@article{14802, abstract = {Frequency-stable lasers form the back bone of precision measurements in science and technology. Such lasers typically attain their stability through frequency locking to reference cavities. State-of-the-art locking performances to date had been achieved using frequency modulation based methods, complemented with active drift cancellation systems. We demonstrate an all passive, modulation-free laser-cavity locking technique (squash locking) that utilizes changes in spatial beam ellipticity for error signal generation, and a coherent polarization post-selection for noise resilience. By comparing two identically built proof-of-principle systems, we show a frequency locking instability of 5×10−7 relative to the cavity linewidth at 10 s averaging. The results surpass the demonstrated performances of methods engineered over the last five decades, potentially enabling an advancement in the precision control of lasers, while creating avenues for bridging the performance gaps between industrial grade lasers with scientific ones due to the afforded simplicity and scalability.}, author = {Diorico, Fritz R and Zhutov, Artem and Hosten, Onur}, issn = {2334-2536}, journal = {Optica}, keywords = {Atomic and Molecular Physics, and Optics, Electronic, Optical and Magnetic Materials}, number = {1}, pages = {26--31}, publisher = {Optica Publishing Group}, title = {{Laser-cavity locking utilizing beam ellipticity: accessing the 10−7 instability scale relative to cavity linewidth}}, doi = {10.1364/optica.507451}, volume = {11}, year = {2024}, } @article{15045, abstract = {Coupling of orbital motion to a spin degree of freedom gives rise to various transport phenomena in quantum systems that are beyond the standard paradigms of classical physics. Here, we discuss features of spin-orbit dynamics that can be visualized using a classical model with two coupled angular degrees of freedom. Specifically, we demonstrate classical ‘spin’ filtering through our model and show that the interplay between angular degrees of freedom and dissipation can lead to asymmetric ‘spin’ transport.}, author = {Varshney, Atul and Ghazaryan, Areg and Volosniev, Artem}, issn = {1432-5411}, journal = {Few-Body Systems}, keywords = {Atomic and Molecular Physics, and Optics}, publisher = {Springer Nature}, title = {{Classical ‘spin’ filtering with two degrees of freedom and dissipation}}, doi = {10.1007/s00601-024-01880-x}, volume = {65}, year = {2024}, } @article{14749, abstract = {We unveil a powerful method for the stabilization of laser injection locking based on sensing variations in the output beam ellipticity of an optically seeded laser. The effect arises due to an interference between the seeding beam and the injected laser output. We demonstrate the method for a commercial semiconductor laser without the need for any internal changes to the readily operational injection locked laser system that was used. The method can also be used to increase the mode-hop free tuning range of lasers, and has the potential to fill a void in the low-noise laser industry.}, author = {Mishra, Umang and Li, Vyacheslav and Wald, Sebastian and Agafonova, Sofya and Diorico, Fritz R and Hosten, Onur}, issn = {1539-4794}, journal = {Optics Letters}, keywords = {Atomic and Molecular Physics, and Optics}, number = {15}, pages = {3973--3976}, publisher = {Optica Publishing Group}, title = {{Monitoring and active stabilization of laser injection locking using beam ellipticity}}, doi = {10.1364/ol.495553}, volume = {48}, year = {2023}, } @article{14759, abstract = {Proper operation of electro-optic I/Q modulators relies on precise adjustment and control of the relative phase biases between the modulator’s internal interferometer arms. We present an all-analog phase bias locking scheme where error signals are obtained from the beat between the optical carrier and optical tones generated by an auxiliary 2 MHz 𝑅𝐹 tone to lock the phases of all three involved interferometers for operation up to 10 GHz. With the developed method, we demonstrate an I/Q modulator in carrier-suppressed single-sideband mode, where the suppressed carrier and sideband are locked at optical power levels <−27dB relative to the transmitted sideband. We describe a simple analytical model for calculating the error signals and detail the implementation of the electronic circuitry for the implementation of the method.