Abstract Dynamical control of the nonlinear optical properties of solids – with light itself – will be essential for future ultrafast photonic technologies. Previously, methods to modulate nonlinear processes including second-harmonic generation (SHG) have relied primarily on non-resonant light-matter interaction or photo-generation of hot electrons in nanoscale materials. However, these approaches are typically constrained by limited interaction lengths and the initial frequency conversion is relatively weak under equilibrium conditions. Here, a ~ 30% modulation of efficient phase-matched SHG in bulk beta-barium borate (β-BaB2O4) is achieved through transient lattice deformation by intense terahertz (THz) pulses that are tuned to resonance with an infrared-active phonon mode. The effect originates from modification of the index of refraction ellipsoid and the corresponding nonlinear phase-matching conditions, rather than from direct modulation of the nonlinear susceptibility through THz-mediated $${\chi }^{(3)}$$ χ ( 3 ) processes. This mechanism, of resonant selective lattice excitation, points toward novel THz-control schemes to tune the nonlinear optical response in materials.

Visualizing the spatial profile of light beams is essential for evaluating irradiance, characterizing beam quality, and achieving precise alignment. In the optical spectral range, this is readily performed using silicon-based CCD and CMOS cameras. In the terahertz (THz) range, however, it typically requires specialized detectors with prohibitive costs. Here, we show that an infrared (IR) camera can be used outside of its labeled specifications to achieve similar performance as a dedicated microbolometric THz camera, at under 1

Each cycle of a quantum computation requires a quantum state initialisation. For semiconductor-based quantum platforms, initialisation is typically performed via slow microwave processes and usually requires cooling to temperatures where only the lowest quantum level is occupied. In silicon, boron atoms are the most common impurities. They bind holes in orbitals including an effective spin-3/2 ground state as well as excited states analogous to the Rydberg series for hydrogen. Here we show that initialisation temperature demands may be relaxed and speeds increased over a thousand-fold by importing, from atomic physics, the procedure of optical pumping via excited orbital states to preferentially occupy a target ground state spin. Spin relaxation within the orbital ground state of unstrained silicon is too fast to measure for conventional pulsed microwave technology, except at temperatures below 2 K, implying a need not only for fast state preparation but also fast state readout. Circularly polarised ~10 THz photon pulses from a free electron laser meet both needs at temperatures above 3 K: a 9 ps pulse enhances the population of one spin eigenstate for the "1s"-like ground state orbital, and the second interrogates this imbalance in spin population. Using parameters given by our data, we calculate that it should be possible to initialise 99% of spins for boron in strained silicon within 250 ps at 3 K. The speedup of both state preparation and measurement gained for THz rather than microwave photons should be explored for the many other solid state quantum systems hosting THz excitations potentially useful as intermediate states.

Rydberg states of atoms in vacuum are now well recognized as a resource for quantum technologies. Donors in semiconductors also display analogous states, which have been proposed for similar applications. While they benefit from permanent locations in their host crystals, electron-lattice coupling leads to much shorter excited-state lifetimes than for neutral atoms in vacuum. Here we provide a quantitative description of donor-phonon kinetics, creating a basis for engineering donor systems in realistic material stacks for quantum devices. Our theory incorporates both form factors for the Rydberg states, which given their large extents in real space provide strong selectivity in momentum space, and tabulated deformation potentials for all six phonon branches throughout the Brillouin zone. By confronting this framework with carefully controlled time-resolved free electron laser measurements, we show that the widely quoted position of the silicon conduction band minimum, k_0, is inconsistent with observed donor relaxation rates and that quantitative agreement is obtained for a value further from the X-point than commonly assumed. This stringent experiment-theory comparison establishes donor relaxation as a precision metrology for conduction band parameters and scattering processes in silicon, with consequences spanning from quantum devices to classical electronics.

Because it is easily switched from insulator to metal either via chemical doping or electrical gating, silicon is at the core of modern information technology and remains a candidate platform for quantum computing. The metal-to-insulator transition in this material has therefore been one of the most studied phenomena in condensed matter physics, and has been revisited with considerable profit each time a new fabrication technology has been introduced. Here we take advantage of recent advances in creating ultra-thin layers of Bohr-atom-like dopants to realize the two-dimensional disordered Hubbard model at half-filling and its metal-to-insulator transition (MIT) as a function of mean distance between atoms. We use gas-phase dosing of dopant precursor molecules on silicon to create arsenic and phosphorus δ-layers as thin as 0.4 nm and as dilute as 10^13 cm^-2. On approaching the insulating state, the conventional weak localization effects, prevalent at high dopant densities and due to orbital motion of the electrons in the plane, become dominated by electron-electron interaction contributions which obey a paramagnetic Zeeman scaling law. The latter make a negative contribution to the conductance, and thus cannot be interpreted in terms of an emergent Kondo regime near the MIT.

