Patrick M. Vora

Binary nanocrystal superlattice membranes self-assembled at the liquid-air interface

The spontaneous organization of multicomponent micrometre-sized colloids or nanocrystals into superlattices is of scientific importance for understanding the assembly process on the nanometre scale and is of great interest for bottom-up fabrication of functional devices. In particular, co-assembly of two types of nanocrystal into binary nanocrystal superlattices (BNSLs) has recently attracted significant attention, as this provides a low-cost, programmable way to design metamaterials with precisely controlled properties that arise from the organization and interactions of the constituent nanocrystal components. Although challenging, the ability to grow and manipulate large-scale BNSLs is critical for extensive exploration of this new class of material. Here we report a general method of growing centimetre-scale, uniform membranes of BNSLs that can readily be transferred to arbitrary substrates. Our method is based on the liquid–air interfacial assembly of multicomponent nanocrystals and circumvents the limitations associated with the current assembly strategies, allowing integration of BNSLs on any substrate for the fabrication of nanocrystal-based devices. We demonstrate the construction of magnetoresistive devices by incorporating large-area (1.5 mm × 2.5 mm) BNSL membranes; their magnetotransport measurements clearly show that device magnetoresistance is dependent on the structure (stoichiometry) of the BNSLs. The ability to transfer BNSLs also allows the construction of free-standing membranes and other complex architectures that have not been accessible previously.

Photoluminescence and band gap modulation in graphene oxide

We report broadband visible photoluminescence from solid graphene oxide, and modifications of the emission spectrum by progressive chemical reduction. The data suggest a gapping of the two-dimensional electronic system by removal of π-electrons. We discuss possible gapping mechanisms, and propose that a Kekule pattern of bond distortions may account for the observed behavior.

Influence of probe pressure on the diffuse correlation spectroscopy blood flow signal: extra-cerebral contributions

A pilot study explores relative contributions of extra-cerebral (scalp/skull) versus brain (cerebral) tissues to the blood flow index determined by diffuse correlation spectroscopy (DCS). Microvascular DCS flow measurements were made on the head during baseline and breath-holding/hyperventilation tasks, both with and without pressure. Baseline (resting) data enabled estimation of extra-cerebral flow signals and their pressure dependencies. A simple two-component model was used to derive baseline and activated cerebral blood flow (CBF) signals, and the DCS flow indices were also cross-correlated with concurrent Transcranial Doppler Ultrasound (TCD) blood velocity measurements. The study suggests new pressure-dependent experimental paradigms for elucidation of blood flow contributions from extra-cerebral and cerebral tissues.

Leveraging Crystal Anisotropy for Deterministic Growth of InAs Quantum Dots with Narrow Optical Linewidths

Crystal growth anisotropy in molecular beam epitaxy usually prevents deterministic nucleation of individual quantum dots when a thick GaAs buffer is grown over a nanopatterned substrate. Here, we demonstrate how this anisotropy can actually be used to mold nucleation sites for single dots on a much thicker buffer than has been achieved by conventional techniques. This approach greatly suppresses the problem of defect-induced line broadening for single quantum dots in a charge-tunable device, giving state-of-the-art optical linewidths for a system widely studied as a spin qubit for quantum information.

Spin–cavity interactions between a quantum dot molecule and a photonic crystal cavity

The integration of InAs/GaAs quantum dots into nanophotonic cavities has led to impressive demonstrations of cavity quantum electrodynamics. However, these demonstrations are primarily based on two-level excitonic systems. Efforts to couple long-lived quantum dot electron spin states with a cavity are only now succeeding. Here we report a two-spin–cavity system, achieved by embedding an InAs quantum dot molecule within a photonic crystal cavity. With this system we obtain a spin singlet–triplet Λ-system where the ground-state spin splitting exceeds the cavity linewidth by an order of magnitude. This allows us to observe cavity-stimulated Raman emission that is highly spin-selective. Moreover, we demonstrate the first cases of cavity-enhanced optical nonlinearities in a solid-state Λ-system. This provides an all-optical, local method to control the spin exchange splitting. Incorporation of a highly engineerable quantum dot molecule into the photonic crystal architecture advances prospects for a quantum network.

