This invention is concerning a method of generating local electric fields that drive spatially varying currents within an optical spot of a semiconductor.
The spatial and temporal dynamics of charged particles at the interfaces of materials is of vital consequence to several modern technologies, including but not limited to light-harvesting and semiconductor devices. For example, the mobility of carriers and the underlying nature of diffusion raise important questions relevant to semiconductor device technology. In the case of photocatalysis, where light energy is converted to chemical energy at the surface of a semiconductor, spatio-temporal dynamics of the photocarriers can directly impact chemical reactions at that surface. To further these scientific and technological aims, over the past few years, a handful of techniques have begun to study the dynamics of photocarriers simultaneously in space and time with high resolution.
Ultrafast micro pump-probe techniques which interpret the measured, spatially resolved optical response to understand the underlying carrier dynamics, have observed drift and diffusion phenomena in semiconductor nanostructures. One such method of measurement is scanning ultrafast electron microscopy (SUEM), which utilizes ultrafast electronic packets to obtain high spatio-temporal resolution. SUEM can be used to measure secondary electrons emitted by a probe electron packet to access the photoexcited carrier dynamics. As a result, SUEM has recently observed anomalous and anisotropic diffusion phenomena in amorphous silicon and black phosphorous respectively. However, the measurements achieved this way still lack certainty and rigor.
Consequently, an improved system and method for study the dynamics of photocarriers simultaneously in space and time with high resolution is desired.
A system and method for redistributing photoexcited electrons and generate local currents within an optical spot on ultrafast timescales achieving in high-speed, high-resolution control of opto-electronic phenomena is disclosed. Selectively addressing sub-populations of photoexcited electrons within the distribution is necessary. By exploiting the spatial intensity variations in an ultrafast light pulse, local surface fields are generated within the photoexcitation spot of a doped semiconductor, which pull apart the photoexcited electrons into two separate distributions. Using time-resolved photoemission microscopy, it is then possible to directly record a movie of this redistribution process, which can be controlled via the spatial profile and intensity of the photoexciting pulse. An intuitive and quantitative model explains the underlying charge transport phenomena, thus providing a roadmap to the more generalized ability to manipulate photocarrier distributions with high spatio-temporal resolution.
The embodiments herein demonstrate a novel capability to move and redistribute photoexcited electrons within the optical spot on ultrafast timescales. This is achieved by generating local electric fields with high spatiotemporal resolution using light that drives current within an optical spot, and manipulating the distribution of photoelectrons.
In the past, a conventional example of manipulating the distribution of photocarriers is the separation of unlike charges—e.g. electrons and holes, via an electric field or energy gradient. This has been the cornerstone of various opto-electronic technologies to date solar cells, photodetectors, and others. On the other hand, being able to manipulate distributions of like photocarriers, say electrons, with high spatio-temporal resolution would provide another, perhaps even more powerful, platform for future opto-electronic control. For example, one could generate local currents that rapidly pull apart portions of the photoexcited electron distribution, and use them to power tiny opto-electronic devices, or to drive site-specific, temporally gated photocatalytic reactions, or to study quantum coherent effects that develop between the spatially separated electron sub-populations.
One difficulty with achieving the above is that manipulating distributions of like photocharges is quite challenging—it requires one to selectively address just one part of the distribution, which can then be separately manipulated from the whole. Even in the broader physics literature, techniques to separate electron populations, such as the Stern-Gerlach apparatus or the partial quantum tunneling through a barrier, are scarce. Moreover, they do not operate on ultrafast timescales and are of limited utility in the case of photoelectrons in materials.
The embodiments herein overcome these and other difficulties. Specifically, using intensity variations in the optical pulse, it is possible to generate local electric fields in a doped semiconductor, which selectively address photo-electron sub-populations and thereby pull apart the original Gaussian distribution of the electrons into two separate distributions on ultrafast timescales. Using a theoretical model to explain and quantitatively reproduce the results of the above steps and procedures, a clear roadmap into arbitrary manipulation of the distribution of photoelectrons (as well as other quasiparticles) with high spatio-temporal resolution is provided.
It is also possible to capture movies of the above redistribution process. These movies may have a duration of only several trillionths of a second, but can be controlled by making alterations to the shape and intensity of an optical pulse.
As stated, SUEM has recently observed anomalous and anisotropic diffusion phenomena in amorphous silicon and black phosphorous respectively.
In contrast, time-resolved photoemission electron microscopy (TR-PEEM) techniques combines the high temporal resolution provided by ultrafast optical pulses with the high spatial resolution provided by photoemitted electrons to study dynamic in metals and semiconductors. In semiconductors, TR-PEEM can directly image the density of photoexcited electrons as they evolve in space and time, as exemplified through observation of the motion of electrons in a type-II semiconductor heterostructure.
