Resonant Photon Absorption Research Articles

Effects of Autoionizing Resonances on Wave-Packet Dynamics Studied by Time-Resolved Photoelectron Spectroscopy.

We report a combined experimental and theoretical study on the effect of autoionizing resonances in time-resolved photoelectron spectroscopy. The coherent excitation of N_{2} by ∼14.15 eV extreme-ultraviolet photons prepares a superposition of three dominant adjacent vibrational levels (v^{'}=14-16) in the valence b^{'} ^{1}Σ_{u}^{+} state, which are probed by the absorption of two or three near-infrared photons (800nm). The superposition manifests itself as coherent oscillations in the measured photoelectron spectra. A quantum-mechanical simulation confirms that two autoionizing Rydberg states converging to the excited A ^{2}Π_{u} and B ^{2}Σ_{u}^{+} N_{2}^{+} cores are accessed by the resonant absorption of near-infrared photons. We show that these resonances apply different filters to the observation of the vibrational wave packet, which results in different phases and amplitudes of the oscillating photoelectron signal depending on the nature of the autoionizing resonance. This work clarifies the importance of resonances in time-resolved photoelectron spectroscopy and particularly reveals the phase of vibrational quantum beats as a powerful observable for characterizing the properties of such resonances.

Structurally engineered colloidal quantum dot phosphor using TiO2 photonic crystal backbone

Photonic crystal (PhC) phosphor, in which the phosphor material is periodically modulated for an enhancement in color-conversion efficiency via resonant absorption of excitation photons, is a paradigm-shifting structural phosphor platform. Two-dimensional (2D) square-lattice PhC phosphor is currently considered the most advanced platform because of not only its high efficiency, but also its immunity to excitation polarization. In the present study, two major modifications are made to further improve the performance of the 2D PhC phosphor: increasing the refractive index contrast and planarizing the surface. The index contrast is improved by replacing the PhC backbone material with TiO2 whereas the surface planarization is achieved by removing excessive colloidal quantum dots from the surface. In comparison with the reference phosphor, the upgraded PhC phosphor exhibits ~59 times enhanced absorption (in simulations) and ~7 times enhanced emission (in experiments), both of which are unprecedentedly high. Our results not only brighten the viability and applicability of the PhC phosphor but also spur the phosphor development through structural engineering of phosphor materials.

Acoustically induced transparency for synchrotron hard x-ray photons

The induced transparency of opaque medium for resonant electromagnetic radiation is a powerful tool for manipulating the field-matter interaction. Various techniques to make different physical systems transparent for radiation from microwaves to x-rays were implemented. Most of them are based on the modification of the quantum-optical properties of the medium under the action of an external coherent electromagnetic field. Recently, an observation of acoustically induced transparency (AIT) of the 57Fe absorber for resonant 14.4-keV photons from the radioactive 57Co source was reported. About 150-fold suppression of the resonant absorption of photons due to collective acoustic oscillations of the nuclei was demonstrated. In this paper, we extend the AIT phenomenon to a novel phase-locked regime, when the transmitted photons are synchronized with the absorber vibration. We show that the advantages of synchrotron Mössbauer sources such as the deterministic periodic emission of radiation and controlled spectral-temporal characteristics of the emitted photons along with high-intensity photon flux in a tightly focused beam, make it possible to efficiently implement this regime, paving the way for the development of the acoustically controlled interface between hard x-ray photons and nuclear ensembles.

The quantized chemical reaction resonantly driven by multiple MIR-photons: From nature to the artificial

Biochemical reactions in vivo occur at the temperature usually lower than that in vitro, however the underlying mechanism still remains a challenge. Inspired by our recent studies of adenosine triphosphate (ATP) releasing photons to resonantly drive DNA replication in a quantum way, we propose a quantized chemical reaction driven by multiple mid-infrared (MIR) photons. The space confinement effect of enzymes on a reactant molecule increases the lifetime of excitation state of its bond vibration, providing a chance for the bond to resonantly absorb multiple photons. Although the energy of each MIR photon is significantly lower than that of chemical bond, the resonant absorption of multiple photons can break the appointed bond of confined molecules. Different from the traditional thermochemistry and photochemistry, the quantized chemical reactions could have a high energy efficiency and ultrahigh selectivity. In addition, we also suggest a quantum driving source for our quantum-confined superfluid reactions proposed previously. The quantized chemical reaction resonantly driven by multiple MIR photons holds great promise to develop novel approaches for the chemical engineering in future.

