Hot Electron Tunneling in Pt/LaAlO₃/SrTiO₃ Heterostructures for Enhanced Photodetection

LaAlO3/SrTiO3 (LAO/STO) heterostructures, in which a highly mobile two-dimensional electron gas (2DEG) is formed, have great potential for optoelectronic applications. However, the inherently high density of the 2DEG hinders the observation of photo-excitation effects in oxide heterostructures. Herein, a strong photoresponse of the 2DEG in a Pt/LAO/STO heterostructure is achieved by adopting a vertical tunneling configuration. The tunneling of the 2DEG through an ultrathin LAO layer is significantly enhanced by UV light irradiation, showing a maximum photoresponsivity of ∼1.11 × 107%. The strong and reversible photoresponse is attributed to the thermionic emission of photoexcited hot electrons from the oxygen-deficient STO. Notably, the oxygen vacancy defects play a critical role in enhancing the tunneling photocurrent. Our systematic study on the hysteresis behavior and the light power dependency of the tunneling current consistently support the fact that the photoexcited hot electrons from the oxygen vacancies strongly contribute to the tunneling conduction under the UV light. This work offers valuable insights into a novel photodetection mechanism based on the 2DEG as well as into developing ultrathin optoelectronic devices based on the oxide heterostructures

Gate-Tunable Optical Extinction of Graphene Nanoribbon Nanoclusters

We investigate the optical response of graphene nanoribbons (GNRs) using the broadband nonlinear generation and detection capabilities of nanoscale junctions created at the LaAlO$_3$/SrTiO$_3$ interface. GNR nanoclusters measured to be as small as 1-2 GNRs in size are deposited on the LaAlO$_3$ surface with an atomic force microscope tip. Time-resolved nonlinear optical probes of GNR nanoclusters reveal a strong, gate-tunable second and third harmonic response, as well as strong extinction of visible to near-infrared (VIS-NIR) light at distinct wavelengths, similar to previous reports with graphene

Broadband Terahertz Generation and Detection at 10 nm Scale

Terahertz (0.1–30 THz) radiation reveals a wealth of information that is relevant for material, biological, and medical sciences with applications that span chemical sensing, high-speed electronics, and coherent control of semiconductor quantum bits. To date, there have been no methods capable of controlling terahertz (THz) radiation at molecular scales. Here we report both generation and detection of broadband terahertz field from 10 nm scale oxide nanojunctions. Frequency components of ultrafast optical radiation are mixed at these nanojunctions, producing broadband THz emission. These same devices detect THz electric fields with comparable spatial resolution. This unprecedented control, on a scale of 4 orders of magnitude smaller than the diffraction limit, creates a pathway toward THz-bandwidth spectroscopy and control of individual nanoparticles and molecules

Gate-Tunable Optical Nonlinearities and Extinction in Graphene/LaAlO3_3/SrTiO3_3 Nanostructures

Pristine, undoped graphene has a constant absorption of 2.3 % across the visible to near-infrared (VIS-NIR) region of the electromagnetic spectrum. Under certain conditions, such as nanostructuring and intense gating, graphene can interact more robustly with VIS-NIR light and exhibit a large nonlinear optical response. Here, we explore the optical properties of graphene/LaAlO$_3$/SrTiO$_3$ nanostructures, where nanojunctions formed at the LaAlO$_3$/SrTiO$_3$ interface enable large (~10$^8$ V/m) electric fields to be applied to graphene over a scale of ~10 nm. Upon illumination with ultrafast VIS-NIR light, graphene/LaAlO$_3$/SrTiO$_3$ nanostructures produce broadband THz emission as well as a sum-frequency generated (SFG) response. Strong spectrally sharp, gate-tunable extinction features (>99.99%) are observed in both the VIS-NIR and SFG regions alongside significant intensification of the nonlinear response. The observed gate-tunable strong graphene-light interaction and nonlinear optical response are of fundamental interest and open the way for future exploitation in graphene-based optical devices

Strong Interfacial Charge Trapping in Ultrathin SrRuO₃ on SrTiO₃ Probed by Noise Spectroscopy

SrRuO3 (SRO) has emerged as a promising quantum material due to its exotic electron correlations and topological properties. In epitaxial SRO films, electron scattering against lattice phonons or defects has been considered as only a predominant mechanism accounting for electronic properties. Although the charge trapping by polar defects can also strongly influence the electronic behavior, it has often been neglected. Herein, we report strong interfacial charge trapping in ultrathin SRO films on SrTiO3 (STO) substrates probed by noise spectroscopy. We find that oxygen vacancies in the STO cause stochastic interfacial charge trapping, resulting in high electrical noise. Spectral analyses of the photoinduced noise prove that the oxygen vacancies buried deep in the STO can effectively contribute to the charge trapping process. These results unambiguously reveal that electron transport in ultrathin SRO films is dominated by the carrier number fluctuation that correlates with interfacial charge trapping

