THz Control in Correlated Electron Solids: Sources and Applications

Först, Michael; Hoffmann, Matthias C.; Dienst, A.; Kaiser, Stefan; Rini, Matteo; Tobey, R. I.; Gensch, Michael; Manzoni, Cristian; Cavalleri, Andrea

doi:10.1007/978-3-642-29564-5_23

Cited by 6 publications

(7 citation statements)

References 99 publications

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“…Since then the concept has been demonstrated at synchrotrons [21,22]; however, its true potential has been revealed once it has been observed at linacs [20,23] since the longitudinal electron bunch length is typically much shorter than that of an usual storage ring. In recent years, we are witnessing a continuation of the rapid development at linear accelerators being developed for the generation of laser-like x-rays such as the FEL in Hamburg FLASH [17,24,25], the Linac Coherent Light Source (LCLS) [26,27], PAL-FEL [28], FERMI [29], Frascati FEL [30], and femtosecond linacs like the one in Shanghai [31,32], FLUTE [33] and TELBE [34]. For generation of high peak THz power at these facilities, short electron bunches are mandatory.…”

Section: Accelerator-based Thz Sourcesmentioning

confidence: 99%

“…High intensity and field in the focus of THz pulses generated by CTR, together with the relative simplicity of design and operation motivate further development and use of these sources at fourth generation photon facilities around the world. At present, new CTR sources are under commissioning or construction at TELBE [34], FLUTE [33], FLASH and FERMI [29], to just name a few.…”

Section: Single Cycle Thz Sourcesmentioning

confidence: 99%

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Accelerator- and laser-based sources of high-field terahertz pulses

Stojanović¹,

Drescher²

2013

J. Phys. B: At. Mol. Opt. Phys.

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At present we are witnessing a rapid development of sources for terahertz (THz) pulses with very strong electromagnetic fields. These pulses are reaching a stage where they can be used to not only probe, but also uniquely control a variety of processes that range from fundamental dynamics in individual atoms and molecules, through phase transitions in solids to a wealth of interactions in biological materials. In this review, we are presenting an overview of two major directions in the generation of such radiation. Large-scale accelerator-based sources offer unprecedented pulse energies coupled with a wide tuning range and extreme repetition rates. Laser-based sources, on the other hand, are laboratory-scale instruments and thus are very attractive in their availability to the wide scientific community. The capabilities of different variants of these THz sources are evaluated and compared with each other. In addition, powerful techniques for the temporal characterization of THz pulses are discussed.

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Section: Accelerator-based Thz Sourcesmentioning

confidence: 99%

Section: Single Cycle Thz Sourcesmentioning

confidence: 99%

Accelerator- and laser-based sources of high-field terahertz pulses

Stojanović¹,

Drescher²

2013

J. Phys. B: At. Mol. Opt. Phys.

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“…This point of view is different from that of light-induced excited spin-state trapping (LIESST), where the spin states of transition-metal complexes are switched between high-and low-spins by photoexcitations at low temperature [1][2][3][4][5][6][7][8][9]. Additionally, the abovementioned point of view is also different from that of photo-induced phase transitions (PIPTs), where phase transitions, such as metal-insulator and ionic-neutral transitions at certain temperatures (T C s), are brought about by photo-irradiation near the T C s [10,11]. The purpose of the present work is the control of spin distribution and anisotropy independent of thermodynamic conditions, unlike PIPTs.…”

Section: Introductionmentioning

confidence: 99%

Direct Control of Spin Distribution and Anisotropy in Cu-Dithiolene Complex Anions by Light

2016

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Electrical and magnetic properties are dominated by the (de)localization and the anisotropy in the distribution of unpaired electrons in solids. In molecular materials, these properties have been indirectly controlled through crystal structures using various chemical modifications to affect molecular structures and arrangements. In the molecular crystals, since the energy band structures can be semi-quantitatively known using band calculations and solid state spectra, one can anticipate the (de)localization of unpaired electrons in particular bands/levels, as well as interactions with other electrons. Thus, direct control of anisotropy and localization of unpaired electrons by locating them in selected energy bands/levels would realize more efficient control of electrical and magnetic properties. In this work, it has been found that the unpaired electrons on Cu(II)-complex anions can be optically controlled to behave as anisotropically-delocalized electrons (under dark) or isotropically-localized electrons like free electrons (under UV), the latter of which has hardly been observed in the ground states of Cu(II)-complexes by any chemical modifications. Although the compounds examined in this work did not switch between conductors and magnets, these findings indicate that optical excitation in the [Cu(dmit) 2 ] 2´s alts should be an effective method to control spin distribution and anisotropy.

