Electron Tunneling Spectroscopy Research Articles

Sensitizers in inelastic electron tunneling spectroscopy: a first-principles study of functional aromatics on Cu(111)

Low sensitivity is a key problem in inelastic electron tunneling spectroscopy (IETS) with the scanning tunneling microscope. Using first-principles simulations, we predict different means to tune the IETS sensitivity of symmetrical functional aromatics on a Cu(111) surface. We show how the IET-spectra of phenyl-NO2 compounds can be greatly enhanced as compared to pristine phenyl. More precisely, the NO2 substituent qualifies as a sensitizer of low-frequency wagging modes, but also as a quencher of high-frequency stretching modes. At variance, the CO2 substituent is found to suppress the whole IET-activity. The head-up (non-anchoring) and head-down (anchoring) configurations of the functional group lead to minor changes in the signals, nevertheless allowing access to discriminate configurational features. It is shown how to disentangle the electronic and steric effects of the substituent in the STM junction.

Spin inelastic currents in molecular ring junctions

Within a simple model, we discuss spin inelastic currents in molecular ring junctions. We generalize considerations of the spin-flip inelastic electron tunneling spectroscopy (IETS) to the case of multisite molecular system, and formulate a conserving approximation, which takes into account renormalization of elastic channel. We also extend recent studies of circular currents in molecular junctions beyond scattering theory formulation. We demonstrate control of the spin-flip IETS signal and discuss spin polarization of total and circular currents in a benzene ring junction.

A theoretical rationalization of a total inelastic electron tunneling spectrum: The comparative cases of formate and benzoate on Cu(111)

Inelastic electron tunneling spectroscopy (IETS) performed with the scanning tunneling microscope (STM) has been deemed as the ultimate tool for identifying chemicals at the atomic scale. However, direct IETS-based chemical analysis remains difficult due to the selection rules that await a definite understanding. We present IETS simulations of single formate and benzoate species adsorbed in the same upright bridge geometry on a (111)-cleaved Cu surface. In agreement with measurements on a related substrate, the simulated IET-spectra of formate/Cu(111) clearly resolve one intense C-H stretching mode whatever the tip position in the vicinity of the molecular fragment. At variance, benzoate/Cu(111) has no detectable IET signal. The dissimilar IETS responses of chemically related molecules--formate and benzoate adsorbates--permit us to unveil another factor that complements the selection rules, namely the degree of the vacuum extension of the tunneling active states perturbed by the vibrations. As a consequence, the lack of a topmost dangling bond orbital is entirely detrimental for STM-based inelastic spectroscopy but not for STM elastic imaging.

ON THE ELECTRONIC DENSITY OF STATES IN INELASTIC ELECTRON TUNNELING SPECTROSCOPY

In agreement with experimental results relative to acetylene and deuterated-acetylene molecules on copper, a quantitative study relative to electronic density of states and tunneling current in terms of voltage is carried out within the context of inelastic electron tunneling spectroscopy. Our starting point is regarding the corresponding differential tunneling conductance as a function of the tunneling voltage. In particular, as a relevant figure of merit, the first derivative of the above conductance is determined. A numerical computation relative to this figure of merit is also carried out.

Single molecule electronics and devices.

The manufacture of integrated circuits with single-molecule building blocks is a goal of molecular electronics. While research in the past has been limited to bulk experiments on self-assembled monolayers, advances in technology have now enabled us to fabricate single-molecule junctions. This has led to significant progress in understanding electron transport in molecular systems at the single-molecule level and the concomitant emergence of new device concepts. Here, we review recent developments in this field. We summarize the methods currently used to form metal-molecule-metal structures and some single-molecule techniques essential for characterizing molecular junctions such as inelastic electron tunnelling spectroscopy. We then highlight several important achievements, including demonstration of single-molecule diodes, transistors, and switches that make use of electrical, photo, and mechanical stimulation to control the electron transport. We also discuss intriguing issues to be addressed further in the future such as heat and thermoelectric transport in an individual molecule.