}, author = {Wald, Sebastian and Diorico, Fritz R and Hosten, Onur}, issn = {2155-3165}, journal = {Applied Optics}, keywords = {Atomic and Molecular Physics, and Optics, Engineering (miscellaneous), Electrical and Electronic Engineering}, number = {1}, pages = {1--7}, publisher = {Optica Publishing Group}, title = {{Analog stabilization of an electro-optic I/Q modulator with an auxiliary modulation tone}}, doi = {10.1364/ao.474118}, volume = {62}, year = {2023}, } @article{13277, abstract = {Recent experimental advances have inspired the development of theoretical tools to describe the non-equilibrium dynamics of quantum systems. Among them an exact representation of quantum spin systems in terms of classical stochastic processes has been proposed. Here we provide first steps towards the extension of this stochastic approach to bosonic systems by considering the one-dimensional quantum quartic oscillator. We show how to exactly parameterize the time evolution of this prototypical model via the dynamics of a set of classical variables. We interpret these variables as stochastic processes, which allows us to propose a novel way to numerically simulate the time evolution of the system. We benchmark our findings by considering analytically solvable limits and providing alternative derivations of known results.}, author = {Tucci, Gennaro and De Nicola, Stefano and Wald, Sascha and Gambassi, Andrea}, issn = {2666-9366}, journal = {SciPost Physics Core}, keywords = {Statistical and Nonlinear Physics, Atomic and Molecular Physics, and Optics, Nuclear and High Energy Physics, Condensed Matter Physics}, number = {2}, publisher = {SciPost Foundation}, title = {{Stochastic representation of the quantum quartic oscillator}}, doi = {10.21468/scipostphyscore.6.2.029}, volume = {6}, year = {2023}, } @article{13352, abstract = {Optoelectronic effects differentiating absorption of right and left circularly polarized photons in thin films of chiral materials are typically prohibitively small for their direct photocurrent observation. Chiral metasurfaces increase the electronic sensitivity to circular polarization, but their out-of-plane architecture entails manufacturing and performance trade-offs. Here, we show that nanoporous thin films of chiral nanoparticles enable high sensitivity to circular polarization due to light-induced polarization-dependent ion accumulation at nanoparticle interfaces. Self-assembled multilayers of gold nanoparticles modified with L-phenylalanine generate a photocurrent under right-handed circularly polarized light as high as 2.41 times higher than under left-handed circularly polarized light. The strong plasmonic coupling between the multiple nanoparticles producing planar chiroplasmonic modes facilitates the ejection of electrons, whose entrapment at the membrane–electrolyte interface is promoted by a thick layer of enantiopure phenylalanine. Demonstrated detection of light ellipticity with equal sensitivity at all incident angles mimics phenomenological aspects of polarization vision in marine animals. The simplicity of self-assembly and sensitivity of polarization detection found in optoionic membranes opens the door to a family of miniaturized fluidic devices for chiral photonics.}, author = {Cai, Jiarong and Zhang, Wei and Xu, Liguang and Hao, Changlong and Ma, Wei and Sun, Maozhong and Wu, Xiaoling and Qin, Xian and Colombari, Felippe Mariano and de Moura, André Farias and Xu, Jiahui and Silva, Mariana Cristina and Carneiro-Neto, Evaldo Batista and Gomes, Weverson Rodrigues and Vallée, Renaud A. L. and Pereira, Ernesto Chaves and Liu, Xiaogang and Xu, Chuanlai and Klajn, Rafal and Kotov, Nicholas A. and Kuang, Hua}, issn = {1748-3395}, journal = {Nature Nanotechnology}, keywords = {Electrical and Electronic Engineering, Condensed Matter Physics, General Materials Science, Biomedical Engineering, Atomic and Molecular Physics, and Optics, Bioengineering}, number = {4}, pages = {408--416}, publisher = {Springer Nature}, title = {{Polarization-sensitive optoionic membranes from chiral plasmonic nanoparticles}}, doi = {10.1038/s41565-022-01079-3}, volume = {17}, year = {2022}, } @article{13991, abstract = {The prediction and realization of topological insulators have sparked great interest in experimental approaches to the