Chiral high-harmonic generation and spectroscopy on solid surfaces using polarization-tailored strong fields.

Strong-field methods in solids enable new strategies for ultrafast nonlinear spectroscopy and provide all-optical insights into the electronic properties of condensed matter in reciprocal and real space. Additionally, solid-state media offers unprecedented possibilities to control high-harmonic generation using modified targets or tailored excitation fields. Here we merge these important points and demonstrate circularly-polarized high-harmonic generation with polarization-matched excitation fields for spectroscopy of chiral electronic properties at surfaces. The sensitivity of our approach is demonstrated for structural helicity and termination-mediated ferromagnetic order at the surface of silicon-dioxide and magnesium oxide, respectively. Circularly polarized radiation emanating from a solid sample now allows to add basic symmetry properties as chirality to the arsenal of strong-field spectroscopy in solids. Together with its inherent temporal (femtosecond) resolution and non-resonant broadband spectrum, the polarization control of high harmonics from condensed matter can illuminate ultrafast and strong field dynamics of surfaces, buried layers or thin films.

Lithography for robust and editable atomic-scale silicon devices and memories.

At the atomic scale, there has always been a trade-off between the ease of fabrication of structures and their thermal stability. Complex structures that are created effortlessly often disorder above cryogenic conditions. Conversely, systems with high thermal stability do not generally permit the same degree of complex manipulations. Here, we report scanning tunneling microscope (STM) techniques to substantially improve automated hydrogen lithography (HL) on silicon, and to transform state-of-the-art hydrogen repassivation into an efficient, accessible error correction/editing tool relative to existing chemical and mechanical methods. These techniques are readily adapted to many STMs, together enabling fabrication of error-free, room-temperature stable structures of unprecedented size. We created two rewriteable atomic memories (1.1 petabits per in2), storing the alphabet letter-by-letter in 8 bits and a piece of music in 192 bits. With HL no longer faced with this trade-off, practical silicon-based atomic-scale devices are poised to make rapid advances towards their full potential.

All-electronic Nanosecond-resolved Scanning Tunneling Microscopy: Facilitating the Investigation of Single Dopant Charge Dynamics.

The miniaturization of semiconductor devices to scales where small numbers of dopants can control device properties requires the development of new techniques capable of characterizing their dynamics. Investigating single dopants requires sub-nanometer spatial resolution, which motivates the use of scanning tunneling microscopy (STM). However, conventional STM is limited to millisecond temporal resolution. Several methods have been developed to overcome this shortcoming, including all-electronic time-resolved STM, which is used in this study to examine dopant dynamics in silicon with nanosecond resolution. The methods presented here are widely accessible and allow for local measurement of a wide variety of dynamics at the atomic scale. A novel time-resolved scanning tunneling spectroscopy technique is presented and used to efficiently search for dynamics.

Resolving and Tuning Carrier Capture Rates at a Single Silicon Atom Gap State.

We report on tuning the carrier capture events at a single dangling bond (DB) midgap state by varying the substrate temperature, doping type, and doping concentration. All-electronic time-resolved scanning tunneling microscopy (TR-STM) is employed to directly measure the carrier capture rates on the nanosecond time scale. A characteristic negative differential resistance (NDR) feature is evident in the scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS) measurements of DBs on both n- and p-type doped samples. We find that a common model accounts for both observations. Atom-specific Kelvin probe force microscopy (KPFM) measurements confirm the energetic position of the DB's charge transition levels, corroborating STS studies. We show that under different tip-induced fields the DB can be supplied with electrons from two distinct reservoirs: the bulk conduction band and/or the valence band. We measure the filling and emptying rates of the DBs in the energy regime where electrons are supplied by the bulk valence band. We show that adding point charges in the vicinity of a DB shifts observed STS and NDR features due to Coulombic interactions.

Tailored semiconductors for high-harmonic optoelectronics.