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“…Various ways are now established to create short, high-intensity THz pulses. − Low-frequency THz pulses in the regime from 0.1 to 3 THz are generated using optical rectification in nonlinear crystals, such as LiNbO 3 , reaching a field strength of more than 1 MV/cm and pulse duration of a few ps. ,− THz pulses in the range of about 2 to 10 THz can be efficiently generated from table top sources using organic crystals like DSTMS or DAST. , These pulses can reach field strengths of up to 80 MV/cm with a duration of several hundred fs. , Pulses from organic crystals can get as short as 130 fs in full width at half-maximum (FWHM) while maintaining field strengths of about 0.3 MV/cm. , Also pulses beyond 10 THz have been generated with organic crystals at field strengths of up to 0.5 MV/cm . THz fields beyond 10 THz can be efficiently generated with difference-frequency generation in GaSe crystals with field strength surpassing 100 MV/cm. , High-intensity THz pulses reaching up to tens of MV/cm and spanning the frequency range from 0.1 to 30 THz with pulse lengths of tens of fs to several ps can be generated using free-electron laser (FEL) facilities ,, such as FLASH, , LCLS, PAL-FEL, FERMI, , or TELBE . The highest field strength, up to 200 MV/cm, can be achieved by creating coherent transition radiation from relativistic electron bunches passing through Beryllium foils .…”

Section: Introductionmentioning

confidence: 99%

“…55,56 High-intensity THz pulses reaching up to tens of MV/cm and spanning the frequency range from 0.1 to 30 THz with pulse lengths of tens of fs to several ps can be generated using free-electron laser (FEL) facilities 40,57,58 such as FLASH, 59,60 LCLS, 61 PAL-FEL, 62 FERMI, 63,64 or TELBE. 65 The highest field strength, up to 200 MV/cm, can be achieved by creating coherent transition radiation from relativistic electron bunches passing through Beryllium foils. 66 However, these pulses typically have a very broad spectral width of tens of THz.…”

Section: Introductionmentioning

confidence: 99%

Prospects of Using High-Intensity THz Pulses To Induce Ultrafast Temperature-Jumps in Liquid Water

Mishra¹,

Bettaque

Vendrell

et al. 2018

J. Phys. Chem. A

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Ultrashort, high-intensity terahertz (THz) pulses, e.g., generated at free-electron laser facilities, allow for direct investigation as well as the driving of intermolecular modes in liquids like water and thus will deepen our understanding of the hydrogen bonding network. In this work, the temperature-jump (T-jump) of water induced by THz radiation is simulated for ten different THz frequencies in the range from 3 to 30 THz and five different pulse intensities in the range from 1 × 10 to 5 × 10 W/cm employing both ab initio molecular dynamics (AIMD) and force field molecular dynamics (FFMD) approaches. The most efficient T-jump can be achieved with 16 THz pulses. Three distinct T-jump mechanisms can be uncovered. For all cases, the T-jump mechanism proceeds within tens of femtoseconds (fs). For frequencies between 10 and 25 THz, most of the energy is initially transferred to the rotational degrees of freedom. Subsequently, the energy is redistributed to the translational and intramolecular vibrational degrees of freedom within a maximum of 500 fs. For the lowest frequencies considered (7 THz and below), translational and rotational degrees of freedom are heated within tens of fs as the THz pulse also couples to the intermolecular vibrations. Subsequently, the intramolecular vibrational modes are heated within a few hundred fs. At the highest frequencies considered (25 THz and above), vibrational and rotational degrees of freedom are heated within tens of fs, and energy redistribution to the translational degrees of freedom happens within several hundred fs. Both AIMD and FFMD simulations show a similar dependence of the T-jump on the frequency employed. However, the FFMD simulations overestimate the total energy transfer around the main peak and drop off too fast toward frequencies higher and lower than the main peak. These differences can be rationalized by missing elements, such as the polarizability, in the TIP4P/2005f force field employed. The feasibility of performing experiments at the studied frequencies and intensities as well as important issues such as energy efficiency, penetration depth, and focusing are discussed.

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THz Control in Correlated Electron Solids: Sources and Applications

Cited by 6 publications

References 99 publications

Accelerator- and laser-based sources of high-field terahertz pulses

Accelerator- and laser-based sources of high-field terahertz pulses

Direct Control of Spin Distribution and Anisotropy in Cu-Dithiolene Complex Anions by Light

Prospects of Using High-Intensity THz Pulses To Induce Ultrafast Temperature-Jumps in Liquid Water

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