Two-dimensional (2D) materials are easily fabricated when their bulk form has a layered structure. The monolayer form in layered transition-metal dichalcogenides is typically the same as a single layer of the bulk material. However, ${\mathrm{PdSe}}_2$ presents a puzzle. Its monolayer form has been theoretically shown to be stable, but there have been no reports that monolayer ${\mathrm{PdSe}}_2$ has been fabricated. Here, combining atomic-scale imaging in a scanning transmission electron microscope and density functional theory, we demonstrate that the preferred monolayer form of this material amounts to a melding of two bulk monolayers accompanied by the emission of Se atoms so that the resulting stoichiometry is ${\mathrm{Pd}}_2{\mathrm{Se}}_3$. We further verify the interlayer melding mechanism by creating Se vacancies in situ in the layered ${\mathrm{PdSe}}_2$ matrix using electron irradiation. The discovery that strong interlayer interactions can be induced by defects and lead to the formation of new 2D materials opens a new venue for the exploration of defect engineering and novel 2D structures.

We study the effects of local perturbations on the dynamics of disordered fermionic systems in order to characterize time irreversibility. We focus on three different systems: the noninteracting Anderson and Aubry-André-Harper (AAH) models and the interacting spinless disordered $t\text{−}V$ chain. First, we consider the effect on the full many-body wave functions by measuring the Loschmidt echo (LE). We show that in the extended or ergodic phase the LE decays exponentially fast with time, while in the localized phase the decay is algebraic. We demonstrate that the exponent of the decay of the LE in the localized phase diverges proportionally to the single-particle localization length as we approach the metal-insulator transition in the AAH model. Second, we probe different phases of disordered systems by studying the time expectation value of local observables evolved with two Hamiltonians that differ by a spatially local perturbation. Remarkably, we find that many-body localized systems could lose memory of the initial state in the long-time limit, in contrast to the noninteracting localized phase where some memory is always preserved.

We report evidence of a nonadiabatic Kohn anomaly in boron-doped diamond, using a joint theoretical and experimental analysis of the phonon dispersion relations. We demonstrate that standard calculations of phonons using density-functional perturbation theory are unable to reproduce the dispersion relations of the high-energy phonons measured by high-resolution inelastic x-ray scattering. On the contrary, by taking into account nonadiabatic effects within a many-body field-theoretic framework, we obtain excellent agreement with our experimental data. This result indicates a breakdown of the Born-Oppenheimer approximation in the phonon dispersion relations of boron-doped diamond.

Using the sensitivity of optical second harmonic generation to currents, we demonstrate the generation of 250-fs long spin current pulses in $\mathrm{Fe}/\mathrm{Au}/\mathrm{Fe}/\mathrm{MgO}(001)$ spin valves. The temporal profile of these pulses indicates ballistic transport of hot electrons across a sub-100 nm Au layer. The pulse duration is primarily determined by the thermalization time of laser-excited hot carriers in Fe. Considering the calculated spin-dependent $\mathrm{Fe}/\mathrm{Au}$ interface transmittance we conclude that a nonthermal spin-dependent Seebeck effect is responsible for the generation of ultrashort spin current pulses. The demonstrated rotation of spin polarization of hot electrons upon interaction with noncollinear magnetization at $\mathrm{Au}/\mathrm{Fe}$ interfaces holds high potential for future spintronic devices.

We have utilized a plethora of transient and steady state optical and magneto-optical spectroscopies in a broad spectral range (0.25–2.5 eV) for elucidating the primary and long-lived photoexcitations in a low band-gap $\pi$-conjugated donor-acceptor (DA) copolymer used for efficient photovoltaic solar cells. We show that both singlet excitons (SE) and intrachain triplet-triplet (TT) pairs are photogenerated in the DA-copolymer chains. From the picosecond transient magnetic field response of these species we conclude that the SE and TT spin states are coupled. The TT decomposition into two intrachain geminate triplet excitons maintains spin coherence and thus their spin entanglement lasts into the microsecond time domain.

We demonstrate a new method for projective single-shot measurement of two electron spin states (singlet versus triplet) in an array of gate-defined lateral quantum dots in GaAs. The measurement has very high fidelity and is robust with respect to electric and magnetic fluctuations in the environment. It exploits a long-lived metastable charge state, which increases both the contrast and the duration of the charge signal distinguishing the two measurement outcomes. This method allows us to evaluate the charge measurement error and the spin-to-charge conversion error separately. We specify conditions under which this method can be used, and project its general applicability to scalable quantum dot arrays in GaAs or silicon.