We report the generation of extremely narrowband, micro-Joule-level, frequency-tunable THz pulses between 3 and 4 THz in organic DSTMS, without applying any spectral filtering techniques (e.g., bandpass filters). Using difference frequency generation with > 10 ps duration linearly chirped near-infrared (NIR) pulses, THz pulses with 300 nJ output energy and an extremely narrow spectrum of 83 GHz at 3.87 THz were achieved with a relative bandwidth of 2

Quantum sensors and qubits are usually two-level systems (TLS), the quantum analogues of classical bits assuming binary values 0 or 1. They are useful to the extent to which superpositions of 0 and 1 persist despite a noisy environment. The standard prescription to avoid decoherence of solid-state qubits is their isolation by means of extreme dilution in ultrapure materials. We demonstrate a different strategy using the rare-earth insulator LiY 1− x Tb x F 4 ( x = 0.001) which realizes a dense random network of TLS. Some TLS belong to strongly interacting Tb 3+ pairs whose quantum states, thanks to localization effects, form highly coherent qubits with 100-fold longer coherence times than single ions. Our understanding of the underlying decoherence mechanisms—and of their suppression—suggests that coherence in networks of dipolar coupled TLS can be enhanced rather than reduced by the interactions.

Fabrication of semiconductor heterostructures is now so precise that metrology has become a key challenge for progress in science and applications. It is now relatively straightforward to characterize classic III-V and group IV heterostructures consisting of slabs of different semiconductor alloys with thicknesses of ∼5 nm and greater using sophisticated tools such as diffraction, high energy X-ray photoemission spectroscopy, and secondary ion mass spectrometry. However, profiling thin layers with nm or sub-nm thickness, e.g. atomically thin dopant layers (), of impurities required for modulation doping and spin-based quantum and classical information technologies is more challenging. Here, we present theory and experiment showing how resonant-contrast reflectometry meets this challenge. The technique takes advantage of the change in the scattering factor of atoms as their core level resonances are scanned by varying the energy. We demonstrate the capability of the resulting element-selective, non-destructive profilometry for single arsenic δ-layers within silicon, and show that the sub-nm electronic thickness of the corresponds to sub-nm chemical thickness. In combination with X-ray fluorescence imaging, this enables non-destructive three-dimensional characterization of nano-structured quantum devices. Due to the strong resonances at soft X-ray wavelengths, the technique is also ideally suited to characterize layered quantum materials, such as cuprates or the topical infinite-layer nickelates.

Abstract The progress of miniaturization in integrated electronics has led to atomic and nanometer‐sized dopant devices in silicon. Such structures can be fabricated routinely by hydrogen resist lithography, using various dopants such as P and As. However, the ability to non‐destructively obtain atomic‐species‐specific images of the final structure, which would be an indispensable tool for building more complex nano‐scale devices, such as quantum co‐processors, remains an unresolved challenge. Here, X‐ray fluorescence is exploited to create an element‐specific image of As dopants in Si, with dopant densities in absolute units and a resolution limited by the beam focal size (here ≈1 µm), without affecting the device's low temperature electronic properties. The As densities provided by the X‐ray data are compared to those derived from Hall effect measurements as well as the standard non‐repeatable, scanning tunneling microscopy and secondary ion mass spectroscopy, techniques. Before and after the X‐ray experiments, we also measured the magneto‐conductance, which is dominated by weak localization, a quantum interference effect extremely sensitive to sample dimensions and disorder. Notwithstanding the 1.5 × 1010 Sv (1.5 × 1016 Rad cm−2) exposure of the device to X‐rays, all transport data are unchanged to within experimental errors, corresponding to upper bounds of 0.2 Angstroms for the radiation‐induced motion of the typical As atom and 3% for the loss of activated, carrier‐contributing dopants. With next generation synchrotron radiation sources and more advanced optics, the authors foresee that it will be possible to obtain X‐ray images of single dopant atoms within resolved radii of 5 nm.