classification of materials1,2,3. The phase transition between non-trivial and trivial topological states is important, not only for basic materials science but also for next-generation technology, such as dissipation-free electronics4. It is therefore crucial to develop advanced probes that are suitable for a wide range of samples and environments. Here we demonstrate that circularly polarized laser-field-driven high-harmonic generation is distinctly sensitive to the non-trivial and trivial topological phases in the prototypical three-dimensional topological insulator bismuth selenide5. The phase transition is chemically initiated by reducing the spin–orbit interaction strength through the substitution of bismuth with indium atoms6,7. We find strikingly different high-harmonic responses of trivial and non-trivial topological surface states that manifest themselves as a conversion efficiency and elliptical dichroism that depend both on the driving laser ellipticity and the crystal orientation. The origins of the anomalous high-harmonic response are corroborated by calculations using the semiconductor optical Bloch equations with pairs of surface and bulk bands. As a purely optical approach, this method offers sensitivity to the electronic structure of the material, including its nonlinear response, and is compatible with a wide range of samples and sample environments.}, author = {Heide, Christian and Kobayashi, Yuki and Baykusheva, Denitsa Rangelova and Jain, Deepti and Sobota, Jonathan A. and Hashimoto, Makoto and Kirchmann, Patrick S. and Oh, Seongshik and Heinz, Tony F. and Reis, David A. and Ghimire, Shambhu}, issn = {1749-4893}, journal = {Nature Photonics}, keywords = {Atomic and Molecular Physics, and Optics, Electronic, Optical and Magnetic Materials}, number = {9}, pages = {620--624}, publisher = {Springer Nature}, title = {{Probing topological phase transitions using high-harmonic generation}}, doi = {10.1038/s41566-022-01050-7}, volume = {16}, year = {2022}, } @article{13367, abstract = {Confining molecules can fundamentally change their chemical and physical properties. Confinement effects are considered instrumental at various stages of the origins of life, and life continues to rely on layers of compartmentalization to maintain an out-of-equilibrium state and efficiently synthesize complex biomolecules under mild conditions. As interest in synthetic confined systems grows, we are realizing that the principles governing reactivity under confinement are the same in abiological systems as they are in nature. In this Review, we categorize the ways in which nanoconfinement effects impact chemical reactivity in synthetic systems. Under nanoconfinement, chemical properties can be modulated to increase reaction rates, enhance selectivity and stabilize reactive species. Confinement effects also lead to changes in physical properties. The fluorescence of light emitters, the colours of dyes and electronic communication between electroactive species can all be tuned under confinement. Within each of these categories, we elucidate design principles and strategies that are widely applicable across a range of confined systems, specifically highlighting examples of different nanocompartments that influence reactivity in similar ways.}, author = {Grommet, Angela B. and Feller, Moran and Klajn, Rafal}, issn = {1748-3395}, journal = {Nature Nanotechnology}, keywords = {Electrical and Electronic Engineering, Condensed Matter Physics, General Materials Science, Biomedical Engineering, Atomic and Molecular Physics, and Optics, Bioengineering}, pages = {256--271}, publisher = {Springer Nature}, title = {{Chemical reactivity under nanoconfinement}}, doi = {10.1038/s41565-020-0652-2}, volume = {15}, year = {2020}, } @article{13998, abstract = {The interaction of strong near-infrared (NIR) laser pulses with wide-bandgap dielectrics produces high harmonics in the extreme ultraviolet (XUV) wavelength range. These observations have opened up the possibility of attosecond metrology in solids, which would benefit from a precise measurement of the emission times of individual harmonics with respect to the NIR laser field. Here we show that, when high-harmonics are detected from the input surface of a magnesium oxide crystal, a bichromatic probing of the XUV emission shows a clear synchronization largely consistent with a semiclassical model of electron–hole recollisions in bulk solids. On the other hand, the bichromatic spectrogram of harmonics originating from the exit surface of the 200 μm-thick crystal is strongly modified, indicating the influence of laser field distortions during propagation. Our tracking of sub-cycle electron and hole re-collisions at XUV energies is relevant to the development of solid-state sources of attosecond pulses.