In this article we describe the OpenMolcas environment and invite the computational chemistry community to collaborate. The open-source project already includes a large number of new developments realized during the transition from the commercial MOLCAS product to the open-source platform. The paper initially describes the technical details of the new software development platform. This is followed by brief presentations of many new methods, implementations, and features of the OpenMolcas program suite. These developments include novel wave function methods such as stochastic complete active space self-consistent field, density matrix renormalization group (DMRG) methods, and hybrid multiconfigurational

Reliable quantum chemical methods for the description of molecules with denselying frontier orbitals are needed in the context of many chemical compounds and reactions. Here, we review developments that led to our new computational toolbox which implements the quantum chemical density matrix renormalization group in a second-generation algorithm. We present an overview of the different components of this toolbox.

A novel fast electron beam emitting along the surface of a target irradiated by intense laser pulses is observed. The beam is found to appear only when the plasma density scale length is small. Numerical simulations reveal that the electron beam is formed due to the confinement of the surface quasistatic electromagnetic fields. The results are of interest for potential applications of fast electron beams and deep understanding of the cone-target physics in the fast ignition related experiments.

We present a matrix-product state (MPS)-based quadratically convergent densitymatrix renormalization group self-consistent-field (DMRG-SCF) approach. Following a proposal by Werner and Knowles (J. Chem. Phys. 82, 5053, (1985)), our DMRG-SCF algorithm is based on a direct minimization of an energy expression which is correct to second-order with respect to changes in the molecular orbital basis. We exploit a simultaneous optimization of the MPS wave function and molecular orbitals in order to achieve quadratic convergence. In contrast to previously reported (augmented Hessian) Newton-Raphson and super-configuration-interaction algorithms for DMRG-SCF, energy convergence beyond a quadratic scaling is possible in our ansatz.Discarding the set of redundant active-active orbital rotations, the DMRG-SCF energy converges typically within two to four cycles of the self-consistent procedure.