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arXiv:2405.02723 · Physical Review A

Role of chirping in pulsed single-photon spectroscopy

Elnaz Darsheshdar, Aiman Khan, Francesco Albarelli, Animesh Datta

Published Oct 11, 2024• 8 citations
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Abstract

We investigate the precision of estimating the interaction strength between a two-level system (TLS) and a single-photon pulse when the latter is subject to chirping. We consider linear, quadratic, and sinusoidal temporal phases applied to Gaussian and exponential temporal profiles. At the asymptotic time, when the TLS has fully decayed to its ground state, the fundamental precision depends solely on the magnitude of its spectral amplitude. For quadratically phase-modulated Gaussian pulses, this is entirely determined by the spectral bandwidth. We provide expressions for evaluating the fundamental precision for general temporal profiles and phase modulations. Finally, we show that experimentally feasible mode-resolved measurements are optimal, or close to it, for chirped, pulsed single-photon spectroscopy. Published by the American Physical Society 2024

DOI
10.1103/physreva.110.043710

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We investigate the precision of estimating the interaction strength between a two-level system (TLS) and a single-photon pulse when the latter is subject to chirping. We consider linear, quadratic, and sinusoidal temporal phases applied to Gaussian and exponential temporal profiles. At the asymptotic time, when the TLS has fully decayed to its ground state, the fundamental precision depends solely on the magnitude of its spectral amplitude. For quadratically phase-modulated Gaussian pulses, this is entirely determined by the spectral bandwidth. We provide expressions for evaluating the fundamental precision for general temporal profiles and phase modulations. Finally, we show that experimentally feasible mode-resolved measurements are optimal, or close to it, for chirped, pulsed single-photon spectroscopy. Published by the American Physical Society 2024
Abstract Two complementary properties, such as frequency and duration of a pulse, cannot be precisely measured simultaneously. The lower bound on the time-bandwidth product, known also as uncertainty relation, plays a very important role in quantum theory. In this work, we consider single-photon pulses with arbitrary temporal and spectral profiles, and derive a lower bound for the single-photon time-bandwidth product. We investigate how this bound depends on the modal purity, the single-mode fidelity, and the effective number of modes. Our results can be used to solve the inverse problem, namely, to estimate characteristics of the single-photon pulse based on the time-bandwidth product obtained from temporal and spectral measurements of the pulse.
The role of weakly chirped pulses (time bandwidth product, DeltanuDeltatau<0.61) on three-pulse photon echo signals has been systematically studied. Pulses with varying chirp were characterized with frequency resolved optical gating (FROG) and used to measure spectrally resolved three-pulse photon echoes of a dye in solution. The weakly chirped pulses give rise to markedly different echo signals for population times below approximately 100 fs. The chirped pulses can decrease or enhance spectral signatures of an excited state absorption transition in the echo signal. Furthermore, the observed dephasing dynamics depend on the phase of the electric fields. Simulations based on a three-level model and the electric fields retrieved from the FROG traces give a good agreement for photon echo experiments with both transform limited and chirped pulses. The simulations also allow for a numerical investigation of effects of chirp in two-dimensional spectroscopy. For a two-level system, the chirped pulses result in nonelliptical two-dimensional spectra that can erroneously be interpreted as spectral heterogeneity with frequency dependent dephasing dynamics. Furthermore, chirped pulses can give rise to "false" cross peaks when strong vibrational modes are involved in the system-bath interaction.
We present a detailed quantum theory and simulations of few-photon Fock state pulses interacting with a two-level system (TLS) in an open waveguide-QED system. For a rectangular pulse shape, we present an exact temporal scattering theory to derive analytical expressions for the TLS population, using one-photon and two-photon pulses, for both chiral and symmetric emitters. We also derive the stationary (long-time) and time-dependent spectra for one-photon excitation, and show how these differ at a fundamental level when considering TLS population effects. Numerically, we also present matrix product state (MPS) simulations, which allow us to compute more general photon correlation functions for arbitrary quantum pulses, and we use this approach to also show results for Gaussian quantum pulses and to confirm the accuracy of our analytical solutions. In the case of a chiral TLS, we show how a one-photon pulse, of any temporal shape, yields a transmitted long-time spectrum that is identical to the input pulse, despite significant TLS population effects. However, the dynamical spectra and spectral intensity show rich population effects, allowing for their detection in spectroscopic experiments. We also show the striking differences between one-photon and two-photon excitation, where the latter shows clear signatures of nonlinear saturation effects. In addition, we demonstrate how significant population TLS dynamics also occur for pulses that are relatively long compared to the radiative decay time (showing that a weak excitation approximation, which neglects finite TLS population effects, cannot be made) and investigate the population signatures, nonlinear features and dynamical behavior as a function of quantum pulse length.
