arXiv subjects

Benjamin P. P. Mallett

Publications and source records attributed to Benjamin P. P. Mallett.

6 recordsLinked to original sources

arXiv2021

Non-collinear and strongly asymmetric polar moments at back-gated SrTiO3 interfaces

The highly mobile electrons at the interface of SrTiO3 with other oxide insulators, such as LaAlO3 or AlOx, are of great current interest. A vertical gate voltage allows controlling a metal/superconductor-to-insulator transition, as well as electrical modulation of the spin-orbit Rashba coupling for spin-charge conversion. These findings raise important questions about the origin of the confined electrons as well as the mechanisms that govern the interfacial electric field. Here we use infrared ellipsometry and confocal Raman spectroscopy to show that an anomalous polar moment is induced at the interface that is non-collinear, highly asymmetric and hysteretic with respect to the vertical gate electric field. Our data indicate that an important role is played by the electromigration of oxygen vacancies and their clustering at the antiferrodistortive domain boundaries of SrTiO3, which generates local electric and possibly also flexoelectric fields and subsequent polar moments with a large lateral component. Our results open new perspectives for the defect engineering of lateral devices with strongly enhanced and hysteretic local electric fields that can be manipulated with various other parameters, like strain, temperature, or photons.

cond-mat.mtrl-sci↗

arXiv2019

Systematic Raman study of optical phonons in $R$Ba$_2$Cu$_3$O$_{6+δ}$ ($R$ = Y, Dy, Gd, Sm, Nd): Antiferromagnetic coupling strength versus lattice parameters

We present a systematic study of the interplay between lattice parameters and the energy of the optical phonons as well as the antiferromagnetic coupling strength, $J$, in the high-$T_{\text{c}}$ superconducting cuprate $R$Ba$_2$Cu$_3$O$_{6+δ}$ (\mbox{R-123}, $R =$ Y, Dy, Gd, Sm, Nd) with hole-doping $p$ ($0.00<p \lesssim 0.04$). The energy of the $B_{1g}$-mode at $ν_{B1g}\approx~335$ cm$^{-1}$ has been found to relate systematically to the inverse of the lattice parameter $a$. Our results confirm the temperature dependent phonon splitting for Nd-123 at low doping, which has been reported for optimally-doped Nd-123. Surprisingly, $J$ is independent of $a$ for the first four $R$ families, and a general consistency between $T_{\text{c}}^{\text{max}}$ and $J$, as suggested in a previous investigation, could not be confirmed.

cond-mat.str-el↗

arXiv2018

Lattice-Mediated Magnetic Order Melting in TbMnO3

Recent ultrafast magnetic-sensitive measurements [Phys. Rev. B 92, 184429 (2015) and Phys. Rev. B 96, 184414 (2017)] have revealed a delayed melting of the long-range cycloid spin-order in TbMnO$_3$ following photoexcitation across the fundamental Mott-Hubbard gap. The microscopic mechanism behind this slow transfer of energy from the photoexcited carriers to the spin degrees of freedom is still elusive and not understood. Here, we address this problem by combining spectroscopic ellipsometry, ultrafast broadband optical spectroscopy and ab initio calculations. Upon photoexcitation, we observe the emergence of a complex collective response, which is due to high-energy coherent optical phonons coupled to the out-of-equilibrium charge density. This response precedes the magnetic order melting and is interpreted as the fingerprint of the formation of anti-Jahn Teller polarons. We propose that the charge localization in a long-lived self-trapped state hinders the emission of magnons and other spin-flip mechanisms, causing the energy transfer from the charge to the spin system to be mediated by the reorganization of the lattice. Furthermore, we provide evidence for the coherent excitation of a phonon mode associated with the ferroelectric phase transition.

cond-mat.str-el↗

arXiv2017

Strongly bound excitons in anatase TiO2 single crystals and nanoparticles

Anatase TiO$_2$ is among the most studied materials for light-energy conversion applications, but the nature of its fundamental charge excitations is still unknown. Yet it is crucial to establish whether light absorption creates uncorrelated electron-hole pairs or bound excitons and, in the latter case, to determine their character. Here, by combining steady-state angle-resolved photoemission spectroscopy and spectroscopic ellipsometry with state-of-the-art ab initio calculations, we demonstrate that the direct optical gap of single crystals is dominated by a strongly bound exciton rising over the continuum of indirect interband transitions. This exciton possesses an intermediate character between the Wannier-Mott and Frenkel regimes and displays a peculiar two-dimensional wavefunction in the three-dimensional lattice. The nature of the higher-energy excitations is also identified. The universal validity of our results is confirmed up to room temperature by observing the same elementary excitations in defect-rich samples (doped single crystals and nanoparticles) via ultrafast two-dimensional deep-ultraviolet spectroscopy.

cond-mat.mtrl-sci↗

arXiv2016

Clocking the Onset of Bilayer Coherence in a High-$\mathrm{T_C}$ Cuprate

In cuprates, a precursor state of superconductivity is speculated to exist above the critical temperature $\mathrm{T_C}$. Here we show via a combination of far-infrared ellipsometry and ultrafast broadband optical spectroscopy that signatures of such a state can be obtained via three independent observables in an underdoped sample of NdBa$_2$Cu$_3$O$_{6+δ}$. The pseudogap correlations were disentangled from the response of laser-broken pairs by clocking their characteristic time-scales. The onset of a superconducting precursor state was found at a temperature $\mathrm{T_{ONS}}$ $>$ $\mathrm{T_C}$, consistent with the temperature scale identified via static optical spectroscopy. Furthermore, the temperature evolution of the coherent vibration of the Ba ion, strongly renormalized by the onset of superconductivity, revealed a pronounced anomaly at the same temperature $\mathrm{T_{ONS}}$. The microscopic nature of such a precursor state is discussed in terms of pre-formed pairs and enhanced bilayer coherence.

cond-mat.supr-con↗

arXiv2015

Terahertz ellipsometry study of the soft mode behavior in ultrathin SrTiO3 films

We present a combined study with conventional far-infrared and time-domain terahertz ellipsometry of the temperature dependent optical response of SrTiO3 thin films (85 and 8.5 nm) that are grown by pulsed-laser deposition on LSAT substrates. We demonstrate that terahertz ellipsometry is very sensitive to the optical response of these thin films, in particular, to the soft mode of SrTiO3. We show that for the 85 nm film the eigenfrequency of the soft mode is strongly reduced by annealing at 1200 C, whereas for the 8.5 nm film it is hardy affected. For the latter, after annealing the mode remains at 125 cm-1 at 300 K and exhibits only a weak softening to about 90 cm-1 at 10 K. This suggests that this ultrathin film undergoes hardly any relaxation of the compressive strain due to the LSAT substrate.

cond-mat.mtrl-sci↗