Resonant Pumping of d-d Crystal Field Electronic Transitions as a Mechanism of Ultrafast Optical Control of the Exchange Interactions in Iron Oxides.

The microscopic origin of ultrafast modification of the ratio between the symmetric (J) and antisymmetric (D) exchange interaction in antiferromagnetic iron oxides is revealed, using femtosecond laser excitation as a pump and terahertz emission spectroscopy as a probe. By tuning the photon energy of the laser pump pulse we show that the effect of light on the D/J ratio in two archetypical iron oxides FeBO_{3} and ErFeO_{3} is maximized when the photon energy is in resonance with a spin and parity forbidden d-d transition between the crystal-field split states of Fe^{3+} ions. The experimental findings are supported by a multielectron model, which accounts for the resonant absorption of photons by Fe^{3+} ions. Our results reveal the importance of the parity and spin-change forbidden, and therefore often underestimated, d-d transitions in ultrafast optical control of magnetism.

Efficient single-photon absorption by a trapped moving atom

The influence of the center of mass motion of a trapped two level system on efficient resonant single photon absorption is investigated. It is shown that this absorption process depends strongly on the ratio between the characteristic time scales of spontaneous photon emission and of the two level system's center of mass motion. In particular, if the spontaneous photon emission process occurs almost instantaneously on the time scale of the center of mass motion coherent control of the center of mass motion offers interesting perspectives for optimizing single photon absorption. It is demonstrated that this way time dependent modulation of a harmonic trapping frequency allows to squeeze the two level system's center of mass motion so strongly that high efficient single photon absorption is possible even in cases of weak confinement by a trapping potential.

Infrared Action Spectroscopy of Low-Temperature Neutral Gas-Phase Molecules of Arbitrary Structure.

We demonstrate a technique for IR action spectroscopy that enables measuring IR spectra in a background-free fashion for low-temperature neutral gas-phase molecules of arbitrary structure. The method is exemplified experimentally for N-methylacetamide molecules in the mid-IR spectral range of 1000-1800 cm^{-1}, utilizing the free electron laser FELIX. The technique involves the resonant absorption of multiple mid-IR photons, which induces molecular dissociation. The dissociation products are probed with 10.49eV vacuum ultraviolet photons and analyzed with a mass spectrometer. We also demonstrate the capability of this method to record, with unprecedented ease, mid-IR spectra for the molecular associates, such as clusters and oligomers, present in a molecular beam. In this way the mass-selected spectra of low-temperature gas-phase dimers and trimers of N-methylacetamide are measured in the full amide I-III range.

Design for strong absorption in a nanowire array tandem solar cell.

Semiconductor nanowires are a promising candidate for next-generation solar cells. However, the optical response of nanowires is, due to diffraction effects, complicated to optimize. Here, we optimize through optical modeling the absorption in a dual-junction nanowire-array solar cell in terms of the Shockley-Quessier detailed balance efficiency limit. We identify efficiency maxima that originate from resonant absorption of photons through the HE11 and the HE12 waveguide modes in the top cell. An efficiency limit above 40% is reached in the band gap optimized Al0.10Ga0.90As/In0.34Ga0.66As system when we allow for different diameter for the top and the bottom nanowire subcell. However, for experiments, equal diameter for the top and the bottom cell might be easier to realize. In this case, we find in our modeling a modest 1–2% drop in the efficiency limit. In the Ga0.51In0.49P/InP system, an efficiency limit of η = 37.3% could be reached. These efficiencies, which include reflection losses and sub-optimal absorption, are well above the 31.0% limit of a perfectly-absorbing, idealized single-junction bulk cell, and close to the 42.0% limit of the idealized dual-junction bulk cell. Our results offer guidance in the choice of materials and dimensions for nanowires with potential for high efficiency tandem solar cells.