We introduce a method, based on a novel thermodynamic integration scheme, to extract the Flory-Huggins $\chi$ parameter as small as ${10}^{-3}kT$ for polymer blends from molecular dynamics (MD) simulations. We obtain $\chi$ for the archetypical coarse-grained model of nonpolar polymer blends: flexible bead-spring chains with different Lennard-Jones interactions between $A$ and $B$ monomers. Using these $\chi$ values and a lattice version of self-consistent field theory (SCFT), we predict the shape of planar interfaces for phase-separated binary blends. Our SCFT results agree with MD simulations, validating both the predicted $\chi$ values and our thermodynamic integration method. Combined with atomistic simulations, our method can be applied to predict $\chi$ for new polymers from their chemical structures.

We study the response of a film of colloidal spherocylinders to compression by combining pressure-area isotherm measurements, microscopy, and computer simulations. We find that the behavior of the film depends strongly on the geometry of the particles. For a small aspect ratio, a uniform monolayer forms and then buckles. For a higher aspect ratio, particles flip to orient perpendicular to the interface; we show that flipping occurs in locations where the nematic ordering is low. Our experiments and simulations further demonstrate that the longest particles rearrange to self-assemble a colloidal bilayer, which is stable due to the unique geometry of spherocylinders at an interface.

We present a numerical study of dense colloidal suspensions in a pressure-driven microchannel flow in two dimensions. The colloids are modeled as elastic and frictional spheres suspended in a Newtonian fluid, which we simulate using the method of multiparticle collision dynamics. The model reproduces periodic velocity and density pulse trains, traveling upstream in the microchannel, which are found in experiments conducted by Isa et al. [Phys. Rev. Lett. 102, 058302 (2009)]. We show that colloid-wall friction and the resultant force chains are crucial for the formation of these pulses. With an increasing colloid density, first solitary jams occur, which become periodic pulse trains at intermediate densities and unstable solitary pulses at high densities. We formulate a phenomenological continuum model and show how these spatiotemporal flow and density profiles can be understood as homoclinic and periodic orbits in traveling-wave equations.

Directly in the thermodynamic limit, we show how to combine local imaginary and real-time evolution of tensor networks to efficiently and accurately find the nonequilibrium steady states (NESSs) of one-dimensional dissipative quantum lattices governed by a local Lindblad master equation. The imaginary time evolution first bypasses any highly correlated portions of the real-time evolution trajectory by directly converging to the weakly correlated subspace of the NESS, after which, real-time evolution completes the convergence to the NESS with high accuracy. We demonstrate the power of the method with the dissipative transverse field quantum Ising chain. We show that a crossover of an order parameter shown to be smooth in previous finite-size studies remains smooth in the thermodynamic limit.

Collective spins of large atomic samples trapped inside optical resonators can carry quantum information that can be processed in a way similar to quantum computation with continuous variables. It is shown here that by combining the resonators in multipath interferometers one can realize coupling between different samples, and that polynomial Hamiltonians can be constructed by repeated spin rotations and twisting induced by dispersive interaction of the atoms with light. Application can be expected in the efficient simulation of quantum systems.

We consider ground states of quantum spin chains with symmetry-protected topological (SPT) order as resources for measurement-based quantum computation (MBQC). We show that, for a wide range of SPT phases, the computational power of ground states is uniform throughout each phase. This computational power, defined as the Lie group of executable gates in MBQC, is determined by the same algebraic information that labels the SPT phase itself. We prove that these Lie groups always contain a full set of single-qubit gates, thereby affirming the long-standing conjecture that general SPT phases can serve as computationally useful phases of matter.

Nonequilibrium time evolution in isolated many-body quantum systems generally results in thermalization. However, the relaxation process can be very slow, and quasistationary nonthermal plateaux are often observed at intermediate times. The paradigmatic example is a quantum quench in an integrable model with weak integrability breaking; for a long time, the state cannot escape the constraints imposed by the approximate integrability. We unveil a new mechanism of prethermalization, based on the presence of a symmetry of the prequench Hamiltonian, which is spontaneously broken at zero temperature and is explicitly broken by the postquench Hamiltonian. The typical time scale of the phenomenon is proportional to the thermal correlation length of the initial state, which diverges as the temperature is lowered. We show that the prethermal quasistationary state can be approximated by a mixed state that violates cluster decomposition property. We consider two examples: the transverse-field Ising chain, where the full-time evolution is computed analytically, and the (nonintegrable) anisotropic next-nearest-neighbor Ising model, which is investigated numerically.

