We simulate the pump-probe experiments of lasing in molecular nitrogen ions with particular interest on the effects of rotational wave-packet dynamics. Our computations demonstrate that the coherent preparation of rotational wave packets in N$_2^+$ by an intense short non-resonant pulse results in a modulation of the subsequent emission from $B^2Σ_u^+ \rightarrow X^2Σ_g^+$ transitions induced by a resonant seed pulse. We model the dynamics of such pumping and emission using density matrix theory to describe the N$_2^+$ dynamics and the Maxwell wave equation to model the seed pulse propagation. We show that the gain and absorption of a delayed seed pulse is dependent on the pump-seed delay, that is, the rotational coherences excited by the pump pulse can modulate the gain and absorption of the delayed seed pulse. Further, we demonstrate that the coherent rotational dynamics of the nitrogen ions can cause lasing without electronic inversion.
We experimentally investigated the rotationally resolved polarization characteristics of N$_2^+$ lasing at 391 and 428 nm using a pump-seed scheme. By varying the relative angle between the linear polarizations of the pump and seed, it is found that the polarizations of the P and R branches of 391-nm lasing are counter-rotated. By contrast, both branches of 428-nm lasing remain polarized along the pump. The origin of the puzzled abnormal polarization characteristics is found based on a complete physical model that simultaneously includes the transient photoionization and the subsequent couplin…
In standard lasers, light amplification requires population inversion between an upper and a lower state to break the reciprocity between absorption and stimulated emission. However, in a medium prepared in a specific superposition state, quantum interference may fully suppress absorption while leaving stimulated emission intact, opening the possibility of lasing without inversion. Here we show that lasing without inversion arises naturally during propagation of intense femtosecond laser pulses in air. It is triggered by the combination of molecular ionization and molecular alignment, both una…
A new class of laser, which harnesses coherence in both light and atoms, is possible with the use of ultra-cold alkaline earth atoms trapped in an optical lattice inside an optical cavity. Different lasing regimes, including superradiance, superradiant and conventional lasing, are distinguished by the relative coherence stored in the atoms and in the cavity mode. We analyze the physics in two different experimentally achievable regions of the superradiant lasing regime. Our calculations confirm the narrow linewidth of superradiant lasing for the doubly forbidden clock transition ${}^3 P_0 \to …
Gaseous ammonia has previously been demonstrated as a compelling gain medium for a quantum cascade laser pumped molecular laser (QPML), exhibiting good power efficiency but limited tunability. Here we explore the potential of the ammonia QPML to produce powerful, broadly tunable terahertz frequency lasing on rotational and pure inversion transitions. After theoretically predicting possible laser frequencies, pump thresholds, and efficiencies, we experimentally demonstrate unprecedented tunability -- from 0.762 to more than 4.5 THz -- by pumping Q- and R-branch infrared transitions with widely …
Lasers differ from other light sources in that they are coherent, and their coherence makes them indispensable to both fundamental research and practical application. In optomechanical cavities, phonon and photon lasing is facilitated by the ability of photons and phonons to interact intensively and excite one another coherently. The lasing linewidths of both phonons and photons are critical for practical application. However, thus far, these linewidths have not been explored in detail in cavity optomechanical systems. This study investigates the underlying dynamics of lasing in optomechanical…
We describe a superconducting device capable of producing laser light in the visible range at half the Josephson generation frequency, with the optical phase of the light locked to the superconducting phase difference. An earlier proposed device, the so called "half-Josephson laser" [Phys. Rev. Lett. 107, 073901 (2011)], cannot provide long coherence times, because of spontaneous switchings between the emitter states. To circumvent this we consider N >> 1 emitters driving an optical resonator mode. We derive a general model that captures essential physics of such devices while not depending on…
A cavity-free laser in the sky could lead to revolutionary improvements in optical remote sensing for atmospheric science. Abundant in air, nitrogen molecules are prime candidates as an active medium for such a laser. Nitrogen molecules, either neutral or singly ionized, exhibit a significant optical gain in the UV regime when pumped by an intense femtosecond laser. Despite numerous works, the physical origin of this lasing is still not understood. Here we offer a consistent interpretation of all experimental facts by introducing a concept drawn from the field of quantum optics: transient lasi…
We design and fabricate an on-chip laser source that produces a directional beam with low spatial coherence. The lasing modes are based on the axial orbit in a stable cavity and have good directionality. To reduce the spatial coherence of emission, the number of transverse lasing modes is maximized by fine-tuning the cavity geometry. Decoherence is reached in a few nanoseconds. Such rapid decoherence will facilitate applications in ultrafast speckle-free full-field imaging.