Temporal-spectral modes of light provide a fundamental window into the nature of quantum systems and offer a robust means for information encoding. Methods to precisely characterize the temporal-spectral state of light at the single-photon level thus play a central role in understanding single-photon sources and their applications in emerging optical quantum technologies. Here we demonstrate an optical reference-free method, which melds techniques from ultrafast metrology and single-photon spectral detection, to characterize the pulse-mode structure of heralded single photons.
Spectral-temporal manipulation of optical pulses has enabled numerous developments within a broad range of research topics, ranging from fundamental science to practical applications. Within quantum optics spectral-temporal degree of freedom of light offers a promising platform for integrated photonic quantum information processing. An important challenge in experimentally realizing spectral-temporal manipulation of quantum states of light is the need for highly efficient manipulation tools. In this context the intrinsically deterministic electro-optic methods show great promise for quantum applications. We experimentally demonstrate application of electro-optic platform for spectral-temporal manipulation of ultrashort pulsed quantum light. Using techniques analogous to serrodyne frequency shifting we show active spectral translation of few-picosecond single photon pulses by up to 0.5 THz. By employing an approach based on an electro-optic time lens we demonstrate up to 6-fold spectral compression of heralded single photon pulses with efficiency that enables us to significantly increase single photon flux through a narrow bandpass filter. We realize the required temporal phase manipulation by driving a lithium niobate waveguided electrooptic modulator with 33 dBm sinusoidal RF field at the frequency of either 10 GHz or 40 GHz. We use a phase lock loop to temporally lock the RF field to the 80 MHz repetition rate of approximately 1 ps long optical pulses. Heralded single photon wavepackets are generated by means of spontaneous parametric down-conversion in potassium dihydrogen phosphate (KDP) crystal, which enables preparation of spectrally pure single photon wavepackets without the need for spectral filtering. Spectral shifting is achieved by locking single-photon pulses to the linear slope of sinusoidal 40 GHz RF phase modulation. We verify the spectral shift by performing spectrally resolved heralded single photon counting, using frequency-to-time conversion by means of a highly dispersive chirped fiber Bragg grating. We verify the non-classicality of spectrally shifted single photons by measuring high-visibility Hong-Ou-Mandel interference using a reference single photon pulse. Spectral compression is based on the time lens principle, which requires locking optical pulses to approximately quadratic region of sinusoidal phase modulation. We utilize both 10 GHz and 40 GHz RF driving frequencies. Bandwidth compression is achieved by chirping the single photon pulse using an appropriate length of single-mode fibre and subsequently subjecting it to the action of the time lens. We verify spectral compression directly using the aforementioned spectrally-resolved heralded single photon counting method. We achieve 3-fold spectral compression of 2 nm bandwidth single photon pulses using 40 GHZ modulation frequency, and 6-fold spectral compression of 0.9 nm bandwidth single photon pulses using 10 GHz modulation frequency. Overall transmission of our set-up exceeding 30% enables practical usability of our spectral compression method which we demonstrate experimentally by showing an increased photon flux through a narrowband filter. Our results present an important contribution towards implementing quantum information processing in the spectral-temporal degree of freedom of a photon. In the context of quantum networks they present an enabling tool towards efficient photonic interfacing of different quantum information processing platforms.
A novel coherent transient spectroscopy, cw photon echo, is described. A medium is exposed to broadband cw laser radiation and then to a pulsed laser, resulting in a continuous emission signal from the medium. The temporal profile of this signal is studied using full density-matrix theory for the cases of a two-level system and a multilevel system. It is shown that such signal decays with a homogeneous dephasing time T2{\mathit{T}}_{2}T2​ and can have a quantum-beat-type modulation, reproducing in a single shot the conventional two-pulse photon echo plot versus first-to-second pulse separation. Experimental demonstrations are given for the 7^{7}7F0{\mathit{F}}_{0}F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathit{D}}_{0}D0​ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ and the 3^{3}3H4{\mathit{H}}_{4}H4​${\mathrm{\ensuremath{-}}}^{1}$D2{\mathit{D}}_{2}D2​ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+; both ions are doped in YAlO3{\mathrm{YAlO}}_{3}YAlO3​. The Eu ions exhibit a single exponential decay with a slight modulation due to the ground-state hyperfine splittings. The temperature dependence of the signal is also studied. The Pr ions show a very deep modulation pattern, which provides excellent agreement with the independent two pulse echo measurement. A numerical simulation based on the modulation theory also agrees with the observed decay curves and the nuclear axis configuration in this crystal is discussed.