The advent of high-harmonic generation in gases 30 years ago set the foundation for attosecond science and facilitated ultrafast spectroscopy in atoms, molecules, and solids. We explore high-harmonic generation in the solid state by means of nanostructured and ion-implanted semiconductors. We use wavelength-selective microscopic imaging to map enhanced harmonic emission and show that the generation medium and the driving field can be locally tailored in solids by modifying the chemical composition and morphology. This enables the control of high-harmonic technology within precisely engineered solid targets. We demonstrate customized high-harmonic wave fields with wavelengths down to 225 nanometers (ninth-harmonic order of 2-micrometer laser pulses) and present an integrated Fresnel zone plate target in silicon, which leads to diffraction-limited self-focusing of the generated harmonics down to 1-micrometer spot sizes.

Time-resolved single dopant charge dynamics in silicon.

As the ultimate miniaturization of semiconductor devices approaches, it is imperative that the effects of single dopants be clarified. Beyond providing insight into functions and limitations of conventional devices, such information enables identification of new device concepts. Investigating single dopants requires sub-nanometre spatial resolution, making scanning tunnelling microscopy an ideal tool. However, dopant dynamics involve processes occurring at nanosecond timescales, posing a significant challenge to experiment. Here we use time-resolved scanning tunnelling microscopy and spectroscopy to probe and study transport through a dangling bond on silicon before the system relaxes or adjusts to accommodate an applied electric field. Atomically resolved, electronic pump-probe scanning tunnelling microscopy permits unprecedented, quantitative measurement of time-resolved single dopant ionization dynamics. Tunnelling through the surface dangling bond makes measurement of a signal that would otherwise be too weak to detect feasible. Distinct ionization and neutralization rates of a single dopant are measured and the physical process controlling those are identified.

Time-Resolved Imaging of Negative Differential Resistance on the Atomic Scale.

Negative differential resistance remains an attractive but elusive functionality, so far only finding niche applications. Atom scale entities have shown promising properties, but the viability of device fabrication requires a fuller understanding of electron dynamics than has been possible to date. Using an all-electronic time-resolved scanning tunneling microscopy technique and a Green's function transport model, we study an isolated dangling bond on a hydrogen terminated silicon surface. A robust negative differential resistance feature is identified as a many body phenomenon related to occupation dependent electron capture by a single atomic level. We measure all the time constants involved in this process and present atomically resolved, nanosecond time scale images to simultaneously capture the spatial and temporal variation of the observed feature.

New fabrication technique for highly sensitive qPlus sensor with well-defined spring constant.

A new technique for the fabrication of highly sensitive qPlus sensor for atomic force microscopy (AFM) is described. The focused ion beam was used to cut then weld onto a bare quartz tuning fork a sharp micro-tip from an electrochemically etched tungsten wire. The resulting qPlus sensor exhibits high resonance frequency and quality factor allowing increased force gradient sensitivity. Its spring constant can be determined precisely which allows accurate quantitative AFM measurements. The sensor is shown to be very stable and could undergo usual UHV tip cleaning including e-beam and field evaporation as well as in situ STM tip treatment. Preliminary results with STM and AFM atomic resolution imaging at 4.5 K of the silicon Si(111)-7×7 surface are presented.

Single-electron dynamics of an atomic silicon quantum dot on the H-Si(100)-(2×1) surface.

Here we report the direct observation of single electron charging of a single atomic dangling bond (DB) on the H-Si(100)-2×1 surface. The tip of a scanning tunneling microscope is placed adjacent to the DB to serve as a single-electron sensitive charge detector. Three distinct charge states of the dangling bond--positive, neutral, and negative--are discerned. Charge state probabilities are extracted from the data, and analysis of current traces reveals the characteristic single-electron charging dynamics. Filling rates are found to decay exponentially with increasing tip-DB separation, but are not a function of sample bias, while emptying rates show a very weak dependence on tip position, but a strong dependence on sample bias, consistent with the notion of an atomic quantum dot tunnel coupled to the tip on one side and the bulk silicon on the other.