Ionizations and fragmentations of benzene, methylbenzene, and chlorobenzene in strong IR and UV laser fields**Project supported by the National Basic Research Program of China (Grant No. 2013CB922200) and the National Natural Science Foundation of China (GrantNo. 11274140).

Ionizations and fragmentations of benzene, methylbenzene, and chlorobenzene are studied in linearly polarized 50-fs, 800-nm and 400-nm strong laser fields using a time-of-flight mass spectrometer. It is shown that at low laser intensity, the parent ions are dominant for any one of the molecules in an 800-nm strong laser field, while extensive fragmentation is observed in a 400-nm laser field, which can be understood by the resonant photon absorption of molecular cations. The ratio of the yield of the parent ion to the yield of the total ion for each molecule is measured as a function of laser intensity in a range from 1.0 × 1013 W/cm2 to 4.0 × 1014 W/cm2, in either the 800-nm or 400-nm laser field. The results show that the fragmentation of the aromatic molecules increases significantly as the laser intensity is increased. Possible mechanisms for fragmentation in strong laser fields are discussed. Finally, the saturation intensity of ionization of the titled molecules is also determined.

SYNCHROTRON SELF-COMPTON EMISSION FROM THE CRAB AND OTHER PULSARS

Results of a simulation of synchrotron-self Compton (SSC) emission from a rotation-powered pulsar are presented. The radiating particles are assumed to be both accelerated primary electrons and a spectrum of electron-positron pairs produced in cascades near the polar cap. They follow trajectories in a slot gap using 3D force-free magnetic field geometry, gaining pitch angles through resonant cyclotron absorption of radio photons, radiating and scattering synchrotron emission at high altitudes out to and beyond the light cylinder. Full angular dependence of the synchrotron photon density is simulated in the scattering and all processes are treated in the inertial observer frame. Spectra for the Crab and Vela pulsars as well as two energetic millisecond pulsars, B1821-24 and B1937+21 are simulated using this model. The simulation of the Crab pulsar radiation can reproduce both the flux level and the shape of the observed optical to hard X-ray emission assuming a pair multiplicity of $M_+ = 3 \times 10^5$, as well as the very-high-energy emission above 50 GeV detected by MAGIC and VERITAS, with both the synchrotron and SSC components reflecting the shape of the pair spectrum. Simulations of Vela, B1821$-$24 and B1937+21, for $M_+$ up to $10^5$, do not produce pair SSC emission that is detectable by current telescopes, indicating that only Crab-like pulsars produce significant SSC components. The pair synchrotron emission matches the observed X-ray spectrum of the millisecond pulsars and the predicted peak of this emission at 1 - 10 MeV would be detectable with planned Compton telescopes.

Radiation-induced quantum Fano-type resonances in the transport ofn−p−ngraphene-based junctions

We present a theoretical study of quantum resonances in the ballistic transport of graphene based $N$-$P$-$N$ junction subject to an externally applied electromagnetic field (EF). By making use of the Floquet analysis and the quasi-classical approach we analyze the dynamics of electrons in the presence of time and coordinate dependent potential $U(z,t)$. In the absence of EF the resonant tunneling results in a set of sharp resonances in the dependence of dc conductance $\sigma$ on the gate voltage $V_g$. In irradiated $N$-$P$-$N$ junctions we obtain the Fano-type resonances in the dependence of $\sigma(V_g)$. This \emph{coherent quantum-mechanical phenomenon} is due to the interplay of two effects: the resonant tunneling through quasi-bound states and the quantum-interference effect in the region between the "resonant points", where the resonant absorption (emission) of photons occurs, and junction interfaces.

Multiphoton photochemistry of red fluorescent proteins in solution and live cells.