}, author = {Vampa, Giulio and Lu, Jian and You, Yong Sing and Baykusheva, Denitsa Rangelova and Wu, Mengxi and Liu, Hanzhe and Schafer, Kenneth J and Gaarde, Mette B and Reis, David A and Ghimire, Shambhu}, issn = {1361-6455}, journal = {Journal of Physics B: Atomic, Molecular and Optical Physics}, keywords = {Condensed Matter Physics, Atomic and Molecular Physics, and Optics}, number = {14}, publisher = {IOP Publishing}, title = {{Attosecond synchronization of extreme ultraviolet high harmonics from crystals}}, doi = {10.1088/1361-6455/ab8e56}, volume = {53}, year = {2020}, } @article{8411, abstract = {Studying protein dynamics on microsecond‐to‐millisecond (μs‐ms) time scales can provide important insight into protein function. In magic‐angle‐spinning (MAS) NMR, μs dynamics can be visualized by R1p rotating‐frame relaxation dispersion experiments in different regimes of radio‐frequency field strengths: at low RF field strength, isotropic‐chemical‐shift fluctuation leads to “Bloch‐McConnell‐type” relaxation dispersion, while when the RF field approaches rotary resonance conditions bond angle fluctuations manifest as increased R1p rate constants (“Near‐Rotary‐Resonance Relaxation Dispersion”, NERRD). Here we explore the joint analysis of both regimes to gain comprehensive insight into motion in terms of geometric amplitudes, chemical‐shift changes, populations and exchange kinetics. We use a numerical simulation procedure to illustrate these effects and the potential of extracting exchange parameters, and apply the methodology to the study of a previously described conformational exchange process in microcrystalline ubiquitin.}, author = {Marion, Dominique and Gauto, Diego F. and Ayala, Isabel and Giandoreggio-Barranco, Karine and Schanda, Paul}, issn = {1439-4235}, journal = {ChemPhysChem}, keywords = {Physical and Theoretical Chemistry, Atomic and Molecular Physics, and Optics}, number = {2}, pages = {276--284}, publisher = {Wiley}, title = {{Microsecond protein dynamics from combined Bloch-McConnell and Near-Rotary-Resonance R1p relaxation-dispersion MAS NMR}}, doi = {10.1002/cphc.201800935}, volume = {20}, year = {2019}, } @article{8412, abstract = {Microsecond to millisecond timescale backbone dynamics of the amyloid core residues in Y145Stop human prion protein (PrP) fibrils were investigated by using 15N rotating frame (R1ρ) relaxation dispersion solid‐state nuclear magnetic resonance spectroscopy over a wide range of spin‐lock fields. Numerical simulations enabled the experimental relaxation dispersion profiles for most of the fibril core residues to be modelled by using a two‐state exchange process with a common exchange rate of 1000 s−1, corresponding to protein backbone motion on the timescale of 1 ms, and an excited‐state population of 2 %. We also found that the relaxation dispersion profiles for several amino acids positioned near the edges of the most structured regions of the amyloid core were better modelled by assuming somewhat higher excited‐state populations (∼5–15 %) and faster exchange rate constants, corresponding to protein backbone motions on the timescale of ∼100–300 μs. The slow backbone dynamics of the core residues were evaluated in the context of the structural model of human Y145Stop PrP amyloid.}, author = {Shannon, Matthew D. and Theint, Theint and Mukhopadhyay, Dwaipayan and Surewicz, Krystyna and Surewicz, Witold K. and Marion, Dominique and Schanda, Paul and Jaroniec, Christopher P.