Beyond the observation of drift and diffusion phenomena in semiconductor structures, it is advantageous to directly control the distribution of charge densities and local currents in space and time with high resolution. Arguably, one of the most potent and useful examples of manipulating photocarrier distribution for modern technology is the separation of unlike photocharges—e.g. electrons and holes, using macroscopic electric fields or energy gradients formed in material heterostructures, such as type-II heterostructures. However, manipulating the distribution of photocarriers of the same charge, e.g. just the electrons, can be challenging due to the relatively few ways to separately address sub-populations of the photocarrier. Furthermore, tools to achieve control with both high spatial and temporal resolution remain scarce.
Light would provide a natural tool to achieve high-speed effects, but it would still be necessary to develop ways to selectively manipulate electrons within the optical spot size to achieve spatial resolution beyond the diffraction limit. Ultimately, such an ability to manipulate the distribution of photoexcited electrons and thereby generate local, spatially varying currents with high spatio-temporal resolution could have significant implications for fast, nanoscale opto-electronic devices, or for site-specific, temporally gated photocatalytic reactions, as well as many other opto-electronic technologies.
Utilizing the spatial variations in the intensity of a Gaussian ultrafast optical beam, it is possible to generate local electric fields that drive spatially varying currents within the optical spot of a p-doped GaAs semiconductor. The local electric fields act to pull apart and separate a single Gaussian distribution into two separate Gaussian distributions of photoexcited electrons. Using TR-PEEM, it is possible to directly image the evolving electron density with high spatial and temporal resolution, and thereby make a movie of the process of separation of the photoexcited electron distribution. By varying the spatial profile and intensity of the ultrafast optical beam, one can control the in-plane electric fields and thus the degree and rate of the separation process.
The photoemitted electrons 124 are imaged in the photoemission electron microscope 132 with high spatial resolution at varying pump-probe delays. Assembling a plurality of these images sequentially can provide a movie demonstrating how to control the redistribution of the photoexcited electrons via optically induced spatially varying in-plane electric fields within the photoexcitation spot 136.
For the embodiments herein, a p-doped GaAs wafer is cleaved in-situ in the ultrahigh vacuum chamber of the photoemission electron microscope (PEEM), thereby exposing a clean surface. The wafer is then photoexcited with a 1.55 eV, 45 fs pump pulse. The photoexcited electrons are then photoemitted with a time-delayed 4.6 eV probe pulse. As shown in
Meanwhile, within
With the experimental capability shown in
A grazing angle of incidence of the pulse from the pump 104 creates an elliptical photoexcitation profile, which provides a strong electric field along the short axis (as explained in more detail below). At the instant of photoexcitation i.e. at 0 ps, the density profile of the photoexcited electrons inherits the Gaussian (bell curve) distribution of the photoexcitation beam.
The intensity profile of the photoexcitation beam provides a strong degree of control over the rate and degree of separation of the photoexcited electrons. This is advantageous and has a wide variety of useful applications.
In
Some context may be helpful at this point, starting with an explanation of generating in-plane electric fields arising from intensity variations in the photoexciting Gaussian pulse. Within the embodiments herein, prior to photoexcitation, a layer of positive charge exists at the surface of a p-doped semiconductor, which in turn is balanced by the depletion layer of negatively charged dopants and results in the well-known band bending seen in doped semiconductors. Within this disclosure, the expression surface bands will be understood to mean valence and conduction bands which are found at the surface of a typical semiconductor.
Upon the optical injection of carriers from the pump 104 in
In the embodiments herein, under the right intensity conditions, an almost completely screened region at the center of the Gaussian pulse and regions with a finite intrinsic field away from the center are left behind. Thus, as shown in
By using a grazing angle of incidence corresponding to an elliptical photoexcitation profile, it is possible to weaken the strength of the electric field along the long axis of the ellipse thereby ensuring the electrons are pulled apart only in the direction of the short axis. This is another example of the utility and usefulness of the embodiments herein. The ability to control the pulling of the electrons is advantageous and has many practical and industrial applications.
The axes labelled ‘Distance’ in
An important semantic consideration exists with regard to
For additional clarification,
In both
Comparing
The Point of all this
After having digested the above, it should now be more apparent that the embodiments herein provide a new paradigm in the spatio-temporal control of charge carriers with high resolution. In general, the ability to alter photoexcited electronic distributions within the optical spot 136 opens up the possibility to go beyond the diffraction limit of light to the nanoscale. Further, using spatial light modulators to imprint other non-trivial intensity patterns on the surface, it becomes possible to obtain arbitrary control of charge currents on a nano-scale, or even a femto-scale. These charge currents in turn can be used to drive nanoscale opto-electronic devices, or for localized, temporally-gated photocatalysis with high resolution and unprecedented control.
Another interesting consequence of the ability to spatially separate, and then potentially recombine sub-populations of photoexcited electrons, could be spatial coherences in the photoelectron population. The ability to manipulate spatial quantum coherent effects in photoexcited electron populations would have fundamental as well as technological value. Lastly, the ability to create lateral energy potential differences at the surface via lateral variations in the amount of band bending could allow the flow of other quasi-particle species such as neutral, tightly bound excitons, thus enabling next-generation excitonic technologies.