We present a comprehensive study of the polarization and spatial coherence properties of the lasing modes supported by a 4-fold symmetric plasmonic lattice. By modifying only, the scattering properties of the individual particles while keeping the lattice geometry constant, we are able to distinguish the scattering induced effects from the lattice geometry induced effects. Customized interferometric measurements reveal that the lasing emission undergoes a drastic change from 1D to 2D spatial coherence with increasing particle size, accompanied with dramatic changes in the far field polarizatio…
We report on the lasing in air and pure nitrogen gas pumped by a single 800 nm femtosecond laser pulse. Depending on gas pressure, incident laser power and beam convergence, different lasing lines are observed in the forward direction with rapid change of their relative intensities. The lines are attributed to transitions between vibrational and rotational levels of the first negative band of the singly charged nitrogen molecule-ion. We show that self-seeding plays an important role in the observed intensity changes.
Since the advent of x-ray free-electron lasers (XFELs), considerable efforts have been devoted to achieve x-ray pulses with better temporal coherence. Here, we put forward a scheme to generate fully coherent x-ray lasers (XRLs) based on population inversion in highly charged ions (HCIs), created by fast inner-shell photoionization using XFEL pulses in a laser-produced plasma. Numerical simulations show that one can obtain high-intensity, femtosecond x-ray pulses of relative bandwidths $Δω/ω=10^{-5}$ - $10^{-7}$ by orders of magnitude narrower than in XFEL pulses for wavelengths down to the sub…
We report generation of cascaded rotational Raman scattering up to 58th orders in coherently excited CO_2 molecules. The high-order Raman scattering, which produces a quasiperiodic frequency comb with more than 600 sidebands, is obtained using an intense femtosecond laser to impulsively excite rotational coherence and the femtosecond-laser-induced N_2^+ lasing to generate cascaded Raman signals. The novel configuration allows this experiment to be performed with a single femtosecond laser beam at free-space standoff locations. It is revealed that the efficient spectral extension of Raman signa…
A near-infrared laser generates gain on transitions between the $\text{B}^{\text{2}} Σ_{\text{u}}^{\text{+}}$ and $\text{X}^{\text{2}} Σ_{\text{g}}^{\text{+}}$ states of the nitrogen molecular cation in part by coupling the $\text{X}^{\text{2}} Σ_{\text{g}}^{\text{+}}$ and $\text{A}^{\text{2}} Π_{\text{u}}$ states in the V-system. Traditional time resolved pump-probe measurements rely on post-ionization coupling by the pump pulse to initialize dynamics in the $\text{A}^{\text{2}} Π_{\text{u}}$ state. Here we show that a weak second excitation pulse reduces ambiguity because it acts only on the…
Kagome lattices supporting Dirac cone and flatband dispersions are well known as a highly frustrated, two-dimensional lattice system. Particularly the flatbands therein are attracting continuous interest based on their link to topological order, correlations and frustration. In this work, we realize coupled microcavity implementations of Kagome lattices hosting exciton-polariton quantum fluids of light. We demonstrate precise control over the dispersiveness of the flatband as well as selective condensation of exciton-polaritons into the flatband. Subsequently, we focus on the spatial and tempo…
Singly ionized nitrogen molecules in ambient air pumped by near-infrared femtosecond laser give rise to superradiant emission. Here we demonstrate coherent control of this superradiance by injecting a pair of resonant seeding pulses inside the nitrogen gas plasma. Strong modulation of the 391.4 nm superradiance with a period of 1.3 fs is observed when the delay between the two seeding pulses are finely tuned, pinpointing the essential role of macroscopic coherence in this lasing process. Based on this time-resolved method, the complex temporal evolution of the macroscopic coherence between two…
A pump source is one of the essential prerequisites in order to achieve lasing, and, in most cases, a stronger pump leads to higher laser power at the output. However, this behavior may be suppressed if two pump beams are used. In this work, it is shown that lasing around the 1600 nm band can be suppressed completely if two pumps, at wavelengths of 980 nm and 1550 nm, are applied simultaneously to a Yb:Er-doped microlaser, whereas it can be revived by switching one of them off. This phenomenon can be explained by assuming that the existence of one pump (980 nm) changes the role of the other pu…
A directional random laser mediated by transverse Anderson localization in a disordered glass optical fiber is reported. Previous demonstrations of random lasers have found limited applications because of their multi-directionality and chaotic fluctuations in the laser emission. The random laser presented in this paper operates in the Anderson localization regime. The disorder induced localized states form isolated local channels that make the output laser beam highly directional and stabilize its spectrum. The strong transverse disorder and longitudinal invariance result in isolated lasing mo…
Two-dimensional infrared (2DIR) spectroscopy is widely used to study molecular dynamics but it is typically restricted to solid and liquid phase samples and modest spectral resolution. Only recently, its potential to study gas-phase dynamics is beginning to be realized. Moreover, the recently proposed technique of cavity-enhanced 2D spectroscopy using frequency combs and developments in multi-comb spectroscopy are expected to dramatically advance capabilities for acquisition of rotationally-resolved 2DIR spectra. This demonstrates the need for rigorous and quantitative treatment of rotationall…
