Here we present an evaluation of the binding affinity prediction accuracy of the free energy calculation method FEP+ on internal active drug discovery projects and on a large new public benchmark set. File list (3) download file view on ChemRxiv manuscript.pdf (4.23 MiB) download file view on ChemRxiv supplementary.pdf (0.92 MiB) download file view on ChemRxiv tables.zip (5.99 KiB)

1 Solids with strong electron correlations generally develop exotic phases of electron matter at low temperatures [1,2,3,4,5]. Among such systems, the heavyfermion semi-metal URu 2 Si 2 presents an enigmatic transition at T o = 17.5 K to a 'hidden order' state whose order parameter remains unknown after 23 years of intense research [6,7]. Various experiments point to the reconstruction and partial gapping of the Fermi surface when the hidden-order establishes [8,9,10,11,12,13,14,15,16,17,18]. However, up to now, the question of how this transition affects the electronic spectrum at the Fermi surface has not been directly addressed by a spectroscopic probe. Here we show, using angleresolved photoemission spectroscopy, that a band of heavy quasi-particles drops below the Fermi level upon the transition to the hidden-order state. Our data provide the first direct evidence of a large reorganization of the electronic structure across the Fermi surface of URu 2 Si 2 occurring during this transition, and unveil a new kind of Fermi-surface instability in correlated electron systems.Earlier angle-resolved photoemission spectroscopy (ARPES) experiments mapped the basic band structure of URu 2 Si 2 in the paramagnetic state (above T o ), establishing the existence of hole-pockets at the Γ, Z and X points of the Brillouin zone [19,20,21]. These experiments revealed strong disagreements with the calculations for the electronic structure and Fermi surface of URu 2 Si 2 . It was speculated that this was due to the presence of narrow features from the U-5f states, not taken into account by the calculations, and difficult to characterize experimentally with the resolutions available at the time [21]. To date, no reports exist of high-resolution ARPES experiments below or across T o . The pressing question is to determine experimentally the electronic structure near the Fermi level (E F ), inlcuding the heavy 5f states, above and below T o . Figure 1 summarizes our findings for the temperature evolution of the electronic structure near E F . Figure 1a shows the angle-integrated spectra of electrons with k , the momentum component parallel to the sample surface, along the (110) direction at two temperatures across the transition. At T = 26 K, the only apparent feature is a surface state (SS) at binding energies E B < −35 meV, observed at all the investigated temperatures (see Supple-mentary Material). In contrast, at 13 K a narrow peak at E B ≈ −7 meV appears, signaling the presence of a quasi-particle (QP) band. The temperature dependence of this QP band was systematically studied, and is shown in Figures 1b-d. In these figures we normalized 2 the spectra by the Fermi-Dirac distribution, following a well established procedure [22], to reveal the thermally occupied part of the spectral function up to energies ∼ 5k B T above E F .The angle-integrated data of Fig. 1b shows that at 26 K the QP band lies at E B ≈ 5 meV, at 18 K ≈ T o it appears right at E F , and below T o the band shifts to energies below E F . At 10 K the QP peak is ...

A comparison of high-resolution, angle-resolved photoemission spectroscopy (ARPES) data with ab initio band-structure calculations by density functional theory for the anticipated Kondo insulator FeSi shows that the experimental dispersions can quantitatively be described by an itinerant behavior provided that an appropriate self-energy correction is included, whose real part describes the band renormalization due to interactions of the Fe 3d electrons. The imaginary part of the self-energy, on the other hand, determines the linewidth of the quasiparticle peaks in the ARPES data. We use a model self-energy which consistently describes both the renormalized single-particle dispersion and the energy-dependent linewidth of the Fe 3d bands. These results are clear evidence that FeSi is an itinerant semiconductor whose properties can be explained without a local Kondo-like interaction.

A quantum phase transition in a heavy-fermion compound may destroy the Fermi-liquid ground state. However, the conditions for this breakdown have remained obscure. We report the first direct investigation of heavy quasiparticle formation and breakdown in the canonical system CeCu(6-x)Au(x) by ultraviolet photoemission spectroscopy at elevated temperatures without the complications of lattice coherence. Surprisingly, the single-ion Kondo energy scale T(K) exhibits an abrupt step near the quantum critical Au concentration of x(c) = 0.1. We show theoretically that this step is expected from a highly nonlinear renormalization of the local spin coupling at each Ce site, induced by spin fluctuations on neighboring sites. It provides a general high-temperature indicator for heavy-fermion quasiparticle breakdown at a quantum phase transition.

We report on the results of a high-resolution angle-resolved photoemission study on the ordered surface alloy CePt(5). The temperature dependence of the spectra show the formation of the coherent low-energy heavy-fermion band near the Fermi level. These experimental data are supported by a multiband model calculation in the framework of the dynamical mean-field theory.