arXiv subjects

Douglas Natelson

Publications and source records attributed to Douglas Natelson.

At least 37 records · Page 2Linked to original sources

arXiv2023

Nernst-Ettingshausen effect in thin Pt and W films at low temperatures

As spin caloritronic measurements become increasingly common techniques for characterizing material properties, it is important to quantify potentially confounding effects. We report measurements of the Nernst-Ettingshausen response from room temperature to 5 K in thin film wires of Pt and W, metals commonly used as inverse spin Hall detectors in spin Seebeck characterization. Johnson-Nyquist noise thermometry is used to assess the temperature change of the metals with heater power at low temperatures, and the thermal path is analyzed via finite-element modeling. The Nernst-Ettingshausen response of W is found to be approximately temperature-independent, while the response of Pt increases at low temperatures. These results are discussed in the context of theoretical expectations and the possible role of magnetic impurities in Pt.

cond-mat.mes-hall↗

arXiv2022

Tuning light emission crossovers in atomic-scale aluminum plasmonic tunnel junctions

Atomic sized plasmonic tunnel junctions are of fundamental interest, with great promise as the smallest on-chip light sources in various optoelectronic applications. Several mechanisms of light emission in electrically driven plasmonic tunnel junctions have been proposed, from single-electron or higher order multi-electron inelastic tunneling to recombination from a steady-state population of hot carriers. By progressively altering the tunneling conductance of an aluminum junction, we tune the dominant light emission mechanism through these possibilities for the first time, finding quantitative agreement with theory in each regime. Improved plasmonic resonances in the energy range of interest increase photon yields by two orders of magnitude. These results demonstrate that the dominant emission mechanism is set by a combination of tunneling rate, hot carrier relaxation timescales, and junction plasmonic properties.

cond-mat.mes-hall↗

arXiv2022

Spin Seebeck effect at low temperatures in the nominally paramagnetic insulating state of vanadium dioxide

The low temperature monoclinic, insulating phase of vanadium dioxide is ordinarily considered nonmagnetic, with dimerized vanadium atoms forming spin singlets, though paramagnetic response is seen at low temperatures. We find a nonlocal spin Seebeck signal in VO2 films that appears below 30 K and which increases with decreasing temperature. The spin Seebeck response has a non-hysteretic dependence on in-plane external magnetic field. This paramagnetic spin Seebeck response is discussed in terms of prior findings on paramagnetic spin Seebeck effects and expected magnetic excitations of the monoclinic ground state.

cond-mat.str-el↗

arXiv2021

Thousand-fold Increase in Plasmonic Light Emission via Combined Electronic and Optical Excitations

Surface plasmon enhanced processes and hot-carrier dynamics in plasmonic nanostructures are of great fundamental interest to reveal light-matter interactions at the nanoscale. Using plasmonic tunnel junctions as a platform supporting both electrically- and optically excited localized surface plasmons, we report a much greater (over 1000x) plasmonic light emission at upconverted photon energies under combined electro-optical excitation, compared with electrical or optical excitation separately. Two mechanisms compatible with the form of the observed spectra are interactions of plasmon-induced hot carriers and electronic anti-Stokes Raman scattering. Our measurement results are in excellent agreement with a theoretical model combining electro-optical generation of hot carriers through non-radiative plasmon excitation and hot-carrier relaxation. We also discuss the challenge of distinguishing relative contributions of hot carrier emission and the anti-Stokes electronic Raman process. This observed increase in above-threshold emission in plasmonic systems may open avenues in on-chip nanophotonic switching and hot carrier photocatalysis.

physics.optics↗

arXiv2021

Thermoelectric response from grain boundaries and lattice distortions in crystalline gold devices

The electronic Seebeck response in a conductor involves the energy-dependent mean free path of the charge carriers and is affected by crystal structure, scattering from boundaries and defects, and strain. Previous photothermoelectric (PTE) studies have suggested that the thermoelectric properties of polycrystalline metal nanowires are related to grain structure, though direct evidence linking crystal microstructure to the PTE response is difficult to elucidate. Here, we show that room temperature scanning PTE measurements are sensitive probes that can detect subtle changes in the local Seebeck coefficient of gold tied to the underlying defects and strain that mediate crystal deformation. This connection is revealed through a combination of scanning PTE and electron microscopy measurements of single crystal and bicrystal gold microscale devices. Unexpectedly, the photovoltage maps strongly correlate with gradually varying crystallographic misorientations detected by electron backscatter diffraction. The effects of individual grain boundaries and differing grain orientations on the PTE signal are minimal. This scanning PTE technique shows promise for identifying minor structural distortions in nanoscale materials and devices.

cond-mat.mtrl-sci↗

arXiv2020

Electron pairing in the pseudogap state revealed by shot noise in copper-oxide junctions