Dual-comb lasers from which asynchronous ultrashort pulses can be simultaneously generated have recently become an interesting research subject. They could be an intriguing alternative to the current dual-laser optical-frequency-comb source with highly sophisticated electronic control systems. If generated through a common light path traveled by all pulses, the common-mode noises between the spectral lines of different pulse trains could be significantly reduced. Therefore, coherent dual-comb generation from a completely common-path, unidirectional lasing cavity would be an interesting territo…
It was widely accepted that embedding of metallic layers into optoelectronic structures is detrimental to lasing due absorption in metal. However, recently macroscopic optical coherence and lasing was observed in microcavities with intra-cavity single metallic layer. Here we propose the design of the of microcavity-type structure with two intra-cavity metallic layers which could serve as contacts for electrical pumping. The design of optical modes based on utilizing peculiarities of Tamm plasmon provides vanishing absorption due to fixing of the node of electric field of optical mode to metall…
Encapsulation of a single water molecule in fullerene-C60 via chemical surgery provides a unique opportunity to study the distinct rotational dynamics of the water spin isomers at cryogenic temperatures. Here, we employ single-cycle terahertz (THz) pulses to coherently excite the low-frequency rotational motion of ortho- and para-water, encapsulated in fullerene-C60. The THz pulse slightly orients the water electric dipole moments along the field polarization leading to the subsequent emission of electromagnetic waves, which we resolve via the field-free electro-optic sampling technique. At te…
Generation of laser-like narrow bandwidth emissions from nitrogen molecular ions generated in intense near- and mid-infrared femtosecond laser fields has aroused much interest because of the mysterious physics underlying such a phenomenon as well as the potential application of such an effect in atmospheric spectroscopic sensing. Here, we perform a pump-probe measurement on the nonlinear interaction of rotational quantum wavepackets of nitrogen molecular ions generated in mid-infrared (e.g., at a wavelength centered at 1580 nm) femtosecond laser fields with an ultrashort probe pulse whose broa…
We show from ab initio laser theory that by choosing an appropriate spatial pump profile, many different spatial modes of a typical microlaser can be turned on at the same pump energy, substantially increasing the number, N, of simultaneous lasing modes. The optimal pump profile can be obtained simply from knowledge of the space-dependent saturated gain profile when the system is uniformly pumped up to the Nth modal threshold. We test this general result by applying it to a two-dimensional diffusive random laser and a microdisk laser. Achieving highly multimode lasing at reasonable pump powers…
The ray dynamics of optical cavities exhibits bifurcation points: special geometries at which ray trajectories switch abruptly between stable and unstable. A prominent example is the Fabry-Perot cavity with two planar mirrors, which is widely employed for broad-area semiconductor lasers. Such cavities support lasing in a relatively small number of transverse modes, and the laser is highly susceptible to filamentation and irregular pulsations. Here we demonstrate experimentally that a slight deviation from this bifurcation point (planar cavity) dramatically changes the laser performance. In a n…
Energy transfer through quantum coherences plays an essential role in diverse natural phenomena and technological applications, such as human vision, light-harvesting complexes, quantum heat engines, and quantum information and computing. The understanding of the long-lived coherence involved in these phenomena requires a detailed modeling of the system-bath interactions beyond the so-called secular and/or Markovian approximations. Despite continuous theoretical progress on understanding nonsecular dynamics in the last decades, convincing experimental observations are still lacking. By using t…
We investigate the prospects of creating broad rotational wave packets by means of molecular interaction with long sequences of intense femtosecond pulses. Using state-resolved rotational Raman spectroscopy of oxygen, subject to a sequence of more than 20 laser pulses with peak intensities exceeding $10^{13}$ W/cm$^{2}$ per pulse, we show that the centrifugal distortion is the main obstacle on the way to reaching high rotational states. We demonstrate that the timing of the pulses can be optimized to partially mitigate the centrifugal limit. The cumulative effect of a long pulse sequence resul…
We present diagrammatic transport theory including self-consistent nonlinear enhancement and dissipation in the multiple scattering regime. Our model of Vollhardt-Wölfle transport of photons is fit-parameter-free and raises the claim that the results hold up to the closest packed volume of randomly arranged ZnO Mie scatterers. We find that a symmetry breaking caused by dissipative effects of a lossy underlying substrate leads to qualitatively different physics of coherence and lasing in granular amplifying media. According to our results, confined and extended mode and their laser thresholds c…
Semiconductor lasers are notoriously sensitive to optical feedback, and their dynamics and coherence can be significantly modified through optical reinjection. We concentrate on the dynamical properties of a very small (i.e., microscale) Vertical Cavity Surface Emitting Laser (VCSEL) operated in the low coherence region between the emission of (partially) coherent pulses and ending below the accepted macroscopic lasing threshold, with the double objective of: 1. studying the feedback influence in a regime of very low energy consumption; 2. using the micro-VCSEL as a surrogate for nanolasers, w…
