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arXiv:2606.11516

Single Photon Cross-Phase Shifts Can Be Enhanced by Localization in both Frequency and Time

Xinyu Jiao, Vida-Michelle Nixon, Kyle Thompson, Aephraim Steinberg

quant-phSubmitted Jun 9, 2026• Announced Jun 11, 2026• 0 citations
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Abstract

Single-photon optical nonlinearities face a fundamental trade-off: maximum nonlinearity requires both spectral resonance (narrow bandwidth) and high peak intensity (short duration), constraints that are incompatible due to the time-energy uncertainty relation. We demonstrate experimentally that this limitation does not need to exist in cases involving post-selection. We measure a cross-phase shift (XPS) produced by a resonant photon from a narrow-band source that is first transmitted through a cold atomic cloud and then localized in time through detection. The peak size of this XPS is greatly enhanced compared to that of Gaussian single-photon-level pulses without post-selection, benefiting from the narrow bandwidth of the resonant prepared state and the high intensity of the post-selected state simultaneously. We measure enhancements in the peak XPS of 6$\pm$1 at an optical depth (OD) of 2.4$\pm$0.1, and our results are in qualitative agreement across a range of optical depths with the recently developed weak value theory of atomic excitation [Thompson et al., APL Quantum 2, 036108 (2025)] for such post-selected photons. This work uncovers new consequences of having simultaneous knowledge of frequency and time, raising new foundational questions about how a particle behaves, and interacts with other systems, when its preparation and post-selection are non-commuting.

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Electromagnetically induced transparency (EIT) has been proposed as a way to greatly enhance cross-phase modulation, with the possibility of leading to few-photon-level optical nonlinearities [Schmidt and Imamoglu, Opt. Lett. 21, 1936 (1996)]. This enhancement grows as the transparency window width, ${\mathrm{\ensuremath{\Delta}}}_{\mathrm{EIT}}$, is narrowed. Decreasing ${\mathrm{\ensuremath{\Delta}}}_{\mathrm{EIT}}$, however, has been shown to increase the response time of the nonlinear medium. This suggests that, for a given pulse duration, the nonlinearity would diminish once the window width became narrower than this pulse bandwidth. We show that this is not the case: the peak phase shift saturates but does not decrease. We show that in the regimes of most practical interest---narrow EIT windows perturbed by short signal pulses---the enhancement offered by EIT is not only in the magnitude of the nonlinear phase shift but also in its increased duration. That is, for the case of signal pulses much shorter (temporally) than the inverse EIT bandwidth, the narrow window serves to prolong the effect of the passing signal pulse, leading to an integrated phase shift that grows linearly with $1/{\mathrm{\ensuremath{\Delta}}}_{\mathrm{EIT}}$; this continued growth of the integrated phase shift improves the detectability of the phase shift, in principle, without bound. For many purposes, it is this detectability which is of more interest than the absolute magnitude of the peak phase shift. We present analytical expressions based on a linear time-invariant model that accounts for the temporal behavior of the cross-phase modulation for several parameter ranges of interest. We conclude that in order to optimize the detectability of the EIT-based cross-phase shift, one should use the narrowest possible EIT window and a signal pulse that is as broadband as the excited-state linewidth and detuned by half a linewidth.