In the quest to understand high-temperature superconductivity in copper oxides, a vigorous debate has been focused on the pseudogap - a partial gap that opens over portions of the Fermi surface in the 'normal' state above the bulk critical temperature ($T_{c}$). The pseudogap has been attributed to precursor superconductivity, to the existence of preformed pairs, or to competing orders such as charge-density waves. A direct determination of the charge of carriers as a function of temperature and bias could help resolve among these alternatives. Here, we report measurements of the shot noise of tunneling current in high-quality La$_{2-x}$Sr$_{x}$CuO$_{4}$/La$_{2}$CuO$_{4}$/La$_{2-x}$Sr$_{x}$CuO$_{4}$ (LSCO/LCO/LSCO) heterostructures fabricated using atomic-layer-by-layer molecular beam epitaxy, for several doping levels. The data delineate three distinct regions in the bias voltage-temperature ($V-T$) space. Well outside the superconducting gap region, the shot noise agrees quantitatively with independent tunneling of charge-e carriers. Deep within the gap, shot noise is greatly enhanced, reminiscent of multiple Andreev reflections. Starting above $T_{c}$ and extending to biases much larger than the gap, there is a broad region in which the noise substantially exceeds the expectations of single-charge tunneling, indicating pairing of carriers. Pairs are detectable deep into the pseudogap region of temperature and bias.

cond-mat.supr-con↗

arXiv2020

Electrically Driven Hot-Carrier Generation and Above-threshold Light Emission in Plasmonic Tunnel Junctions

Above-threshold light emission from plasmonic tunnel junctions, when emitted photons have energies significantly higher than the energy scale of the incident electrons, has attracted much recent interest in nano-optics, while the underlying physical mechanism remains elusive. We examine above-threshold light emission in electromigrated tunnel junctions. Our measurements over a large ensemble of devices demonstrate a giant material dependence of photon yield (emitted photons per incident electrons), as large as four orders of magnitude. This dramatic effect cannot be explained only by the radiative field enhancement effect due to the localized plasmons in the tunneling gap. Emission is well described by a Boltzmann spectrum with an effective temperature exceeding 2000 K, coupled to a plasmon-modified photonic density of states. The effective temperature is approximately linear in the applied bias, consistent with a suggested theoretical model in which hot carriers are generated by non-radiative decay of electrically excited localized plasmons. Electrically driven hot-carrier generation and the associated non-traditional light emission could open new possibilities for active photochemistry, optoelectronics and quantum optics.

cond-mat.mes-hall↗

arXiv2020

Tunneling spectroscopy of c-axis epitaxial cuprate junctions

Atomically precise epitaxial structures are unique systems for tunneling spectroscopy that minimize extrinsic effects of disorder. We present a systematic tunneling spectroscopy study, over a broad doping, temperature, and bias range, in epitaxial c-axis La$_{2-x}$Sr$_{x}$CuO$_{4}$/La$_{2}$CuO$_{4}$/La$_{2-x}$Sr$_{x}$CuO$_{4}$ heterostructures. The behavior of these superconductor/insulator/superconductor (SIS) devices is unusual. Down to 20 mK there is complete suppression of c-axis Josephson critical current with a barrier of only 2 nm of La$_{2}$CuO$_{4}$, and the zero-bias conductance remains at 20-30% of the normal-state conductance, implying a substantial population of in-gap states. Tunneling spectra show greatly suppressed coherence peaks. As the temperature is raised, the superconducting gap fills in rather than closing at $T_{c}$. For all doping levels, the spectra show an inelastic tunneling feature at $\sim$ 80 meV, suppressed as $T$ exceeds $T_{c}$. These nominally simple epitaxial cuprate junctions deviate markedly from expectations based on the standard Bardeen-Cooper-Schrieffer (BCS) theory.

cond-mat.supr-con↗

arXiv2018

Room Temperature Magnetic Order in Air-Stable Ultra-Thin Iron Oxide

Certain two-dimensional (2D) materials exhibit intriguing properties such as valley polarization, ferroelectricity, superconductivity and charge-density waves. Many of these materials can be manually assembled into atomic-scale multilayer devices under ambient conditions, owing to their exceptional chemical stability. Efforts have been made to add a magnetic degree of freedom to these 2D materials via defects, but only local magnetism has been achieved. Only with the recent discoveries of 2D materials supporting intrinsic ferromagnetism have stacked spintronic devices become realistic. Assembling 2D multilayer devices with these ferromagnets under ambient conditions remains challenging due to their sensitivity to environmental degradation, and magnetic order at room temperature is rare in van der Waals materials. Here, we report the growth of air-stable ultra-thin epsilon-phase iron oxide crystals that exhibit magnetic order at room temperature. These crystals require no passivation and can be prepared in large quantity by cost-effective chemical vapor deposition (CVD). We find that the epsilon phase, which is energetically unfavorable and does not form in bulk, can be easily made in 2D down to a seven unit-cell thickness. Magneto-optical Kerr effect (MOKE) magnetometry of individual crystals shows that even at this ultrathin limit the epsilon phase exhibits robust magnetism with coercive fields of hundreds of mT. These measurements highlight the advantages of ultrathin iron oxide as a promising candidate towards air-stable 2D magnetism and integration into 2D spintronic devices.