Strong nonlinearity at the single photon level represents a crucial enabling tool for optical quantum technologies. Here we report on experimental implementation of a strong Kerr nonlinearity by measurement-induced quantum operations on weak quantum states of light. Our scheme coherently combines two sequences of single photon addition and subtraction to induce a nonlinear phase shift at the single photon level. We probe the induced nonlinearity with weak coherent states and characterize the output non-Gaussian states with quantum state tomography. The strong nonlinearity is clearly witnessed as a change of sign of specific off-diagonal density matrix elements in the Fock basis.

We investigate the near-field interaction between an isolated free-base phthalocyanine molecule and a plasmon localized in the gap between an NaCl-covered Ag(111) surface and the tip apex of a scanning tunneling microscope. When the tip is located in the close proximity of the molecule, asymmetric dips emerge in the broad luminescence spectrum of the plasmon generated by the tunneling current. The origin of the dips is explained by energy transfer between the plasmon and molecular excitons and a quantum mechanical interference effect, where molecular vibrations provide additional degrees of freedom in the dynamic process.

This Letter reports the successful use of feedback from a spin polarization measurement to the revolution frequency of a $0.97\mathrm{GeV}/c$ bunched and polarized deuteron beam in the Cooler Synchrotron (COSY) storage ring in order to control both the precession rate ($\approx 121\mathrm{kHz}$) and the phase of the horizontal polarization component. Real time synchronization with a radio frequency (rf) solenoid made possible the rotation of the polarization out of the horizontal plane, yielding a demonstration of the feedback method to manipulate the polarization. In particular, the rotation rate shows a sinusoidal function of the horizontal polarization phase (relative to the rf solenoid), which was controlled to within a 1 standard deviation range of $\sigma =0.21\mathrm{rad}$. The minimum possible adjustment was 3.7 mHz out of a revolution frequency of 753 kHz, which changes the precession rate by $26\mathrm{mrad}/\mathrm{s}$. Such a capability meets a requirement for the use of storage rings to look for an intrinsic electric dipole moment of charged particles.

It has been predicted for over a decade that low-recycling plasma-facing components in fusion devices would allow high edge temperatures and flat or nearly flat temperature profiles. In recent experiments with lithium wall coatings in the Lithium Tokamak Experiment (LTX), a hot edge ($>200\mathrm{eV}$) and flat electron temperature profiles have been measured following the termination of external fueling. Reduced recycling was demonstrated by retention of $\sim 60\%$ of the injected hydrogen in the walls following the discharge. Electron energy confinement followed typical Ohmic confinement scaling during fueling, but did not decrease with density after fueling terminated, ultimately exceeding the scaling by $\sim 200\%$. Achievement of the low-recycling, hot edge regime has been an important goal of LTX and lithium plasma-facing component research in general, as it has potentially significant implications for the operation, design, and cost of fusion devices.

We develop a computationally efficient scheme to determine the potentials of zero charge (PZC) of metal-water interfaces with respect to the standard hydrogen electrode. We calculate the PZC of Pt(111), Au(111), Pd(111) and Ag(111) at a good accuracy using this scheme. Moreover, we find that the interface dipole potentials are almost entirely caused by charge transfer from water to the surfaces, the magnitude of which depends on the bonding strength between water and the metals, while water orientation hardly contributes at the PZC conditions.

We investigate the magnetic dynamics in the spinel-type vanadium oxide ${\mathrm{MnV}}_2{\mathrm{O}}_4$. Inelastic neutron scattering around 10 meV and a Heisenberg model analysis have revealed that ${\mathrm{V}}^{3+}$ spin-wave modes exist at a lower-energy region than previously reported. The scattering around 20 meV cannot be reproduced with the spin-wave analysis. We propose that this scattering could originate from the spin-orbital coupled excitation. This scattering is most likely attributable to ${\mathrm{V}}^{3+}$ spin-wave modes, entangled with the orbital hybridization between $t_{2g}$ orbitals.