In an embodiment, the composition of the wafer can be Zn-doped GaAs <100> wafer of thickness 350±25 μm. The dopant concentration of the sample was confirmed via Hall Effect measurement to be ˜1.0×1017 cm−3. The sample was heated to 150° C. in an ultrahigh vacuum chamber (˜10−10 Torr) for at least an hour for desorption of gases from the surface. After cooling, the sample was cleaved in-situ and transferred into the main chamber for measurements. The cleaved surface was confirmed with both low energy electron diffraction (LEED) and photoemission imaging (PEEM) to be clean and free of any microscopic ridges.
The TR-PEEM measurements were performed in a LEEM/PEEM system (e.g. SPELEEM, manufactured by Elmitec GmbH) using femtosecond pump-probe technique. The cathode lens design of the microscope allows for non-scanning, high-resolution imaging of the photoemitted electrons with a lateral resolution of ˜40 nm. The femtosecond pulses at a central wavelength of 800 nm and a pulse duration of 45 fs are generated by a high-power (e.g. 2.6 W) high repetition rate (4 MHz) oscillator system. The fundamental pulses were split into two parts: the first part was used as a pump pulse to photoexcite the GaAs sample; the second part was frequency tripled via BBO crystals to 266 nm and used as a time-delayed probe pulse to photoemit electrons from the sample.
Due to the low photon energy of the probe and the electron affinity of the sample, only the photoexcited electrons are photoemitted from the sample. Both the pump and the probe pulses were focused onto the sample at a grazing angle of 18°. The diameter of the short axis of the pump elliptical spot 136 was ˜30 μm FWHM. The probe spot was a few hundred micrometers wide to achieve uniform illumination of the field-of-view of the sample. The temporal resolution of the measurement is obtained from the rise time of the pump-probe signal to be ˜280 fs, due to the stretching of the frequency-tripled probe. The LEED pattern of the sample was taken both before and after the measurements to rule out any significant surface change over the course of the measurements.
At equilibrium, the surface band bending of a p-type GaAs leaves behind a positively charged surface that is balanced by the negatively charged regions beneath the surface, i.e. the depletion region. Upon photoexcitation, this intrinsic surface space charge field causes the photoexcited electrons to drift towards the surface and the holes to drift towards the bulk. This separation of the photoexcited carriers will in turn lead to the buildup of an opposite electric field that will then “screen” the intrinsic surface space charge field. The inhomogeneous distribution of the photoexcited carriers leads to a spatially nonuniform screening of the intrinsic field. The gradient of unscreened positive surface charges gives rise to an in-plane surface electric field that acts upon the photoexcited electrons, pulling them apart as observed at least within
The layer 508 refers to a layer of negative charges in a depletion region. The X-axis is the surface of the wafer 120, the +++ is the layer of positive charges, and the e− are the photoexcited charges at the surface.
Due to the longer distance, the photoelectrons closer to the positive surface charges in the +x direction will experience a net attractive pull towards the +x direction, and vice versa for the electrons closer to the positive surface charges in the −x direction. Finally,
As such, the surface electric field due to these positive surface charges is
where σ is the surface charge density. Correspondingly, the surface electric field in the x-direction due to the negative charges at z=−w is
and the resultant surface electric field due to this layer of dipoles is as shown in
Using this surface electric field, it is then possible to model the lateral transport of the photoelectrons at the surface with the following drift-diffusion equation:
where N is the electron density, D is the diffusion coefficient, μ is the electron mobility, and τ is the recombination rate. Using the three parameters, D, μ, and τ as fitting parameters, it is possible to qualitatively reproduce the photoexcited electrons distribution profile as shown in
A field programmable gate array (FPGA) is a semiconductor device made up of reconfigurable logic blocks. Unlike integrated circuits that are designed and fabricated specifically for an application. FPGAs can be reprogram by end users to desired new application or functionality after manufacturing. This has greatly reduced the cost and time for application-specific circuit design as incremental changes to the circuit can now be done within hours instead of weeks spent fabricating the new circuit.
One of the principles of the embodiments herein is the ultrafast, sub-diffraction control of the local surface potential. By manipulating the surface potential with an ultrafast light, we can potentially imprint a temporary logic gate on the sample for as long as the photocarrier lifetime, after which the gate will be erased allowing the sample surface to be reprogram with another logic gate.
By selecting a material with higher bandgap and shorter photocarrier lifetime, nanoscale devices can be reprogrammed with picosecond intervals.
This application is a U.S. National Stage Application filed under 35 U.S.C. § 371 of International Patent Application No. PCT/JP2019/016464 entitled “METHOD OF GENERATING LOCAL ELECTRIC FIELDS”, filed Apr. 17, 2019, which claims priority to U.S. Application No. 62/660,818, filed Apr. 20, 2018, the contents of which are incorporated by reference for all purposes as if fully set forth herein.
| Filing Document | Filing Date | Country | Kind |
|---|---|---|---|
| PCT/JP2019/016464 | 4/17/2019 | WO | 00 |
| Number | Date | Country | |
|---|---|---|---|
| 62660818 | Apr 2018 | US |