Tunable far infrared laser spectrometers

The state of the art in far infrared (FIR) spectroscopy is reviewed. The development of tunable, coherent FIR radiation sources is discussed. Applications of tunable FIR laser spectrometers for measurement of rotational spectra and dipole moments of molecular ions and free radicals, vibration-rotation-tunneling (VRT) spectra of weakly bound complexes, and vibration-rotation spectra of linear carbon clusters are presented. A detailed description of the Berkeley tunable FIR laser spectrometers is presented in the following article

The Berkeley tunable far infrared laser spectrometers

A detailed description is presented for a tunable far infrared laser spectrometer based on frequency mixing of an optically pumped molecular gas laser with tunable microwave radiation in a Schottky point contact diode. The system has been operated on over 30 laser lines in the range 10–100 cm^–1 and exhibits a maximum absorption sensitivity near one part in 10^6. Each laser line can be tuned by ±110 GHz with first-order sidebands. Applications of this instrument are detailed in the preceding paper

Nonlinear electromagnetic response of graphene: Frequency multiplication and the self-consistent-field effects

Graphene is a recently discovered carbon based material with unique physical properties. This is a monolayer of graphite, and the two-dimensional electrons and holes in it are described by the effective Dirac equation with a vanishing effective mass. As a consequence, electromagnetic response of graphene is predicted to be strongly non-linear. We develop a quasi-classical kinetic theory of the non-linear electromagnetic response of graphene, taking into account the self-consistent-field effects. Response of the system to both harmonic and pulse excitation is considered. The frequency multiplication effect, resulting from the non-linearity of the electromagnetic response, is studied under realistic experimental conditions. The frequency up-conversion efficiency is analysed as a function of the applied electric field and parameters of the samples. Possible applications of graphene in terahertz electronics are discussed.Comment: 14 pages, 7 figures, invited paper written for a special issue of JPCM "Terahertz emitters

Electrically driven spin excitation in a ferroelectric magnet DyMnO_3

Temperature (5--250 K) and magnetic field (0--70 kOe) variations of the low-energy (1--10 meV) electrodynamics of spin excitations have been investigated for a complete set of light-polarization configurations for a ferroelectric magnet DyMnO$_3$ by using terahertz time-domain spectroscopy. We identify the pronounced absorption continuum (1--8 meV) with a peak feature around 2 meV, which is electric-dipole active only for the light $E$-vector along the a-axis. This absorption band grows in intensity with lowering temperature from the spin-collinear paraelectric phase above the ferroelectric transition, but is independent of the orientation of spiral spin plane ($bc$ or $ab$), as shown on the original $P_{\rm s}$ (ferroelectric polarization) $\parallel c$ phase as well as the magnetic field induced $P_{\rm s}\parallel a$ phase. The possible origin of this electric-dipole active band is argued in terms of the large fluctuations of spins and spin-current.Comment: New version, 11 pages including colored 8 figure

Dynamics of Excited Electrons in Copper: Role of Auger Electrons

Within a theoretical model based on the Boltzmann equation, we analyze in detail the structure of the unusual peak recently observed in the relaxation time in Cu. In particular, we discuss the role of Auger electrons in the electron dynamics and its dependence on the d-hole lifetime, the optical transition matrix elements and the laser pulse duration. We find that the Auger contribution to the distribution is very sensitive to both the d-hole lifetime tau_h and the laser pulse duration tau_l and can be expressed as a monotonic function of tau_l/tau_h. We have found that for a given tau_h, the Auger contribution is significantly smaller for a short pulse duration than for a longer one. We show that the relaxation time at the peak depends linearly on the d-hole lifetime, but interestingly not on the amount of Auger electrons generated. We provide a simple expression for the relaxation time of excited electrons which shows that its shape can be understood by a phase space argument and its amplitude is governed by the d-hole lifetime. We also find that the height of the peak depends on both the ratio of the optical transition matrix elements R=|M_{d \to sp}|^2/|M_{sp \to sp}|^2 and the laser pulse duration. Assuming a reasonable value for the ratio, namely R = 2, and a d-hole lifetime of tau_h=35 fs, we obtain for the calculated height of the peak Delta tau_{th}=14 fs, in fair agreement with Delta tau_{exp} \approx 17 fs measured for polycrystalline Cu.Comment: 6 pages, 6 figure