Genetically encoded fluorescent proteins (FPs), and biosensors based on them, provide new insights into how living cells and tissues function. Ultimately, the goal of the bioimaging community is to use these probes deep in tissues and even in entire organisms, and this will require two-photon laser scanning microscopy (TPLSM), with its greater tissue penetration, lower autofluorescence background, and minimum photodamage in the out-of-focus volume. However, the extremely high instantaneous light intensities of femtosecond pulses in the focal volume dramatically increase the probability of further stepwise resonant photon absorption, leading to highly excited, ionizable and reactive states, often resulting in fast bleaching of fluorescent proteins in TPLSM. Here, we show that the femtosecond multiphoton excitation of red FPs (DsRed2 and mFruits), both in solution and live cells, results in a chain of consecutive, partially reversible reactions, with individual rates driven by a high-order (3–5 photon) absorption. The first step of this process corresponds to a three- (DsRed2) or four-photon (mFruits) induced fast isomerization of the chromophore, yielding intermediate fluorescent forms, which then subsequently transform into nonfluorescent products. Our experimental data and model calculations are consistent with a mechanism in which ultrafast electron transfer from the chromophore to a neighboring positively charged amino acid residue triggers the first step of multiphoton chromophore transformations in DsRed2 and mFruits, consisting of decarboxylation of a nearby deprotonated glutamic acid residue.

New results in high-resolution X-ray fluorescence spectroscopy

We present some recent results dealing with resonant inelastic X-ray scattering (RIXS) on atomic targets in the 3-5 keV enegy region. In this so-called tender spectral region, the K-shell fluorescence branching ratios become reasonably large, but a full vacuum enclosure is still preferable to avoid detection efficiency loss due to the sizeable arms of high resolution crystal spectrometers. By squeezing energy resolution in the fluorescence decay channel, one may improve the spectral resolution of photoabsorption, enable separation of multielectron excitation and relaxation channels, and completely eliminate the need to scan across the selected energy range of the photon probe in order to acquire the photoabsorption spectrum. On the other hand, the spectra may be untrivially modified by effects such as interference of absorption-emission paths or structured relaxation modes, and a more elaborated modelling is needed to understand the emitted signal. We illustrate these aspects by presenting four cases: the reconstruction of Ar KM and Ar KL absorption edges from a series of highly resolved emission spectra recorded at different probe energies, the reconstruction of the Xe L3 edge from a single X-ray emission spectrum, and the analysis of the radiative Ar K-MM Auger decay preceeded by the resonant or nonresonant photon absorption.

Mechanisms of Multiphoton Bleaching of Red Fluorescent Proteins

Two-photon laser scanning microscopy (TPLSM) has several advantages over one-photon confocal microscopy, including deeper tissue penetration, higher signal-to-background ratio, and less photodamage in the out-of-focus volume. However, due to very high instantaneous light intensities in the focal volume, the probability of further, stepwise resonant photon(s) absorption increases dramatically, leading to very efficient bleaching of a probe. To deal with this challenge one has to understand the underlying mechanisms. Here we measured the power dependence of multiphoton bleaching rates of several red fluorescent proteins expressed in live E. coli cells under two-photon microscope conditions. To clarify the photophysical mechanisms, we also used much lower repetition rate (1 kHz) and different pulse durations in experiments in vitro with Ti:Sa amplifier excitation. Our experimental data supported by quantum mechanical calculations of the chromophore in protein environment are consistent with the mechanism of ultrafast (<150 fs) singlet-singlet stepwise absorption of one or two additional photons following initial simultaneous two-photon absorption. In the DsRed2 protein, the third photon absorption most probably results in an ultrafast electron transfer (ET) from the anionic chromophore to an excited Rydberg state of a nearby positive amino acid residue (e.g. K163+). The transient radical state of the chromophore tends to accept an electron from the deprotonated E215- amino acid, thus promoting the first step of the recently established decarboxylation reaction. In mFruits proteins, the third photon promotes an ET from the chromophore to the 4S Rydberg state of nearby K70+ residue with its subsequent photoionization by the fourth photon.

