Using optical, TEM, and ultrafast electron diffraction experiments we find that single crystal VO(2) microbeams gently placed on insulating substrates or metal grids exhibit different behaviors, with structural and metal-insulator transitions occurring at the same temperature for insulating substrates, while for metal substrates a new monoclinic metal phase lies between the insulating monoclinic phase and the metallic rutile phase. The structural and electronic phase transitions in these experiments are strongly first order and we discuss their origins in the context of current understanding of multiorbital splitting, strong correlation effects, and structural distortions that act cooperatively in this system.
We study the strain state of doubly clamped VO2 nanobeam devices by dynamically probing resonant frequency of the nanoscale electromechanical device across the metal-insulator transition. Simultaneous resistance and resonance measurements indicate M1-M2 phase transition in the insulating state with a drop in resonant frequency concomitant with an increase in resistance. The resonant frequency increases by ~7 MHz with the growth of metallic domain (M2-R transition) due to the development of tensile strain in the nanobeam. Our approach to dynamically track strain coupled with simultaneous resistance and resonance measurements using electromechanical resonators enables the study of lattice-involved interactions more precisely than static strain measurements. This technique can be extended to other phase change systems important for device applications.
We have systematically measured the room-temperature thermal conductivity of epitaxial layers of InxGa1−xN alloys with 15 different Indium compositions ranging from 0.08 to 0.98 by time-domain thermoreflectance method. The data are compared to the estimates of the strength of phonon scattering by cation disorder. The thermal conductivity is in good agreement with the theoretical modeling results based on the mass difference for In-rich (x > 0.9) and Ga-rich (x < 0.2) compositions. At intermediate compositions (0.2 < x < 0.9), the thermal conductivity is strongly suppressed below the values expected for homogeneous alloys. We attribute this suppression of thermal conductivity to phonon scattering by nanometer-scale compositional inhomogeneities in alloys.
Two-dimensional electron systems offer enormous opportunities for science discoveries and technological innovations. Here we report a dense electron system on the surface of single-crystal vanadium dioxide nanobeam via electrolyte gating. The overall conductance of the nanobeam increases by nearly 100 times at a gate voltage of 3 V. A series of experiments were carried out which rule out electrochemical reaction, impurity doping, and oxygen vacancy diffusion as the dominant mechanism for the conductance modulation. A surface insulator-to-metal transition is electrostatically triggered, thereby collapsing the bandgap and unleashing an extremely high density of free electrons from the original valence band within a depth self-limited by the energetics of the system. The dense surface electron system can be reversibly tuned by the gating electric field, which provides direct evidence of the electron correlation driving mechanism of the phase transition in VO(2). It also offers a new material platform for implementing Mott transistor and novel sensors and investigating low-dimensional correlated electron behavior.
We studied the insulator-metal transition (IMT) in single-domain, single crystalline vanadium dioxide (VO(2)) microbeams with infrared microspectroscopy. The unique nature of such samples allowed us to probe the intrinsic behavior of both insulating and metallic phases in the close vicinity of IMT, and investigate the IMT driven by either strain or temperature independently. We found that the VO(2) insulating band gap narrows rapidly upon heating, and the infrared response undergoes an abrupt transition at both strain- and temperature-induced IMT. The results are consistent with recent studies attributing the opening of VO(2) insulating band gap to a correlation-assisted Peierls transition.
Read moreIn contrast to most semiconductors, electrical conductivity of InN is known to increase upon high-energy particle irradiation. The effects of irradiation on its thermal and thermoelectric properties have yet to be investigated. Here we report the thermal conductivity of high-quality InN to be 120 W/m K and examine the effects of point defects generated by irradiation on the thermal conductivity and Seebeck coefficient. We show that irradiation can be used to modulate the thermal and thermoelectric properties of InN by controlling point defect concentrations. The thermoelectric figure of merit of InN was found to be insensitive to irradiation.
Read moreWe study field-effect transistors realized from VO2 nanobeams with HfO2 as the gate dielectric. When heated up from low to high temperatures, VO2 undergoes an insulator-to-metal transition. We observe a change in conductance (∼6%) of our devices induced by gate voltage when the system is in the insulating phase. The response is reversible and hysteretic, and the area of hysteresis loop becomes larger as the rate of gate sweep is slowed down. A phase lag exists between the response of the conductance and the gate voltage. This indicates the existence of a memory of the system and we discuss its possible origins.
Read moreActive heat flow control is essential for broad applications of heating, cooling, and energy conversion. Like electronic devices developed for the control of electric power, it is very desirable to develop advanced all-thermal solid-state devices that actively control heat flow without consuming other forms of energy. Here we demonstrate temperature-gated thermal rectification using vanadium dioxide beams in which the environmental temperature actively modulates asymmetric heat flow. In this three terminal device, there are two switchable states, which can be regulated by global heating. In the "Rectifier" state, we observe up to 28% thermal rectification. In the "Resistor" state, the thermal rectification is significantly suppressed (<1%). To the best of our knowledge, this is the first demonstration of solid-state active-thermal devices with a large rectification in the Rectifier state. This temperature-gated rectifier can have substantial implications ranging from autonomous thermal management of heating and cooling systems to efficient thermal energy conversion and storage.