The insulating rare-earth magnet LiY1-xHoxF4 has received great attention because a laboratory field applied perpendicular to its crystallographic c axis converts the low-energy electronic spin Hamiltonian into the (dilute) transverse field Ising model. The mapping between the real magnet and the transverse field Ising model is strongly dependent on the exact nature of the low-energy Hamiltonian for the material, which can be determined by spectroscopy in the dilute limit. The energies of the eigenstates are in the difficult terahertz (THz) regime, and here we use THz time domain and Fourier transform spectroscopy to directly measure the lowest crystal-field levels of LiY1-xHoxF4 in the dilute limit, including nuclear hyperfine substructure. The high resolution of our measurements allows us to observe the nonequidistantly spaced Ho (I = 7/2) hyperfine transitions originating from dipolar and quadrupolar hyperfine interactions. We provide refined crystal-field parameters and extract the dipolar and quadrupolar hyperfine constants A(J) = 0.027 03 +/- 0.000 03 cm(-1) (810.3 +/- 0.9 MHz) and B = 0.04 +/- 0.01 cm(-1)(1.2 +/- 0.3 GHz), respectively. Thereupon we determine all crystal-field energy levels and magnetic moments of the I-5(8) ground-state manifold, including the (nonlinear) hyperfine corrections. The latter improve the prediction precision by a factor of 60 compared to previous crystal-field parameters. Additionally, we establish the far-infrared, low-temperature refractive index of LiY1-xHoxF4.

We report a family of organometallic rare-earth complexes with the general formula (COT)M(Cpttt) (where (COT)2- = cyclooctatetraenide, (Cpttt)- = 1,2,4-tri(tert-butyl)cyclopentadienide, M = Y(iii), Nd(iii), Dy(iii) and Er(iii)). Similarly to the prototypical Er(iii) analog featuring pentamethylcyclopentadienyl ligand (Cp*)-, (COT)Er(Cpttt) behaves as a single-ion magnet. However, the introduction of the sterically demanding (Cpttt)- imposes geometric constraints that lead to a simplified magnetic relaxation behavior compared to the (Cp*)- containing complexes. Consequently, (COT)Er(Cpttt) can be viewed as a model representative of this organometallic single-ion magnet architecture. In addition, we demonstrate that the increased steric profile associated with the (Cpttt)- ligand permits preparation, structural characterization and interrogation of magnetic properties of the early-lanthanide complex, (COT)Nd(Cpttt). Such a mononuclear derivative could not be obtained when a (Cp*)- ligand was employed, a testament to larger ionic radius of this early lanthanide ion.

Quantum sensors and qubits are usually two-level systems (TLS), the quantum analogs of classical bits which assume binary values '0' or '1'. They are useful to the extent to which they can persist in quantum superpositions of '0' and '1' in real environments. However, such TLS are never alone in real materials and devices, and couplings to other degrees of freedom limit the lifetimes - called decoherence times - of the superposition states. Decoherence occurs via two major routes - excitation hopping and fluctuating electromagnetic fields. Common mitigation strategies are based on material improvements, exploitation of clock states which couple only to second rather than first order to external perturbations, and reduction of interactions via extreme dilution of pure materials made from isotopes selected to minimize noise from nuclear spins. We demonstrate that for a dense TLS network in a noisy nuclear spin bath, we can take advantage of interactions to pass from hopping to fluctuation dominance, increasing decoherence times by almost three orders of magnitude. In the dilute rare-earth insulator LiY1-xTbxF4, Tb ions realize TLS characterized by a 30GHz splitting and readily implemented clock states. Dipolar interactions lead to coherent, localized pairs of Tb ions, that decohere due to fluctuating quantum mechanical ring-exchange interaction, sensing the slow dynamics of the surrounding, nearly localized Tb spins. The hopping and fluctuation regimes are sharply distinguished by their Rabi oscillations and the invisible vs. strong effect of classic 'error correcting' microwave pulse sequences. Laying open the decoherence mechanisms at play in a dense, disordered and noisy network of interacting TLS, our work expands the search space for quantum sensors and qubits to include clusters in dense, disordered materials, that can be explored for localization effects.

Refractive indices of high resistivity Si and Ge were measured at temperatures between 4–296 K and at frequencies between 4.2–7.7 THz using a Fourier-transform spectrometer (FTS) in transmission mode. A phenomenological model of the temperature dependence of the refractive index is proposed.

Modern techniques for the investigation of correlated materials in the time domain combine selective excitation in the THz frequency range with selective probing of coupled structural, electronic and magnetic degrees of freedom using x-ray scattering techniques. Cryogenic sample temperatures are commonly required to prevent thermal occupation of the low energy modes and to access relevant material ground states. Here, we present a chamber optimized for high-field THz excitation and (resonant) x-ray diffraction at sample temperatures between 5 and 500 K. Directly connected to the beamline vacuum and featuring both a Beryllium window and an in-vacuum detector, the chamber covers the full (2–12.7) keV energy range of the femtosecond x-ray pulses available at the Bernina endstation of the SwissFEL free electron laser. Successful commissioning experiments made use of the energy tunability to selectively track the dynamics of the structural, magnetic and orbital order of Ca 2 RuO 4 and Tb 2 Ti 2 O 7 at the Ru (2.96 keV) and Tb (7.55 keV) L -edges, respectively. THz field amplitudes up to 1.12 MV cm −1 peak field were demonstrated and used to excite the samples at temperatures as low as 5 K.

