In this thesis, high harmonic radiation is studied which is generated by the relativistic interaction of intense laser pulses with dense plasma surfaces. Laser plasma simulations are performed by the author and by colleagues from the University of Dusseldorf for interpreting the experimental results. At first glance, these simulations predict such a high generation efficiency of harmonics from relativistically oscillating mirrors (ROM) that they have been considered as the next generation attosecond light source for the last 15 years. The objective of this thesis is the spectral characterization of the harmonics' efficiency and the ROM process utilizing calibrated XUV diagnostics. The first step, that has been pursued in the thesis work, is the generation of ROM harmonics at the terawatt laser systems JETI and ARCTURUS operated by the University of Jena and the University of Düsseldorf, respectively. According to the wide-spread belief, the efficient generation of ROM harmonics requires extremely short plasma density gradients which calls for high intensity laser pulses with excellent temporal contrast. For this reason, a plasma mirror system has been installed at both laser systems to improve the pulse contrast by two or three orders of magnitude depending of the target material. In experiments using contrast-enhanced laser pulses, a stable emission of ROM harmonics was observed. However, the highest yield has been measured for the intermediate pulse contrast which results in a plasma scale length L^ROM_P=lambda/5. Surprisingly, the overall efficiency of ROM harmonics decreases for shorter scale lengths < lambda/10 or high contrast, respectively. A strong signal of ROM harmonics could even be measured - indeed unstable - without any contrast improvement. Laser plasma simulations confirm the experimental observation of an optimum plasma scale length L^ROM_P=lambda/5. Two effects have been identified which lead to the reduction of the ROM harmonics' yield for short plasma scale lengths: First, the laser field at the plasma surface is reduced for very short plasma scale lengths. Second, the oscillating electron plasma at the plasma surface is held back by strong electrostatic fields due to the immobile ion background for short plasma density gradients. As a conclusion, the use of an intermediate plasma density gradient for generating ROM harmonics with highest efficiency has to be considered as a paradigm shift in this research field since previous work has called for the highest possible pulse contrast or the shortest plasma scale length, respectively, in order to generate ROM harmonics at all. Using the optimized plasma scale length, a significant modulation and broadening of the ROM harmonic lines has been observed which is unfavorable for most of the potential applications of ROM harmonics. Laser plasma simulations reproduce the fine structure of the harmonic lines. They further reveal an unequally spaced attosecond pulse train and a positive chirp of the harmonics which is associated with the line broadening. This positive chirp is characteristic for ROM harmonics generated at expanded plasma density profiles and is explained by a temporal denting of the plasma surface due to radiation pressure. It is shown by simulations and experiments that the harmonics' linewidth can be minimized when the harmonics' chirp is compensated by chirped driving laser pulses. For optimized preplasma conditions, the efficiency of the ROM harmonics was measured to be 10^-4 at 40nm and 10^-6 at 20nm per harmonic order and falls short of expectations nurtured by 1D PIC-simulations and plasma theory. Having a pulse energy in the order of a µJ per harmonic order, ROM harmonics are indeed suited, e. g., for seeding XUV free-electron lasers or coherent diffraction imaging. However, the efficiency of ROM harmonics of 10^-4 at 40nm is comparable to that of high harmonic generation in gaseous media which is state-of-the-art and technologically much less demanding. Considering the present results of the ROM harmonics' efficiency, the high expectations of a highly-efficient, next-generation attosecond source have not been met yet. The reason for the rather low efficiency of ROM harmonics has been investigated by means of 2D simulations. These simulations reveal surface plasma waves which can be generated in addition to the ROM oscillation and lead to a reduced harmonic emisson in the direction of reflection. Surface plasma waves could thus be responsible for the low efficiency of ROM harmonics measured in the experiments. The simulations suggest that shorter pulses with few-cycle pulse duration should be used in the future for a more efficient generation since surface plasma waves can not be built up at these time scales. A prerequisite for most of the potential applications of ROM harmonics is the generation with a high repetition rate. Using fast-rotating targets and frequency-doubled laser pulses surface harmonics have been generated with the 10-Hz repetition rate of the JETI laser system. Due to the frequency-doubling process the pulse contrast is enhanced by several orders of magnitude such that extremely short plasma density gradients are obtained. Surprisingly, an effect was discovered which was not predicted by theory so far: The high harmonic spectra show a significant enhancement of particular harmonic orders located at twice the maximum plasma frequency 2 omega_P or 2 omega_P +- 2 omega_L. By using targets of different density we were able to tune the enhancement in a certain frequency range in the XUV. Moreover, the efficiency of the amplified harmonics is even higher than the one which is measured for the optimized plasma scale length. Laser plasma simulations confirm then experimental results and reveal the origin of the enhancement: The plasma surface oscillates relativistically with the laser frequency omega_L and the plasma frequency omega_P. The enhanced harmonics are due to a ROM-like oscillation at omega_P. A simple model based on the ROM model can explain the enhanced harmonics as a frequency-mixing process which utilizes the relativistic nonlinearity induced by retardation. This relativistic frequency synthesis at plasma surfaces can be regarded as a new regime of nonlinear optics in the XUV which employs plasma frequencies of dense surface plasmas in the order of several PHz. At the end of the thesis, two selected applications of ROM harmonics are discussed: The generation of intense attosecond pulses by the ROM process would enable XUV-XUV pump-probe experiments providing attosecond time resolution. However, such experiments would require the determination of the attosecond time structure of ROM harmonics first. An apparatus has been constructed which allows the measurement of an attosecond pulse train by using a nonlinear autocorrelation technique. The second potential application of ROM harmonics is a non-invasive cross-sectional imaging technique which has been developed during the thesis work. This method provides a depth resolution of a few nanometers and employs broad-bandwidth XUV or soft x-ray radiation. ROM harmonics with a nearly continuous spectrum could be a suitable radiation source for this application of technical and industrial relevance.