Effects of substrate strain and electrical stress on lattice dynamics, defects, and traps in strained-Si/Si0.81Ge0.19 n-type metal-oxide-semiconductor field effect transistors

Defects and traps in strained-Si n-type metal-oxide-semiconductor field effect transistors (MOSFETs) are studied in detail. The inelastic electron tunneling spectroscopy (IETS) technique is shown to be capable of probing traps in ultrathin gate dielectrics and obtain the energies and spatial locations of the traps. Detailed analyses of electrical stress-induced build-up of traps and electrically active bonding defects and identification of the trap-features including trap-assisted conduction and charge-trapping have been performed. The location and energies of the traps are estimated from the IETS spectra measured at both bias polarities. Identification of the acoustic and optical phonon modes (inelastic) as well as trap-features (elastic) helps in better understandings of the complex transport-mechanisms in gate dielectrics on strained layers.

Many-body effects in magnetic inelastic electron tunneling spectroscopy

Magnetic inelastic electron tunneling spectroscopy (IETS) shows sharp increases in conductance when a new conductance channel associated to a change in magnetic structure is open. Typically, the magnetic moment carried by an adsorbate can be changed by collision with a tunneling electron; in this process the spin of the electron can flip or not. A previous one-electron theory [Phys. Rev. Lett. {\bf 103}, 176601 (2009)] successfully explained both the conductance thresholds and the magnitude of the conductance variation. The elastic spin flip of conduction electrons by a magnetic impurity leads to the well known Kondo effect. In the present work, we compare the theoretical predictions for inelastic magnetic tunneling obtained with a one-electron approach and with a many-body theory including Kondo-like phenomena. We apply our theories to a singlet-triplet transition model system that contains most of the characteristics revealed in magnetic IETS. We use two self-consistent treatments (non-crossing approximation and self-consistent ladder approximation). We show that, although the one-electron limit is properly recovered, new intrinsic many-body features appear. In particular, sharp peaks appear close to the inelastic thresholds; these are not localized exactly at thresholds and could influence the determination of magnetic structures from IETS experiments.Analysis of the evolution with temperature reveals that these many-body features involve an energy scale different from that of the usual Kondo peaks. Indeed, the many-body features perdure at temperatures much larger than the one given by the Kondo energy scale of the system.

Spin-dependent tunneling spectroscopy in MgO-based double-barrier magnetic tunnel junctions

We investigated the dynamic conductance and inelastic electron tunneling spectroscopy in MgO-based double barrier magnetic tunnel junctions with Co50Fe50/Co40Fe40B20 hybrid free layers. The tunneling is coherent through the MgO (001) barriers but nonresonant, and the highest tunneling magnetoresistance reaches 260% at 2 K. Based on the detailed discussion of the tunneling mechanisms, the double-barrier junctions investigated here can be considered as two single-barrier junctions in series.

Electron Transport through Single π‐Conjugated Molecules Bridging between Metal Electrodes

Understanding electron transport through a single molecule bridging between metal electrodes is a central issue in the field of molecular electronics. This review covers the fabrication and electron-transport properties of single π-conjugated molecule junctions, which include benzene, fullerene, and π-stacked molecules. The metal/molecule interface plays a decisive role in determining the stability and conductivity of single-molecule junctions. The effect of the metal-molecule contact on the conductance of the single π-conjugated molecule junction is reviewed. The characterization of the single benzene molecule junction is also discussed using inelastic electron tunneling spectroscopy and shot noise. Finally, electron transport through the π-stacked system using π-stacked aromatic molecules enclosed within self-assembled coordination cages is reviewed. The electron transport in the π-stacked systems is found to be efficient at the single-molecule level, thus providing insight into the design of conductive materials.