Response theory for time-resolved second-harmonic generation and two-photon photoemission

A unified response theory for the time-resolved nonlinear light generation and two-photon photoemission (2PPE) from metal surfaces is presented. The theory allows to describe the dependence of the nonlinear optical response and the photoelectron yield, respectively, on the time dependence of the exciting light field. Quantum-mechanical interference effects affect the results significantly. Contributions to 2PPE due to the optical nonlinearity of the surface region are derived and shown to be relevant close to a plasmon resonance. The interplay between pulse shape, relaxation times of excited electrons, and band structure is analyzed directly in the time domain. While our theory works for arbitrary pulse shapes, we mainly focus on the case of two pulses of the same mean frequency. Difficulties in extracting relaxation rates from pump-probe experiments are discussed, for example due to the effect of detuning of intermediate states on the interference. The theory also allows to determine the range of validity of the optical Bloch equations and of semiclassical rate equations, respectively. Finally, we discuss how collective plasma excitations affect the nonlinear optical response and 2PPE.Comment: 27 pages, including 11 figures, version as publishe

Lifetimes of image-potential states on copper surfaces

The lifetime of image states, which represent a key quantity to probe the coupling of surface electronic states with the solid substrate, have been recently determined for quantum numbers $n\le 6$ on Cu(100) by using time-resolved two-photon photoemission in combination with the coherent excitation of several states (U. H\"ofer et al, Science 277, 1480 (1997)). We here report theoretical investigations of the lifetime of image states on copper surfaces. We evaluate the lifetimes from the knowledge of the self-energy of the excited quasiparticle, which we compute within the GW approximation of many-body theory. Single-particle wave functions are obtained by solving the Schr\"odinger equation with a realistic one-dimensional model potential, and the screened interaction is evaluated in the random-phase approximation (RPA). Our results are in good agreement with the experimentally determined decay times.Comment: 4 pages, 1 figure, to appear in Phys. Rev. Let

Excitation and Abundance of C3 in star forming cores:Herschel/HIFI observations of the sight-lines to W31C and W49N

We present spectrally resolved observations of triatomic carbon (C3) in several ro-vibrational transitions between the vibrational ground state and the low-energy nu2 bending mode at frequencies between 1654-1897 GHz along the sight-lines to the submillimeter continuum sources W31C and W49N, using Herschel's HIFI instrument. We detect C3 in absorption arising from the warm envelope surrounding the hot core, as indicated by the velocity peak position and shape of the line profile. The sensitivity does not allow to detect C3 absorption due to diffuse foreground clouds. From the column densities of the rotational levels in the vibrational ground state probed by the absorption we derive a rotation temperature (T_rot) of ~50--70 K, which is a good measure of the kinetic temperature of the absorbing gas, as radiative transitions within the vibrational ground state are forbidden. It is also in good agreement with the dust temperatures for W31C and W49N. Applying the partition function correction based on the derived T_rot, we get column densities N(C3) ~7-9x10^{14} cm^{-2} and abundance x(C3)~10^{-8} with respect to H2. For W31C, using a radiative transfer model including far-infrared pumping by the dust continuum and a temperature gradient within the source along the line of sight we find that a model with x(C3)=10^{-8}, T_kin=30-50 K, N(C3)=1.5 10^{15} cm^{-2} fits the observations reasonably well and provides parameters in very good agreement with the simple excitation analysis.Comment: Accepted for publication in Astronomy and Astrophysics (HIFI first results issue