Band-gap profiling by laser writing of hydrogen-containing III-N-Vs

We show that the dissociation of the N-H complex in hydrogenated III-N-Vs can be laser activated at temperatures that are significantly smaller than those (&gt;200 \ifmmode^\circ\else\textdegree\fi{}C) required for thermal dissociation due to a resonant photon absorption by the N-H complex. This phenomenon provides a mechanism for profiling the band-gap energy in the growth plane of the III-N-Vs with submicron spatial resolution and high energy accuracy; the profiles are erasable and the alloys can be rehydrogenated making any nanoscale in-plane band-gap profile rewritable.

Stimulated emission and absorption of photons in magnetic point contacts

Point contacts between high anisotropy ferromagnetic SmCo5 and normal metal Cu are used to achieve a strong spin-population inversion in the contact core. Subjected to microwave irradiation in resonance with the Zeeman splitting in Cu, the inverted spin population relaxes through stimulated spin-flip photon emission, detected as peaks in the point-contact resistance. Resonant spin-flip photon absorption is detected as resistance minima, corresponding to sourcing the photon field energy into the electrical circuit. These results demonstrate fundamental mechanisms that are potentially useful in designing metallic spin-based lasers.

Unabridged Resonant Contribution to the X-ray Scattering Length

Resonance-enhanced Bragg scattering of x-rays and concomitant dichroic signals are valuable tools for investigation of material properties. In this context parity-odd events E1–E2 and E1–M1 merit special attention. Theoretical analysis of the product of matrix-elements defining the scattering length for the resonant photon absorption and emission process leads to sums of electronic multipoles calculated for equilibrium electron states. The unabridged result retains explicit dependence on the labels of the intermediate state and recovers a common unit tensor present in the formulae describing parity-odd events. In order to add physical insight, the various forms of the unit tensor are correlated with magneto-electric and polar multipoles, which benefit from representations using familiar operators. The description of parity-odd events requires the use of appropriate combinations of photonic tensors and electronic multipoles to achieve correct symmetry properties. After discussing some special cases the new...

Structure Determination of Anionic Metal Clusters via Infrared Resonance Enhanced Multiple Photon Electron Detachment Spectroscopy

We report vibrational spectra of anionic metal clusters, measured via electron detachment following resonant absorption of multiple infrared photons. To facilitate the sequential absorption of the required large number of photons, the cluster beam interacts with the infrared radiation inside the cavity of a free electron laser. Far-infrared spectra of the bare metal cluster anion Nb10– as well as of the Nb6C– anion are measured in the 130–1000 cm–1 range. The structures of these clusters can be unambiguously determined by comparison with calculated spectra of the putative global minima structures, identified by density functional theory calculations.

Photocurrent in a visible-light graphene photodiode

We calculate the photocurrent in a clean graphene sample normally irradiated by a monochromatic electromagnetic field and subject to a step-like electrostatic potential. We consider the photon energies $\hbar\Omega$ that significantly exceed the height of the potential barrier, as is the case in the recent experiments with graphene-based photodetectors. The photocurrent comes from the resonant absorption of photons by electrons and decreases with increasing ratio $\hbar\Omega/U_0$. It is weakly affected by the background gate voltage and depends on the light polarization as $\propto\sin^2\gamma$, $\gamma$ being the angle between the potential and the polarization plane.

ACCELERATING HIGH-ENERGY PULSAR RADIATION CODES

Curvature radiation (CR) is believed to be a dominant mechanism for creating gamma-ray emission from pulsars and is emitted by relativistic particles that are constrained to move along curved magnetic field lines. Additionally, synchrotron radiation (SR) is expected to be radiated by both relativistic primaries (involving cyclotron resonant absorption of radio photons and re-emission of SR photons), or secondary electron-positron pairs (created by magnetic or photon-photon pair production processes involving CR gamma rays in the pulsar magnetosphere). When calculating these high-energy spectra, especially in the context of pulsar population studies where several millions of CR and SR spectra have to be generated, it is profitable to consider approximations that would save computational time without sacrificing too much accuracy. This paper focuses on one such approximation technique, and we show that one may gain significantly in computational speed while preserving the accuracy of the spectral results.