}, issn = {1439-4235}, journal = {ChemPhysChem}, keywords = {Physical and Theoretical Chemistry, Atomic and Molecular Physics, and Optics}, number = {2}, pages = {311--317}, publisher = {Wiley}, title = {{Conformational dynamics in the core of human Y145Stop prion protein amyloid probed by relaxation dispersion NMR}}, doi = {10.1002/cphc.201800779}, volume = {20}, year = {2019}, } @article{8446, abstract = {Solid‐state NMR spectroscopy can provide insight into protein structure and dynamics at the atomic level without inherent protein size limitations. However, a major hurdle to studying large proteins by solid‐state NMR spectroscopy is related to spectral complexity and resonance overlap, which increase with molecular weight and severely hamper the assignment process. Here the use of two sets of experiments is shown to expand the tool kit of 1H‐detected assignment approaches, which correlate a given amide pair either to the two adjacent CO–CA pairs (4D hCOCANH/hCOCAcoNH), or to the amide 1H of the neighboring residue (3D HcocaNH/HcacoNH, which can be extended to 5D). The experiments are based on efficient coherence transfers between backbone atoms using INEPT transfers between carbons and cross‐polarization for heteronuclear transfers. The utility of these experiments is exemplified with application to assemblies of deuterated, fully amide‐protonated proteins from approximately 20 to 60 kDa monomer, at magic‐angle spinning (MAS) frequencies from approximately 40 to 55 kHz. These experiments will also be applicable to protonated proteins at higher MAS frequencies. The resonance assignment of a domain within the 50.4 kDa bacteriophage T5 tube protein pb6 is reported, and this is compared to NMR assignments of the isolated domain in solution. This comparison reveals contacts of this domain to the core of the polymeric tail tube assembly.}, author = {Fraga, Hugo and Arnaud, Charles‐Adrien and Gauto, Diego F. and Audin, Maxime and Kurauskas, Vilius and Macek, Pavel and Krichel, Carsten and Guan, Jia‐Ying and Boisbouvier, Jerome and Sprangers, Remco and Breyton, Cécile and Schanda, Paul}, issn = {1439-4235}, journal = {ChemPhysChem}, keywords = {Physical and Theoretical Chemistry, Atomic and Molecular Physics, and Optics}, number = {19}, pages = {2697--2703}, publisher = {Wiley}, title = {{Solid‐state NMR H–N–(C)–H and H–N–C–C 3D/4D correlation experiments for resonance assignment of large proteins}}, doi = {10.1002/cphc.201700572}, volume = {18}, year = {2017}, } @article{14007, abstract = {In a recent article by Hockett et al (2016 J. Phys. B: At. Mol. Opt. Phys. 49 095602), time delays arising in the context of molecular single-photon ionization are investigated from a theoretical point of view. We argue that one of the central equations given in this article is incorrect and present a reformulation that is consistent with the established treatment of angle-dependent scattering delays (Eisenbud 1948 PhD Thesis Princeton University; Wigner 1955 Phys. Rev. 98 145–7; Smith 1960 Phys. Rev. 118 349–6; Nussenzveig 1972 Phys. Rev. D 6 1534–42).}, author = {Baykusheva, Denitsa Rangelova and Wörner, Hans Jakob}, issn = {1361-6455}, journal = {Journal of Physics B: Atomic, Molecular and Optical Physics}, keywords = {Condensed Matter Physics, Atomic and Molecular Physics, and Optics}, number = {7}, publisher = {IOP Publishing}, title = {{Comment on ‘Time delays in molecular photoionization’}}, doi = {10.1088/1361-6455/aa62b5}, volume = {50}, year = {2017}, } @article{13387, abstract = {Come on in, the water's fine! Non-photoresponsive nanoparticles can be reversibly assembled using light by placing them in an aqueous solution of a photo­acid. Upon exposure to visible light, the photoacid reduces the pH of the solution, which induces attractive interactions between the nanoparticles. In the dark, the resulting nanoparticle aggregates spontaneously disassemble. The process can be repeated many times.}, author = {Samanta, Dipak and Klajn, Rafal}, issn = {2195-1071}, journal = {Advanced Optical Materials}, keywords = {Atomic and Molecular Physics, and Optics, Electronic, Optical and Magnetic Materials}, number = {9}, pages = {1373--1377}, publisher = {Wiley}, title = {{Aqueous light-controlled self-assembly of nanoparticles}}, doi = {10.1002/adom.201600364}, volume = {4}, year = {2016}, } @misc{13388, abstract = {The Inside Cover picture illustrates the fluorescent properties of a gold nanocluster functionalized with several copies of a red-emitting merocyanine (image by Ella Marushchenko). The red fluorescence can be turned on and off reversibly by using an external stimulus.