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arXiv:0808.1924 · Physical Review A

Narrowband spectroscopy by an all-optical correlation of broadband laser pulses

Stanislav O. Konorov, Xiaoji G. Xu, John W. Hepburn, Valery Milner

Published Mar 5, 2009• 14 citations
arXivHTMLPDF

Abstract

High-peak-power ultrafast lasers are widely used in nonlinear spectroscopy, but often limit its spectral resolution because of the broad frequency bandwidth of ultrashort laser pulses. Improving the resolution by achieving spectrally narrow excitation of, or emission from, the resonant medium by means of multiphoton interferences has been the focus of many recent developments in ultrafast spectroscopy. We demonstrate an alternative approach in which high resolution is exercised by detecting narrow spectral correlations between broadband excitation and emission optical fields. All-optical correlation analysis, easily incorporated into a traditional spectroscopic setup, enables direct, robust, and simultaneous detection of multiple narrow resonances in a single measurement.

DOI
10.1103/physreva.79.031801

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High-peak-power ultrafast lasers are widely used in nonlinear spectroscopy, but often limit its spectral resolution because of the broad frequency bandwidth of ultrashort laser pulses. Improving the resolution by achieving spectrally narrow excitation of, or emission from, the resonant medium by means of multiphoton interferences has been the focus of many recent developments in ultrafast spectroscopy. We demonstrate an alternative approach in which high resolution is exercised by detecting narrow spectral correlations between broadband excitation and emission optical fields. All-optical correlation analysis, easily incorporated into a traditional spectroscopic setup, enables direct, robust, and simultaneous detection of multiple narrow resonances in a single measurement.
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The absorption of a single photon that excites a quantum system from a low to a high energy level is an elementary process of light-matter interaction, and a route towards realizing pure single-photon absorption has both fundamental and practical implications in quantum technology. Due to nonlinear optical effects, however, the probability of pure single-photon absorption is usually very low, which is particularly pertinent in the case of strong ultrafast laser pulses with broad bandwidth. Here we demonstrate theoretically a counterintuitive coherent single-photon absorption scheme by eliminating nonlinear interactions of ultrafast laser pulses with quantum systems. That is, a completely linear response of the system with respect to the spectral energy density of the incident light at the transition frequency can be obtained for all transition probabilities between 0 and 100% in multilevel quantum systems. To that end, a multiobjective optimization algorithm is developed to find an optimal spectral phase of an ultrafast laser pulse, which is capable of eliminating all possible nonlinear optical responses while maximizing the probability of single-photon absorption between quantum states. This work not only deepens our understanding of light-matter interactions, but also offers a way to study photophysical and photochemical processes in the ``absence'' of nonlinear optical effects.
Classical time-resolved optical spectroscopy experiments are performed using sequences of ultrashort light pulses, with photon fluxes incident on the sample which are many orders of magnitude higher than real-world conditions corresponding to sunlight illumination. Here we overcome this paradigm by exploiting quantum correlations to perform time-resolved spectroscopy with entangled photons. Starting from spontaneous parametric down-conversion driven by a continuous-wave laser, we exploit the temporal entanglement between randomly generated signal/idler pairs to obtain temporal resolution, and their spectral entanglement to select the excitation frequency. We also add spectral resolution in detection, using a Fourier transform approach which employs a common-path interferometer. We demonstrate the potential of our entangled-photon streak camera by resolving, at the single-photon level, excitation energy transfer cascades from LH2 to LH1 in the photosynthetic membrane and disentangling the lifetimes of two dyes in a mixture. We show that time-resolved spectroscopy with quantum light can be performed without compromising measurement time, recording a fluorescence time trace in less than a minute even for samples with low quantum yield, which can be reduced to sub-second times with acceptable signal-to-noise ratio. Our results provide a new approach to ultrafast optical spectroscopy, where experiments are performed under conditions comparable to real-world sunlight illumination.
Atomic spectroscopy using broadband ultrashort laser pulses with durations in the 100-fs range seems nearly impossible because the large bandwidth of the pulses exceeds the line-width of atomic transitions by several orders of magnitude. Therefore the energy loss of ultrashort pulses crossing a narrow-linewidth medium is very low, even if the center frequency of the pulses is tuned to the transition frequency. For instance, the total absorption of a 100-fs pulse centered at the D/sub 2/-absorption line of Rb near 780 nm is well below 10/sup -3/ if the pulse is sent through a 75-mm-long Rb vapor cell at room temperature. Much more information can be obtained by measurement of the change of the pulse phase rather than the pulse energy after the pulse has crossed the medium. We found that a measurement technique similar to previously published second harmonic generation (SHG) frequency-resolved optical gating (FROG) is very convenient for that purpose. In our first experiments we send light pulses with a duration of 100 fs, a Fourier-limited bandwidth of 10 nm, and a pulse energy of 1 nJ through a 75-mm long Rb vapor cell. The pulses were analyzed with use of a SHG-FROG system composed on a single shot correlator and dispersive optics that depicted temporal and spectral information as two-dimensional images on a CCD sensor. The SHG-FROG signals depended strongly on the Rb vapor pressure inside the cell, which was controlled by the cell temperature. While these experiments analyzed steady states, the new technique principally allows the monitoring of transient states as well. We present first results on the investigation of optical pumped material.
In recent years, nonlinear quantum interferometry has been widely explored for applications like spectroscopy, optical coherence tomography, and imaging [1]. Quantum infrared spectroscopy (QIRS) uses quantum interference of generation processes of frequency-entangled visible-IR photon pairs to perform infrared spectroscopy using visible light sources and silicon-based detectors [2]. This technique utilizes a nonlinear quantum interferometer configuration where the generated IR photons pass through the sample, and the correlated visible photons are detected. The change in the detected visible photon flux with and without the sample helps extract the complex transmittance of the sample in the IR region.
We present a simple and direct method for measuring laser chirp rate, i.e., group delay dispersion (GDD) of ultrashort laser pulses at power levels compatible with single-quantum-emitter excitation. Traditional pulse characterization techniques rely on nonlinear optical processes that require high peak powers, making them unsuitable for the attojoule-to-femtojoule regime relevant to quantum photonics. Our approach utilizes a wavelength-to-time mapping method in which the arrival times of spectrally filtered components of a broadband pulse are recorded using a superconducting nanowire single-photon detector and correlated via a high-resolution time-tagging system. The resulting linear relationship between wavelength and arrival time directly yields the dispersion parameter and, subsequently, the GDD. Beyond single-emitter excitation, this technique can be applied in areas such as single-photon spectroscopy, ultralow-power optical communications, and time-domain quantum control, where linear and non-destructive dispersion characterization is essential.