basic theoretical framework. The observed sound pressure levels for encapsulated argon filled TA transducers (130 dB in air and 200 dB underwater in the near field at 5 cm distance, and 100 and 170 dB in the far field at 1 m distance) are Q times higher than those for open systems, where Q is the resonant quality factor of the thin enclosure plates. Moreover, the sound generation efficiency of the encapsulated system increases toward low frequencies (η [proportionality] 1/f(2)). Another method to increase η in the low frequency region is by modulation of the applied high frequency carrier current with a low frequency resonant envelope. This approach enables sound generation at the frequency of the applied current without the need for additional energy-consuming biasing. The acoustical and geometrical parameters providing further increases in efficiency and transduction performance for resonant systems are discussed.

Mirage effect from thermally modulated transparent carbon nanotube sheets.

The single-beam mirage effect, also known as photothermal deflection, is studied using a free-standing, highly aligned carbon nanotube aerogel sheet as the heat source. The extremely low thermal capacitance and high heat transfer ability of these transparent forest-drawn carbon nanotube sheets enables high frequency modulation of sheet temperature over an enormous temperature range, thereby providing a sharp, rapidly changing gradient of refractive index in the surrounding liquid or gas. The advantages of temperature modulation using carbon nanotube sheets are multiple: in inert gases the temperature can reach > 2500 K; the obtained frequency range for photothermal modulation is ~100 kHz in gases and over 100 Hz in high refractive index liquids; and the heat source is transparent for optical and acoustical waves. Unlike for conventional heat sources for photothermal deflection, the intensity and phase of the thermally modulated beam component linearly depends upon the beam-to-sheet separation over a wide range of distances. This aspect enables convenient measurements of accurate values for thermal diffusivity and the temperature dependence of refractive index for both liquids and gases. The remarkable performance of nanotube sheets suggests possible applications as photo-deflectors and for switchable invisibility cloaks, and provides useful insights into their use as thermoacoustic projectors and sonar. Visibility cloaking is demonstrated in a liquid.

Energy transfer from colloidal nanocrystals into Si substrates studied via photoluminescence photon counts and decay kinetics

NSF (DMR-1207123), NSF (CHE-091197) and the Texas Higher Education Coordinating Board NHARP programs.

Exciton polaritons in transition-metal dichalcogenides and their direct excitation via energy transfer

Excitons, composite electron-hole quasiparticles, are known to play an important role in optoelectronic phenomena in many semiconducting materials. Recent experiments and theory indicate that the band-gap optics of the newly discovered monolayer transition-metal dichalcogenides (TMDs) is dominated by tightly bound valley excitons. The strong interaction of excitons with long-range electromagnetic fields in these 2D systems can significantly affect their intrinsic properties. Here, we develop a semi-classical framework for intrinsic exciton-polaritons in monolayer TMDs that treats their dispersion and radiative decay on the same footing and can incorporate effects of the dielectric environment. It is demonstrated how both inter- and intra-valley long-range interactions influence the dispersion and decay of the polaritonic eigenstates. We also show that exciton-polaritons can be efficiently excited via resonance energy transfer from quantum emitters such as quantum dots, which may be useful for various applications.

Interchain polaron complexes in conducting polymers: Optical transitions and reactions

Abstract The binding energy E β (ξ) of two polarons (P) (or solitons (S)) on adjacent chains arising due to interchain electron hopping t ⊥ is studied at various 3-d orders as a function of PP distance ξ. For out-of-phase order such PP bond is shown to be formed of Ps shifted along the chains. The stability of PP bonds and various decay processes for PP complexes are discussed. The type of 3-d order is found to determine the interchain optical transitions between P levels (through ξ-dependence) which may influence the recombination rate for Ps and could cause quasichemical reactions.

Local field effects for spherical quantum dot emitters in the proximity of a planar dielectric interface

We use numerical solutions of macroscopic Maxwell’s equations to study spontaneous emission rates of model spherical quantum dot (QD) emitters in the vicinity of a highly polarizable dielectric substrate. It is demonstrated that extra polarization of the QD body taking place in the interfacial region may lead to appreciable deviations from the rates that would be expected under the assumption of a fixed magnitude of the effective QD transition dipole moment. Illustrations are given for both radiative and nonradiative decay processes, and potential experimental implications are discussed.