}, author = {Udayabhaskararao, T. and Kundu, Pintu K. and Ahrens, Johannes and Klajn, Rafal}, booktitle = {ChemPhysChem}, issn = {1439-7641}, keywords = {Physical and Theoretical Chemistry, Atomic and Molecular Physics, and Optics}, number = {12}, pages = {1711--1711}, publisher = {Wiley}, title = {{Inside cover: Reversible photoisomerization of spiropyran on the surfaces of Au25 nanoclusters (ChemPhysChem 12/2016)}}, doi = {10.1002/cphc.201600480}, volume = {17}, year = {2016}, } @article{13389, abstract = {Au25 nanoclusters functionalized with a spiropyran molecular switch are synthesized via a ligand-exchange reaction at low temperature. The resulting nanoclusters are characterized by optical and NMR spectroscopies as well as by mass spectrometry. Spiropyran bound to nanoclusters isomerizes in a reversible fashion when exposed to UV and visible light, and its properties are similar to those of free spiropyran molecules in solution. The reversible photoisomerization entails the modulation of fluorescence as well as the light-controlled self-assembly of nanoclusters.}, author = {Udayabhaskararao, T. and Kundu, Pintu K. and Ahrens, Johannes and Klajn, Rafal}, issn = {1439-7641}, journal = {ChemPhysChem}, keywords = {Physical and Theoretical Chemistry, Atomic and Molecular Physics, and Optics}, number = {12}, pages = {1805--1809}, publisher = {Wiley}, title = {{Reversible photoisomerization of spiropyran on the surfaces of Au25 nanoclusters}}, doi = {10.1002/cphc.201500897}, volume = {17}, year = {2016}, } @article{14012, abstract = {Monochromatization of high-harmonic sources has opened fascinating perspectives regarding time-resolved photoemission from all phases of matter. Such studies have invariably involved the use of spectral filters or spectrally dispersive optical components that are inherently lossy and technically complex. Here we present a new technique for the spectral selection of near-threshold harmonics and their spatial separation from the driving beams without any optical elements. We discover the existence of a narrow phase-matching gate resulting from the combination of the non-collinear generation geometry in an extended medium, atomic resonances and absorption. Our technique offers a filter contrast of up to 104 for the selected harmonics against the adjacent ones and offers multiple temporally synchronized beamlets in a single unified scheme. We demonstrate the selective generation of 133, 80 or 56 nm femtosecond pulses from a 400-nm driver, which is specific to the target gas. These results open new pathways towards phase-sensitive multi-pulse spectroscopy in the vacuum- and extreme-ultraviolet, and frequency-selective output coupling from enhancement cavities.}, author = {Rajeev, Rajendran and Hellwagner, Johannes and Schumacher, Anne and Jordan, Inga and Huppert, Martin and Tehlar, Andres and Niraghatam, Bhargava Ram and Baykusheva, Denitsa Rangelova and Lin, Nan and von Conta, Aaron and Wörner, Hans Jakob}, issn = {2047-7538}, journal = {Light: Science & Applications}, keywords = {Atomic and Molecular Physics, and Optics, Electronic, Optical and Magnetic Materials}, number = {11}, pages = {e16170--e16170}, publisher = {Springer Nature}, title = {{In situ frequency gating and beam splitting of vacuum- and extreme-ultraviolet pulses}}, doi = {10.1038/lsa.2016.170}, volume = {5}, year = {2016}, } @article{13392, abstract = {The chemical behaviour of molecules can be significantly modified by confinement to volumes comparable to the dimensions of the molecules. Although such confined spaces can be found in various nanostructured materials, such as zeolites, nanoporous organic frameworks and colloidal nanocrystal assemblies, the slow diffusion of molecules in and out of these materials has greatly hampered studying the effect of confinement on their physicochemical properties. Here, we show that this diffusion limitation can be overcome by reversibly creating and destroying confined environments by means of ultraviolet and visible light irradiation. We use colloidal nanocrystals functionalized with light-responsive ligands that readily self-assemble and trap various molecules from the surrounding bulk solution. Once trapped, these molecules can undergo chemical reactions with increased rates and with stereoselectivities significantly different from those in bulk solution. Illumination with visible light disassembles these nanoflasks, releasing the product in solution and thereby establishes a catalytic cycle. These dynamic nanoflasks can be useful for studying chemical reactivities in confined environments and for synthesizing molecules that are otherwise hard to achieve in bulk solution.