arXiv:1406.0245•Physical Review A•Jan 19, 2016•18 citations
Single-photon optical nonlinearities face a fundamental trade-off: maximum nonlinearity requires both spectral resonance (narrow bandwidth) and high peak intensity (short duration), constraints that are incompatible due to the time-energy uncertainty relation. We demonstrate experimentally that this limitation does not need to exist in cases involving post-selection. We measure a cross-phase shift (XPS) produced by a resonant photon from a narrow-band source that is first transmitted through a cold atomic cloud and then localized in time through detection. The peak size of this XPS is greatly enhanced compared to that of Gaussian single-photon-level pulses without post-selection, benefiting from the narrow bandwidth of the resonant prepared state and the high intensity of the post-selected state simultaneously. We measure enhancements in the peak XPS of 6±\pm±1 at an optical depth (OD) of 2.4±\pm±0.1, and our results are in qualitative agreement across a range of optical depths with the recently developed weak value theory of atomic excitation [Thompson et al., APL Quantum 2, 036108 (2025)] for such post-selected photons. This work uncovers new consequences of having simultaneous knowledge of frequency and time, raising new foundational questions about how a particle behaves, and interacts with other systems, when its preparation and post-selection are non-commuting.
When a photon traverses a cloud of atoms without scattering, how much time does it spend as an atomic excitation? To address this question, we used the cross-Kerr effect to weakly probe the degree of atomic excitation caused by a transmitted resonant "signal" photon by measuring the phase shift induced on a (separate, off-resonant) "probe" beam, postselected on cases when the signal photon is transmitted. The time integral of this observed phase shift, properly normalized and averaged over many runs in which the photon is detected after transmission, is the excitation time of interest, in a weak-valued sense. We measured mean atomic excitation times ranging from (-0.82±0.31)τ_{0} for the most narrow band pulse to (0.54±0.28)τ_{0} for the most broadband signal pulse, where τ_{0} is the non-post-selected excitation time, given by the scattering probability multiplied by the atomic lifetime τ_{sp}. Across a range of pulse durations and optical depths, our results are consistent with the recent theoretical prediction that the weak value of the atomic excitation time caused by a transmitted photon equals the group delay experienced by the light. Our experimental results show that negative times are not limited to describing the shift in the peak of a reshaped wave packet (as resulting from group delay), but they also provide the appropriate description of the weak-valued time the photon spends as an atomic excitation.
The generation of nonclassical photon pairs with a long coherence time is key for applications that range from fundamental to quantum communication and metrology. Spontaneous four-wave mixing with electromagnetically induced transparency has been demonstrated as one of the most efficient methods; however, narrowing the bandwidth and producing photon pairs with a temporal length beyond 1 μs remains a technical challenge due to noise considerations and the need for cold atoms with a high optical depth (OD). In this work, we demonstrate the generation of narrowband photon pairs with a controllable coherence time up to 1.72 μs in a laser-cooled atomic ensemble with an OD as high as 130. At such a high OD, we find that the pump laser field spatial profile has a significant effect on the time–frequency entangled two-photon waveform. We also confirm the quantum particle nature of heralded narrowband single photons generated from this source.
When a resonant photon traverses a sample of absorbing atoms, how much time do atoms spend in the excited state? Does the answer depend on whether the photon is ultimately scattered vs. transmitted? In particular, if it is not scattered, meaning that it emerges in the direction it entered, does it cause atoms to spend any time in the excited state, and if so, how much? In this thesis, I report an experimental measurement of the time a transmitted photon causes atoms to spend in the excited state. The experiment is carried out in an ultra-cold gas of Rubidium 85 atoms and involves simultaneously recording changes to the excited state occupation number induced by incident ("signal") photons and whether those photons are transmitted. The time atoms spend in the excited state, which is defined in terms of the time integral of the average excited state occupation number, is measured weakly using a separate, off-resonant “probe” laser to monitor the index of refraction of the sample—that is, I measure the nonlinear phase shift written by a signal pulse on this probe beam—and direct detection is used to isolate the effect of a single transmitted photon. For short pulses (10 ns, to be compared to the 26 ns atomic lifetime) and an optically thick medium (peak OD = 4, leading to 60% absorption given our broad bandwidth), I report that the average time atoms spend in the excited state due to one transmitted photon is not zero, but rather (77 +/- 16)% of the time the average incident photon causes them to spend in the excited state. This observation of “excitation without loss” is attributed to coherent forward emission, which arises, for instance, due to the sign-flip the instantaneous Rabi frequency (pulse envelope) picks up when a broadband pulse propagates through an optically thick medium with highly frequency-dependent absorption [1]. The results of this thesis reveal the complex history of photons as they propagate through an absorbing medium and illustrate the power of utilizing post-selection to experimentally investigate the past behaviour of observed quantum systems.
Weak value amplification (WVA) is a measurement technique in which the effect of a pre- and post-selected system on a weakly interacting probe is magnified. In this thesis, I present the first experimental observation of WVA of a single photon. We observed that a signal photon - sent through a polarization interferometer and post-selected by photodetection in the almost-dark port - can act like eight photons. The effect of this single photon is measured as a nonlinear phase shift on a separate laser beam. The interaction between the two is mediated by a sample of laser- cooled 85Rb atoms. Electromagnetically induced transparency (EIT) is used to enhance the nonlinearity and overcome resonant absorption. I believe this work to be the first demonstration of WVA where a deterministic interaction is used to entangle two distinct optical systems. In WVA, the amplification is contingent on discarding a large portion of the original data set. While amplification increases measurement sensitivity, discarding data worsens it. Questioning whether these competing effects conspire to improve or diminish measurement accuracy has resulted recently in controversy. I address this question by calculating the maximum amount of information achievable with the WVA technique. By comparing this information to that achievable by the standard technique, where no post-selection is employed, I show that the WVA technique can be advantageous under a certain class of noise models. Finally, I propose a way to optimally apply the WVA technique.
Electromagnetically induced transparency (EIT) has been proposed as a way to greatly enhance cross-phase modulation, with the possibility of leading to few-photon-level optical nonlinearities [Schmidt and Imamoglu, Opt. Lett. 21, 1936 (1996)]. This enhancement grows as the transparency window width, ${\mathrm{\ensuremath{\Delta}}}_{\mathrm{EIT}}$, is narrowed. Decreasing ${\mathrm{\ensuremath{\Delta}}}_{\mathrm{EIT}}$, however, has been shown to increase the response time of the nonlinear medium. This suggests that, for a given pulse duration, the nonlinearity would diminish once the window width became narrower than this pulse bandwidth. We show that this is not the case: the peak phase shift saturates but does not decrease. We show that in the regimes of most practical interest---narrow EIT windows perturbed by short signal pulses---the enhancement offered by EIT is not only in the magnitude of the nonlinear phase shift but also in its increased duration. That is, for the case of signal pulses much shorter (temporally) than the inverse EIT bandwidth, the narrow window serves to prolong the effect of the passing signal pulse, leading to an integrated phase shift that grows linearly with $1/{\mathrm{\ensuremath{\Delta}}}_{\mathrm{EIT}}$; this continued growth of the integrated phase shift improves the detectability of the phase shift, in principle, without bound. For many purposes, it is this detectability which is of more interest than the absolute magnitude of the peak phase shift. We present analytical expressions based on a linear time-invariant model that accounts for the temporal behavior of the cross-phase modulation for several parameter ranges of interest. We conclude that in order to optimize the detectability of the EIT-based cross-phase shift, one should use the narrowest possible EIT window and a signal pulse that is as broadband as the excited-state linewidth and detuned by half a linewidth.