cond-mat.mtrl-sci↗

arXiv2018

Photovoltages and hot electrons in plasmonic nanogaps

In metal nanostructures under illumination, multiple different processes can drive current flow, and in an open- circuit configuration some of these processes lead to the production of open-circuit photovoltages. Structures that have plasmonic resonances at the illumination wavelength can have enhanced photovoltage response, due to both increased interactions with the incident radiation field, and processes made possible through the dynamics of the plasmon excitations themselves. Here we review photovoltage response driven by thermoelectric effects in continuous metal nanowires and photovoltage response driven by hot electron production and tunneling. We discuss the prospects for enhancing and quantifying hot electron generation and response via the combination of local plasmonic resonances and propagating surface plasmon polaritons.

cond-mat.mes-hall↗

arXiv2017

Substantial local variation of Seebeck coefficient in gold nanowires

Nanoscale structuring holds promise to improve thermoelectric properties of materials for energy conversion and photodetection. We report a study of the spatial distribution of the photothermoelectric voltage in thin-film nanowire devices fabricated from single metal. A focused laser beam is used to locally heat the metal nanostructure via a combination of direct absorption and excitation of a plasmon resonance in Au devices. As seen previously, in nanowires shorter than the spot size of the laser, we observe a thermoelectric voltage distribution that is consistent with the local Seebeck coefficient being spatially dependent on the width of the nanostructure. In longer structures, we observe extreme variability of the net thermoelectric voltage as the laser spot is scanned along the length of the nanowire. The sign and magnitude of the thermoelectric voltage is sensitive to the structural defects, metal grain structure, and surface passivation of the nanowire. This finding opens the possibility of improved local control of the thermoelectric properties at the nanoscale.

cond-mat.mes-hall↗

arXiv2017

Photothermoelectric effects and large photovoltages in plasmonic Au nanowires with nanogaps

Nanostructured metals subject to local optical interrogation can generate open-circuit photovoltages potentially useful for energy conversion and photodetection. We report a study of the photovoltage as a function of illumination position in single metal Au nanowires and nanowires with nanogaps formed by electromigration. We use a laser scanning microscope to locally heat the metal nanostructures via excitation of a local plasmon resonance and direct absorption. In nanowires without nanogaps, where charge transport is diffusive, we observe voltage distributions consistent with thermoelectricity, with the local Seebeck coefficient depending on the width of the nanowire. In the nanowires with nanogaps, where charge transport is by tunneling, we observe large photovoltages up to tens of mV, with magnitude, polarization dependence, and spatial localization that follow the plasmon resonance in the nanogap. This is consistent with a model of photocurrent across the nanogap carried by the nonequilibrium, "hot" carriers generated upon the plasmon excitation.

cond-mat.mes-hall↗

arXiv2017

Consecutive Insulator-Metal-Insulator Phase Transitions of Vanadium Dioxide by Hydrogen Doping

We report modulation of a reversible phase transition in VO2 films by hydrogen doping. A metallic phase and a new insulating phase are successively observed at room temperature as the doping concentration increases. It is suggested that the polarized charges from doped hydrogens play an important role. These charges gradually occupy V3d-O2p hybridized orbitals and consequently modulate the filling of the VO2 crystal conduction band-edge states, which eventually evolve into new valence band-edge states. This demonstrates the exceptional sensitivity of VO2 electronic properties to electron concentration and orbital occupancy, providing key information for the phase transition mechanism.

cond-mat.str-el↗

arXiv2017

Potential Fluctuations at Low Temperatures in Mesoscopic-Scale SmTiO$_{3}$/SrTiO$_{3}$/SmTiO$_{3}$ Quantum Well Structures

Heterointerfaces of SrTiO$_{3}$ with other transition metal oxides make up an intriguing family of systems with a bounty of coexisting and competing physical orders. Some examples, such as LaAlO$_{3}$/SrTiO$_{3}$, support a high carrier density electron gas at the interface whose electronic properties are determined by a combination of lattice distortions, spin-orbit coupling, defects, and various regimes of magnetic and charge ordering. Here, we study electronic transport in mesoscale devices made with heterostructures of SrTiO$_{3}$ sandwiched between layers of SmTiO$_{3}$, in which the transport properties can be tuned from a regime of Fermi-liquid like resistivity ($ρ\sim T^{2}$) to a non-Fermi liquid ($ρ\sim T^{5/3}$) by controlling the SrTiO$_{3}$ thickness. In mesoscale devices at low temperatures, we find unexpected voltage fluctuations that grow in magnitude as $T$ is decreased below 20 K, are suppressed with increasing contact electrode size, and are independent of the drive current and contact spacing distance. Magnetoresistance fluctuations are also observed, which are reminiscent of universal conductance fluctuations but not entirely consistent with their conventional properties. Candidate explanations are considered, and a mechanism is suggested based on mesoscopic temporal fluctuations of the Seebeck coefficient. An improved understanding of charge transport in these model systems, especially their quantum coherent properties, may lead to insights into the nature of transport in strongly correlated materials that deviate from Fermi liquid theory.