Tailoring LaAlO₃/SrTiO₃ Interface Metallicity by Oxygen Surface Adsorbates

We report an oxygen surface adsorbates induced metal–insulator transition at the LaAlO₃/SrTiO₃ interfaces. The observed effects were attributed to the terminations of surface Al sites and the resultant electron-accepting surface states. By controlling the local oxygen adsorptions, we successfully demonstrated the nondestructive patterning of the interface two-dimensional electron gas (2DEG). The obtained 2DEG structures are stable in air and also robust against general solvent treatments. This study provides new insights into the metal–insulator transition mechanism at the complex oxide interfaces and also a highly efficient technique for tailoring the interface properties

Large and Reconfigurable Infrared Photothermoelectric Effect at Oxide Interfaces

To maximize the photovoltaic efficiency, it is highly desirable to enable the electricity conversion from low energy photons and to extract the excessive energy from hot carriers. Here we report a large photovoltage generation at the LaAlO3/SrTiO3 interfaces from infrared photons with energies far below the oxide bandgaps. This effect is a result of the photoexcitation of hot carriers in metasurface electrical contacts and the subsequent thermoelectric charge separations by the interfacial two-dimensional electron gas (2DEG). Reaching a room-temperature responsivity of 4.4 V/W, such light-to-charge conversion can be spatially controlled and reconfigured through the patterning of 2DEG using conducting atomic force microscope. Compatible for broadband applications, our results demonstrate a new path toward efficient and programmable light sensing using oxide-based low-dimensional electron systems

Geometrical Doping at the Atomic Scale in Oxide Quantum Materials

Chemical dopants enabling a plethora of emergent physical properties have been treated as randomly and uniformly distributed in the frame of a three-dimensional doped system. However, in nanostructured architectures, the location of dopants relative to the interface or boundary can greatly influence device performance. This observation suggests that chemical dopants need to be considered as discrete defects, meaning that geometric control of chemical dopants becomes a critical aspect as the physical size of materials scales down into the nanotechnology regime. Here we show that geometrical control of dopants at the atomic scale is another fundamental parameter in chemical doping, extending beyond the kind and amount of dopants conventionally used. The geometrical control of dopants extends the class of geometrically controlled structures into an unexplored dimensionality, between 2D and 3D. It is well understood that in the middle of the progressive dimensionality change from 3D to 2D, the electronic state of doped SrTiO3 is altered from a highly symmetric charged fluid to a charge disproportionated insulating state. Our results introduce a geometrical control of dopants, namely, geometrical doping, as another axis to provide a variety of emergent electronic states via tuning of the electronic properties of the solid state

Imprint Control of BaTiO₃ Thin Films via Chemically Induced Surface Polarization Pinning

Surface-adsorbed polar molecules can significantly alter the ferroelectric properties of oxide thin films. Thus, fundamental understanding and controlling the effect of surface adsorbates are crucial for the implementation of ferroelectric thin film devices, such as ferroelectric tunnel junctions. Herein, we report an imprint control of BaTiO₃ (BTO) thin films by chemically induced surface polarization pinning in the top few atomic layers of the water-exposed BTO films. Our studies based on synchrotron X-ray scattering and coherent Bragg rod analysis demonstrate that the chemically induced surface polarization is not switchable but reduces the polarization imprint and improves the bistability of ferroelectric phase in BTO tunnel junctions. We conclude that the chemical treatment of ferroelectric thin films with polar molecules may serve as a simple yet powerful strategy to enhance functional properties of ferroelectric tunnel junctions for their practical applications

Spontaneous Vortex Nanodomain Arrays at Ferroelectric Heterointerfaces

The polarization of the ferroelectric BiFeO3 sub-jected to different electrical boundary conditions by heterointerfaces is imaged with atomic resolution using a spherical aberration-corrected transmission electron microscope. Unusual triangular-shaped nanodomains are seen, and their role in providing polarization closure is understood through phase-field simulations. Heterointerfaces are key to the performance of ferroelectric devices, and this first observation of spontaneous vortex nanodomain arrays at ferroelectric heterointerfaces reveals properties unlike the surrounding film including mixed Ising−Néel domain walls, which will affect switching behavior, and a drastic increase of in-plane polarization. The importance of magnetization closure has long been appreciated in multidomain ferromagnetic systems; imaging this analogous effect with atomic resolution at ferroelectric heterointerfaces provides the ability to see device-relevant interface issues. Extension of this technique to visualize domain dynamics is envisioned