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Spectroscopy with neoclassical light

N. Ph. Georgiades, Robert J. Thompson, Q. A. Turchette, Eugene Simon Polzik, O. Carnal, Harry J. Kimble

Published May 8, 1994• 0 citations
OpenAlex

Abstract

Squeezed and other nondassical fields can be employed for enhanced spectroscopic sensitivity surpassing the standard quantum limit.1 However, beyond improvements in quantitative analysis where the nondassical field acts only as a passive probe are a wealth of possibilities associated with the active alteration of fundamental atomic radiative processes.2 In this regard, we are currently pursuing two experiments which make use of our frequency tunable source of squeezed light. The first studies two- photon excitation by correlated photon pairs,3 while the second investigates line- width alterations in cavity QED with squeezed light.4

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Squeezed and other nondassical fields can be employed for enhanced spectroscopic sensitivity surpassing the standard quantum limit.1 However, beyond improvements in quantitative analysis where the nondassical field acts only as a passive probe are a wealth of possibilities associated with the active alteration of fundamental atomic radiative processes.2 In this regard, we are currently pursuing two experiments which make use of our frequency tunable source of squeezed light. The first studies two- photon excitation by correlated photon pairs,3 while the second investigates line- width alterations in cavity QED with squeezed light.4
Without light, there would be no sight. Light acts as a probe in various measurement techniques ranging from imaging to spectroscopy, from small scale cantilever displace- ment measurement in atomic force microscopy to large scale mirror motion in interfer- ometry, light detection and ranging (LIDAR) and many other fields. As the light probe intensity rises, it not only allows reducing the background noise effect, but it also aids precision to the measurement by reducing the photon noise (shot-noise) contribution. However, increasing intensity beyond certain threshold level is not always advantageous for ultra sensitive measurements. For example in the detection of gravitational waves, the current power circulating in the large scale interferometers can not be increased further without introducing other noise sources like thermal effects on the mirrors, un- wanted scattered photons, and back action due to radiation pressure. In the imaging of delicate photo sensitive sample, high power can causes cell damage or it may lead to disturb the regular process under investigation, viz. favouring certain biochemical reaction, which do not correspond to natural in vitro behaviour. At low intensity, pho- ton noise is an important concern and quantum states of light with correlated photon fluctuation can ideally represent a fruitful way to build specific measurement strategies to surpass the limitation of standard approach based on classical light sources, offering an avenue of solutions for ultra sensitive measurements. This thesis work focuses on two application of quantum enhanced measurement strate- gies. The first part of the thesis work has been dedicated to the realization of the first wide-field microscope with Sub Shot Noise (SSN) sensitivity. This is based on the ex- ploitation of quantum correlations in the Squeezed Vacuum state. In the second part, the investigations have made on the role of the quantum correlated beams in an unusual interferometric scheme, in which two identical optical interferometers are subject to the same phase fluctuation. The scheme, in the classical regime, has been already imple- mented in a large scale experiment devoted to the search of possible quantum gravity (QG) effects at Fermilab.
A frequency-tunable source of squeezed light would allow investigations of the atom-field interaction in a regime where fundamental new phenomena have been predicted.1 There are also opportunities for spectroscopy with sensitivity beyond the shot-noise limit. Toward these objectives, in our experiment we employ a single-frequency Ti-sapphire laser with tuning optimized around 852 nm (cesium resonance transition). The infrared output of the laser is frequency doubled in an external buildup cavity with a KNbO3 crystal as the nonlinear element. Efficient doubling provides 0.65 W of tunable blue output for 1.35 W of infrared input. This blue output is then used to pump an optical parametric oscillator (OPO) containing a second KNbO3 crystal for downconversion back to the infrared. The high power of the blue pump that we have achieved and the large nonlinearity of KNbO3 allows us to employ an OPO that is resonant only for the subharmonic infrared light. This design facilitates tuning of the OPO compared with the case in which the blue pump and the infrared are both resonant. The doubling cavity, OPO, and laser itself are locked relative to a stable reference cavity by an rf sideband technique, thus providing the possibility for tunability of the system with a single knob.
Quantum correlations offer the possibility of surpassing classical limits in optical measurements, but their integration into nonlinear vibrational spectroscopy has remained largely unexplored. Here, we introduce a quantum-enhanced implementation of coherent Raman spectroscopy that employs broadband squeezed-light detection to interrogate relative intensity correlations between Stokes and anti-Stokes fields generated in an ultrafast four-wave-mixing process. By exploiting nonclassical correlations between these fields, we suppress the nonresonant background and enhance the signal-to-noise performance in both temporal and spectral domains, enabling detection sensitivities beyond the classical shot-noise limit. Importantly, the quantum advantage demonstrated here does not arise solely from improved detection statistics. Rather, it originates from microscopic intermolecular correlations mediated by cascaded exchange of a virtual photon between molecular pairs. This mechanism establishes a fundamentally distinct and significant pathway for information extraction in vibrational spectroscopy, providing access to structural and dynamical observables that are intrinsically inaccessible by conventional classical Raman techniques. Numerical simulations illustrate the power of the technique by resolving intradimer [Formula: see text] bond splitting in cyclobutane thymine dimers following ultraviolet excitation, highlighting its potential for probing ultrafast photochemical processes with quantum-limited sensitivity and for label-free biomedical optical sensing and imaging.