cond-mat.mes-hall↗

arXiv2017

Shot noise detection in hBN-based tunnel junctions

High quality Au/hBN/Au tunnel devices are fabricated using transferred atomically thin hexagonal boron nitride as the tunneling barrier. All tunnel junctions show tunneling resistance on the order of several k$Ω$/$μ$m$^{2}$. Ohmic I-V curves at small bias with no signs of resonances indicate the sparsity of defects. Tunneling current shot noise is measured in these devices, and the excess shot noise shows consistency with theoretical expectations. These results show that atomically thin hBN is an excellent tunnel barrier, especially for the study of shot noise properties, and this can enable the study of tunneling density of states and shot noise spectroscopy in more complex systems.

cond-mat.mes-hall↗

arXiv2017

Mesoscopic quantum effects in a bad metal, hydrogen-doped vanadium dioxide

The standard treatment of quantum corrections to semiclassical electronic conduction assumes that charge carriers propagate many wavelengths between scattering events, and succeeds in explaining multiple phenomena (weak localization magnetoresistance (WLMR), universal conductance fluctuations, Aharonov-Bohm oscillations) observed in polycrystalline metals and doped semiconductors in various dimensionalities. We report apparent WLMR and conductance fluctuations in H$_{x}$VO$_{2}$, a poor metal (in violation of the Mott-Ioffe-Regel limit) stabilized by the suppression of the VO$_{2}$ metal-insulator transition through atomic hydrogen doping. Epitaxial thin films, single-crystal nanobeams, and nanosheets show similar phenomenology, though the details of the apparent WLMR seem to depend on the combined effects of the strain environment and presumed doping level. Self-consistent quantitative analysis of the WLMR is challenging given this and the high resistivity of the material, since the quantitative expressions for WLMR are derived assuming good metallicity. These observations raise the issue of how to assess and analyze mesoscopic quantum effects in poor metals.

cond-mat.mes-hall↗

arXiv2017

Evolution of shot noise in suspended lithographic gold break junctions with bias and temperature

Shot noise is a powerful tool to probe correlations and microscopic transport details that conductance measurements alone cannot reveal. Even in atomic-scale Au devices that are well described by Landauer-B{ü}ttiker physics, complications remain such as local heating and electron-phonon interactions. We report systematic rf measurements of shot noise in individual atomic-scale gold break junctions at multiple temperatures, with most bias voltages well above the energy of the Au optical phonon mode. Motivated by the previous experimental evidence that electron-phonon interactions can modify Fano factors and result in kinked features in bias dependence of shot noise, we find that the temperature dependence of shot noise from 4.2~K to 100~K is minimal. Enhanced Fano factors near 0.5$~G_0$ and features beyond simply linear bias dependence of shot noise near the 1$~G_0$ plateau are observed. Both are believed to have non-interacting origins and the latter likely results from slightly bias-dependent transmittance of the dominant quantum channel.

cond-mat.mes-hall↗

arXiv2017

Plasmonic heating in Au nanowires at low Temperatures: The role of thermal boundary resistance

Inelastic electron tunneling and surface-enhanced optical spectroscopies at the molecular scale require cryogenic local temperatures even under illumination - conditions that are challenging to achieve with plasmonically resonant metallic nanostructures. We report a detailed study of the laser heating of plasmonically active nanowires at substrate temperatures from 5 to 60 K. The increase of the local temperature of the nanowire is quantified by a bolometric approach and could be as large as 100 K for a substrate temperature of 5 K and typical values of laser intensity. We also demonstrate that a $\sim 3\times$ reduction of the local temperature increase is possible by switching to a sapphire or quartz substrate. Finite element modeling of the heat dissipation reveals that the local temperature increase of the nanowire at temperatures below $\sim$50 K is determined largely by the thermal boundary resistance of the metal-substrate interface. The model reproduces the striking experimental trend that in this regime the temperature of the nanowire varies nonlinearly with the incident optical power. The thermal boundary resistance is demonstrated to be a major constraint on reaching low temperatures necessary to perform simultaneous inelastic electron tunneling and surface enhanced Raman spectroscopies.

cond-mat.mes-hall↗