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arXiv:2309.04845

Classical Model for Broadband Squeezed Vacuum Driving Two-Photon Absorption or Sum Frequency Generation

Michael G. Raymer, Tiemo S. Landes

Published Sep 9, 2023• 0 citations
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Abstract

We address theoretically the question of classical stochastic fields mimicking quantum states of light in the context of nonlinear spectroscopy and nonlinear optics, in particular two-photon absorption (TPA) and sum-frequency generation (SFG) driven by weak or bright broadband squeezed vacuum with time-frequency entanglement between photons. Upon using a well-defined but ad hoc subtraction of vacuum-energy terms (renormalization), we find that the classical stochastic model yields exactly the same predictions as the full quantum-field theory for all of the phenomena considered here, in both the low-gain and high-gain regimes of squeezed vacuum. Such predictions include the linear-flux scaling of TPA and SFG rates at low incident photon flux, as well as the dependence of TPA and SHG rates on the relative linewidths of the squeezed light and the ground-to-final-state transition in the material system, and the spectrum of SFG generated by bright squeezed vacuum.

DOI
10.48550/arxiv.2309.04845

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We address theoretically the question of classical stochastic fields mimicking quantum states of light in the context of nonlinear spectroscopy and nonlinear optics, in particular two-photon absorption (TPA) and sum-frequency generation (SFG) driven by weak or bright broadband squeezed vacuum with time-frequency entanglement between photons. Upon using a well-defined but ad hoc subtraction of vacuum-energy terms (renormalization), we find that the classical stochastic model yields exactly the same predictions as the full quantum-field theory for all of the phenomena considered here, in both the low-gain and high-gain regimes of squeezed vacuum. Such predictions include the linear-flux scaling of TPA and SFG rates at low incident photon flux, as well as the dependence of TPA and SHG rates on the relative linewidths of the squeezed light and the ground-to-final-state transition in the material system, and the spectrum of SFG generated by bright squeezed vacuum.
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When two-photon interactions are induced by down-converted light with a bandwidth that exceeds the pump bandwidth, they can obtain a behavior that is pulselike temporally, yet spectrally narrow. At low photon fluxes this behavior reflects the time and energy entanglement between the down-converted photons. However, two-photon interactions such as two-photon absorption (TPA) and sum-frequency generation (SFG) can exhibit such a behavior even at high power levels, as long as the final state (i.e., the atomic level in TPA, or the generated light in SFG) is narrow-band enough. This behavior does not depend on the squeezing properties of the light, is insensitive to linear losses, and has potential applications. In this paper we describe analytically this behavior for traveling-wave down conversion with continuous or pulsed pumping, both for high- and low-power regimes. For this we derive a quantum-mechanical expression for the down-converted amplitude generated by an arbitrary pump, and formulate operators that represent various two-photon interactions induced by broadband light. This model is in excellent agreement with experimental results of TPA and SFG with high-power down-converted light and with entangled photons [Dayan et al., Phys. Rev. Lett. 93, 023005 (2004); 94, 043602 (2005); Pe'er et al., ibid. 94, 073601 (2005)].
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Quantum frequency conversion, the process of shifting the frequency of an optical quantum state while preserving quantum coherence, can be used to produce non-classical light at otherwise unapproachable wavelengths. We present experimental results based on highly efficient sum-frequency generation (SFG) between a vacuum squeezed state at 1064 nm and a tunable pump source at 850 nm ± 50 nm for the generation of bright squeezed light at 472 nm ± 4 nm, currently limited by the phase-matching of the used nonlinear crystal. We demonstrate that the SFG process conserves part of the quantum coherence as a 4.2(±0.2) dB 1064 nm vacuum squeezed state is converted to a 1.6(±0.2) dB tunable bright blue squeezed state. We furthermore demonstrate simultaneous frequency- and spatial-mode conversion of the 1064-nm vacuum squeezed state, and measure 1.1(±0.2) dB and 0.4(±0.2) dB of squeezing in the TEM01 and TEM02 modes, respectively. With further development, we foresee that the source may find use within fields such as sensing, metrology, spectroscopy, and imaging.