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1.
Nat Commun ; 15(1): 2116, 2024 Mar 08.
Article in English | MEDLINE | ID: mdl-38459058

ABSTRACT

Altermagnetism represents an emergent collinear magnetic phase with compensated order and an unconventional alternating even-parity wave spin order in the non-relativistic band structure. We investigate directly this unconventional band splitting near the Fermi energy through spin-integrated soft X-ray angular resolved photoemission spectroscopy. The experimentally obtained angle-dependent photoemission intensity, acquired from epitaxial thin films of the predicted altermagnet CrSb, demonstrates robust agreement with the corresponding band structure calculations. In particular, we observe the distinctive splitting of an electronic band on a low-symmetry path in the Brilliouin zone that connects two points featuring symmetry-induced degeneracy. The measured large magnitude of the spin splitting of approximately 0.6 eV and the position of the band just below the Fermi energy underscores the significance of altermagnets for spintronics based on robust broken time reversal symmetry responses arising from exchange energy scales, akin to ferromagnets, while remaining insensitive to external magnetic fields and possessing THz dynamics, akin to antiferromagnets.

2.
Adv Mater ; 36(24): e2312282, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38380859

ABSTRACT

Artificial lattices constructed from individual dopant atoms within a semiconductor crystal hold promise to provide novel materials with tailored electronic, magnetic, and optical properties. These custom-engineered lattices are anticipated to enable new, fundamental discoveries in condensed matter physics and lead to the creation of new semiconductor technologies including analog quantum simulators and universal solid-state quantum computers. This work reports precise and repeatable, substitutional incorporation of single arsenic atoms into a silicon lattice. A combination of scanning tunneling microscopy hydrogen resist lithography and a detailed statistical exploration of the chemistry of arsine on the hydrogen-terminated silicon (001) surface are employed to show that single arsenic dopants can be deterministically placed within four silicon lattice sites and incorporated with 97 ± 2% yield. These findings bring closer to the ultimate frontier in semiconductor technology: the deterministic assembly of atomically precise dopant and qubit arrays at arbitrarily large scales.

3.
Nat Commun ; 15(1): 694, 2024 Jan 24.
Article in English | MEDLINE | ID: mdl-38267459

ABSTRACT

Atomically precise hydrogen desorption lithography using scanning tunnelling microscopy (STM) has enabled the development of single-atom, quantum-electronic devices on a laboratory scale. Scaling up this technology to mass-produce these devices requires bridging the gap between the precision of STM and the processes used in next-generation semiconductor manufacturing. Here, we demonstrate the ability to remove hydrogen from a monohydride Si(001):H surface using extreme ultraviolet (EUV) light. We quantify the desorption characteristics using various techniques, including STM, X-ray photoelectron spectroscopy (XPS), and photoemission electron microscopy (XPEEM). Our results show that desorption is induced by secondary electrons from valence band excitations, consistent with an exactly solvable non-linear differential equation and compatible with the current 13.5 nm (~92 eV) EUV standard for photolithography; the data imply useful exposure times of order minutes for the 300 W sources characteristic of EUV infrastructure. This is an important step towards the EUV patterning of silicon surfaces without traditional resists, by offering the possibility for parallel processing in the fabrication of classical and quantum devices through deterministic doping.

4.
J Phys Chem C Nanomater Interfaces ; 127(33): 16433-16441, 2023 Aug 24.
Article in English | MEDLINE | ID: mdl-37646007

ABSTRACT

We investigate the adsorption and thermal decomposition of triphenyl bismuth (TPB) on the silicon (001) surface using atomic-resolution scanning tunneling microscopy, synchrotron-based X-ray photoelectron spectroscopy, and density functional theory calculations. Our results show that the adsorption of TPB at room temperature creates both bismuth-silicon and phenyl-silicon bonds. Annealing above room temperature leads to increased chemical interactions between the phenyl groups and the silicon surface, followed by phenyl detachment and bismuth subsurface migration. The thermal decomposition of the carbon fragments leads to the formation of silicon carbide at the surface. This chemical understanding of the process allows for controlled bismuth introduction into the near surface of silicon and opens pathways for ultra-shallow doping approaches.

