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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

Measurement of the Phonon Decoherence in Diamond Using Spectral Interference of Stokes Emission

FC. Waldermann, Joshua Nunn, Karl Surmacz, Z. Wang, Dieter Jaksch, Ian A. Walmsley, P. Olivero, Steven Prawer

Published Jun 1, 2007• 0 citations
Publisher

Abstract

In this paper, we measure the decoherence time of phonons using spectral interference of the Stokes emission of diamond. Two 100 femtosecond laser pulses, separated by a delay tau, are sent through a polished diamond sample of 1.2 mm thickness. Optical phonons in the Brillouin zone centre are created by Raman scattering from the ultrafast laser pulses and can be heralded by the Stokes photons emitted, whose superposed spectrum is recorded by a spectrometer.

DOI
10.1109/cleoe-iqec.2007.4386908

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In this paper, we measure the decoherence time of phonons using spectral interference of the Stokes emission of diamond. Two 100 femtosecond laser pulses, separated by a delay tau, are sent through a polished diamond sample of 1.2 mm thickness. Optical phonons in the Brillouin zone centre are created by Raman scattering from the ultrafast laser pulses and can be heralded by the Stokes photons emitted, whose superposed spectrum is recorded by a spectrometer.
We present a new experiment, in which we measure quantum correlations between single photons that are mediated by the exchange of a single phonon. We create and annihilate a single optical phonon in bulk diamond using two ultrashort laser pulses at two different wavelengths, generated by a Ti:Sapph oscillator and a frequency-doubled optical parametric oscillator (APE Berlin). During Stokes Raman scattering, the first pulse creates a photon-phonon pair, while the second pulse convert the same phonon into an anti-Stokes photon. Using spectral filtering and photon counting, we measure the cross-correlations between the Stokes and anti-Stokes photons with a few hundred femtoseconds time resolution. As expected, the non-classical correlation (g(2) much larger than the classical bound) decays within a few picosecond, following to the dynamics of the phonon mode. Our results demonstrate a new source of broadly tunable quantum correlated photons, and can be extended to provide a new way of measuring non-classical dynamics in nanoscale systems — down to individual nanostructures.
Due to their highly coherent emission, tunability, and compactness, integrated single-frequency diamond Raman lasers are interesting tools for applications in integrated quantum technology, high-resolution spectroscopy, or coherent optical communications. While the fundamental emission linewidth of these lasers can be Fourier limited, their thermo-optic characteristics lead to drifts in their carrier frequency, posing important challenges for applications requiring ultrastable emission. We propose here a method for measuring accurately the temperature-dependent index of refraction of diamond by employing standing Stokes waves produced in a monolithic Fabry-P\'erot diamond Raman resonator. Our approach takes into account the influence of temperature on the first-order phonon line and the average lattice phonon frequency under intense stimulated Raman scattering conditions. We further utilize this model to calculate the value of the average phonon frequency and then the temperature-dependent thermo-optic coefficient. The theory is accompanied by the demonstration of tunable Fourier-limited Stokes nanosecond pulses with a stabilized center frequency deviation of less than 444 MHz.
In this work, we study the correlated Stokes-anti-Stokes (SaS) Raman scattering in a diamond sample and the influence that the excitation pulse width has in the intensity of generation of the correlated pairs in the process. For this investigation, we used two excitation systems with different temporal pulse width, one with femtosecond temporal width and one with picosecond temporal width. We did two distinct experiments with this excitation systems with difference in the way of filtering the signal: In the first experiment, the signal filtering is made with band-pass filters, this configuration has a greater efficiency that allow us compare better the correlated pair formation efficiency between the different excitation systems. In the second experiment, we used a monochromator to filtering the signal, this configuration allow us to change the wavelength of the detection so we can measure the formation spectrum of the correlated pairs. The results obtained from these experiments show us that the correlated pairs generation efficiency is larger with the use of the system with femtosecond temporal width, what is expected for a non-linear process. In the resonant Raman frequency region, we observed a intensity 1.5 times larger with the use of femtosecond system, and in the out-of-ressonance Raman region, we observed a intensity 5 times larger in the region with lowest Raman shift and 9 times larger in the region with largest Raman shift. We also measure the formation pairs spectrum around the first order Raman peak of the diamond, confirming the existence of a asymmetry in the formation of this pairs with respect to the positive versus negative detuning from phonon resonance. This asymmetry still remains without a satisfactory theoretical explanation.
The correlated Stokes-anti-Stokes Raman scattering mediated by phonons was introduced in 1977 by Klyshko. In the last two decades, it has been broadly studied experimentally, including results on diamond, graphene and transparent liquid. The theoretical description of non-resonant Stokes-anti-Stokes pair production was shown to be formally similar to the BCS theory of superconductivity, raising attention to the study of pair production as a function of the Raman shift. Intriguingly, the pair production efficiency is not symmetric with respect to the positive versus negative detuning from phonon resonance, a result that was shown for a 180fs pulsed laser, and that remains without a theoretical explanation. Here we show the asymmetry is persistent in diamond measured with lasers of different pulse widths (180 fs and 5 ps) and different wavelengths (633 nm versus 785 nm).
Summary form only given. An amplified pulse of a Ti:sapphire femtosecond laser was split into an intense pump and a weak probe pulse. The delay time 7 between pump and probe pulse was adjusted from 0-50 ps in steps of 10 fs. The interaction volume given by the spatial overlap of pump and probe was in the bulk of the sample. Amorphous samples of glass and different single crystals with a typical thickness of 1 mm were used. Measurements with experimental setup A showed a beam scattering according to the degenerate four wave mixing (DFWM) process with fixed scattering angle, independent of the pump pulse intensity and delay time.