Electron Tunneling Spectroscopic Measurements on Al-doped MgB2 Thin Films

Abstract The effect of Al-doping on the electron-phonon coupling in magnesium diboride films was studied by electron tunneling spectroscopy on planar sandwich-type Mg1-xAlxB2-oxide-indium junctions. The superconducting Mg1-xAlxB2 films (0 ≤ x

Momentum-dependent multiple gaps in magnesium diboride probed by electron tunnelling spectroscopy

The energy gap is the most fundamental property of a superconductor. MgB(2), a superconductor discovered in 2001, exhibits two different superconducting gaps caused by the different electron-phonon interactions in two weakly interacting bands. Theoretical calculations predict that the gap values should also vary across the Fermi surface sheets of MgB(2). However, until now, no such variation has been observed. It has been suggested that two gap values were sufficient to describe real MgB(2) samples. Here we present an electron tunnelling spectroscopy study on MgB(2)/native oxide/Pb tunnel junctions that clearly shows a distribution of gap values, confirming the importance of the anisotropic electron-phonon interaction. The gap values, and their spreads found from the tunnel junction measurements, provide valuable experimental tests for various theoretical approaches to the multi-band superconductivity in MgB(2).

Extracting a More Realistic Pseudopotential for Aluminum, Lead, Niobium and Tantalum from Superconductor Electron Tunnelling Spectroscopy Data

Electron tunnelling spectroscopy when first developed was used to extract the electron-phonon spectral density, α 2 F(ν), from superconductive metals. Here, on revisiting the topic, we show that it further allows the direct extraction of more realistic pseudopotentials for such metals. The pseudopotential so extracted has a range of surprising but physically reasonable properties and regenerates the experimentally derived α 2 F(ν) accurately. Freed from most of its long-standing uncertainties, this pseudopotential may find wide application.

Mechanically controlled molecular orbital alignment in single molecule junctions

Research in molecular electronics often involves the demonstration of devices that are analogous to conventional semiconductor devices, such as transistors and diodes, but it is also possible to perform experiments that have no parallels in conventional electronics. For example, by applying a mechanical force to a molecule bridged between two electrodes, a device known as a molecular junction, it is possible to exploit the interplay between the electrical and mechanical properties of the molecule to control charge transport through the junction. 1,4'-Benzenedithiol is the most widely studied molecule in molecular electronics, and it was shown recently that the molecular orbitals can be gated by an applied electric field. Here, we report how the electromechanical properties of a 1,4'-benzenedithiol molecular junction change as the junction is stretched and compressed. Counterintuitively, the conductance increases by more than an order of magnitude during stretching, and then decreases again as the junction is compressed. Based on simultaneously recorded current-voltage and conductance-voltage characteristics, and inelastic electron tunnelling spectroscopy, we attribute this finding to a strain-induced shift of the highest occupied molecular orbital towards the Fermi level of the electrodes, leading to a resonant enhancement of the conductance. These results, which are in agreement with the predictions of theoretical models, also clarify the origins of the long-standing discrepancy between the calculated and measured conductance values of 1,4'-benzenedithiol, which often differ by orders of magnitude.

Effect of H on interface properties of Al2O3/In0.53Ga0.47As

We report that depositing Al2O3 on InGaAs in an H-containing ambient (e.g., in forming gas) results in significant reduction of interface-trap density and significantly suppressed frequency dispersion of accumulation capacitance. The results of the inelastic electron tunneling spectroscopy study reveal that strong trap features at the Al2O3/InGaAs interface in the InGaAs band gap are largely removed by depositing Al2O3 in an H-containing ambient. Transmission electron microscopy images and x-ray photoelectron spectroscopy data shed some light on the role of hydrogen in improving interface properties of the Al2O3/In0.53Ga0.47As gate stack.