A. Beckert, 2, ∗ R. I. Hermans, M. Grimm, J. R. Freeman, E. H. Linfield, A. G. Davies, M. Müller, H. Sigg, S. Gerber, G. Matmon, and G. Aeppli 2, 6 Laboratory for Micro and Nanotechnology, Paul Scherrer Institut, CH-5232 Villigen PSI, Switzerland Laboratory for Solid State Physics, ETH Zurich, CH-8093 Zurich, Switzerland London Centre for Nanotechnology, University College London, 17-19 Gordon Street, London WC1H 0AH, United Kingdom Condensed Matter Theory Group, LSM, NES, Paul Scherrer Institut, CH-5232 Villigen PSI, Switzerland School of Electronic and Electrical Engineering, University of Leeds, Woodhouse Lane, Leeds LS9 2JT, United Kingdom Institute of Physics, EPF Lausanne, CH-1015 Lausanne, Switzerland (Dated: December 18, 2020)

We use complementary optical spectroscopy methods to directly measure the lowest crystal-field energies of the rare-earth quantum magnet LiY$_{1-x}$Ho$_{x}$F$_{4}$, including their hyperfine splittings, with more than 10 times higher resolution than previous work. We are able to observe energy level splittings due to the $^6\mathrm{Li}$ and $^7\mathrm{Li}$ isotopes, as well as non-equidistantly spaced hyperfine transitions originating from dipolar and quadrupolar hyperfine interactions. We provide refined crystal field parameters and extract the dipolar and quadrupolar hyperfine constants ${A_J=0.02703\pm0.00003}$ $\textrm{cm}^{-1}$ and ${B= 0.04 \pm0.01}$ $\textrm{cm}^{-1}$, respectively. Thereupon we determine all crystal-field energy levels and magnetic moments of the $^5I_8$ ground state manifold, including the (non-linear) hyperfine corrections. The latter match the measurement-based estimates. The scale of the non-linear hyperfine corrections sets an upper bound for the inhomogeneous line widths that would still allow for unique addressing of a selected hyperfine transition. e.g. for quantum information applications. Additionally, we establish the far-infrared, low-temperature refractive index of LiY$_{1-x}$Ho$_{x}$F$_{4}$.

We present a metrological study of a new technique for measuring the complex refractive indices of solids in the THz regime. The technique is widely applicable thanks to requiring only frequency-domain spectroscopy, and is shown to be capable of high accuracy reconstruction of the complex refractive index (RI) spectrum. We quantify the sensitivity to experimental imperfections such as noise, showing that the new technique is more robust than previous methods. We demonstrate the extraction of RI of crystalline Si between 2-20 THz using this method, and comment on the capability to discriminate between absorption and scattering using only a power-transmission measurement.

The selective amplification of DNA in the polymerase chain reaction is used to exponentially increase the signal in molecular diagnostics for nucleic acids, but there are no analogous techniques for signal enhancement in clinical tests for proteins or cells. Instead, the signal from affinity-based measurements of these biomolecules depends linearly on the probe concentration. Substituting antibody-based probes tagged for fluorescent quantification with lasing detection probes would create a new platform for biomarker quantification based on optical rather than enzymatic amplification. Here, we construct a virus laser which bridges synthetic biology and laser physics, and demonstrate virus-lasing probes for biosensing. Our virus-lasing probes display an unprecedented > 10,000 times increase in signal from only a 50% increase in probe concentration, using fluorimeter-compatible optics, and can detect biomolecules at sub-100 fmol mL −1 concentrations.

Doping of silicon via phosphine exposures alternating with molecular beam epitaxy overgrowth is a path to Si:P substrates for conventional microelectronics and quantum information technologies. The technique also provides a new and well-controlled material for systematic studies of two-dimensional lattices with a half-filled band. We show here that for a dense (ns = 2.8 × 1014 cm−2 ) disordered two-dimensional array of P atoms, the full field angle-dependent magnetostransport is remarkably well described by classic weak localization theory with no corrections due to interaction effects. The two- to three-dimensional cross-over seen upon warming can also be interpreted using scaling concepts, developed for anistropic three-dimensional materials, which work remarkably except when the applied fields are nearly parallel to the conducting planes.

Data set for Two- to three-dimensional crossover in a dense electron liquid in silicon paper