Read moreWe investigate the effect of O impurities on the thermoelectric properties of ZnSe from a combination of first-principles and analytic calculations. It is demonstrated that dilute amounts of O impurities introduce peaks in the density of states (DOS) above the conduction band minimum, and that the charge density near the DOS peaks is substantially attracted toward O atoms due to their high electronegativity. The impurity-induced peaks in the DOS result in a sharp increase of the room-temperature Seebeck coefficient and power factor from those of O-free ZnSe by a factor of 30 and 180, respectively. Furthermore, this effect is found to be absent when the impurity electronegativity well matches the host that it substitutes. The results suggest that highly electronegativity-mismatched alloys can be designed for high performance thermoelectric applications.
Read moreLaser-assisted phosphorus doping is demonstrated by J. Wu, C. P. Grigoropoulos, and co-workers on page 341, on ultrathin transition-metal dichalcogenides (TMDCs), including n-type MoS2 and p-type WSe2. Temporal and spatial control of the doping is achieved by varying the laser irradiation power and time, demonstrating wide tunability and high site selectivity with high stability. The laser-assisted doping method may enable a new avenue for functionalizing TMDCs for customized nanodevice applications.
Read moreWe report on measurements of Seebeck effect in single-crystal VO(2) microbeams across their metal-insulator phase transition. One-dimensionally aligned metal-insulator domain walls were reversibly created and eliminated along single VO(2) beams by varying temperature, which allows for accurate extraction of the net contribution to the Seebeck effect from these domain walls. We observed significantly lower Seebeck coefficient in the metal-insulator coexisting regime than predicted by a linear combination of contributions from the insulator and metal domains. This indicates that the net contribution of the domain walls has an opposite sign from that of the insulator and metal phases separately. Possible origins that may be responsible for this unexpected effect were discussed in the context of complications in this correlated electron material.
Read moreWe report synthesis windows for growth of millimeter-long ZnTe nanoribbons and ZnSe nanowires using vapor transport. By tuning the local conditions at the growth substrate, high aspect ratio nanostructures can be synthesized. A Cu-ion immersion doping method was applied, producing strongly p-type conduction in ZnTe and ionic conduction in ZnSe. These extreme aspect ratio wide-bandgap semiconductors have great potential for high density nanostructured optoelectronic circuits.
Read moreAmorphous GaN1−xAsx layers with As content in the range of x=0.1 to 0.6 were grown by molecular beam epitaxy on Pyrex glass substrate. These alloys exhibit a wide range of band gap values from 2.2 to 1.3 eV. We found that the density of the amorphous films is ∼0.8–0.85 of their corresponding crystalline value. These amorphous films have smooth morphology, homogeneous composition, and sharp well defined optical absorption edges. The measured band gap values for the crystalline and amorphous GaN1−xAsx alloys are in excellent agreement with the predictions of the band anticrossing model. The high absorption coefficient of ∼105 cm−1 for the amorphous GaN1−xAsx films suggests that relatively thin films (on the order of 1 μm) are necessary for photovoltaic application.
Read moreCdxZn1−xO alloys, as a transparent conducting oxide, have recently attracted much attention for potential optoelectronic applications. In this letter, we report a hydrostatic pressure-induced phase transition of CdxZn1−xO alloys from the wurtzite to the rocksalt structure and its phase diagram probed using a diamond anvil cell. It is found that the transition pressure, determined by changes in optical and structural properties, depends sensitively on the composition. As the Cd content increases, the critical pressure decreases, until at x = 0.67 where the alloy is intrinsically stable in the rocksalt phase even at ambient pressure. The wurtzite phase is light emitting with a direct bandgap that slightly widens with increasing pressure, while the rocksalt phase has a much wider bandgap that is indirect. The pressure-sensitive light emission and phase transition may find potential applications in fields such as stress sensing and energy storage.
Read moreThermoelectric materials have attracted much attention due to the current interest in energy conversion and recent advancements in nano-engineering. A simple approach to synthesize BiTe and Bi2Te3 micro/nanowires was developed by combining solution chemistry reactions and catalyst-free vapor-solid growth. A pathway to transform the as-grown BiTe nanostructures into Bi2Te3 can be identified through the Bi-Te phase diagram. Structural characterization of these products was identified using standard microscopy practices. Meanwhile, thermoelectric properties of individual Bi-Te compound micro/nanowires were determined by the suspended microdevice technique. This approach provides an applicable route to synthesize advanced high performance thermoelectric materials in quantities and can be used for a wide range of low-dimensional structures.
Read more