}, author = {Zhao, Hui and Sen, Soumyo and Udayabhaskararao, T. and Sawczyk, Michał and Kučanda, Kristina and Manna, Debasish and Kundu, Pintu K. and Lee, Ji-Woong and Král, Petr and Klajn, Rafal}, issn = {1748-3395}, journal = {Nature Nanotechnology}, keywords = {Electrical and Electronic Engineering, Condensed Matter Physics, General Materials Science, Biomedical Engineering, Atomic and Molecular Physics, and Optics, Bioengineering}, pages = {82--88}, publisher = {Springer Nature}, title = {{Reversible trapping and reaction acceleration within dynamically self-assembling nanoflasks}}, doi = {10.1038/nnano.2015.256}, volume = {11}, year = {2015}, } @article{14017, abstract = {The detection of electron motion and electronic wave-packet dynamics is one of the core goals of attosecond science. Recently, choosing the nitric oxide molecule as an example, we have introduced and demonstrated an experimental approach to measure coupled valence electronic and rotational wave packets using high-order-harmonic-generation (HHG) spectroscopy [Kraus et al., Phys. Rev. Lett. 111, 243005 (2013)]. A short outline of the theory to describe the combination of the pump and HHG probe process was published together with an extensive discussion of experimental results [Baykusheva et al., Faraday Discuss. 171, 113 (2014)]. The comparison of theory and experiment showed good agreement on a quantitative level. Here, we present the theory in detail, which is based on a generalized density-matrix approach that describes the pump process and the subsequent probing of the wave packets by a semiclassical quantitative rescattering approach. An in-depth analysis of the different Raman scattering contributions to the creation of the coupled rotational and electronic spin-orbit wave packets is made. We present results for parallel and perpendicular linear polarizations of the pump and probe laser pulses. Furthermore, an analysis of the combined rotational-electronic density matrix in terms of irreducible components is presented that facilitates interpretation of the results.}, author = {Zhang, Song Bin and Baykusheva, Denitsa Rangelova and Kraus, Peter M. and Wörner, Hans Jakob and Rohringer, Nina}, issn = {1094-1622}, journal = {Physical Review A}, keywords = {Atomic and Molecular Physics, and Optics}, number = {2}, publisher = {American Physical Society}, title = {{Theoretical study of molecular electronic and rotational coherences by high-order-harmonic generation}}, doi = {10.1103/physreva.91.023421}, volume = {91}, year = {2015}, } @article{14021, abstract = {We present the detailed analysis of a new two-pulse orientation scheme that achieves macroscopic field-free orientation at the high particle densities required for attosecond and high-harmonic spectroscopies (Kraus et al 2013 arXiv:1311.3923). Carbon monoxide molecules are oriented by combining one-colour and delayed two-colour non-resonant femtosecond laser pulses. High-harmonic generation is used to probe the oriented wave-packet dynamics and reveals that a very high degree of orientation (Nup/Ntotal = 0.73–0.82) is achieved. We further extend this approach to orienting carbonyl sulphide molecules. We show that the present two-pulse scheme selectively enhances orientation created by the hyperpolarizability interaction whereas the ionization-depletion mechanism plays no role. We further control and optimize orientation through the delay between the one- and two-colour pump pulses. Finally, we demonstrate a complementary encoding of electronic-structure features, such as shape resonances, in the even- and odd-harmonic spectrum. The achieved progress makes two-pulse field-free orientation an attractive tool for a broad class of time-resolved measurements.}, author = {Kraus, P M and Baykusheva, Denitsa Rangelova and Wörner, H J}, issn = {1361-6455}, journal = {Journal of Physics B: Atomic, Molecular and Optical Physics}, keywords = {Condensed Matter Physics, Atomic and Molecular Physics, and Optics}, number = {12}, publisher = {IOP Publishing}, title = {{Two-pulse orientation dynamics and high-harmonic spectroscopy of strongly-oriented molecules}}, doi = {10.1088/0953-4075/47/12/124030}, volume = {47}, year = {2014}, }