Ultrafast Electron Trapping in Ligand-Exchanged Quantum Dot Assemblies

We use time-integrated and time-resolved photoluminescence and absorption to characterize the low-temperature optical properties of CdSe quantum dot solids after exchanging native aliphatic ligands for thiocyanate and subsequent thermal annealing. In contrast to trends established at room temperature, our data show that at low temperature the band-edge absorptive bleach is dominated by 1S3/2h hole occupation in the quantum dot interior. We find that our ligand treatments, which bring enhanced interparticle coupling, lead to faster surface state electron trapping, a greater proportion of surface-related photoluminescence, and decreased band-edge photoluminescence lifetimes.

The structural phases and vibrational properties of Mo1−xWxTe2 alloys

The structural polymorphism in transition metal dichalcogenides (TMDs) provides exciting opportunities for developing advanced electronics. For example, MoTe2 crystallizes in the 2H semiconducting phase at ambient temperature and pressure, but transitions into the 1T′ semimetallic phase at high temperatures. Alloying MoTe2 with WTe2 reduces the energy barrier between these two phases, while also allowing access to the Td Weyl semimetal phase. The Mo1−xWxTe2 alloy system is therefore promising for developing phase change memory technology. However, achieving this goal necessitates a detailed understanding of the phase composition in the MoTe2-WTe2 system. We combine polarization-resolved Raman spectroscopy with X-ray diffraction (XRD) and scanning transmission electron microscopy (STEM) to study Mo1−xWxTe2 alloys over the full compositional range x from 0 to 1. We identify Raman and XRD signatures characteristic of the 2H, 1T′, and Td structural phases that agree with density-functional theory (DFT) calculations, and use them to identify phase fields in the MoTe2-WTe2 system, including single-phase 2H, 1T ′, and Td regions, as well as a two-phase 1T ′ + Td region. Disorder arising from compositional fluctuations in Mo1−xWxTe2 alloys breaks inversion and translational symmetry, leading to the activation of an infrared 1T-MoTe2 mode and the enhancement of a double-resonance Raman process in 2H-Mo1−xWxTe2 alloys. Compositional fluctuations limit the phonon correlation length, which we estimate by fitting the observed asymmetric Raman lineshapes with a phonon confinement model. These observations reveal the important role of disorder in Mo1−xWxTe2 alloys, clarify the structural phase boundaries, and provide a foundation for future explorations of phase transitions and electronic phenomena in this system.

Quantum point contacts and resistive switching in Ni/NiO nanowire junctions

Metal oxide devices that exhibit resistive switching are leading candidates for non-volatile memory applications due to their potential for fast switching, low-power operation, and high device density. It is widely accepted in many systems that two-state resistive behavior arises from the formation and rupture of conductive filaments spanning the oxide layer. However, means for controlling the filament geometry, which critically influences conduction, have largely been unexamined. Here, we explore the connection between filament geometry and conductance in a model resistive switching system based on the junction of two nickel/nickel oxide core/shell nanowires. Variable temperature current-voltage measurements indicate that either wide metallic filaments or narrow semiconducting filaments can be preferentially formed by varying the current compliance during electroformation. Metallic filaments behave as a conventional metallic resistance in series with a small barrier, while semiconducting filaments behave...

Increased Transfer Efficiency from Molecular Photonic Wires on Solid Substrates and Cryogenic Conditions

Molecular photonic wires (MPWs) are tunable nanophotonic structures capable of capturing and directing light with high transfer efficiencies. DNA-based assembly techniques provide a simple and economical preparation method for MPWs that allows precise positioning of the molecular transfer components. Unfortunately, the longest DNA-based MPWs (∼30 nm) report only modest transfer efficiencies of ∼2% and have not been demonstrated on solid-state platforms. Here, we demonstrate that DNA-based MPWs can be spin-coated in a polymer matrix onto silicon wafers and exhibit a 5-fold increase in photonic transfer efficiency over solution-phase MPWs. Cooling these MPWs to 5 K led to further efficiency increases ranging from ∼40 to 240% depending on the length of the MPW. The improvement of MPW energy transport efficiencies advances prospects for their incorporation in a variety of optoelectronics technologies and makes them an ideal test bed for further exploration of nanoscale energy transfer.

Correlated structural and optical properties of the MoTe2-WTe2 alloy system (Conference Presentation)

The structural polymorphism intrinsic to select transition metal dichalcogenides provides exciting opportunities for engineering novel devices. Of special interest are memory technologies that rely upon controlled changes in crystal phase, collectively known as phase change memories (PCMs). MoTe