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1.
Proc Natl Acad Sci U S A ; 117(33): 19773-19779, 2020 08 18.
Artículo en Inglés | MEDLINE | ID: mdl-32753379

RESUMEN

The nonlinear optical response of a material is a sensitive probe of electronic and structural dynamics under strong light fields. The induced microscopic polarizations are usually detected via their far-field light emission, thus limiting spatial resolution. Several powerful near-field techniques circumvent this limitation by employing local nanoscale scatterers; however, their signal strength scales unfavorably as the probe volume decreases. Here, we demonstrate that time-resolved atomic force microscopy is capable of temporally and spatially resolving the microscopic, electrostatic forces arising from a nonlinear optical polarization in an insulating dielectric driven by femtosecond optical fields. The measured forces can be qualitatively explained by a second-order nonlinear interaction in the sample. The force resulting from this nonlinear interaction has frequency components below the mechanical resonance frequency of the cantilever and is thus detectable by regular atomic force microscopy methods. The capability to measure a nonlinear polarization through its electrostatic force is a powerful means to revisit nonlinear optical effects at the nanoscale, without the need for emitted photons or electrons from the surface.

2.
ACS Nano ; 16(7): 11251-11258, 2022 Jul 26.
Artículo en Inglés | MEDLINE | ID: mdl-35816615

RESUMEN

Atomically engineered artificial lattices are a useful tool for simulating complex quantum phenomena, but have so far been limited to the study of Hamiltonians where electron-electron interactions do not play a role. However, it is precisely the regime in which these interactions do matter where computational times lend simulations a critical advantage over numerical methods. Here, we propose a platform for constructing artificial matter that relies on the confinement of field-emission resonances, a class of vacuum-localized discretized electronic states. We use atom manipulation of surface vacancies in a chlorine-terminated Cu(100) surface to reveal square patches of the underlying metal, thereby creating atomically precise potential wells that host particle-in-a-box modes. By adjusting the dimensions of the confining potential, we can access states with different quantum numbers, making these patches attractive candidates as quantum dots or artificial atoms. We demonstrate that the lifetime of electrons in these engineered states can be extended and tuned through modification of the confining potential, either via atomic assembly or by changing the tip-sample distance. We also demonstrate control over a finite range of state filling, a parameter which plays a key role in the evolution of quantum many-body states. We model the transport through the localized state to disentangle and quantify the lifetime-limiting processes, illustrating the critical dependence of the electron lifetime on the properties of the underlying bulk band structure. The interplay with the bulk bands gives rise to negative differential resistance, leading to possible applications in engineering custom atomic-scale resonant tunnelling diodes, which exhibit similar current-voltage characteristics.

3.
ACS Nano ; 15(6): 10377-10383, 2021 Jun 22.
Artículo en Inglés | MEDLINE | ID: mdl-34048210

RESUMEN

Inducing an inversion layer in organic semiconductors is a highly nontrivial, but critical, achievement for producing organic field-effect transistor (OFET) devices, which rely on the generation of inversion, accumulation, and depletion regimes for successful operation. Here, we develop a pulsed bias technique to characterize the dopant type of any organic material system, without prior knowledge or characterization of the material in question. We use this technique on a pentacene/PTCDI heterostructure and thus deduce that pentacene is exhibiting n-doped like response. The source of the additional charges in the pentacene island can be identified by charging rings in the dissipation channel of the noncontact atomic force microscopy (AFM) signal, a typical signature for localized charge transfer from the AFM tip to the sample. Additionally, through tip-induced band-bending, we generate inversion, depletion, and accumulation regimes over a 20 nm radius, three monolayer thick n-doped pentacene island. Our findings demonstrate that nanometer-scale lateral extent and thickness are sufficient for an OFET device to operate in the inversion regime.

4.
Science ; 372(6545): 964-968, 2021 05 28.
Artículo en Inglés | MEDLINE | ID: mdl-34045351

RESUMEN

Full insight into the dynamics of a coupled quantum system depends on the ability to follow the effect of a local excitation in real-time. Here, we trace the free coherent evolution of a pair of coupled atomic spins by means of scanning tunneling microscopy. Rather than using microwave pulses, we use a direct-current pump-probe scheme to detect the local magnetization after a current-induced excitation performed on one of the spins. By making use of magnetic interaction with the probe tip, we are able to tune the relative precession of the spins. We show that only if their Larmor frequencies match, the two spins can entangle, causing angular momentum to be swapped back and forth. These results provide insight into the locality of electron spin scattering and set the stage for controlled migration of a quantum state through an extended spin lattice.

5.
J Phys Condens Matter ; 29(49): 495804, 2017 Dec 13.
Artículo en Inglés | MEDLINE | ID: mdl-29091590

RESUMEN

We have determined the magnetic structures of GdCuSn, GdAgSn and GdAuSn using a combination of [Formula: see text]Gd Mössbauer spectroscopy and neutron powder diffraction. Each compound shows the same antiferromagnetic ordering of the Gd sublattice. The magnetic cell is doubled along the crystallographic a-axis (propagation vector [Formula: see text]) with the moments aligned along the hexagonal c-axis, forming alternating ferromagnetic sheets of up/down Gd moments along the a-axis.

6.
J Phys Condens Matter ; 28(26): 266001, 2016 07 06.
Artículo en Inglés | MEDLINE | ID: mdl-27173847

RESUMEN

(151)Eu Mössbauer spectroscopy and neutron powder diffraction are combined to show that the tetragonal (I4mm #107) compound EuNiGe3 orders magnetically below [Formula: see text] K and adopts a complex incommensurate helicoidal magnetic structure at 3.6 K, with a propagation vector [Formula: see text] and a Eu moment of 7.1(2) [Formula: see text]. On warming through 6 K an incommensurate sinusoidal modulation develops and dominates the magnetic order by 12 K.

7.
J Phys Condens Matter ; 28(16): 166003, 2016 Apr 27.
Artículo en Inglés | MEDLINE | ID: mdl-27009349

RESUMEN

The antiferromagnetic structures of both the manganese and europium sublattices in EuMn2Ge2 have been determined using thermal neutron diffraction. T(N)(Mn) = 714(5) K with the 3.35(5) µ(B) (at 285 K) Mn moments ordering according to the I4'/m'm'm space group. The Eu order is incommensurate with the 6.1(2) µ(B) (at 3.6 K) Eu moments oriented parallel to the c-axis with a propagation vector of k = [0.153(2) 0 0]. Both neutron diffraction and (151)Eu Mössbauer spectroscopy reveal evidence of magnetic short-range ordering of the Eu sublattice around and above T(N)(Eu) ∼ 10 K. The ordering temperature of the Eu sublattice is strongly affected by the sample's thermal history and rapid quenching from the melting point may lead to a complete suppression of that ordering.

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