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Physical Review A

Ultrashort pulse generation in a solid medium with long-lived spin coherence

Roman L. Kolesov, Olga A. Kocharovskaya

Published Feb 24, 2003• 4 citations
Publisher

Abstract

We show that utmost possible Raman coherence between equally populated levels can be excited by two-photon resonant bichromatic field far from one photon resonance by means of relaxation processes. On this basis we suggest a mechanism for generation of extremely short pulses with high pulse duty factor and large energy in the pulse. It can be realized in solid materials, such as the rare-earth doped dielectrics with long-lived spin coherence or nitrogen-vacancy $(N\ensuremath{-}V)$ centers in diamond and provide a simple, reliable, and convenient technique for many practical applications.

DOI
10.1103/physreva.67.023810

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We show that utmost possible Raman coherence between equally populated levels can be excited by two-photon resonant bichromatic field far from one photon resonance by means of relaxation processes. On this basis we suggest a mechanism for generation of extremely short pulses with high pulse duty factor and large energy in the pulse. It can be realized in solid materials, such as the rare-earth doped dielectrics with long-lived spin coherence or nitrogen-vacancy (N\ensuremath−V)(N\ensuremath{-}V)(N\ensuremath−V) centers in diamond and provide a simple, reliable, and convenient technique for many practical applications.
An efficient broadband optical continua generation due to stimulated Raman scattering originated from relaxation processes from the excited electronic states is predicted. It is shown that, even when the populations of Raman levels are equal, Raman coherence can be efficiently excited due to coherent population trapping process (CPT). Scattering of the electromagnetic field due to the excited coherence gives rise to a comb of equally spaced spectral components of optical radiation. The generated spectrum can be compressed into a sequence of ultrashort pulses. Estimates for realistic parameters of the medium show that it is possible to produce a sequence of femtosecond and even subfemtosecond pulses with repetition rate several GHz.
Summary form only given. The use of optical Raman interactions to excite spin coherences in solids has numerous potential applications, ranging from low-power nonlinear optics to high-temperature spectral hole burning memories to solid-state quantum computing. The interest in Raman excitation lies in the fact that the spin coherences can be efficiently excited and manipulated using optical laser fields yet are weakly coupled to the environment and hence have the long coherence lifetimes needed for optical memories and quantum computing. The interest in nitrogen-vacancy (N-V) color centers in diamond is its large optical oscillator strength. For memory, a large oscillator strength is important for high temperature operation. For quantum computing, the high optical transition rate enables the higher gate speed and the larger number of quantum logic operations that can be performed within the spin coherence lifetime.
Terahertz radiation has unique potential for applications to material diagnostics including semiconductors, chemical compounds, biomolecules and biotissues, imaging for medical and security applications, remote atmospheric sensing and monitoring, astronomy, etc. The search for efficient, high-power, inexpensive, portable and room temperature suitable methods of generation of THz radiation is one of the main topics in modern optoelectronics and photonics. Specifically, coherent solid-state compact efficient THz sources are desirable. Recently we suggested a new approach to the problem of generation of short coherent THz pulses in molecular gases taking advantage of the dramatic enhancement of a nonlinear response of a medium via quantum coherence. Stimulated Raman adiabatic passage (STIRAP) technique was proposed for preparation of maximal molecular coherence by two optical pump fields, which is further used to efficiently scatter off an IR probe beam and generate a Stokes THz field in a double Λ scheme. The central idea of the crystal-based technique is to generate THz radiation by resonantly inducing coherence at the corresponding transition by coherent optical fields. Electronic levels of the THz transition are coupled by a pair of optical fields to a common ground state forming a V scheme of energy levels. Coherence induced by the optical fields at the THz transition gives rise to polarization provided that the corresponding dipole moment is not zero, which will radiate out a THz pulse. We show that coherently driven molecular (such as methanol, H2F2, CH3Cl, etc.) and solid-state (ruby, alexandrite) media can potentially produce strong, controllable, short pulses of THz radiation. The pulses have energies ranging from hundreds pJ to J and time durations from several fs to ns at room temperature.
Macroscopic quantum coherence, such as in laser, Bose-Einstein condensates, superfluids, and superconductors, is important to fundamental physics and useful for quantum technologies. Superradiance provides a mechanism to produce coherence among a large number of particles and photons. Its implementation, however, has been limited to gaseous systems, solids at very low temperature, or short pulses. Here we demonstrate a solid-state superradiant maser under ambient conditions, which establishes long-lived coherence among about 101410^{14}1014 nitrogen-vacancy center spins in diamond and about 10910^9109 photons in a microwave cavity. By varying the system parameters to access the above-threshold, well-above-threshold, and deep-above-threshold regimes, we observed continuous-wave masing, periodic amplitude modulation, and sequences of superradiant bursts, which are attributed, correspondingly, to macroscopic spin coherence synchronized at a fixed frequency, a coherent time crystal of large spins, and unsynchronized superradiant transients. This work demonstrates that macroscopic quantum coherence can be spontaneously generated and maintained in solids under ambient conditions and provides a solid-state platform for exploring bright quantum lights with many-body correlations.
In coherent Raman beat experiments a laser field coherently scatters off a material excitation that evolves under the internal Hamiltonian of the system. The Raman signal, which is observed as a beat signal between the test laser and the scattered Raman field, provides information on energy-level splittings and dephasing rates. We propose a modification of this technique, which allows, in contrast to the conventional method, the excitation of coherent Raman beats also in systems with large sublevel splittings and small oscillator strengths. For this purpose, we use a bichromatic laser field to excite the coherent superposition in the medium. We calculate the evolution of the coherence during the laser excitation analytically and discuss its dependence on various experimental parameters. We compare the theoretical results with experimental data from Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​.
Robust, long-lived optical quantum memories are important components of many quantum information and communication protocols. We demonstrate coherent generation, storage, and retrieval of excitations on a long-lived spin transition via spontaneous Raman scattering in a rare-earth ion-doped crystal. We further study the time dynamics of the optical correlations in this system. This is the first demonstration of its kind in a solid and an enabling step toward realizing a solid-state quantum repeater.