5.
Adv Sci (Weinh) ; 10(27): e2302101, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37469010

ABSTRACT

Two-dimensional dopant layers (δ-layers) in semiconductors provide the high-mobility electron liquids (2DELs) needed for nanoscale quantum-electronic devices. Key parameters such as carrier densities, effective masses, and confinement thicknesses for 2DELs have traditionally been extracted from quantum magnetotransport. In principle, the parameters are immediately readable from the one-electron spectral function that can be measured by angle-resolved photoemission spectroscopy (ARPES). Here, buried 2DEL δ-layers in silicon are measured with soft X-ray (SX) ARPES to obtain detailed information about their filled conduction bands and extract device-relevant properties. This study takes advantage of the larger probing depth and photon energy range of SX-ARPES relative to vacuum ultraviolet (VUV) ARPES to accurately measure the δ-layer electronic confinement. The measurements are made on ambient-exposed samples and yield extremely thin (< 1 nm) and dense (≈1014  cm-2 ) 2DELs. Critically, this method is used to show that δ-layers of arsenic exhibit better electronic confinement than δ-layers of phosphorus fabricated under identical conditions.

6.
J Am Chem Soc ; 145(23): 12920-12927, 2023 Jun 14.
Article in English | MEDLINE | ID: mdl-37267070

ABSTRACT

Magnetic interactions in combination with nontrivial band structures can give rise to several exotic physical properties such as a large anomalous Hall effect, the anomalous Nernst effect, and the topological Hall effect (THE). Antiferromagnetic (AFM) materials exhibit the THE due to the presence of nontrivial spin structures. EuCuAs crystallizes in a hexagonal structure with an AFM ground state (Néel temperature ∼ 16 K). In this work, we observe a large topological Hall resistivity of ∼7.4 µΩ-cm at 13 K which is significantly higher than the giant topological Hall effect of Gd2PdSi3 (∼3 µΩ-cm). Neutron diffraction experiments reveal that the spins form a transverse conical structure during the metamagnetic transition, resulting in the large THE. In addition, by controlling the magnetic ordering structure of EuCuAs with an external magnetic field, several fascinating topological states such as Dirac and Weyl semimetals have been revealed. These results suggest the possibility of spintronic devices based on antiferromagnets with tailored noncoplanar spin configurations.

7.
Sci Adv ; 9(16): eadf5997, 2023 Apr 21.
Article in English | MEDLINE | ID: mdl-37075116

ABSTRACT

In this work, we show the feasibility of extreme ultraviolet (EUV) patterning on an HF-treated silicon (100) surface in the absence of a photoresist. EUV lithography is the leading lithography technique in semiconductor manufacturing due to its high resolution and throughput, but future progress in resolution can be hampered because of the inherent limitations of the resists. We show that EUV photons can induce surface reactions on a partially hydrogen-terminated silicon surface and assist the growth of an oxide layer, which serves as an etch mask. This mechanism is different from the hydrogen desorption in scanning tunneling microscopy-based lithography. We achieve silicon dioxide/silicon gratings with 75-nanometer half-pitch and 31-nanometer height, demonstrating the efficacy of the method and the feasibility of patterning with EUV lithography without the use of a photoresist. Further development of the resistless EUV lithography method can be a viable approach to nanometer-scale lithography by overcoming the inherent resolution and roughness limitations of photoresist materials.

