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Spin and orbital angular momenta are two intrinsic properties of an electron and are responsible for the physics of a solid. How the spin and orbital evolve with respect to each other on several hundred femtoseconds is largely unknown, but it is at the center of laser-induced ultrafast demagnetization. In this paper, we introduce a concept of the spin-orbital correlation diagram, where spin angular momentum is plotted against orbital angular momentum, much like the position-velocity phase diagram in classical mechanics. We use four sets of highly accurate time-resolved x-ray magnetic circular dichroism (TR-XMCD) data to construct four correlation diagrams for iron and cobalt. To our surprise, a pattern emerges. The trace on the correlation diagram for iron is an arc, and at the end of demagnetization, it has a pronounced cusp. The correlation diagram for cobalt is different and appears more linear, but with kinks. We carry out first-principles calculations with two different methods: time-dependent density functional theory (TDDFT) and time-dependent Liouville density functional theory (TDLDFT). These two methods agree that the experimental findings for both Fe and Co are not due t experimental errors. It is the spin-orbit coupling that correlates the spin dynamics to the orbital dynamics.Microscopically, Fe and Co have different orbital occupations, which leads to distinctive correlation diagrams. We believe that this correlation diagram presents a useful tool to better understand spin and orbital dynamics on an ultrafast time scale. A brief discussion on the magnetic anisotropy energy is also provided., Comment: 19 pages, four figures. Accepted for publication in Journal of Physical Chemistry C

Here we carry out a first-principles time-dependent calculation to investigate how fast electrons actually move under laser excitation and how large the electron transport affects demagnetization on the shortest time scale. To take into account the transport effect, we implement the intraband transition in our theory. In the bulk fcc Ni, we find the effect of the spin transport on the demagnetization is extremely small, no more than 1\%. The collective electron velocity in Ni is 0.4 $\rm \AA/fs$, much smaller than the Fermi velocity, and the collective displacement is no more than 0.1 $\rm \AA$. But this does not mean that electrons do not travel fast; instead we find that electron velocities at two opposite crystal momenta cancel each other. We follow the $\Gamma$-X line and find a huge dispersion in the velocities in the crystal momentum space. In the Fe/W(110) thin film, the overall demagnetization is larger than Ni, and the Fermi velocity is higher than Ni. However, the effect of the spin transport is still small in the Fe/W(110) thin film. Based on our numerical results and existing experimental findings, we propose a different mechanism that can explain two latest experimental results. Our finding sheds new light on the effect of ballistic transport on demagnetization., Comment: 32 pages, 6 figures, (accepted for publication in Journal of Physics: Condensed Matter (2018))

Intra-atomic exchange couplings (IEC) between $5d6s$ and $4f$ electrons are ubiquitous in rare-earth metals and play a critical role in spin dynamics. However, detecting them in real time domain has been difficult. Here we show the direct evidence of IEC between $5d6s$ and $4f$ electrons in gadolinium. Upon femtosecond laser excitation, $5d6s$ electrons are directly excited, their majority bands shift toward the Fermi level while their minority bands do the opposite. For the first time, our first-principles minority shift now agrees with the experiment quantitatively. Excited $5d6s$ electrons lower the exchange potential barrier for $4f$ electrons, so the $4f$ states are also shifted in energy, a prediction that can be tested experimentally. Although a significant number of $5d6s$ electrons, some several eV below the Fermi level, are excited out of the Fermi sea, there is no change in the $4f$ states, a clear manifestation of intra-atomic exchange coupling. Based on our results, we propose that the demagnetization time of a material be inversely proportional to the density of states at the Fermi level and the excited, not the whole, spin moment. This can be tested experimentally., Comment: 18 pages, four figures, one supplementary material file

Elastic and inelastic neutron scattering studies have been carried out on the pyrochlore magnet Ho2Ti2O7. Measurements in zero applied magnetic field show that the disordered spin ice ground state of Ho2Ti2O7 is characterized by a pattern of rectangular diffuse elastic scattering within the [HHL] plane of reciprocal space, which closely resembles the zone boundary scattering seen in its sister compound Dy2Ti2O7. Well-defined peaks in the zone boundary scattering develop only within the spin ice ground state below ~ 2 K. In contrast, the overall diffuse scattering pattern evolves on a much higher temperature scale of ~ 17 K. The diffuse scattering at small wavevectors below [001] is found to vanish on going to Q=0, an explicit signature of expectations for dipolar spin ice. Very high energy-resolution inelastic measurements reveal that the spin ice ground state below ~ 2 K is also characterized by a transition from dynamic to static spin correlations on the time scale of 10^{-9} seconds. Measurements in a magnetic field applied along the [1${\bar1}$0] direction in zero-field cooled conditions show that the system can be broken up into orthogonal sets of polarized alpha chains along [1${\bar1}$0] and quasi-one-dimensional beta chains along [110]. Three dimensional correlations between beta chains are shown to be very sensitive to the precise alignment of the [1${\bar1}$0] externally applied magnetic field., Comment: 11 pages, 10 figures. Submitted for publication

We present results from MiniMax (Fermilab T-864), a small test/experiment at the Tevatron designed to search for the production of disoriented chiral condensate (DCC) in $p - \bar p$ collisions at $\sqrt{s} = 1.8$ TeV in the forward direction, $\sim 3.4 < \eta < \sim 4.2$. Data, consisting of $1.3 \times 10^6$ events, are analyzed using the robust observables developed in an earlier paper. The results are consistent with generic, binomial-distribution partition of pions into charged and neutral species. Limits on DCC production in various models are presented., Comment: 24 pages, 9 figures. Minor clarifications have been added

We report on the progress of a search for disoriented chiral condensates (DCCs) in the far forward region at sqrt(s)=1.8 TeV. MiniMax is a small collider experiment situated at the C0 interaction region of the Tevatron and has been designed to measure the ratio of charged to neutral pions produced at eta near 4.1. The distribution of this ratio is expected to be very different for the generic binomial and DCC particle production models. We present a method used for the search using the factorial moments of particle generating functions, which can be extracted directly from the data. A preliminary comparison of robust ratios of measured values and those expected from the different models is also presented., Comment: Latex, 2 figures, 3 pages, To appear in the proceedings of DPF 96.