On the interpretation of IETS spectra of a small organic molecule

We have investigated vibrational spectra of nitrobenzene molecules adsorbed on Cu(111) by low temperature inelastic electron tunneling spectroscopy. This molecule, which should support 39 internal modes, only gives rise to seven peaks in the spectra. We outline a comparison with ensemble IR data and interpret the small number of vibrational peaks by the superposition of a multitude of almost isoenergetic vibrational modes. The non-detectability of further modes cannot be understood in terms of symmetry considerations. Additional modes in the spectra are attributed to external molecular–metal vibrations.

Inelastic electron tunneling spectroscopy of HfO2 gate stacks: A study based on first-principles modeling

A first-principles modeling approach is used to investigate the vibrational properties of HfO2. The calculated phonon density of states is compared to experimental results obtained from inelastic electron tunneling spectroscopy (IETS) of various metal-oxide-semiconductor devices with HfO2 gate stacks. This comparison provides deep insights into the nature of the signatures of the complicated IETS spectra and provides valuable structural information about the gate stack, such as the possible presence of oxygen vacancies in jet-vapour deposited HfO2. Important structural differences between the interface of atomic-layer or molecular-beam deposited HfO2 and the Si substrate are also revealed.

Nonequilibrium transport through molecular junctions in the quantum regime

We consider a quantum dot, affected by a local vibrational mode and contacted to macroscopic leads, in the non-equilibrium steady-state regime. We apply a variational Lang-Firsov transformation and solve the equations of motion of the Green functions in the Kadanoff-Baym formalism up to second order in the interaction coefficients. The variational determination of the transformation parameter through minimization of the thermodynamic potential allows us to calculate the electron/polaron spectral function and conductance for adiabatic to anti-adiabatic phonon frequencies and weak to strong electron-phonon couplings. We investigate the qualitative impact of the quasi-particle renormalization on the inelastic electron tunneling spectroscopy signatures and discuss the possibility of a polaron induced negative differential conductance. In the high-voltage regime we find that the polaron level follows the lead chemical potential to enhance resonant transport.

Barrier height and tunneling aspects in (110) CrO2 with its natural barrier

We have investigated (110) CrO2/natural barrier/Co magnetic tunnel junctions for their barrier and magneto-transport properties. A negative tunnel magnetoresistance (TMR) of over 5% was observed in micro-fabricated devices at 4.2 K, which is comparable to TMR values obtained with (100) CrO2. Both transport and cross-sectional transmission electron microscopy analysis reveal a natural barrier thickness 3.5 ± 0.5 nm. However, we obtain a low effective barrier height of 0.4 eV from transport measurements. The inelastic electron tunneling spectroscopy showed significant bias dependence with peak positions showing vibrational modes, which deviate from stoichiometric Cr2O3. We conclude that the transport characteristics are controlled by defects within the natural barrier, consistent with recent theoretical reports.

Inelastic Electron Tunneling Spectroscopy of a Single Nuclear Spin

Detection of a single nuclear spin constitutes an outstanding problem in different fields of physics such as quantum computing or magnetic imaging. Here we show that the energy levels of a single nuclear spin can be measured by means of inelastic electron tunneling spectroscopy (IETS). We consider two different systems, a magnetic adatom probed with scanning tunneling microscopy and a single Bi dopant in a silicon nanotransistor. We find that the hyperfine coupling opens new transport channels which can be resolved at experimentally accessible temperatures. Our simulations evince that IETS yields information about the occupations of the nuclear spin states, paving the way towards transport-detected single nuclear spin resonance.

Olfaction is a chemical sense, not a spectral sense

Franco et al. (1) argued that molecular vibrations contribute to odor detection by Drosophila. They claimed that deuterated odorants have a unique C-D stretch vibration that produces a “deuterium odor character” independent of the “structure and chemical properties of the odorant molecules.” The discrimination of normal and deuterated odorants by flies is a clear and convincing finding, but such isotope effects do not prove that the animals are sensing infrared molecular vibrations using inelastic electron tunneling spectroscopy (IETS) (2).