8.
Adv Sci (Weinh) ; 10(13): e2207121, 2023 May.
Article in English | MEDLINE | ID: mdl-36828783

ABSTRACT

Weyl semimetal is a unique topological phase with topologically protected band crossings in the bulk and robust surface states called Fermi arcs. Weyl nodes always appear in pairs with opposite chiralities, and they need to have either time-reversal or inversion symmetry broken. When the time-reversal symmetry is broken the minimum number of Weyl points (WPs) is two. If these WPs are located at the Fermi level, they form an ideal Weyl semimetal (WSM). In this study, intrinsic ferromagnetic (FM) EuCd2 As2 are grown, predicted to be an ideal WSM and studied its electronic structure by angle-resolved photoemission spectroscopy, and scanning tunneling microscopy which agrees closely with the first principles calculations. Moreover, anomalous Hall conductivity and Nernst effect are observed, resulting from the non-zero Berry curvature, and the topological Hall effect arising from changes in the band structure caused by spin canting produced by magnetic fields. These findings can help realize several exotic quantum phenomena in inorganic topological materials that are otherwise difficult to assess because of the presence of multiple pairs of Weyl nodes.

9.
Adv Sci (Weinh) ; 10(6): e2205476, 2023 Feb.
Article in English | MEDLINE | ID: mdl-36592417

ABSTRACT

Pb(Zr,Ti)O3 (PZT) is the most common ferroelectric (FE) material widely used in solid-state technology. Despite intense studies of PZT over decades, its intrinsic band structure, electron energy depending on 3D momentum k, is still unknown. Here, Pb(Zr0.2 Ti0.8 )O3 using soft-X-ray angle-resolved photoelectron spectroscopy (ARPES) is explored. The enhanced photoelectron escape depth in this photon energy range allows sharp intrinsic definition of the out-of-plane momentum k and thereby of the full 3D band structure. Furthermore, the problem of sample charging due to the inherently insulating nature of PZT is solved by using thin-film PZT samples, where a thickness-induced self-doping results in their heavy doping. For the first time, the soft-X-ray ARPES experiments deliver the intrinsic 3D band structure of PZT as well as the FE-polarization dependent electrostatic potential profile across the PZT film deposited on SrTiO3 and Lax SrMn1- x O3 substrates. The negative charges near the surface, required to stabilize the FE state pointing away from the sample (P+), are identified as oxygen vacancies creating localized in-gap states below the Fermi energy. For the opposite polarization state (P-), the positive charges near the surface are identified as cation vacancies resulting from non-ideal stoichiometry of the PZT film as deduced from quantitative XPS measurements.

10.
ACS Nano ; 14(3): 3316-3327, 2020 Mar 24.
Article in English | MEDLINE | ID: mdl-32142256

ABSTRACT

Over the past two decades, prototype devices for future classical and quantum computing technologies have been fabricated by using scanning tunneling microscopy and hydrogen resist lithography to position phosphorus atoms in silicon with atomic-scale precision. Despite these successes, phosphine remains the only donor precursor molecule to have been demonstrated as compatible with the hydrogen resist lithography technique. The potential benefits of atomic-scale placement of alternative dopant species have, until now, remained unexplored. In this work, we demonstrate the successful fabrication of atomic-scale structures of arsenic-in-silicon. Using a scanning tunneling microscope tip, we pattern a monolayer hydrogen mask to selectively place arsenic atoms on the Si(001) surface using arsine as the precursor molecule. We fully elucidate the surface chemistry and reaction pathways of arsine on Si(001), revealing significant differences to phosphine. We explain how these differences result in enhanced surface immobilization and in-plane confinement of arsenic compared to phosphorus, and a dose-rate independent arsenic saturation density of 0.24 ± 0.04 monolayers. We demonstrate the successful encapsulation of arsenic delta-layers using silicon molecular beam epitaxy, and find electrical characteristics that are competitive with equivalent structures fabricated with phosphorus. Arsenic delta-layers are also found to offer confinement as good as similarly prepared phosphorus layers, while still retaining >80% carrier activation and sheet resistances of <2 kΩ/square. These excellent characteristics of arsenic represent opportunities to enhance existing capabilities of atomic-scale fabrication of dopant structures in silicon, and may be important for three-dimensional devices, where vertical control of the position of device components is critical.

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